2012 |
Stein, B; Devaux, E; Genet, C; Ebbesen, T W Self-collimation of surface plasmon beams Journal Article In: OPTICS LETTERS, 37 (11), pp. 1916–1918, 2012, ISSN: 0146-9592. @article{stein_self-collimation_2012, title = {Self-collimation of surface plasmon beams}, author = {Stein, B. and Devaux, E. and Genet, C. and Ebbesen, T. W.}, doi = {10.1364/OL.37.001916}, issn = {0146-9592}, year = {2012}, date = {2012-06-01}, journal = {OPTICS LETTERS}, volume = {37}, number = {11}, pages = {1916--1918}, abstract = {We generate self-collimating surface plasmon beams in a doubly periodic plasmonic grating. The self-collimation effect is understood from the local anisotropy of the isofrequency surface of the grating in the vicinity of the bandgap. The properties of the beams are analyzed by leakage radiation microscopy and show to an unprecedented level significantly reduced diffraction as compared with plasmon beams propagating on a flat metal film. (C) 2012 Optical Society of America}, keywords = {}, pubstate = {published}, tppubtype = {article} } We generate self-collimating surface plasmon beams in a doubly periodic plasmonic grating. The self-collimation effect is understood from the local anisotropy of the isofrequency surface of the grating in the vicinity of the bandgap. The properties of the beams are analyzed by leakage radiation microscopy and show to an unprecedented level significantly reduced diffraction as compared with plasmon beams propagating on a flat metal film. (C) 2012 Optical Society of America |
Liscio, Andrea ; Bonini, Massimo ; Treossi, Emanuele ; Orgiu, Emanuele ; Kastler, Marcel ; Doetz, Florian ; Palermo, Vincenzo ; Samori, Paolo Improving charge transport in poly(3-hexylthiophene) transistors via blending with an alkyl-substituted phenylene-thiophene-thiophene-phenylene molecule Journal Article In: JOURNAL OF POLYMER SCIENCE PART B-POLYMER PHYSICS, 50 (9), pp. 642–649, 2012, ISSN: 0887-6266. @article{liscio_improving_2012, title = {Improving charge transport in poly(3-hexylthiophene) transistors via blending with an alkyl-substituted phenylene-thiophene-thiophene-phenylene molecule}, author = {Liscio, Andrea and Bonini, Massimo and Treossi, Emanuele and Orgiu, Emanuele and Kastler, Marcel and Doetz, Florian and Palermo, Vincenzo and Samori, Paolo}, doi = {10.1002/polb.23044}, issn = {0887-6266}, year = {2012}, date = {2012-05-01}, journal = {JOURNAL OF POLYMER SCIENCE PART B-POLYMER PHYSICS}, volume = {50}, number = {9}, pages = {642--649}, abstract = {A prototypical semiconducting bicomponent system consisting of a conjugated polymer, that is, poly(3-hexylthiophene) (P3HT), blended with a small thiophene containing conjugated molecule, that is, an alkyl-substituted bisphenyl-bithiophene [phenylenethiophenethiophenephenylene (PTTP)], has been used as an electroactive active layer in field-effect transistors (FETs). The self-assembly of this bicomponent system at surfaces has been studied at different length scales, from the nanoscale to the macroscale, and compared with the behavior of monocomponent films of PTTP and P3HT. The correlation between morphology and electric properties of the semiconducting material is explored by fabricating prototypes of FETs varying the relative concentrations of the two-component blend. The maximum charge carrier mobility value, achieved with a few percent of PTTP component, is not simply due to a uniform dispersion of the molecules in the polymer matrix, but rather to the generation of very long percolation paths, whose composition and electrical properties can be tuned with the PTTP concentration. (C) 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2012}, keywords = {}, pubstate = {published}, tppubtype = {article} } A prototypical semiconducting bicomponent system consisting of a conjugated polymer, that is, poly(3-hexylthiophene) (P3HT), blended with a small thiophene containing conjugated molecule, that is, an alkyl-substituted bisphenyl-bithiophene [phenylenethiophenethiophenephenylene (PTTP)], has been used as an electroactive active layer in field-effect transistors (FETs). The self-assembly of this bicomponent system at surfaces has been studied at different length scales, from the nanoscale to the macroscale, and compared with the behavior of monocomponent films of PTTP and P3HT. The correlation between morphology and electric properties of the semiconducting material is explored by fabricating prototypes of FETs varying the relative concentrations of the two-component blend. The maximum charge carrier mobility value, achieved with a few percent of PTTP component, is not simply due to a uniform dispersion of the molecules in the polymer matrix, but rather to the generation of very long percolation paths, whose composition and electrical properties can be tuned with the PTTP concentration. (C) 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2012 |
Dankers, Patricia Y W; Hermans, Thomas M; Baughman, Travis W; Kamikawa, Yuko ; Kieltyka, Roxanne E; Bastings, Maartje M C; Janssen, Henk M; Sommerdijk, Nico A J M; Larsen, Antje ; van Luyn, Marja J A; Bosman, Anton W; Popa, Eliane R; Fytas, George ; Meijer, E W Hierarchical Formation of Supramolecular Transient Networks in Water: A Modular Injectable Delivery System Journal Article In: ADVANCED MATERIALS, 24 (20), pp. 2703–2709, 2012, ISSN: 0935-9648. @article{dankers_hierarchical_2012, title = {Hierarchical Formation of Supramolecular Transient Networks in Water: A Modular Injectable Delivery System}, author = {Dankers, Patricia Y. W. and Hermans, Thomas M. and Baughman, Travis W. and Kamikawa, Yuko and Kieltyka, Roxanne E. and Bastings, Maartje M. C. and Janssen, Henk M. and Sommerdijk, Nico A. J. M. and Larsen, Antje and van Luyn, Marja J. A. and Bosman, Anton W. and Popa, Eliane R. and Fytas, George and Meijer, E. W.}, doi = {10.1002/adma.201104072}, issn = {0935-9648}, year = {2012}, date = {2012-05-01}, journal = {ADVANCED MATERIALS}, volume = {24}, number = {20}, pages = {2703--2709}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Zhao, B; Glaetzle, A W; Pupillo, G; Zoller, P Atomic Rydberg Reservoirs for Polar Molecules Journal Article In: PHYSICAL REVIEW LETTERS, 108 (19), 2012, ISSN: 0031-9007. @article{zhao_atomic_2012, title = {Atomic Rydberg Reservoirs for Polar Molecules}, author = {Zhao, B. and Glaetzle, A. W. and Pupillo, G. and Zoller, P.}, doi = {10.1103/PhysRevLett.108.193007}, issn = {0031-9007}, year = {2012}, date = {2012-05-01}, journal = {PHYSICAL REVIEW LETTERS}, volume = {108}, number = {19}, abstract = {We discuss laser-dressed dipolar and van der Waals interactions between atoms and polar molecules, so that a cold atomic gas with laser admixed Rydberg levels acts as a designed reservoir for both elastic and inelastic collisional processes. The elastic scattering channel is characterized by large elastic scattering cross sections and repulsive shields to protect from close encounter collisions. In addition, we discuss a dissipative (inelastic) collision where a spontaneously emitted photon carries away (kinetic) energy of the collision partners, thus providing a significant energy loss in a single collision. This leads to the scenario of rapid thermalization and cooling of a molecule in the mK down to the mu K regime by cold atoms.}, keywords = {}, pubstate = {published}, tppubtype = {article} } We discuss laser-dressed dipolar and van der Waals interactions between atoms and polar molecules, so that a cold atomic gas with laser admixed Rydberg levels acts as a designed reservoir for both elastic and inelastic collisional processes. The elastic scattering channel is characterized by large elastic scattering cross sections and repulsive shields to protect from close encounter collisions. In addition, we discuss a dissipative (inelastic) collision where a spontaneously emitted photon carries away (kinetic) energy of the collision partners, thus providing a significant energy loss in a single collision. This leads to the scenario of rapid thermalization and cooling of a molecule in the mK down to the mu K regime by cold atoms. |
Buchs, Barbara ; Fieber, Wolfgang ; Drahonovsky, Dusan ; Lehn, Jean-Marie ; Herrmann, Andreas Stabilized Hemiacetal Complexes as Precursors for the Controlled Release of Bioactive Volatile Alcohols Journal Article In: CHEMISTRY & BIODIVERSITY, 9 (4), pp. 689–701, 2012, ISSN: 1612-1872. @article{buchs_stabilized_2012, title = {Stabilized Hemiacetal Complexes as Precursors for the Controlled Release of Bioactive Volatile Alcohols}, author = {Buchs, Barbara and Fieber, Wolfgang and Drahonovsky, Dusan and Lehn, Jean-Marie and Herrmann, Andreas}, doi = {10.1002/cbdv.201100383}, issn = {1612-1872}, year = {2012}, date = {2012-04-01}, journal = {CHEMISTRY & BIODIVERSITY}, volume = {9}, number = {4}, pages = {689--701}, abstract = {Hemiacetals of pyridine-2-carbaldehyde derivatives and volatile alcohols can be stabilized in organic solution in the presence of protons or different metal cations. Despite the inherent instability of hemiacetals in H2O, stabilizing them with zinc(II) triflate and adding them to a cationic surfactant formulation resulted in the slow release of the alcohol from cotton surfaces being treated with the hemiacetal complex. Stabilized hemiacetals might thus be suitable delivery systems of bioactive volatiles by rapid hydrolysis in H2O-based media.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Hemiacetals of pyridine-2-carbaldehyde derivatives and volatile alcohols can be stabilized in organic solution in the presence of protons or different metal cations. Despite the inherent instability of hemiacetals in H2O, stabilizing them with zinc(II) triflate and adding them to a cationic surfactant formulation resulted in the slow release of the alcohol from cotton surfaces being treated with the hemiacetal complex. Stabilized hemiacetals might thus be suitable delivery systems of bioactive volatiles by rapid hydrolysis in H2O-based media. |
Ayme, Jean-Francois ; Lux, Jacques ; Sauvage, Jean-Pierre ; Sour, Angelique [2]Catenanes Built Around Octahedral Transition-Metal Complexes that Contain Two Intertwined Endocyclic but Non-sterically Hindering Tridentate Ligands Journal Article In: CHEMISTRY-A EUROPEAN JOURNAL, 18 (18), pp. 5565–5573, 2012, ISSN: 0947-6539. @article{ayme_[2]catenanes_2012, title = {[2]Catenanes Built Around Octahedral Transition-Metal Complexes that Contain Two Intertwined Endocyclic but Non-sterically Hindering Tridentate Ligands}, author = {Ayme, Jean-Francois and Lux, Jacques and Sauvage, Jean-Pierre and Sour, Angelique}, doi = {10.1002/chem.201104061}, issn = {0947-6539}, year = {2012}, date = {2012-04-01}, journal = {CHEMISTRY-A EUROPEAN JOURNAL}, volume = {18}, number = {18}, pages = {5565--5573}, abstract = {Sterically hindering bidentate chelates, such as 2,9-diphenyl-1,10-phenanthroline, form entwined complexes with copper(I) and other tetrahedrally coordinated transition-metal centres. To prepare octahedral complexes containing two entwined tridentate ligands and thus apply a strategy similar to that used for making catenanes with tetrahedral metal centres, the use of the classical terpy ligand (terpy=2,2':6',2”-terpyridine) appears to be attractive. In fact, 6,6”-diphenyl-2,2':6',2”-terpyridine (dp-terpy) is not appropriate due to strong pinching of the organic backbone by coordination to the metal and thus stable entwined complexes with this ligand cannot be obtained. Herein, we report the synthesis and coordination properties of a new family of tridentate ligands, the main features of which are their endocyclic nature and non-sterically hindering character. The coordinating fragment consists of two 8'-phenylisoquinolin-3'-yl groups attached at the 2 and 6 positions of a pyridine nucleus. Octahedral complexes containing two such entangled ligands around an octahedral metal centre, such as FeII, RuII or CoIII, are highly stable, with no steric congestion around the metal. By using functionalised ligands bearing terminal olefins, double ring-closing metathesis leads to [2]catenanes in good yield with FeII or CoIII as the templating metal centre. The X-ray crystallography structures of the FeII precursor and the FeII catenane are also reported. These show that although significant pinching of the ligand is observed in both FeII complexes, the system is very open and no steric constraints can be detected.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Sterically hindering bidentate chelates, such as 2,9-diphenyl-1,10-phenanthroline, form entwined complexes with copper(I) and other tetrahedrally coordinated transition-metal centres. To prepare octahedral complexes containing two entwined tridentate ligands and thus apply a strategy similar to that used for making catenanes with tetrahedral metal centres, the use of the classical terpy ligand (terpy=2,2':6',2”-terpyridine) appears to be attractive. In fact, 6,6”-diphenyl-2,2':6',2”-terpyridine (dp-terpy) is not appropriate due to strong pinching of the organic backbone by coordination to the metal and thus stable entwined complexes with this ligand cannot be obtained. Herein, we report the synthesis and coordination properties of a new family of tridentate ligands, the main features of which are their endocyclic nature and non-sterically hindering character. The coordinating fragment consists of two 8'-phenylisoquinolin-3'-yl groups attached at the 2 and 6 positions of a pyridine nucleus. Octahedral complexes containing two such entangled ligands around an octahedral metal centre, such as FeII, RuII or CoIII, are highly stable, with no steric congestion around the metal. By using functionalised ligands bearing terminal olefins, double ring-closing metathesis leads to [2]catenanes in good yield with FeII or CoIII as the templating metal centre. The X-ray crystallography structures of the FeII precursor and the FeII catenane are also reported. These show that although significant pinching of the ligand is observed in both FeII complexes, the system is very open and no steric constraints can be detected. |
Karplus, Martin Biomolecular motors: Insights from simulations Journal Article In: ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 243 , 2012, ISSN: 0065-7727. @article{karplus_biomolecular_2012, title = {Biomolecular motors: Insights from simulations}, author = {Karplus, Martin}, issn = {0065-7727}, year = {2012}, date = {2012-03-01}, journal = {ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY}, volume = {243}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Hirsch, Anna K H; Buhler, Eric ; Lehn, Jean-Marie Biodynamers: Self-Organization-Driven Formation of Doubly Dynamic Proteoids Journal Article In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 134 (9), pp. 4177–4183, 2012, ISSN: 0002-7863. @article{hirsch_biodynamers:_2012, title = {Biodynamers: Self-Organization-Driven Formation of Doubly Dynamic Proteoids}, author = {Hirsch, Anna K. H. and Buhler, Eric and Lehn, Jean-Marie}, doi = {10.1021/ja2099134}, issn = {0002-7863}, year = {2012}, date = {2012-03-01}, journal = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY}, volume = {134}, number = {9}, pages = {4177--4183}, abstract = {Polypeptide-type dynamic biopolymers (bio-dynamers) have been generated by polycondensation via acylhydrazone and imine formation of amino-acid-derived components that polymerize driven by self-organization. They have been characterized as globular particles, reminiscent of folded proteins, by cryo-TEM, LS, DOSY NMR, and SANS studies. The reversible polymers obtained show remarkably low dispersity and feature double covalent dynamics allowing for fine-tuning of both exchange and incorporation processes through pH control. In the course of build-up, they perform a selection of the most suitable building block, as indicated by the preferential incorporation of the more hydrophobic amino-acid component with increased rate and higher molecular weight of the polymer formed. The system described displays nucleation-elongation behavior driven by hydrophobic effects and represents a model for the operation of adaptation processes in the evolution of complex matter.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Polypeptide-type dynamic biopolymers (bio-dynamers) have been generated by polycondensation via acylhydrazone and imine formation of amino-acid-derived components that polymerize driven by self-organization. They have been characterized as globular particles, reminiscent of folded proteins, by cryo-TEM, LS, DOSY NMR, and SANS studies. The reversible polymers obtained show remarkably low dispersity and feature double covalent dynamics allowing for fine-tuning of both exchange and incorporation processes through pH control. In the course of build-up, they perform a selection of the most suitable building block, as indicated by the preferential incorporation of the more hydrophobic amino-acid component with increased rate and higher molecular weight of the polymer formed. The system described displays nucleation-elongation behavior driven by hydrophobic effects and represents a model for the operation of adaptation processes in the evolution of complex matter. |
Bronner, Catherine ; Veiga, Manoel ; Guenet, Aurelie ; De Cola, Luisa ; Hosseini, Mir Wais ; Strassert, Cristian A; Baudron, Stephane A Excited State Properties and Energy Transfer within Dipyrrin-Based Binuclear Iridium/Platinum Dyads: The Effect of ortho-Methylation on the Spacer Journal Article In: CHEMISTRY-A EUROPEAN JOURNAL, 18 (13), pp. 4041–4050, 2012, ISSN: 0947-6539. @article{bronner_excited_2012, title = {Excited State Properties and Energy Transfer within Dipyrrin-Based Binuclear Iridium/Platinum Dyads: The Effect of ortho-Methylation on the Spacer}, author = {Bronner, Catherine and Veiga, Manoel and Guenet, Aurelie and De Cola, Luisa and Hosseini, Mir Wais and Strassert, Cristian A. and Baudron, Stephane A.}, doi = {10.1002/chem.201103836}, issn = {0947-6539}, year = {2012}, date = {2012-03-01}, journal = {CHEMISTRY-A EUROPEAN JOURNAL}, volume = {18}, number = {13}, pages = {4041--4050}, abstract = {Luminescent cyclometalated iridium complexes based on pyridyl appended dipyrrin ligands were prepared and characterized both in the solid state and in solution. The functionalization of the peripheral pyridyl moiety causes dramatic changes on the emission properties of both mono- and hetero- binuclear complexes. A detailed photophysical investigation of the two mononuclear derivatives of the [(Ppy)2Ir(dpm-py)] family (Ppy=2-phenylpyridine}, keywords = {}, pubstate = {published}, tppubtype = {article} } Luminescent cyclometalated iridium complexes based on pyridyl appended dipyrrin ligands were prepared and characterized both in the solid state and in solution. The functionalization of the peripheral pyridyl moiety causes dramatic changes on the emission properties of both mono- and hetero- binuclear complexes. A detailed photophysical investigation of the two mononuclear derivatives of the [(Ppy)2Ir(dpm-py)] family (Ppy=2-phenylpyridine |
Theberge, Ashleigh B; Mayot, Estelle ; Harrak, Abdeslam El ; Kleinschmidt, Felix ; Huck, Wilhelm T S; Griffiths, Andrew D Microfluidic platform for combinatorial synthesis in picolitre droplets Journal Article In: Lab on a Chip, 12 (7), pp. 1320–1326, 2012, ISSN: 1473-0189. @article{theberge_microfluidic_2012, title = {Microfluidic platform for combinatorial synthesis in picolitre droplets}, author = {Theberge, Ashleigh B. and Mayot, Estelle and Harrak, Abdeslam El and Kleinschmidt, Felix and Huck, Wilhelm T. S. and Griffiths, Andrew D.}, url = {http://pubs.rsc.org/en/content/articlelanding/2012/lc/c2lc21019c}, doi = {10.1039/C2LC21019C}, issn = {1473-0189}, year = {2012}, date = {2012-03-01}, urldate = {2016-05-30}, journal = {Lab on a Chip}, volume = {12}, number = {7}, pages = {1320--1326}, abstract = {This paper presents a droplet-based microfluidic platform for miniaturized combinatorial synthesis. As a proof of concept, a library of small molecules for early stage drug screening was produced. We present an efficient strategy for producing a 7 × 3 library of potential thrombin inhibitors that can be utilized for other combinatorial synthesis applications. Picolitre droplets containing the first type of reagent (reagents A1, A2, …, Am) were formed individually in identical microfluidic chips and then stored off chip with the aid of stabilizing surfactants. These droplets were then mixed to form a library of droplets containing reagents A1–m, each individually compartmentalized, which was reinjected into a second microfluidic chip and combinatorially fused with picolitre droplets containing the second reagent (reagents B1, B2, …, Bn) that were formed on chip. The concept was demonstrated with a three-component Ugi-type reaction involving an amine (reagents A1–3), an aldehyde (reagents B1–7), and an isocyanide (held constant), to synthesize a library of small molecules with potential thrombin inhibitory activity. Our technique produced 106 droplets of each reaction at a rate of 2.3 kHz. Each droplet had a reaction volume of 3.1 pL, at least six orders of magnitude lower than conventional techniques. The droplets can then be divided into aliquots for different downstream screening applications. In addition to medicinal chemistry applications, this combinatorial droplet-based approach holds great potential for other applications that involve sampling large areas of chemical parameter space with minimal reagent consumption; such an approach could be beneficial when optimizing reaction conditions or performing combinatorial reactions aimed at producing novel materials.}, keywords = {}, pubstate = {published}, tppubtype = {article} } This paper presents a droplet-based microfluidic platform for miniaturized combinatorial synthesis. As a proof of concept, a library of small molecules for early stage drug screening was produced. We present an efficient strategy for producing a 7 × 3 library of potential thrombin inhibitors that can be utilized for other combinatorial synthesis applications. Picolitre droplets containing the first type of reagent (reagents A1, A2, …, Am) were formed individually in identical microfluidic chips and then stored off chip with the aid of stabilizing surfactants. These droplets were then mixed to form a library of droplets containing reagents A1–m, each individually compartmentalized, which was reinjected into a second microfluidic chip and combinatorially fused with picolitre droplets containing the second reagent (reagents B1, B2, …, Bn) that were formed on chip. The concept was demonstrated with a three-component Ugi-type reaction involving an amine (reagents A1–3), an aldehyde (reagents B1–7), and an isocyanide (held constant), to synthesize a library of small molecules with potential thrombin inhibitory activity. Our technique produced 106 droplets of each reaction at a rate of 2.3 kHz. Each droplet had a reaction volume of 3.1 pL, at least six orders of magnitude lower than conventional techniques. The droplets can then be divided into aliquots for different downstream screening applications. In addition to medicinal chemistry applications, this combinatorial droplet-based approach holds great potential for other applications that involve sampling large areas of chemical parameter space with minimal reagent consumption; such an approach could be beneficial when optimizing reaction conditions or performing combinatorial reactions aimed at producing novel materials. |
Fallah-Araghi, Ali ; Baret, Jean-Christophe ; Ryckelynck, Michael ; Griffiths, Andrew D A completely in vitro ultrahigh-throughput droplet-based microfluidic screening system for protein engineering and directed evolution Journal Article In: Lab on a Chip, 12 (5), pp. 882–891, 2012, ISSN: 1473-0189. @article{fallah-araghi_completely_2012, title = {A completely in vitro ultrahigh-throughput droplet-based microfluidic screening system for protein engineering and directed evolution}, author = {Fallah-Araghi, Ali and Baret, Jean-Christophe and Ryckelynck, Michael and Griffiths, Andrew D.}, doi = {10.1039/c2lc21035e}, issn = {1473-0189}, year = {2012}, date = {2012-03-01}, journal = {Lab on a Chip}, volume = {12}, number = {5}, pages = {882--891}, abstract = {In vitro screening systems based on the coupled transcription and translation of genes using cell-free systems have a number of attractive features for protein engineering and directed evolution. We present a completely in vitro ultrahigh-throughput screening platform using droplet-based microfluidics. Single genes are compartmentalized in aqueous droplets, dispersed in inert carrier oil, and amplified using the polymerase chain reaction (PCR). After amplification, the droplets, now containing 30,000 copies of each gene, are fused one-to-one with droplets containing a cell-free coupled transcription-translation (IVTT) system and the reagents for a fluorogenic assay. Fluorescence-activated electrocoalescence with an aqueous stream is then used to selectively recover genes from droplets containing the desired activity. We demonstrate, by selecting mixtures of lacZ genes encoding the enzyme β-galactosidase and lacZmut genes encoding an inactive variant, that this system can sort at 2000 droplets s(-1): lacZ genes were enriched 502-fold from a 1 : 100 molar ratio of lacZ : lacZmut genes. Indeed, the false positive and false negative error rates were both textbackslashtextbackslashtextbackslashtextless0.004 and the results indicate that enrichment is not limited by the sorting efficiency, but by the co-encapsulation of multiple genes in droplets, which is described by the Poisson distribution. Compared to screening using microtiter plate-based systems, the volume and cost of PCR and IVTT reagents are reduced by almost 10(5)-fold, allowing the screening of 10(6) genes using only 150 μL of reagents.}, keywords = {}, pubstate = {published}, tppubtype = {article} } In vitro screening systems based on the coupled transcription and translation of genes using cell-free systems have a number of attractive features for protein engineering and directed evolution. We present a completely in vitro ultrahigh-throughput screening platform using droplet-based microfluidics. Single genes are compartmentalized in aqueous droplets, dispersed in inert carrier oil, and amplified using the polymerase chain reaction (PCR). After amplification, the droplets, now containing 30,000 copies of each gene, are fused one-to-one with droplets containing a cell-free coupled transcription-translation (IVTT) system and the reagents for a fluorogenic assay. Fluorescence-activated electrocoalescence with an aqueous stream is then used to selectively recover genes from droplets containing the desired activity. We demonstrate, by selecting mixtures of lacZ genes encoding the enzyme β-galactosidase and lacZmut genes encoding an inactive variant, that this system can sort at 2000 droplets s(-1): lacZ genes were enriched 502-fold from a 1 : 100 molar ratio of lacZ : lacZmut genes. Indeed, the false positive and false negative error rates were both textbackslashtextbackslashtextbackslashtextless0.004 and the results indicate that enrichment is not limited by the sorting efficiency, but by the co-encapsulation of multiple genes in droplets, which is described by the Poisson distribution. Compared to screening using microtiter plate-based systems, the volume and cost of PCR and IVTT reagents are reduced by almost 10(5)-fold, allowing the screening of 10(6) genes using only 150 μL of reagents. |
Stein, Benedikt ; Laluet, Jean-Yves ; Devaux, Eloise ; Genet, Cyriaque ; Ebbesen, Thomas W Fano Resonances and Leakage Radiation for High-Resolution Plasmonic Sensing Journal Article In: JOURNAL OF PHYSICAL CHEMISTRY C, 116 (10), pp. 6092–6096, 2012, ISSN: 1932-7447. @article{stein_fano_2012, title = {Fano Resonances and Leakage Radiation for High-Resolution Plasmonic Sensing}, author = {Stein, Benedikt and Laluet, Jean-Yves and Devaux, Eloise and Genet, Cyriaque and Ebbesen, Thomas W.}, doi = {10.1021/jp2120675}, issn = {1932-7447}, year = {2012}, date = {2012-03-01}, journal = {JOURNAL OF PHYSICAL CHEMISTRY C}, volume = {116}, number = {10}, pages = {6092--6096}, abstract = {We demonstrate that the asymmetric profiles of Fano resonances lead to important figure of merit (FOM) improvements of surface plasmon (SP)-based refractive index sensors. Exploiting the high angular resolution of a leakage radiation microscope, our sensor shows a 75% improvement over the optimal FOM of classic SP-based sensors, reaching a FOM as high as 234 +/- 1 RIU-1. We also perform a full noise assessment of the system and achieve a final resolution of O(10(-7)) RIU.}, keywords = {}, pubstate = {published}, tppubtype = {article} } We demonstrate that the asymmetric profiles of Fano resonances lead to important figure of merit (FOM) improvements of surface plasmon (SP)-based refractive index sensors. Exploiting the high angular resolution of a leakage radiation microscope, our sensor shows a 75% improvement over the optimal FOM of classic SP-based sensors, reaching a FOM as high as 234 +/- 1 RIU-1. We also perform a full noise assessment of the system and achieve a final resolution of O(10(-7)) RIU. |
Zenin, Vladimir A; Volkov, Valentyn S; Han, Zhanghua ; Bozhevolnyi, Sergey I; Devaux, Eloise ; Ebbesen, Thomas W Directional coupling in channel plasmon-polariton waveguides Journal Article In: OPTICS EXPRESS, 20 (6), pp. 6124–6134, 2012, ISSN: 1094-4087. @article{zenin_directional_2012, title = {Directional coupling in channel plasmon-polariton waveguides}, author = {Zenin, Vladimir A. and Volkov, Valentyn S. and Han, Zhanghua and Bozhevolnyi, Sergey I. and Devaux, Eloise and Ebbesen, Thomas W.}, doi = {10.1364/OE.20.006124}, issn = {1094-4087}, year = {2012}, date = {2012-03-01}, journal = {OPTICS EXPRESS}, volume = {20}, number = {6}, pages = {6124--6134}, abstract = {We investigate directional couplers (DCs) formed by channel plasmon-polariton (CPP) waveguides (CPPWs). DCs comprising 5-mu m-offset S-bends and 40-mu m-long parallel CPPWs with different separations (0.08, 0.25, 0.5 and 2 mu m) between V-groove channels are fabricated by using a focused ion-beam (FIB) technique in a 2-mu m-thick gold film and characterized at telecom wavelengths (1425-1630 nm) with near-field optical microscopy. Experimental results reveal strong coupling, resulting in approximately equal power splitting between DC-CPPWs, for small CPPW separations (0.08 and 0.25 mu m). The coupling gradually deteriorates with the increase of separation between V-grooves and practically vanishes for the separation of 2 mu m. The DC-CPPW characteristics observed are found in good agreement with finite-element method (implemented in COMSOL) simulations. (C) 2012 Optical Society of America}, keywords = {}, pubstate = {published}, tppubtype = {article} } We investigate directional couplers (DCs) formed by channel plasmon-polariton (CPP) waveguides (CPPWs). DCs comprising 5-mu m-offset S-bends and 40-mu m-long parallel CPPWs with different separations (0.08, 0.25, 0.5 and 2 mu m) between V-groove channels are fabricated by using a focused ion-beam (FIB) technique in a 2-mu m-thick gold film and characterized at telecom wavelengths (1425-1630 nm) with near-field optical microscopy. Experimental results reveal strong coupling, resulting in approximately equal power splitting between DC-CPPWs, for small CPPW separations (0.08 and 0.25 mu m). The coupling gradually deteriorates with the increase of separation between V-grooves and practically vanishes for the separation of 2 mu m. The DC-CPPW characteristics observed are found in good agreement with finite-element method (implemented in COMSOL) simulations. (C) 2012 Optical Society of America |
El Gemayel, Mirella ; Treier, Matthias ; Musumeci, Chiara ; Li, Chen ; Muellen, Klaus ; Samori, Paolo Tuning the Photoresponse in Organic Field-Effect Transistors Journal Article In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 134 (4), pp. 2429–2433, 2012, ISSN: 0002-7863. @article{el_gemayel_tuning_2012, title = {Tuning the Photoresponse in Organic Field-Effect Transistors}, author = {El Gemayel, Mirella and Treier, Matthias and Musumeci, Chiara and Li, Chen and Muellen, Klaus and Samori, Paolo}, doi = {10.1021/ja211515b}, issn = {0002-7863}, year = {2012}, date = {2012-02-01}, journal = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY}, volume = {134}, number = {4}, pages = {2429--2433}, abstract = {We report on the fabrication of solution-processed organic phototransistors (OPTs) based on perylenebis(dicarboximide)s (PDIs). We found that the responsivity to the photoillumination depends on the transistor's channel length and that it can be tuned by varying the device geometry. The analysis of different morphologies of the active semiconducting layer revealed. that single PDI fibers exhibit the higher photoresponse when compared to more poorly organized films. The highest responsivity value of 4.08 +/- 1.65 x 10(5) A/W was achieved on a multifiber-based OPT. These findings represent a step forward toward the use of organic based phototransistors as photosensors.}, keywords = {}, pubstate = {published}, tppubtype = {article} } We report on the fabrication of solution-processed organic phototransistors (OPTs) based on perylenebis(dicarboximide)s (PDIs). We found that the responsivity to the photoillumination depends on the transistor's channel length and that it can be tuned by varying the device geometry. The analysis of different morphologies of the active semiconducting layer revealed. that single PDI fibers exhibit the higher photoresponse when compared to more poorly organized films. The highest responsivity value of 4.08 +/- 1.65 x 10(5) A/W was achieved on a multifiber-based OPT. These findings represent a step forward toward the use of organic based phototransistors as photosensors. |
Meme, Aurelie ; Stefankiewicz, Artur R; Harrowfield, Jack ; Cao, Xiao-Yu ; Huuskonen, Juhani ; Rissanen, Kari ; Lehn, Jean-Marie ; Nierengarten, Helene ; Leize, Emmanuelle A Novel MALDI-MS Approach for the Analysis of Neutral Metallosupramolecular Architectures Journal Article In: EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, (4), pp. 647–654, 2012, ISSN: 1434-1948. @article{meme_novel_2012, title = {A Novel MALDI-MS Approach for the Analysis of Neutral Metallosupramolecular Architectures}, author = {Meme, Aurelie and Stefankiewicz, Artur R. and Harrowfield, Jack and Cao, Xiao-Yu and Huuskonen, Juhani and Rissanen, Kari and Lehn, Jean-Marie and Nierengarten, Helene and Leize, Emmanuelle}, doi = {10.1002/ejic.201101008}, issn = {1434-1948}, year = {2012}, date = {2012-02-01}, journal = {EUROPEAN JOURNAL OF INORGANIC CHEMISTRY}, number = {4}, pages = {647--654}, abstract = {Matrix assisted laser desorption/ionisation mass spectrometry (MALDI-MS) methods have been developed for the characterisation of neutral [2 x 2] metallogrids derived from diimine, dihydrazone and diacylhydrazone ligands. Such grids may be protonated in solution to give cationic species but in most cases these are labile, so that rather delicate conditions are required for observation of the intact metallogrids as monoprotonated derivatives in the gas phase. As a MALDI matrix, 2,4,6-trihydroxyacetophenone (THAP) is sufficiently acidic to enable monoprotonation of the grids unaccompanied by dissociation, and if the grid sample is initially deposited by a layering technique to avoid any preliminary dissociation in solution the mass spectrum of the intact mono-protonated grid is readily obtainable. The stoichiometry of 24 grids obtained from several different ligands and metals was confirmed with this optimized protocol. The deposition technique used means that the best signal-to-noise ratio in the spectra is obtained with only a small number of laser shots (ca. 5) to volatilise the sample. This MALDI-MS protocol can be applied to the study of grid dissociation in solution and in the case of Cu-II grids, in particular, has revealed the formation of various unusual clusters. The crystal structure is reported of one such cluster that was isolated and contains a nonionisable ligand that is related to that incorporated within the grids analysed by the MALDI-MS protocol.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Matrix assisted laser desorption/ionisation mass spectrometry (MALDI-MS) methods have been developed for the characterisation of neutral [2 x 2] metallogrids derived from diimine, dihydrazone and diacylhydrazone ligands. Such grids may be protonated in solution to give cationic species but in most cases these are labile, so that rather delicate conditions are required for observation of the intact metallogrids as monoprotonated derivatives in the gas phase. As a MALDI matrix, 2,4,6-trihydroxyacetophenone (THAP) is sufficiently acidic to enable monoprotonation of the grids unaccompanied by dissociation, and if the grid sample is initially deposited by a layering technique to avoid any preliminary dissociation in solution the mass spectrum of the intact mono-protonated grid is readily obtainable. The stoichiometry of 24 grids obtained from several different ligands and metals was confirmed with this optimized protocol. The deposition technique used means that the best signal-to-noise ratio in the spectra is obtained with only a small number of laser shots (ca. 5) to volatilise the sample. This MALDI-MS protocol can be applied to the study of grid dissociation in solution and in the case of Cu-II grids, in particular, has revealed the formation of various unusual clusters. The crystal structure is reported of one such cluster that was isolated and contains a nonionisable ligand that is related to that incorporated within the grids analysed by the MALDI-MS protocol. |
Przybilla, Frederic ; Genet, Cyriaque ; Ebbesen, Thomas W Long vs. short-range orders in random subwavelength hole arrays Journal Article In: OPTICS EXPRESS, 20 (4), pp. 4697–4709, 2012, ISSN: 1094-4087. @article{przybilla_long_2012, title = {Long vs. short-range orders in random subwavelength hole arrays}, author = {Przybilla, Frederic and Genet, Cyriaque and Ebbesen, Thomas W.}, doi = {10.1364/OE.20.004697}, issn = {1094-4087}, year = {2012}, date = {2012-02-01}, journal = {OPTICS EXPRESS}, volume = {20}, number = {4}, pages = {4697--4709}, abstract = {We analyze the progressive introduction of disorder in periodic subwavelength hole arrays. Two models of disorder are discussed from their associated Fourier transforms and correlation functions. The optical transmission properties of the corresponding arrays are closely related with the evolutions of structure factors, as experimentally detailed. Remarkably, the optical properties of random arrays are not in general equal to those of the single hole as a result of short-range correlations corresponding to hole-to-hole interactions. These correlations are due to packing constraints that are controlled through the careful generation of random patterns. For high density pattern, short-range order can take over long-range order associated with the periodic array. (C) 2012 Optical Society of America}, keywords = {}, pubstate = {published}, tppubtype = {article} } We analyze the progressive introduction of disorder in periodic subwavelength hole arrays. Two models of disorder are discussed from their associated Fourier transforms and correlation functions. The optical transmission properties of the corresponding arrays are closely related with the evolutions of structure factors, as experimentally detailed. Remarkably, the optical properties of random arrays are not in general equal to those of the single hole as a result of short-range correlations corresponding to hole-to-hole interactions. These correlations are due to packing constraints that are controlled through the careful generation of random patterns. For high density pattern, short-range order can take over long-range order associated with the periodic array. (C) 2012 Optical Society of America |
Sauvage, Jean-Pierre ; Amabilino, David B The Beauty of Knots at the Molecular Level Incollection In: {Fabbrizzi, L} (Ed.): BEAUTY IN CHEMISTRY: ARTISTRY IN THE CREATION OF NEW MOLECULES, 323 , pp. 107–125, 2012, ISBN: 978-3-642-28341-3. @incollection{sauvage_beauty_2012, title = {The Beauty of Knots at the Molecular Level}, author = {Sauvage, Jean-Pierre and Amabilino, David B.}, editor = {{Fabbrizzi, L}}, doi = {10.1007/128_2011_292}, isbn = {978-3-642-28341-3}, year = {2012}, date = {2012-01-01}, booktitle = {BEAUTY IN CHEMISTRY: ARTISTRY IN THE CREATION OF NEW MOLECULES}, volume = {323}, pages = {107--125}, series = {Topics in Current Chemistry}, abstract = {What makes a given object look beautiful to the observer, be it in the macroscopic world or at the molecular level? This very general question will be briefly addressed at the beginning of this essay, in relation to contemporary molecular chemistry and biology, leading to the general statement that, most of the time, beauty is tightly connected to function as well as to the cultural background of the observer. The main topic of the present article will be that of topologically non-trivial molecules or molecular ensembles and the fascination that such species have exerted on molecular or solid state chemists. Molecules with a graph identical to Kuratowski's K-5 or K-3,K-3 graphs are indeed highly attractive from an aesthetical viewpoint, but perhaps even more fascinating and beautiful are molecular knots. A general discussion will be devoted to these compounds, which are still considered as exotic species because of the very limited number of efficient synthetic strategies leading to their preparation. Particularly efficient are templated approaches based either on transition metals such as copper(I) or on organic groups able to form hydrogen bonds or acceptor-donor stacks. A particularly noteworthy property of knots, and in particular of the trefoil knot, is their topological chirality. The isolation of both enantiomers of the trefoil knot (3(1)) could be achieved and showed that such species have fascinating chiroptical properties. Finally, various routes to more complex and beautiful knots than the trefoil knot, which is the simplest non-trivial knot, will be discussed in line with the remarkable ability of transition metals to gather and orient in a very precise fashion several organic components in their coordination spheres, thus leading to synthetic precursors displaying geometries which are perfectly well adapted to the preparation of the desired knots or links.}, keywords = {}, pubstate = {published}, tppubtype = {incollection} } What makes a given object look beautiful to the observer, be it in the macroscopic world or at the molecular level? This very general question will be briefly addressed at the beginning of this essay, in relation to contemporary molecular chemistry and biology, leading to the general statement that, most of the time, beauty is tightly connected to function as well as to the cultural background of the observer. The main topic of the present article will be that of topologically non-trivial molecules or molecular ensembles and the fascination that such species have exerted on molecular or solid state chemists. Molecules with a graph identical to Kuratowski's K-5 or K-3,K-3 graphs are indeed highly attractive from an aesthetical viewpoint, but perhaps even more fascinating and beautiful are molecular knots. A general discussion will be devoted to these compounds, which are still considered as exotic species because of the very limited number of efficient synthetic strategies leading to their preparation. Particularly efficient are templated approaches based either on transition metals such as copper(I) or on organic groups able to form hydrogen bonds or acceptor-donor stacks. A particularly noteworthy property of knots, and in particular of the trefoil knot, is their topological chirality. The isolation of both enantiomers of the trefoil knot (3(1)) could be achieved and showed that such species have fascinating chiroptical properties. Finally, various routes to more complex and beautiful knots than the trefoil knot, which is the simplest non-trivial knot, will be discussed in line with the remarkable ability of transition metals to gather and orient in a very precise fashion several organic components in their coordination spheres, thus leading to synthetic precursors displaying geometries which are perfectly well adapted to the preparation of the desired knots or links. |
Fabre, Bruno ; Samori, Cristian ; Bianco, Alberto Immobilization of double functionalized carbon nanotubes on glassy carbon electrodes for the electrochemical sensing of the biotin-avidin affinity Journal Article In: JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 665 , pp. 90–94, 2012, ISSN: 1572-6657. @article{fabre_immobilization_2012, title = {Immobilization of double functionalized carbon nanotubes on glassy carbon electrodes for the electrochemical sensing of the biotin-avidin affinity}, author = {Fabre, Bruno and Samori, Cristian and Bianco, Alberto}, doi = {10.1016/j.jelechem.2011.11.029}, issn = {1572-6657}, year = {2012}, date = {2012-01-01}, journal = {JOURNAL OF ELECTROANALYTICAL CHEMISTRY}, volume = {665}, pages = {90--94}, abstract = {Multi-walled carbon nanotubes (MWCNTs) double functionalized with redox-active ferrocene and biotin (Fc-Biot-MWCNTs) were synthesized and used for the electrochemical detection of avidin. After dispersion in perfluorosulfonated polymer Nation and immobilization on the electrode surfaces, the cyclic voltammetry response of the modified electrodes showed in aqueous medium a quasi-reversible one-electron system at 0.46 V vs. SCE, assigned to the bound ferrocene/ferrocenium redox couple. Upon the addition of avidin in the range 0.9-20 nM, a stepwise decrease of both anodic and cathodic peak currents ascribed to the ferrocene was observed. These electrochemical changes are specifically due to the formation of biotin-avidin complex and are explained by complexation-induced modifications in the environment of covalently bound ferrocene. (C) 2011 Elsevier B.V. All rights reserved.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Multi-walled carbon nanotubes (MWCNTs) double functionalized with redox-active ferrocene and biotin (Fc-Biot-MWCNTs) were synthesized and used for the electrochemical detection of avidin. After dispersion in perfluorosulfonated polymer Nation and immobilization on the electrode surfaces, the cyclic voltammetry response of the modified electrodes showed in aqueous medium a quasi-reversible one-electron system at 0.46 V vs. SCE, assigned to the bound ferrocene/ferrocenium redox couple. Upon the addition of avidin in the range 0.9-20 nM, a stepwise decrease of both anodic and cathodic peak currents ascribed to the ferrocene was observed. These electrochemical changes are specifically due to the formation of biotin-avidin complex and are explained by complexation-induced modifications in the environment of covalently bound ferrocene. (C) 2011 Elsevier B.V. All rights reserved. |
Rinaldi, R; Maruccio, G; Arima, V; Spada, G P; Samori, P; Cuniberti, G; Boland, J; Bramanti, A P Molarnet Project: Molecular Architectures for QCA-Inspired Boolean Networks Journal Article In: INTERNATIONAL JOURNAL OF UNCONVENTIONAL COMPUTING, 8 (4, SI), pp. 301–305, 2012, ISSN: 1548-7199. @article{rinaldi_molarnet_2012, title = {Molarnet Project: Molecular Architectures for QCA-Inspired Boolean Networks}, author = {Rinaldi, R. and Maruccio, G. and Arima, V. and Spada, G. P. and Samori, P. and Cuniberti, G. and Boland, J. and Bramanti, A. P.}, issn = {1548-7199}, year = {2012}, date = {2012-01-01}, journal = {INTERNATIONAL JOURNAL OF UNCONVENTIONAL COMPUTING}, volume = {8}, number = {4, SI}, pages = {301--305}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Crivillers, Nuria ; Favaretto, Laura ; Zanelli, Alberto ; Manet, Ilse ; Treier, Matthias ; Morandi, Vittorio ; Gazzano, Massimo ; Samori, Paolo ; Melucci, Manuela Self-assembly and electrical properties of a novel heptameric thiophene-benzothiadiazole based architectures Journal Article In: CHEMICAL COMMUNICATIONS, 48 (100), pp. 12162–12164, 2012, ISSN: 1359-7345. @article{crivillers_self-assembly_2012, title = {Self-assembly and electrical properties of a novel heptameric thiophene-benzothiadiazole based architectures}, author = {Crivillers, Nuria and Favaretto, Laura and Zanelli, Alberto and Manet, Ilse and Treier, Matthias and Morandi, Vittorio and Gazzano, Massimo and Samori, Paolo and Melucci, Manuela}, doi = {10.1039/c2cc36510c}, issn = {1359-7345}, year = {2012}, date = {2012-01-01}, journal = {CHEMICAL COMMUNICATIONS}, volume = {48}, number = {100}, pages = {12162--12164}, abstract = {A novel semiconducting benzothiadiazole (BTZ)-thiophene (T) co-oligomer having an unprecedented BTZ-T alternated motif has been synthesized and self-assembled into micrometer sized fibers by simple solution processing. The electrical properties of these low-dimensional architectures have been characterized by integrating them in an organic field-effect transistor.}, keywords = {}, pubstate = {published}, tppubtype = {article} } A novel semiconducting benzothiadiazole (BTZ)-thiophene (T) co-oligomer having an unprecedented BTZ-T alternated motif has been synthesized and self-assembled into micrometer sized fibers by simple solution processing. The electrical properties of these low-dimensional architectures have been characterized by integrating them in an organic field-effect transistor. |
Samori, Paolo Paolo Samori Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (32), pp. 7889, 2012, ISSN: 1433-7851. @article{samori_paolo_2012, title = {Paolo Samori}, author = {Samori, Paolo}, issn = {1433-7851}, year = {2012}, date = {2012-01-01}, journal = {ANGEWANDTE CHEMIE-INTERNATIONAL EDITION}, volume = {51}, number = {32}, pages = {7889}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Palma, Carlos-Andres ; Cecchini, Marco ; Samori, Paolo Predicting self-assembly: from empirism to determinism Journal Article In: CHEMICAL SOCIETY REVIEWS, 41 (10), pp. 3713–3730, 2012, ISSN: 0306-0012. @article{palma_predicting_2012, title = {Predicting self-assembly: from empirism to determinism}, author = {Palma, Carlos-Andres and Cecchini, Marco and Samori, Paolo}, doi = {10.1039/c2cs15302e}, issn = {0306-0012}, year = {2012}, date = {2012-01-01}, journal = {CHEMICAL SOCIETY REVIEWS}, volume = {41}, number = {10}, pages = {3713--3730}, abstract = {Self-assembly is one of the most important concepts of the 21st century. Strikingly, despite the rational design of molecules for biological and pharmaceutical applications is rather well established, only few are the attempts to formally refine predictions of self-assembly in material science. In the present tutorial review, we encompass some of the most significant efforts towards the systematic study of (thermodynamically stable) self-assembly. We discuss experimental and computer-simulated self-assembly events in hard-matter, soft-matter and higher symmetry architectures under the common framework of partition functions. In this framework, we endeavor to correlate state-of-the-art chemical design, programming and/or engineering of reversible (thermal and chemical equilibrium) self-assembly with knowledge of the underlying partition function landscape in a step towards quantitative predictions and ab initio molecular design.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Self-assembly is one of the most important concepts of the 21st century. Strikingly, despite the rational design of molecules for biological and pharmaceutical applications is rather well established, only few are the attempts to formally refine predictions of self-assembly in material science. In the present tutorial review, we encompass some of the most significant efforts towards the systematic study of (thermodynamically stable) self-assembly. We discuss experimental and computer-simulated self-assembly events in hard-matter, soft-matter and higher symmetry architectures under the common framework of partition functions. In this framework, we endeavor to correlate state-of-the-art chemical design, programming and/or engineering of reversible (thermal and chemical equilibrium) self-assembly with knowledge of the underlying partition function landscape in a step towards quantitative predictions and ab initio molecular design. |
Treier, Matthias ; Arlin, Jean-Baptiste ; Ruzie, Christian ; Geerts, Yves H; Lemaur, Vincent ; Cornil, Jerome ; Samori, Paolo Ambipolar organic field-effect transistors with balanced mobilities through solvent-vapour annealing induced phase-separation of bi-component mixtures Journal Article In: JOURNAL OF MATERIALS CHEMISTRY, 22 (19), pp. 9509–9512, 2012, ISSN: 0959-9428. @article{treier_ambipolar_2012, title = {Ambipolar organic field-effect transistors with balanced mobilities through solvent-vapour annealing induced phase-separation of bi-component mixtures}, author = {Treier, Matthias and Arlin, Jean-Baptiste and Ruzie, Christian and Geerts, Yves H. and Lemaur, Vincent and Cornil, Jerome and Samori, Paolo}, doi = {10.1039/c2jm31063e}, issn = {0959-9428}, year = {2012}, date = {2012-01-01}, journal = {JOURNAL OF MATERIALS CHEMISTRY}, volume = {22}, number = {19}, pages = {9509--9512}, abstract = {Thin films of bi-component mixtures of two commonly used n- and p-type organic semiconductors are found to undergo spontaneous phase-separation with the formation of well-ordered nanoneedles/crystals upon solvent-vapour annealing. The de-mixing is used to fabricate ambipolar organic field-effect transistors where balanced mobilities were achieved by adjusting the relative amount of the constituent in solution.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Thin films of bi-component mixtures of two commonly used n- and p-type organic semiconductors are found to undergo spontaneous phase-separation with the formation of well-ordered nanoneedles/crystals upon solvent-vapour annealing. The de-mixing is used to fabricate ambipolar organic field-effect transistors where balanced mobilities were achieved by adjusting the relative amount of the constituent in solution. |
Savage, Rebecca C; Orgiu, Emanuele ; Mativetsky, Jeffrey M; Pisula, Wojciech ; Schnitzler, Tobias ; Eversloh, Christian Luetke ; Li, Chen ; Muellen, Klaus ; Samori, Paolo Charge transport in fibre-based perylene-diimide transistors: effect of the alkyl substitution and processing technique Journal Article In: NANOSCALE, 4 (7), pp. 2387–2393, 2012, ISSN: 2040-3364. @article{savage_charge_2012, title = {Charge transport in fibre-based perylene-diimide transistors: effect of the alkyl substitution and processing technique}, author = {Savage, Rebecca C. and Orgiu, Emanuele and Mativetsky, Jeffrey M. and Pisula, Wojciech and Schnitzler, Tobias and Eversloh, Christian Luetke and Li, Chen and Muellen, Klaus and Samori, Paolo}, doi = {10.1039/c2nr30088e}, issn = {2040-3364}, year = {2012}, date = {2012-01-01}, journal = {NANOSCALE}, volume = {4}, number = {7}, pages = {2387--2393}, abstract = {We report a comparative study on the self-assembly from solution and electrical characterization of n-type semiconducting fibres obtained from five different perylenebis(dicarboximide) (PDI) derivatives. In particular we investigated the role of the nature of the alkyl chain covalently linked to the N,N' sites of the PDI in modulating the molecular solubility and aggregation capacity. We explored the morphologies of the self-assembled architectures physisorbed on dielectric surfaces and in particular how they can be modified by tuning the deposition and post-deposition procedures, i.e. by modulating the kinetics of the self-assembly process. To this end, alongside the conventional spin-coating, solvent vapour annealing (SVA) and solvent induced precipitation (SIP) have been employed. Both approaches led to fibres having widths of several hundred nanometres and lengths up to tens of micrometres. SVA formed isolated fibres which were tens of nanometres high, flat, and tapered at the ends. Conversely, SIP fibres exhibited nearly matching heights and widths, but organized into bundles. Despite these morphological differences, the same intermolecular packing is found by XRD in each type of structure, albeit with differing degrees of long-range order. The study of the electrical characteristics of the obtained low dimensional nano-assemblies has been accomplished by fabricating and characterizing organic field-effect transistors.}, keywords = {}, pubstate = {published}, tppubtype = {article} } We report a comparative study on the self-assembly from solution and electrical characterization of n-type semiconducting fibres obtained from five different perylenebis(dicarboximide) (PDI) derivatives. In particular we investigated the role of the nature of the alkyl chain covalently linked to the N,N' sites of the PDI in modulating the molecular solubility and aggregation capacity. We explored the morphologies of the self-assembled architectures physisorbed on dielectric surfaces and in particular how they can be modified by tuning the deposition and post-deposition procedures, i.e. by modulating the kinetics of the self-assembly process. To this end, alongside the conventional spin-coating, solvent vapour annealing (SVA) and solvent induced precipitation (SIP) have been employed. Both approaches led to fibres having widths of several hundred nanometres and lengths up to tens of micrometres. SVA formed isolated fibres which were tens of nanometres high, flat, and tapered at the ends. Conversely, SIP fibres exhibited nearly matching heights and widths, but organized into bundles. Despite these morphological differences, the same intermolecular packing is found by XRD in each type of structure, albeit with differing degrees of long-range order. The study of the electrical characteristics of the obtained low dimensional nano-assemblies has been accomplished by fabricating and characterizing organic field-effect transistors. |
Treier, Matthias ; Liscio, Andrea ; Mativetsky, Jeffrey M; Kastler, Marcel ; Muellen, Klaus ; Palermo, Vincenzo ; Samori, Paolo Photoconductive and supramolecularly engineered organic field-effect transistors based on fibres from donor-acceptor dyads Journal Article In: NANOSCALE, 4 (5), pp. 1677–1681, 2012, ISSN: 2040-3364. @article{treier_photoconductive_2012, title = {Photoconductive and supramolecularly engineered organic field-effect transistors based on fibres from donor-acceptor dyads}, author = {Treier, Matthias and Liscio, Andrea and Mativetsky, Jeffrey M. and Kastler, Marcel and Muellen, Klaus and Palermo, Vincenzo and Samori, Paolo}, doi = {10.1039/c2nr11635a}, issn = {2040-3364}, year = {2012}, date = {2012-01-01}, journal = {NANOSCALE}, volume = {4}, number = {5}, pages = {1677--1681}, abstract = {We report on the formation of photoconductive self-assembled fibres by solvent induced precipitation of a HBC-PMI donor-acceptor dyad. Kelvin Probe Force Microscopy revealed that upon illumination with white light the surface potential of the fibres shifted to negative values due to a build-up of negative charge. When integrated in a field-effect transistor (FET) configuration, the devices can be turned `on' much more efficiently using light than conventional bias triggered field-effect, suggesting that these structures could be used for the fabrication of light sensing devices. Such a double gating represents an important step towards bi-functional organic FETs, in which the current through the junction can be modulated both optically (by photoexcitation) and electrically (by gate control).}, keywords = {}, pubstate = {published}, tppubtype = {article} } We report on the formation of photoconductive self-assembled fibres by solvent induced precipitation of a HBC-PMI donor-acceptor dyad. Kelvin Probe Force Microscopy revealed that upon illumination with white light the surface potential of the fibres shifted to negative values due to a build-up of negative charge. When integrated in a field-effect transistor (FET) configuration, the devices can be turned `on' much more efficiently using light than conventional bias triggered field-effect, suggesting that these structures could be used for the fabrication of light sensing devices. Such a double gating represents an important step towards bi-functional organic FETs, in which the current through the junction can be modulated both optically (by photoexcitation) and electrically (by gate control). |
Orgiu, Emanuele ; Masillamani, Appan Merari ; Vogel, Joern-Oliver ; Treossi, Emanuele ; Kiersnowski, Adam ; Kastler, Marcel ; Pisula, Wojciech ; Doetz, Florian ; Palermo, Vincenzo ; Samori, Paolo Enhanced mobility in P3HT-based OTFTs upon blending with a phenylene-thiophene-thiophene-phenylene small molecule Journal Article In: CHEMICAL COMMUNICATIONS, 48 (10), pp. 1562–1564, 2012, ISSN: 1359-7345. @article{orgiu_enhanced_2012, title = {Enhanced mobility in P3HT-based OTFTs upon blending with a phenylene-thiophene-thiophene-phenylene small molecule}, author = {Orgiu, Emanuele and Masillamani, Appan Merari and Vogel, Joern-Oliver and Treossi, Emanuele and Kiersnowski, Adam and Kastler, Marcel and Pisula, Wojciech and Doetz, Florian and Palermo, Vincenzo and Samori, Paolo}, doi = {10.1039/c1cc15477j}, issn = {1359-7345}, year = {2012}, date = {2012-01-01}, journal = {CHEMICAL COMMUNICATIONS}, volume = {48}, number = {10}, pages = {1562--1564}, abstract = {An enhancement in charge transport capacity in a poly(3-hexylthiophene) (P3HT) semicrystalline film, up to field-effect mobilities approaching 0.1 cm(2) V-1 s(-1), has been achieved by co-deposition with a small molecule, i.e. 5,5'-bis(4-n-hexylphenyl)-2,2'-bithiophene (dH-PTTP), forming highly ordered crystals bridging large polymeric domains.}, keywords = {}, pubstate = {published}, tppubtype = {article} } An enhancement in charge transport capacity in a poly(3-hexylthiophene) (P3HT) semicrystalline film, up to field-effect mobilities approaching 0.1 cm(2) V-1 s(-1), has been achieved by co-deposition with a small molecule, i.e. 5,5'-bis(4-n-hexylphenyl)-2,2'-bithiophene (dH-PTTP), forming highly ordered crystals bridging large polymeric domains. |
El Malah, Tamer ; Ciesielski, Artur ; Piot, Luc ; Troyanov, Sergey I; Mueller, Uwe ; Weidner, Steffen ; Samori, Paolo ; Hecht, Stefan Conformationally pre-organized and pH-responsive flat dendrons: synthesis and self-assembly at the liquid-solid interface Journal Article In: NANOSCALE, 4 (2), pp. 467–472, 2012, ISSN: 2040-3364. @article{el_malah_conformationally_2012, title = {Conformationally pre-organized and pH-responsive flat dendrons: synthesis and self-assembly at the liquid-solid interface}, author = {El Malah, Tamer and Ciesielski, Artur and Piot, Luc and Troyanov, Sergey I. and Mueller, Uwe and Weidner, Steffen and Samori, Paolo and Hecht, Stefan}, doi = {10.1039/c1nr11434d}, issn = {2040-3364}, year = {2012}, date = {2012-01-01}, journal = {NANOSCALE}, volume = {4}, number = {2}, pages = {467--472}, abstract = {Efficient Cu-catalyzed 1,3-dipolar cycloaddition reactions have been used to prepare two series of three regioisomers of G-1 and G-2 poly(triazole-pyridine) dendrons. The G-1 and G-2 dendrons consist of branched yet conformationally pre-organized 2,6-bis(phenyl/pyridyl-1,2,3-triazol-4-yl) pyridine (BPTP) monomeric and trimeric cores, respectively, carrying one focal and either two or four peripheral alkyl side chains. In the solid state, the conformation and supramolecular organization were studied by means of a single crystal X-ray structure analysis of one derivative. At the liquid-solid interface, the self-assembly behavior was investigated by scanning tunneling microscopy (STM) on graphite surfaces. Based on the observed supramolecular organization, it appears that the subtle balance between conformational preferences inherent in the dendritic backbone on the one side and the adsorption and packing of the alkyl side chains on the graphite substrate on the other side dictate the overall structure formation in 2D.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Efficient Cu-catalyzed 1,3-dipolar cycloaddition reactions have been used to prepare two series of three regioisomers of G-1 and G-2 poly(triazole-pyridine) dendrons. The G-1 and G-2 dendrons consist of branched yet conformationally pre-organized 2,6-bis(phenyl/pyridyl-1,2,3-triazol-4-yl) pyridine (BPTP) monomeric and trimeric cores, respectively, carrying one focal and either two or four peripheral alkyl side chains. In the solid state, the conformation and supramolecular organization were studied by means of a single crystal X-ray structure analysis of one derivative. At the liquid-solid interface, the self-assembly behavior was investigated by scanning tunneling microscopy (STM) on graphite surfaces. Based on the observed supramolecular organization, it appears that the subtle balance between conformational preferences inherent in the dendritic backbone on the one side and the adsorption and packing of the alkyl side chains on the graphite substrate on the other side dictate the overall structure formation in 2D. |
Qi, Yan ; Nam, Kwangho ; Spong, Marie C; Banerjee, Anirban ; Sung, Rou-Jia ; Zhang, Michael ; Karplus, Martin ; Verdine, Gregory L Strandwise translocation of a DNA glycosylase on undamaged DNA Journal Article In: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 109 (4), pp. 1086–1091, 2012, ISSN: 0027-8424. @article{qi_strandwise_2012, title = {Strandwise translocation of a DNA glycosylase on undamaged DNA}, author = {Qi, Yan and Nam, Kwangho and Spong, Marie C. and Banerjee, Anirban and Sung, Rou-Jia and Zhang, Michael and Karplus, Martin and Verdine, Gregory L.}, doi = {10.1073/pnas.1111237108}, issn = {0027-8424}, year = {2012}, date = {2012-01-01}, journal = {PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA}, volume = {109}, number = {4}, pages = {1086--1091}, abstract = {Base excision repair of genotoxic nucleobase lesions in the genome is critically dependent upon the ability of DNA glycosylases to locate rare sites of damage embedded in a vast excess of undamaged DNA, using only thermal energy to fuel the search process. Considerable interest surrounds the question of how DNA glycosylases translocate efficiently along DNA while maintaining their vigilance for target damaged sites. Here, we report the observation of strandwise translocation of 8-oxoguanine DNA glycosylase, MutM, along undamaged DNA. In these complexes, the protein is observed to translocate by one nucleotide on one strand while remaining untranslocated on the complementary strand. We further report that alterations of single base-pairs or a single amino acid substitution (R112A) can induce strandwise translocation. Molecular dynamics simulations confirm that MutM can translocate along DNA in a strandwise fashion. These observations reveal a previously unobserved mode of movement for a DNA-binding protein along the surface of DNA.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Base excision repair of genotoxic nucleobase lesions in the genome is critically dependent upon the ability of DNA glycosylases to locate rare sites of damage embedded in a vast excess of undamaged DNA, using only thermal energy to fuel the search process. Considerable interest surrounds the question of how DNA glycosylases translocate efficiently along DNA while maintaining their vigilance for target damaged sites. Here, we report the observation of strandwise translocation of 8-oxoguanine DNA glycosylase, MutM, along undamaged DNA. In these complexes, the protein is observed to translocate by one nucleotide on one strand while remaining untranslocated on the complementary strand. We further report that alterations of single base-pairs or a single amino acid substitution (R112A) can induce strandwise translocation. Molecular dynamics simulations confirm that MutM can translocate along DNA in a strandwise fashion. These observations reveal a previously unobserved mode of movement for a DNA-binding protein along the surface of DNA. |
Stefankiewicz, Artur R; Rogez, Guillaume ; Harrowfield, Jack ; Sobolev, Alexandre N; Madalan, Augustin ; Huuskonen, Juhani ; Rissanen, Kari ; Lehn, Jean-Marie Self-ordering of metallogrid complexes via directed hydrogen-bonding Journal Article In: DALTON TRANSACTIONS, 41 (45), pp. 13848–13855, 2012, ISSN: 1477-9226. @article{stefankiewicz_self-ordering_2012, title = {Self-ordering of metallogrid complexes via directed hydrogen-bonding}, author = {Stefankiewicz, Artur R. and Rogez, Guillaume and Harrowfield, Jack and Sobolev, Alexandre N. and Madalan, Augustin and Huuskonen, Juhani and Rissanen, Kari and Lehn, Jean-Marie}, doi = {10.1039/c2dt31384g}, issn = {1477-9226}, year = {2012}, date = {2012-01-01}, journal = {DALTON TRANSACTIONS}, volume = {41}, number = {45}, pages = {13848--13855}, abstract = {Reaction of imidazole aldehydes with dihydrazino derivatives of 2-phenylpyrimidine provides a family of bis(acylhydrazone) ligands which form [2 x 2] metallogrid complexes with transition metal ions including Fe(II), Co(II), Cu(II) and Zn(II). The free ligands show H-bonding interactions, both donor and acceptor, largely involving the imidazole units, while binding of the metal ions occupies all the acceptor sites and leaves only the pyrrolic-NH site as an H-bond donor, although its deprotonation by a strong base can regenerate an acceptor. These H-bonding interactions have been studied by H-1 NMR spectroscopy in solution and in the solid state by means of several crystal structure determinations. The Fe(II) grids appear to be exclusively high-spin species over a wide temperature range in solution. In the solid state various forms of spin-crossover behaviour can be observed between 1.8 and 300 K, which has been rationalised in terms of the varied forms of hydrogen-bonding possible in the crystalline state.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Reaction of imidazole aldehydes with dihydrazino derivatives of 2-phenylpyrimidine provides a family of bis(acylhydrazone) ligands which form [2 x 2] metallogrid complexes with transition metal ions including Fe(II), Co(II), Cu(II) and Zn(II). The free ligands show H-bonding interactions, both donor and acceptor, largely involving the imidazole units, while binding of the metal ions occupies all the acceptor sites and leaves only the pyrrolic-NH site as an H-bond donor, although its deprotonation by a strong base can regenerate an acceptor. These H-bonding interactions have been studied by H-1 NMR spectroscopy in solution and in the solid state by means of several crystal structure determinations. The Fe(II) grids appear to be exclusively high-spin species over a wide temperature range in solution. In the solid state various forms of spin-crossover behaviour can be observed between 1.8 and 300 K, which has been rationalised in terms of the varied forms of hydrogen-bonding possible in the crystalline state. |
Lehn, Jean-Marie Constitutional Dynamic Chemistry: Bridge from Supramolecular Chemistry to Adaptive Chemistry Incollection In: {Barboiu, M} (Ed.): CONSTITUTIONAL DYNAMIC CHEMISTRY, 322 , pp. 1–32, 2012, ISBN: 978-3-642-28344-4 978-3-642-28343-7. @incollection{lehn_constitutional_2012, title = {Constitutional Dynamic Chemistry: Bridge from Supramolecular Chemistry to Adaptive Chemistry}, author = {Lehn, Jean-Marie}, editor = {{Barboiu, M}}, doi = {10.1007/128_2011_256}, isbn = {978-3-642-28344-4 978-3-642-28343-7}, year = {2012}, date = {2012-01-01}, booktitle = {CONSTITUTIONAL DYNAMIC CHEMISTRY}, volume = {322}, pages = {1--32}, series = {Topics in Current Chemistry-Series}, abstract = {Supramolecular chemistry aims at implementing highly complex chemical systems from molecular components held together by non-covalent intermolecular forces and effecting molecular recognition, catalysis and transport processes. A further step consists in the investigation of chemical systems undergoing self-organization, i.e. systems capable of spontaneously generating well-defined functional supramolecular architectures by self-assembly from their components, thus behaving as programmed chemical systems. Supramolecular chemistry is intrinsically a dynamic chemistry in view of the lability of the interactions connecting the molecular components of a supramolecular entity and the resulting ability of supramolecular species to exchange their constituents. The same holds for molecular chemistry when the molecular entity contains covalent bonds that may form and break reversibility, so as to allow a continuous change in constitution by reorganization and exchange of building blocks. These features define a Constitutional Dynamic Chemistry (CDC) on both the molecular and supramolecular levels. CDC introduces a paradigm shift with respect to constitutionally static chemistry. The latter relies on design for the generation of a target entity, whereas CDC takes advantage of dynamic diversity to allow variation and selection. The implementation of selection in chemistry introduces a fundamental change in outlook. Whereas self-organization by design strives to achieve full control over the output molecular or supramolecular entity by explicit programming, self-organization with selection operates on dynamic constitutional diversity in response to either internal or external factors to achieve adaptation. The merging of the features: -information and programmability, -dynamics and reversibility, -constitution and structural diversity, points to the emergence of adaptive and evolutive chemistry, towards a chemistry of complex matter.}, keywords = {}, pubstate = {published}, tppubtype = {incollection} } Supramolecular chemistry aims at implementing highly complex chemical systems from molecular components held together by non-covalent intermolecular forces and effecting molecular recognition, catalysis and transport processes. A further step consists in the investigation of chemical systems undergoing self-organization, i.e. systems capable of spontaneously generating well-defined functional supramolecular architectures by self-assembly from their components, thus behaving as programmed chemical systems. Supramolecular chemistry is intrinsically a dynamic chemistry in view of the lability of the interactions connecting the molecular components of a supramolecular entity and the resulting ability of supramolecular species to exchange their constituents. The same holds for molecular chemistry when the molecular entity contains covalent bonds that may form and break reversibility, so as to allow a continuous change in constitution by reorganization and exchange of building blocks. These features define a Constitutional Dynamic Chemistry (CDC) on both the molecular and supramolecular levels. CDC introduces a paradigm shift with respect to constitutionally static chemistry. The latter relies on design for the generation of a target entity, whereas CDC takes advantage of dynamic diversity to allow variation and selection. The implementation of selection in chemistry introduces a fundamental change in outlook. Whereas self-organization by design strives to achieve full control over the output molecular or supramolecular entity by explicit programming, self-organization with selection operates on dynamic constitutional diversity in response to either internal or external factors to achieve adaptation. The merging of the features: -information and programmability, -dynamics and reversibility, -constitution and structural diversity, points to the emergence of adaptive and evolutive chemistry, towards a chemistry of complex matter. |
Stephan, D W; Wright, D S; Atwood, J L; Cloke, F G N; Tsang, S C E; Lehn, J -M; Moody, C J; O'Reilly, R K; Taylor, R J K; Houk, Kendall N; Colacot, T J Royal Society of Chemistry Awards Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (37), pp. 9214–9215, 2012, ISSN: 1433-7851. @article{stephan_royal_2012, title = {Royal Society of Chemistry Awards}, author = {Stephan, D. W. and Wright, D. S. and Atwood, J. L. and Cloke, F. G. N. and Tsang, S. C. E. and Lehn, J. -M. and Moody, C. J. and O'Reilly, R. K. and Taylor, R. J. K. and Houk, Kendall N. and Colacot, T. J.}, doi = {10.1002/anie.201205769}, issn = {1433-7851}, year = {2012}, date = {2012-01-01}, journal = {ANGEWANDTE CHEMIE-INTERNATIONAL EDITION}, volume = {51}, number = {37}, pages = {9214--9215}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Fukuda, Kazuyuki ; Shimoda, Manabu ; Sukegawa, Makoto ; Nobori, Tadahito ; Lehn, Jean-Marie Doubly degradable dynamers: dynamic covalent polymers based on reversible imine connections and biodegradable polyester units Journal Article In: GREEN CHEMISTRY, 14 (10), pp. 2907–2911, 2012, ISSN: 1463-9262. @article{fukuda_doubly_2012, title = {Doubly degradable dynamers: dynamic covalent polymers based on reversible imine connections and biodegradable polyester units}, author = {Fukuda, Kazuyuki and Shimoda, Manabu and Sukegawa, Makoto and Nobori, Tadahito and Lehn, Jean-Marie}, doi = {10.1039/c2gc35875a}, issn = {1463-9262}, year = {2012}, date = {2012-01-01}, journal = {GREEN CHEMISTRY}, volume = {14}, number = {10}, pages = {2907--2911}, abstract = {We report the preparation and features of environmentally friendly “Green Dynamers” (GDs), dynamic polymers presenting sequential double-degradation features, chemical and biological. They were obtained by connecting biodegradable oligomers (such as small units of polybutylene adipate, PBA, and polybutylene succinate, PBS) through chemically degradable reversible imine bonds. The GDs possess water disintegratability, mendability and biodegradability. Their degradation rate may be modulated through and increases with the number of imine groups in the polymeric chain. The GDs were thermodynamically stable and maintained their molecular weight and their mechanical strength in air. However, when they were contacted with water, the imine bonds easily hydrolyzed, breaking up the polymer chains into oligomers. After such water disintegration, the residual oligomers were biodegraded into CO2 and water. In addition, the imine bonds were restored by evaporation of the water, leading to recovery of the molecular weight and of the mechanical properties of the GDs. The present GDs may be considered to represent a class of doubly-degradable polymers, combining chemical and biological degradability features, that operate in mild environmental conditions. This concept may contribute to solve the problem of waste elimination associated with the use of non-degradable polymeric materials.}, keywords = {}, pubstate = {published}, tppubtype = {article} } We report the preparation and features of environmentally friendly “Green Dynamers” (GDs), dynamic polymers presenting sequential double-degradation features, chemical and biological. They were obtained by connecting biodegradable oligomers (such as small units of polybutylene adipate, PBA, and polybutylene succinate, PBS) through chemically degradable reversible imine bonds. The GDs possess water disintegratability, mendability and biodegradability. Their degradation rate may be modulated through and increases with the number of imine groups in the polymeric chain. The GDs were thermodynamically stable and maintained their molecular weight and their mechanical strength in air. However, when they were contacted with water, the imine bonds easily hydrolyzed, breaking up the polymer chains into oligomers. After such water disintegration, the residual oligomers were biodegraded into CO2 and water. In addition, the imine bonds were restored by evaporation of the water, leading to recovery of the molecular weight and of the mechanical properties of the GDs. The present GDs may be considered to represent a class of doubly-degradable polymers, combining chemical and biological degradability features, that operate in mild environmental conditions. This concept may contribute to solve the problem of waste elimination associated with the use of non-degradable polymeric materials. |
Clegg, Jack K; Harrowfield, Jack ; Kim, Yang ; Lee, Young Hoon ; Lehn, Jean-Marie ; Lim, Woo Taik ; Thuery, Pierre Chelation-controlled molecular morphology: aminal to imine rearrangements Journal Article In: DALTON TRANSACTIONS, 41 (15), pp. 4335–4357, 2012, ISSN: 1477-9226. @article{clegg_chelation-controlled_2012, title = {Chelation-controlled molecular morphology: aminal to imine rearrangements}, author = {Clegg, Jack K. and Harrowfield, Jack and Kim, Yang and Lee, Young Hoon and Lehn, Jean-Marie and Lim, Woo Taik and Thuery, Pierre}, doi = {10.1039/c2dt12250b}, issn = {1477-9226}, year = {2012}, date = {2012-01-01}, journal = {DALTON TRANSACTIONS}, volume = {41}, number = {15}, pages = {4335--4357}, abstract = {Reactions between the tripodal hydroxytriamine, 2,2-bis(aminomethyl)-3-aminopropan-1-ol, “hytame”, and the isomeric pyridine aldehydes generate in all cases the tris(aminal) species based on a 1,3,5-triaza-adamantane skeleton. In all cases also, the product from water under basic conditions consists of an approximately 1:9 mixture of the triequatorial and monoaxial-diequatorial isomers. While all these tripyridyltriaza-adamantanes appear capable of acting as Lewis bases, in particular cases metal ion binding leads to a radical structural rearrangement. These cases involve the pyridine-2-aldehyde derivatives only and certain transition metal ions (notably Fe(II)), and result in the conversion of the tris (aminal) into its isomeric tris(imine) form. This is apparently favoured because it can act as a hexadentate ligand towards a single metal ion, although kinetic influences are clearly important in this chemistry because template reactions of the triamine, pyridine-2-aldehyde and several metal ions give much better yields of the tris(imine) complex than do analogous rearrangement reactions. For the low-spin, kinetically inert Fe(II) complex of the tris(imine), its formation is apparently so favourable that it is generated via aldehyde unit exchange when the aza-adamantanes derived from pyridine-3- and -4-aldehyde are heated with a mixture of Fe(II) and pyridine-2-aldehyde. When the kinetically labile Zn(II) complex is treated with EDTA, the metal ion is extracted but the released ligand does not undergo valence tautomerisation to what would be expected to be the triaxial isomer of the tripyridyltriaza-adamantane but instead rapidly undergoes partial hydrolysis before slowly forming the mixture of triequatorial and monoaxial-diequatorial isomers.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Reactions between the tripodal hydroxytriamine, 2,2-bis(aminomethyl)-3-aminopropan-1-ol, “hytame”, and the isomeric pyridine aldehydes generate in all cases the tris(aminal) species based on a 1,3,5-triaza-adamantane skeleton. In all cases also, the product from water under basic conditions consists of an approximately 1:9 mixture of the triequatorial and monoaxial-diequatorial isomers. While all these tripyridyltriaza-adamantanes appear capable of acting as Lewis bases, in particular cases metal ion binding leads to a radical structural rearrangement. These cases involve the pyridine-2-aldehyde derivatives only and certain transition metal ions (notably Fe(II)), and result in the conversion of the tris (aminal) into its isomeric tris(imine) form. This is apparently favoured because it can act as a hexadentate ligand towards a single metal ion, although kinetic influences are clearly important in this chemistry because template reactions of the triamine, pyridine-2-aldehyde and several metal ions give much better yields of the tris(imine) complex than do analogous rearrangement reactions. For the low-spin, kinetically inert Fe(II) complex of the tris(imine), its formation is apparently so favourable that it is generated via aldehyde unit exchange when the aza-adamantanes derived from pyridine-3- and -4-aldehyde are heated with a mixture of Fe(II) and pyridine-2-aldehyde. When the kinetically labile Zn(II) complex is treated with EDTA, the metal ion is extracted but the released ligand does not undergo valence tautomerisation to what would be expected to be the triaxial isomer of the tripyridyltriaza-adamantane but instead rapidly undergoes partial hydrolysis before slowly forming the mixture of triequatorial and monoaxial-diequatorial isomers. |
Hardy, John George ; Cao, Xiao-yu ; Harrowfield, Jack ; Lehn, Jean-Marie Generation of metallosupramolecular polymer gels from multiply functionalized grid-type complexes Journal Article In: NEW JOURNAL OF CHEMISTRY, 36 (3), pp. 668–673, 2012, ISSN: 1144-0546. @article{hardy_generation_2012, title = {Generation of metallosupramolecular polymer gels from multiply functionalized grid-type complexes}, author = {Hardy, John George and Cao, Xiao-yu and Harrowfield, Jack and Lehn, Jean-Marie}, doi = {10.1039/c2nj20898a}, issn = {1144-0546}, year = {2012}, date = {2012-01-01}, journal = {NEW JOURNAL OF CHEMISTRY}, volume = {36}, number = {3}, pages = {668--673}, abstract = {A ditopic ligand (1), containing two tridentate bis(acylhydrazone) subunits and bearing both long alkyl chains and hydrogen-bonding groups, has been synthesised. Metal cation binding in the presence of a base leads to hierarchical self-assembly, forming first a neutral [2 x 2] grid-type complex (2) that hierarchically assembles into metallosupramolecular polymer gels in toluene.}, keywords = {}, pubstate = {published}, tppubtype = {article} } A ditopic ligand (1), containing two tridentate bis(acylhydrazone) subunits and bearing both long alkyl chains and hydrogen-bonding groups, has been synthesised. Metal cation binding in the presence of a base leads to hierarchical self-assembly, forming first a neutral [2 x 2] grid-type complex (2) that hierarchically assembles into metallosupramolecular polymer gels in toluene. |
Han, Shuangbing ; Hermans, Thomas M; Fuller, Patrick E; Wei, Yanhu ; Grzybowski, Bartosz A Transport into Metal-Organic Frameworks from Solution Is Not Purely Diffusive Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (11), pp. 2662–2666, 2012, ISSN: 1433-7851. @article{han_transport_2012, title = {Transport into Metal-Organic Frameworks from Solution Is Not Purely Diffusive}, author = {Han, Shuangbing and Hermans, Thomas M. and Fuller, Patrick E. and Wei, Yanhu and Grzybowski, Bartosz A.}, doi = {10.1002/anie.201108492}, issn = {1433-7851}, year = {2012}, date = {2012-01-01}, journal = {ANGEWANDTE CHEMIE-INTERNATIONAL EDITION}, volume = {51}, number = {11}, pages = {2662--2666}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Mueller, Markus ; Diehl, Sebastian ; Pupillo, Guido ; Zoller, Peter Engineered Open Systems and Quantum Simulations with Atoms and Ions Incollection In: {Arimondo, E; Berman, PR ; Lin, CC} (Ed.): ADVANCES IN ATOMIC, MOLECULAR, AND OPTICAL PHYSICS, VOL 61, 61 , pp. 1–80, 2012, ISBN: 978-0-12-396482-3. @incollection{mueller_engineered_2012, title = {Engineered Open Systems and Quantum Simulations with Atoms and Ions}, author = {Mueller, Markus and Diehl, Sebastian and Pupillo, Guido and Zoller, Peter}, editor = {{Arimondo, E and Berman, PR and Lin, CC}}, doi = {10.1016/B978-0-12-396482-3.00001-6}, isbn = {978-0-12-396482-3}, year = {2012}, date = {2012-01-01}, booktitle = {ADVANCES IN ATOMIC, MOLECULAR, AND OPTICAL PHYSICS, VOL 61}, volume = {61}, pages = {1--80}, series = {Advances In Atomic Molecular and Optical Physics}, abstract = {The enormous experimental progress in atomic, molecular, and optical (AMO) physics during the last decades allows us nowadays to isolate single, a few or even many-body ensembles of microscopic particles, and to manipulate their quantum properties at a level of precision, which still seemed unthinkable some years ago. This versatile set of tools has enabled the development of the well-established concept of engineering of many-body Hamiltonians in various physical platforms. These available tools, however, can also be harnessed to extend the scenario of Hamiltonian engineering to a more general Liouvillian setting, which in addition to coherent dynamics also includes controlled dissipation in many-body quantum systems. Here, we review recent theoretical and experimental progress in different directions along these lines, with a particular focus on physical realizations with systems of atoms and ions. This comprises digital quantum simulations in a general open system setting, as well as engineering and understanding new classes of systems far away from thermodynamic equilibrium. In the context of digital quantum simulation, we first outline the basic concepts and illustrate them on the basis of a recent experiment with trapped ions. We also discuss theoretical work proposing an intrinsically scalable simulation architecture for spin models with high-order interactions such as Kitaev's toric code, based on Rydberg atoms stored in optical lattices. We then turn to the digital simulation of dissipative many-body dynamics, pointing out a route for the general quantum state preparation in complex spin models, and discuss a recent experiment demonstrating the basic building blocks of a full-fledged open-system quantum simulator. In view of creating novel classes of out-of-equilibrium systems, we focus on ultracold atoms. We point out how quantum mechanical long-range order can be established via engineered dissipation, and present genuine many-body aspects of this setting: in the context of bosons, we discuss dynamical phase transitions resulting from competing Hamiltonian and dissipative dynamics. In the context of fermions, we present a purely dissipative pairing mechanism, and show how this could pave the way for the quantum simulation of the Fermi-Hubbard model. We also propose and analyze the key properties of dissipatively targeted topological phases of matter.}, keywords = {}, pubstate = {published}, tppubtype = {incollection} } The enormous experimental progress in atomic, molecular, and optical (AMO) physics during the last decades allows us nowadays to isolate single, a few or even many-body ensembles of microscopic particles, and to manipulate their quantum properties at a level of precision, which still seemed unthinkable some years ago. This versatile set of tools has enabled the development of the well-established concept of engineering of many-body Hamiltonians in various physical platforms. These available tools, however, can also be harnessed to extend the scenario of Hamiltonian engineering to a more general Liouvillian setting, which in addition to coherent dynamics also includes controlled dissipation in many-body quantum systems. Here, we review recent theoretical and experimental progress in different directions along these lines, with a particular focus on physical realizations with systems of atoms and ions. This comprises digital quantum simulations in a general open system setting, as well as engineering and understanding new classes of systems far away from thermodynamic equilibrium. In the context of digital quantum simulation, we first outline the basic concepts and illustrate them on the basis of a recent experiment with trapped ions. We also discuss theoretical work proposing an intrinsically scalable simulation architecture for spin models with high-order interactions such as Kitaev's toric code, based on Rydberg atoms stored in optical lattices. We then turn to the digital simulation of dissipative many-body dynamics, pointing out a route for the general quantum state preparation in complex spin models, and discuss a recent experiment demonstrating the basic building blocks of a full-fledged open-system quantum simulator. In view of creating novel classes of out-of-equilibrium systems, we focus on ultracold atoms. We point out how quantum mechanical long-range order can be established via engineered dissipation, and present genuine many-body aspects of this setting: in the context of bosons, we discuss dynamical phase transitions resulting from competing Hamiltonian and dissipative dynamics. In the context of fermions, we present a purely dissipative pairing mechanism, and show how this could pave the way for the quantum simulation of the Fermi-Hubbard model. We also propose and analyze the key properties of dissipatively targeted topological phases of matter. |
Joosten, Antoine ; Trolez, Yann ; Collin, Jean-Paul ; Heitz, Valerie ; Sauvage, Jean-Pierre Copper(I)-Assembled [3]Rotaxane Whose Two Rings Act as Flapping Wings Journal Article In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 134 (3), pp. 1802–1809, 2012, ISSN: 0002-7863. @article{joosten_copperi-assembled_2012, title = {Copper(I)-Assembled [3]Rotaxane Whose Two Rings Act as Flapping Wings}, author = {Joosten, Antoine and Trolez, Yann and Collin, Jean-Paul and Heitz, Valerie and Sauvage, Jean-Pierre}, doi = {10.1021/ja210113y}, issn = {0002-7863}, year = {2012}, date = {2012-01-01}, journal = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY}, volume = {134}, number = {3}, pages = {1802--1809}, abstract = {A new copper-complexed [3]rotaxane consisting of two coordinating 30-membered rings threaded by a two-binding-site axis has been prepared in good yield from relatively simple organic fragments. The main specificity of the system originates from the stoppering reaction, based on “click” chemistry, and thus from the presence of two triazole groups at positions next to the bidentate chelates of the axis central part. The geometry of the coordinating atoms belonging to the axis is such that the triazole groups can either be part of the coordinating fragments when the metal center is 5-coordinate or be not at all involved in coordination to the metal when the latter is 4-coordinate. To be more specific, when the two complexed metal centers are monovalent copper(I) centers, the triazoles are not included in the metal coordination sphere, whereas when the metal centers are Cu(II) or Zn2+, the triazole groups are bound to the metals. This is easily explained by the fact that Cu(I) is preferably 4-coordinate and Cu(II) and Zn2+ are 5-coordinate. The interconversion between both situations (4- or 5-coordinate) can be quantitatively induced by metal exchange (Cu(I)/Zn2+) or by a redox process (Cu(II)/Cu(I). It leads to important geometrical changes and in particular to a strong modification of the angle between the two rings. As a consequence, the two threaded rings undergo a motion which is reminiscent of a wing-flapping movement similar to that of birds. This flapping motion is fast and quantitative. It should lead to new functional molecular machines in the future.}, keywords = {}, pubstate = {published}, tppubtype = {article} } A new copper-complexed [3]rotaxane consisting of two coordinating 30-membered rings threaded by a two-binding-site axis has been prepared in good yield from relatively simple organic fragments. The main specificity of the system originates from the stoppering reaction, based on “click” chemistry, and thus from the presence of two triazole groups at positions next to the bidentate chelates of the axis central part. The geometry of the coordinating atoms belonging to the axis is such that the triazole groups can either be part of the coordinating fragments when the metal center is 5-coordinate or be not at all involved in coordination to the metal when the latter is 4-coordinate. To be more specific, when the two complexed metal centers are monovalent copper(I) centers, the triazoles are not included in the metal coordination sphere, whereas when the metal centers are Cu(II) or Zn2+, the triazole groups are bound to the metals. This is easily explained by the fact that Cu(I) is preferably 4-coordinate and Cu(II) and Zn2+ are 5-coordinate. The interconversion between both situations (4- or 5-coordinate) can be quantitatively induced by metal exchange (Cu(I)/Zn2+) or by a redox process (Cu(II)/Cu(I). It leads to important geometrical changes and in particular to a strong modification of the angle between the two rings. As a consequence, the two threaded rings undergo a motion which is reminiscent of a wing-flapping movement similar to that of birds. This flapping motion is fast and quantitative. It should lead to new functional molecular machines in the future. |
Ventura, Barbara ; Durola, Fabien ; Frey, Julien ; Heitz, Valerie ; Sauvage, Jean-Pierre ; Flamigni, Lucia Near-infrared dual luminescence from an extended zinc porphyrin Journal Article In: CHEMICAL COMMUNICATIONS, 48 (7), pp. 1021–1023, 2012, ISSN: 1359-7345. @article{ventura_near-infrared_2012, title = {Near-infrared dual luminescence from an extended zinc porphyrin}, author = {Ventura, Barbara and Durola, Fabien and Frey, Julien and Heitz, Valerie and Sauvage, Jean-Pierre and Flamigni, Lucia}, doi = {10.1039/c1cc16739a}, issn = {1359-7345}, year = {2012}, date = {2012-01-01}, journal = {CHEMICAL COMMUNICATIONS}, volume = {48}, number = {7}, pages = {1021--1023}, abstract = {The photophysical characterization of an extended zinc porphyrin is reported. Fusion of bis-tetraazaanthracene on the porphyrin ring causes an unusual dual luminescence ascribed to two non-equilibrated singlet excited states.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The photophysical characterization of an extended zinc porphyrin is reported. Fusion of bis-tetraazaanthracene on the porphyrin ring causes an unusual dual luminescence ascribed to two non-equilibrated singlet excited states. |
Huang, Jier ; Buyukcakir, Onur ; Mara, Michael W; Coskun, Ali ; Dimitrijevic, Nada M; Barin, Gokhan ; Kokhan, Oleksandr ; Stickrath, Andrew B; Ruppert, Romain ; Tiede, David M; Stoddart, Fraser J; Sauvage, Jean-Pierre ; Chen, Lin X Highly Efficient Ultrafast Electron Injection from the Singlet MLCT Excited State of Copper(I) Diimine Complexes to TiO2 Nanoparticles Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (51), pp. 12711–12715, 2012, ISSN: 1433-7851. @article{huang_highly_2012, title = {Highly Efficient Ultrafast Electron Injection from the Singlet MLCT Excited State of Copper(I) Diimine Complexes to TiO2 Nanoparticles}, author = {Huang, Jier and Buyukcakir, Onur and Mara, Michael W. and Coskun, Ali and Dimitrijevic, Nada M. and Barin, Gokhan and Kokhan, Oleksandr and Stickrath, Andrew B. and Ruppert, Romain and Tiede, David M. and Stoddart, J. Fraser and Sauvage, Jean-Pierre and Chen, Lin X.}, doi = {10.1002/anie.201204341}, issn = {1433-7851}, year = {2012}, date = {2012-01-01}, journal = {ANGEWANDTE CHEMIE-INTERNATIONAL EDITION}, volume = {51}, number = {51}, pages = {12711--12715}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Ventura, Barbara ; Flamigni, Lucia ; Collin, Jean-Paul ; Durola, Fabien ; Heitz, Valerie ; Reviriego, Felipe ; Sauvage, Jean-Pierre ; Trolez, Yann NIR emission of cyclic [4]rotaxanes containing pi-extended porphyrin chromophores Journal Article In: PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 14 (30), pp. 10589–10594, 2012, ISSN: 1463-9076. @article{ventura_nir_2012, title = {NIR emission of cyclic [4]rotaxanes containing pi-extended porphyrin chromophores}, author = {Ventura, Barbara and Flamigni, Lucia and Collin, Jean-Paul and Durola, Fabien and Heitz, Valerie and Reviriego, Felipe and Sauvage, Jean-Pierre and Trolez, Yann}, doi = {10.1039/c2cp41381g}, issn = {1463-9076}, year = {2012}, date = {2012-01-01}, journal = {PHYSICAL CHEMISTRY CHEMICAL PHYSICS}, volume = {14}, number = {30}, pages = {10589--10594}, abstract = {The photophysical properties of a Cu(I) [4]rotaxane 4(4+) and of the demetalated [4] rotaxane 3 have been determined and compared to those of the component Zn porphyrin 2. All samples emit in the NIR region (700-1200 nm). The luminescence from the interlocked structures is bathochromically shifted with respect to 2 and displays a lower emission quantum yield, much lower for 4(4+) than for 3. The occurrence of intra-molecular electron or energy transfer is excluded and the decrease in luminescence yield is discussed in terms of the energy gap law and of electronic interactions between components of the cyclic interlocked structure. In toluene a dual emission behavior, similar to that of 2, is observed for 3 and ascribed to the presence of two non-equilibrated excited states, pi-pi* and CT in nature with lifetimes of 0.80 and 0.14 ns, respectively.}, keywords = {}, pubstate = {published}, tppubtype = {article} } The photophysical properties of a Cu(I) [4]rotaxane 4(4+) and of the demetalated [4] rotaxane 3 have been determined and compared to those of the component Zn porphyrin 2. All samples emit in the NIR region (700-1200 nm). The luminescence from the interlocked structures is bathochromically shifted with respect to 2 and displays a lower emission quantum yield, much lower for 4(4+) than for 3. The occurrence of intra-molecular electron or energy transfer is excluded and the decrease in luminescence yield is discussed in terms of the energy gap law and of electronic interactions between components of the cyclic interlocked structure. In toluene a dual emission behavior, similar to that of 2, is observed for 3 and ascribed to the presence of two non-equilibrated excited states, pi-pi* and CT in nature with lifetimes of 0.80 and 0.14 ns, respectively. |
Coskun, Ali ; Hmadeh, Mohamad ; Barin, Gokhan ; Gandara, Felipe ; Li, Qiaowei ; Choi, Eunwoo ; Strutt, Nathan L; Cordes, David B; Slawin, Alexandra M Z; Stoddart, Fraser J; Sauvage, Jean-Pierre ; Yaghi, Omar M Metal-Organic Frameworks Incorporating Copper-Complexed Rotaxanes Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (9), pp. 2160–2163, 2012, ISSN: 1433-7851. @article{coskun_metal-organic_2012, title = {Metal-Organic Frameworks Incorporating Copper-Complexed Rotaxanes}, author = {Coskun, Ali and Hmadeh, Mohamad and Barin, Gokhan and Gandara, Felipe and Li, Qiaowei and Choi, Eunwoo and Strutt, Nathan L. and Cordes, David B. and Slawin, Alexandra M. Z. and Stoddart, J. Fraser and Sauvage, Jean-Pierre and Yaghi, Omar M.}, doi = {10.1002/anie.201107873}, issn = {1433-7851}, year = {2012}, date = {2012-01-01}, journal = {ANGEWANDTE CHEMIE-INTERNATIONAL EDITION}, volume = {51}, number = {9}, pages = {2160--2163}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Mazutis, Linas ; Griffiths, Andrew D Selective droplet coalescence using microfluidic systems Journal Article In: Lab on a Chip, 12 (10), pp. 1800, 2012, ISSN: 1473-0197, 1473-0189. @article{mazutis_selective_2012, title = {Selective droplet coalescence using microfluidic systems}, author = {Mazutis, Linas and Griffiths, Andrew D.}, url = {http://xlink.rsc.org/?DOI=c2lc40121e}, doi = {10.1039/c2lc40121e}, issn = {1473-0197, 1473-0189}, year = {2012}, date = {2012-01-01}, urldate = {2016-05-30}, journal = {Lab on a Chip}, volume = {12}, number = {10}, pages = {1800}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Najah, Majdi ; Griffiths, Andrew D; Ryckelynck, Michael Teaching Single-Cell Digital Analysis Using Droplet-Based Microfluidics Journal Article In: Analytical Chemistry, 84 (3), pp. 1202–1209, 2012, ISSN: 0003-2700. @article{najah_teaching_2012, title = {Teaching Single-Cell Digital Analysis Using Droplet-Based Microfluidics}, author = {Najah, Majdi and Griffiths, Andrew D. and Ryckelynck, Michael}, url = {http://dx.doi.org/10.1021/ac202645m}, doi = {10.1021/ac202645m}, issn = {0003-2700}, year = {2012}, date = {2012-01-01}, urldate = {2016-05-30}, journal = {Analytical Chemistry}, volume = {84}, number = {3}, pages = {1202--1209}, abstract = {Microfluidics allows the manipulation of small quantities of reagents in a high-throughput manner and is therefore highly amenable to single cell characterization and more generally to digital analysis, with applications in fields as varied as genomics, diagnostics, directed evolution, and drug screening. The growing place of microfluidics in biology laboratories encouraged us to develop a teaching method where advanced undergraduate or first-year graduate-level students are taught to fabricate droplet-based microfluidic devices, characterize them, and finally use them to perform a digital analysis of bacterial samples based on a phenotypic marker.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Microfluidics allows the manipulation of small quantities of reagents in a high-throughput manner and is therefore highly amenable to single cell characterization and more generally to digital analysis, with applications in fields as varied as genomics, diagnostics, directed evolution, and drug screening. The growing place of microfluidics in biology laboratories encouraged us to develop a teaching method where advanced undergraduate or first-year graduate-level students are taught to fabricate droplet-based microfluidic devices, characterize them, and finally use them to perform a digital analysis of bacterial samples based on a phenotypic marker. |
Miller, Oliver J; Harrak, Abdeslam El ; Mangeat, Thomas ; Baret, Jean-Christophe ; Frenz, Lucas ; Debs, Bachir El ; Mayot, Estelle ; Samuels, Michael L; Rooney, Eamonn K; Dieu, Pierre ; Galvan, Martin ; Link, Darren R; Griffiths, Andrew D High-resolution dose–response screening using droplet-based microfluidics Journal Article In: Proceedings of the National Academy of Sciences, 109 (2), pp. 378–383, 2012, ISSN: 0027-8424, 1091-6490. @article{miller_high-resolution_2012, title = {High-resolution dose–response screening using droplet-based microfluidics}, author = {Miller, Oliver J. and Harrak, Abdeslam El and Mangeat, Thomas and Baret, Jean-Christophe and Frenz, Lucas and Debs, Bachir El and Mayot, Estelle and Samuels, Michael L. and Rooney, Eamonn K. and Dieu, Pierre and Galvan, Martin and Link, Darren R. and Griffiths, Andrew D.}, url = {http://www.pnas.org/content/109/2/378}, doi = {10.1073/pnas.1113324109}, issn = {0027-8424, 1091-6490}, year = {2012}, date = {2012-01-01}, urldate = {2016-05-30}, journal = {Proceedings of the National Academy of Sciences}, volume = {109}, number = {2}, pages = {378--383}, abstract = {A critical early step in drug discovery is the screening of a chemical library. Typically, promising compounds are identified in a primary screen and then more fully characterized in a dose–response analysis with 7–10 data points per compound. Here, we describe a robust microfluidic approach that increases the number of data points to approximately 10,000 per compound. The system exploits Taylor–Aris dispersion to create concentration gradients, which are then segmented into picoliter microreactors by droplet-based microfluidics. The large number of data points results in IC50 values that are highly precise (± 2.40% at 95% confidence) and highly reproducible (CV = 2.45%}, keywords = {}, pubstate = {published}, tppubtype = {article} } A critical early step in drug discovery is the screening of a chemical library. Typically, promising compounds are identified in a primary screen and then more fully characterized in a dose–response analysis with 7–10 data points per compound. Here, we describe a robust microfluidic approach that increases the number of data points to approximately 10,000 per compound. The system exploits Taylor–Aris dispersion to create concentration gradients, which are then segmented into picoliter microreactors by droplet-based microfluidics. The large number of data points results in IC50 values that are highly precise (± 2.40% at 95% confidence) and highly reproducible (CV = 2.45% |
Cuche, A; Mahboub, O; Devaux, E; Genet, C; Ebbesen, T W Plasmonic Coherent Drive of an Optical Trap Journal Article In: PHYSICAL REVIEW LETTERS, 108 (2), 2012, ISSN: 0031-9007. @article{cuche_plasmonic_2012, title = {Plasmonic Coherent Drive of an Optical Trap}, author = {Cuche, A. and Mahboub, O. and Devaux, E. and Genet, C. and Ebbesen, T. W.}, doi = {10.1103/PhysRevLett.108.026801}, issn = {0031-9007}, year = {2012}, date = {2012-01-01}, journal = {PHYSICAL REVIEW LETTERS}, volume = {108}, number = {2}, abstract = {We demonstrate that optical trapping can be driven by delocalized surface plasmon modes resonantly excited within a standing wave trap. Dynamical modifications are shown to be determined by the near-field symmetry of the plasmonic modes with negligible thermal effect. With low trapping powers and polarization control, remarkable stiffness enhancements are recorded, the larger the smaller the particle. The results can be simply modeled accounting for a coherent interaction between the plasmon field and the Gaussian standing wave of the trap.}, keywords = {}, pubstate = {published}, tppubtype = {article} } We demonstrate that optical trapping can be driven by delocalized surface plasmon modes resonantly excited within a standing wave trap. Dynamical modifications are shown to be determined by the near-field symmetry of the plasmonic modes with negligible thermal effect. With low trapping powers and polarization control, remarkable stiffness enhancements are recorded, the larger the smaller the particle. The results can be simply modeled accounting for a coherent interaction between the plasmon field and the Gaussian standing wave of the trap. |
Hutchison, James A; Schwartz, Tal ; Genet, Cyriaque ; Devaux, Eloise ; Ebbesen, Thomas W Modifying Chemical Landscapes by Coupling to Vacuum Fields Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (7), pp. 1592–1596, 2012, ISSN: 1433-7851. @article{hutchison_modifying_2012, title = {Modifying Chemical Landscapes by Coupling to Vacuum Fields}, author = {Hutchison, James A. and Schwartz, Tal and Genet, Cyriaque and Devaux, Eloise and Ebbesen, Thomas W.}, doi = {10.1002/anie.201107033}, issn = {1433-7851}, year = {2012}, date = {2012-01-01}, journal = {ANGEWANDTE CHEMIE-INTERNATIONAL EDITION}, volume = {51}, number = {7}, pages = {1592--1596}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Sondergaard, Thomas ; Bozhevolnyi, Sergey I; Beermann, Jonas ; Novikov, Sergey M; Devaux, Eloise ; Ebbesen, Thomas W Extraordinary optical transmission with tapered slits: effect of higher diffraction and slit resonance orders Journal Article In: JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 29 (1), pp. 130–137, 2012, ISSN: 0740-3224. @article{sondergaard_extraordinary_2012, title = {Extraordinary optical transmission with tapered slits: effect of higher diffraction and slit resonance orders}, author = {Sondergaard, Thomas and Bozhevolnyi, Sergey I. and Beermann, Jonas and Novikov, Sergey M. and Devaux, Eloise and Ebbesen, Thomas W.}, doi = {10.1364/JOSAB.29.000130}, issn = {0740-3224}, year = {2012}, date = {2012-01-01}, journal = {JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS}, volume = {29}, number = {1}, pages = {130--137}, abstract = {Transmission through thin metal films with a periodic arrangement of tapered slits is considered. Transmission maps covering a wide range of periods, film thicknesses, and taper angles are presented. The maps show resonant transmission when fundamental and higher-order slit resonances are excited. A study of the effect on transmission of different combinations of available transmission and reflection diffraction orders show optimum total transmission when only the fundamental reflection order and higher transmission diffraction orders are available. The optimum taper angle is shown to be in the range of 6 degrees-10 degrees. Both theory and experiments show split-peak spectra and shifted-peak spectra due to interference between a slit resonance and Rayleigh-Wood anomalies. (C) 2011 Optical Society of America}, keywords = {}, pubstate = {published}, tppubtype = {article} } Transmission through thin metal films with a periodic arrangement of tapered slits is considered. Transmission maps covering a wide range of periods, film thicknesses, and taper angles are presented. The maps show resonant transmission when fundamental and higher-order slit resonances are excited. A study of the effect on transmission of different combinations of available transmission and reflection diffraction orders show optimum total transmission when only the fundamental reflection order and higher transmission diffraction orders are available. The optimum taper angle is shown to be in the range of 6 degrees-10 degrees. Both theory and experiments show split-peak spectra and shifted-peak spectra due to interference between a slit resonance and Rayleigh-Wood anomalies. (C) 2011 Optical Society of America |
2011 |
Faramarzi, V; Raimondo, C; Reinders, F; Mayor, M; Samori, P; Doudin, B Optically switchable molecular device using microsphere based junctions Journal Article In: APPLIED PHYSICS LETTERS, 99 (23), 2011, ISSN: 0003-6951. @article{faramarzi_optically_2011, title = {Optically switchable molecular device using microsphere based junctions}, author = {Faramarzi, V. and Raimondo, C. and Reinders, F. and Mayor, M. and Samori, P. and Doudin, B.}, doi = {10.1063/1.3665940}, issn = {0003-6951}, year = {2011}, date = {2011-12-01}, journal = {APPLIED PHYSICS LETTERS}, volume = {99}, number = {23}, abstract = {Metallic planar electrodes are bridged using microspheres coated with chemisorbed azobenzene self-assembled monolayers. The circuit exhibits light-induced switching, with reproducibility over 90%, as statistically determined and compared to junctions incorporating photo-insensitive alkanethiol layers. Microsphere interconnects provide direct access to molecular transport properties, with reliability and stability, making multifunctional molecular electronics devices possible. (C) 2011 American Institute of Physics. [doi:10.1063/1.3665940]}, keywords = {}, pubstate = {published}, tppubtype = {article} } Metallic planar electrodes are bridged using microspheres coated with chemisorbed azobenzene self-assembled monolayers. The circuit exhibits light-induced switching, with reproducibility over 90%, as statistically determined and compared to junctions incorporating photo-insensitive alkanethiol layers. Microsphere interconnects provide direct access to molecular transport properties, with reliability and stability, making multifunctional molecular electronics devices possible. (C) 2011 American Institute of Physics. [doi:10.1063/1.3665940] |
Chambron, Jean-Claude ; Sauvage, Jean-Pierre Transition metal-templated synthesis of catenanes and rotaxanes Journal Article In: SCIENCE CHINA-CHEMISTRY, 54 (12), pp. 2028–2031, 2011, ISSN: 1674-7291. @article{chambron_transition_2011, title = {Transition metal-templated synthesis of catenanes and rotaxanes}, author = {Chambron, Jean-Claude and Sauvage, Jean-Pierre}, doi = {10.1007/s11426-011-4420-x}, issn = {1674-7291}, year = {2011}, date = {2011-12-01}, journal = {SCIENCE CHINA-CHEMISTRY}, volume = {54}, number = {12}, pages = {2028--2031}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
Durola, Fabien ; Durot, Stephanie ; Heitz, Valerie ; Joosten, Antoine ; Sauvage, Jean-Pierre ; Trolez, Yann Formation of copper(I)-templated [2]rotaxanes using “click” methodology: influence of the base, the thread and the catalyst Journal Article In: JOURNAL OF INCLUSION PHENOMENA AND MACROCYCLIC CHEMISTRY, 71 (3-4, SI), pp. 507–515, 2011, ISSN: 1388-3127. @article{durola_formation_2011, title = {Formation of copper(I)-templated [2]rotaxanes using “click” methodology: influence of the base, the thread and the catalyst}, author = {Durola, Fabien and Durot, Stephanie and Heitz, Valerie and Joosten, Antoine and Sauvage, Jean-Pierre and Trolez, Yann}, doi = {10.1007/s10847-011-9986-6}, issn = {1388-3127}, year = {2011}, date = {2011-12-01}, journal = {JOURNAL OF INCLUSION PHENOMENA AND MACROCYCLIC CHEMISTRY}, volume = {71}, number = {3-4, SI}, pages = {507--515}, abstract = {Three new copper(I)-assembled [2]rotaxanes incorporating the same macrocycle and different axes containing a bipy, a phen or a terpy have been synthesized thanks to CuAAC reaction for attaching the stoppers. The influence of the nature of the base used for the stoppering reaction was investigated on the formation of the bipy-containing rotaxane. The yield of the [2]rotaxane synthesis was increased when using a phen as a coordinating unit in the thread with [Cu(CH3CN)(4)](PF6) as catalyst. The strong influence of the nature of the catalyst was clearly evidenced for the formation of the terpy rotaxane, increasing the yield of the stoppering reaction from 0 to 95% by just substituting the Cu(I) catalyst. Finally, the best conditions found for our systems are the use of Na2CO3 as a base and Cu(tren')Br as a catalyst.}, keywords = {}, pubstate = {published}, tppubtype = {article} } Three new copper(I)-assembled [2]rotaxanes incorporating the same macrocycle and different axes containing a bipy, a phen or a terpy have been synthesized thanks to CuAAC reaction for attaching the stoppers. The influence of the nature of the base used for the stoppering reaction was investigated on the formation of the bipy-containing rotaxane. The yield of the [2]rotaxane synthesis was increased when using a phen as a coordinating unit in the thread with [Cu(CH3CN)(4)](PF6) as catalyst. The strong influence of the nature of the catalyst was clearly evidenced for the formation of the terpy rotaxane, increasing the yield of the stoppering reaction from 0 to 95% by just substituting the Cu(I) catalyst. Finally, the best conditions found for our systems are the use of Na2CO3 as a base and Cu(tren')Br as a catalyst. |
Publications
2012 |
Self-collimation of surface plasmon beams Journal Article In: OPTICS LETTERS, 37 (11), pp. 1916–1918, 2012, ISSN: 0146-9592. |
Improving charge transport in poly(3-hexylthiophene) transistors via blending with an alkyl-substituted phenylene-thiophene-thiophene-phenylene molecule Journal Article In: JOURNAL OF POLYMER SCIENCE PART B-POLYMER PHYSICS, 50 (9), pp. 642–649, 2012, ISSN: 0887-6266. |
Hierarchical Formation of Supramolecular Transient Networks in Water: A Modular Injectable Delivery System Journal Article In: ADVANCED MATERIALS, 24 (20), pp. 2703–2709, 2012, ISSN: 0935-9648. |
Atomic Rydberg Reservoirs for Polar Molecules Journal Article In: PHYSICAL REVIEW LETTERS, 108 (19), 2012, ISSN: 0031-9007. |
Stabilized Hemiacetal Complexes as Precursors for the Controlled Release of Bioactive Volatile Alcohols Journal Article In: CHEMISTRY & BIODIVERSITY, 9 (4), pp. 689–701, 2012, ISSN: 1612-1872. |
[2]Catenanes Built Around Octahedral Transition-Metal Complexes that Contain Two Intertwined Endocyclic but Non-sterically Hindering Tridentate Ligands Journal Article In: CHEMISTRY-A EUROPEAN JOURNAL, 18 (18), pp. 5565–5573, 2012, ISSN: 0947-6539. |
Biomolecular motors: Insights from simulations Journal Article In: ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 243 , 2012, ISSN: 0065-7727. |
Biodynamers: Self-Organization-Driven Formation of Doubly Dynamic Proteoids Journal Article In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 134 (9), pp. 4177–4183, 2012, ISSN: 0002-7863. |
Excited State Properties and Energy Transfer within Dipyrrin-Based Binuclear Iridium/Platinum Dyads: The Effect of ortho-Methylation on the Spacer Journal Article In: CHEMISTRY-A EUROPEAN JOURNAL, 18 (13), pp. 4041–4050, 2012, ISSN: 0947-6539. |
Microfluidic platform for combinatorial synthesis in picolitre droplets Journal Article In: Lab on a Chip, 12 (7), pp. 1320–1326, 2012, ISSN: 1473-0189. |
A completely in vitro ultrahigh-throughput droplet-based microfluidic screening system for protein engineering and directed evolution Journal Article In: Lab on a Chip, 12 (5), pp. 882–891, 2012, ISSN: 1473-0189. |
Fano Resonances and Leakage Radiation for High-Resolution Plasmonic Sensing Journal Article In: JOURNAL OF PHYSICAL CHEMISTRY C, 116 (10), pp. 6092–6096, 2012, ISSN: 1932-7447. |
Directional coupling in channel plasmon-polariton waveguides Journal Article In: OPTICS EXPRESS, 20 (6), pp. 6124–6134, 2012, ISSN: 1094-4087. |
Tuning the Photoresponse in Organic Field-Effect Transistors Journal Article In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 134 (4), pp. 2429–2433, 2012, ISSN: 0002-7863. |
A Novel MALDI-MS Approach for the Analysis of Neutral Metallosupramolecular Architectures Journal Article In: EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, (4), pp. 647–654, 2012, ISSN: 1434-1948. |
Long vs. short-range orders in random subwavelength hole arrays Journal Article In: OPTICS EXPRESS, 20 (4), pp. 4697–4709, 2012, ISSN: 1094-4087. |
The Beauty of Knots at the Molecular Level Incollection In: {Fabbrizzi, L} (Ed.): BEAUTY IN CHEMISTRY: ARTISTRY IN THE CREATION OF NEW MOLECULES, 323 , pp. 107–125, 2012, ISBN: 978-3-642-28341-3. |
Immobilization of double functionalized carbon nanotubes on glassy carbon electrodes for the electrochemical sensing of the biotin-avidin affinity Journal Article In: JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 665 , pp. 90–94, 2012, ISSN: 1572-6657. |
Molarnet Project: Molecular Architectures for QCA-Inspired Boolean Networks Journal Article In: INTERNATIONAL JOURNAL OF UNCONVENTIONAL COMPUTING, 8 (4, SI), pp. 301–305, 2012, ISSN: 1548-7199. |
Self-assembly and electrical properties of a novel heptameric thiophene-benzothiadiazole based architectures Journal Article In: CHEMICAL COMMUNICATIONS, 48 (100), pp. 12162–12164, 2012, ISSN: 1359-7345. |
Paolo Samori Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (32), pp. 7889, 2012, ISSN: 1433-7851. |
Predicting self-assembly: from empirism to determinism Journal Article In: CHEMICAL SOCIETY REVIEWS, 41 (10), pp. 3713–3730, 2012, ISSN: 0306-0012. |
Ambipolar organic field-effect transistors with balanced mobilities through solvent-vapour annealing induced phase-separation of bi-component mixtures Journal Article In: JOURNAL OF MATERIALS CHEMISTRY, 22 (19), pp. 9509–9512, 2012, ISSN: 0959-9428. |
Charge transport in fibre-based perylene-diimide transistors: effect of the alkyl substitution and processing technique Journal Article In: NANOSCALE, 4 (7), pp. 2387–2393, 2012, ISSN: 2040-3364. |
Photoconductive and supramolecularly engineered organic field-effect transistors based on fibres from donor-acceptor dyads Journal Article In: NANOSCALE, 4 (5), pp. 1677–1681, 2012, ISSN: 2040-3364. |
Enhanced mobility in P3HT-based OTFTs upon blending with a phenylene-thiophene-thiophene-phenylene small molecule Journal Article In: CHEMICAL COMMUNICATIONS, 48 (10), pp. 1562–1564, 2012, ISSN: 1359-7345. |
Conformationally pre-organized and pH-responsive flat dendrons: synthesis and self-assembly at the liquid-solid interface Journal Article In: NANOSCALE, 4 (2), pp. 467–472, 2012, ISSN: 2040-3364. |
Strandwise translocation of a DNA glycosylase on undamaged DNA Journal Article In: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 109 (4), pp. 1086–1091, 2012, ISSN: 0027-8424. |
Self-ordering of metallogrid complexes via directed hydrogen-bonding Journal Article In: DALTON TRANSACTIONS, 41 (45), pp. 13848–13855, 2012, ISSN: 1477-9226. |
Constitutional Dynamic Chemistry: Bridge from Supramolecular Chemistry to Adaptive Chemistry Incollection In: {Barboiu, M} (Ed.): CONSTITUTIONAL DYNAMIC CHEMISTRY, 322 , pp. 1–32, 2012, ISBN: 978-3-642-28344-4 978-3-642-28343-7. |
Royal Society of Chemistry Awards Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (37), pp. 9214–9215, 2012, ISSN: 1433-7851. |
Doubly degradable dynamers: dynamic covalent polymers based on reversible imine connections and biodegradable polyester units Journal Article In: GREEN CHEMISTRY, 14 (10), pp. 2907–2911, 2012, ISSN: 1463-9262. |
Chelation-controlled molecular morphology: aminal to imine rearrangements Journal Article In: DALTON TRANSACTIONS, 41 (15), pp. 4335–4357, 2012, ISSN: 1477-9226. |
Generation of metallosupramolecular polymer gels from multiply functionalized grid-type complexes Journal Article In: NEW JOURNAL OF CHEMISTRY, 36 (3), pp. 668–673, 2012, ISSN: 1144-0546. |
Transport into Metal-Organic Frameworks from Solution Is Not Purely Diffusive Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (11), pp. 2662–2666, 2012, ISSN: 1433-7851. |
Engineered Open Systems and Quantum Simulations with Atoms and Ions Incollection In: {Arimondo, E; Berman, PR ; Lin, CC} (Ed.): ADVANCES IN ATOMIC, MOLECULAR, AND OPTICAL PHYSICS, VOL 61, 61 , pp. 1–80, 2012, ISBN: 978-0-12-396482-3. |
Copper(I)-Assembled [3]Rotaxane Whose Two Rings Act as Flapping Wings Journal Article In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 134 (3), pp. 1802–1809, 2012, ISSN: 0002-7863. |
Near-infrared dual luminescence from an extended zinc porphyrin Journal Article In: CHEMICAL COMMUNICATIONS, 48 (7), pp. 1021–1023, 2012, ISSN: 1359-7345. |
Highly Efficient Ultrafast Electron Injection from the Singlet MLCT Excited State of Copper(I) Diimine Complexes to TiO2 Nanoparticles Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (51), pp. 12711–12715, 2012, ISSN: 1433-7851. |
NIR emission of cyclic [4]rotaxanes containing pi-extended porphyrin chromophores Journal Article In: PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 14 (30), pp. 10589–10594, 2012, ISSN: 1463-9076. |
Metal-Organic Frameworks Incorporating Copper-Complexed Rotaxanes Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (9), pp. 2160–2163, 2012, ISSN: 1433-7851. |
Selective droplet coalescence using microfluidic systems Journal Article In: Lab on a Chip, 12 (10), pp. 1800, 2012, ISSN: 1473-0197, 1473-0189. |
Teaching Single-Cell Digital Analysis Using Droplet-Based Microfluidics Journal Article In: Analytical Chemistry, 84 (3), pp. 1202–1209, 2012, ISSN: 0003-2700. |
High-resolution dose–response screening using droplet-based microfluidics Journal Article In: Proceedings of the National Academy of Sciences, 109 (2), pp. 378–383, 2012, ISSN: 0027-8424, 1091-6490. |
Plasmonic Coherent Drive of an Optical Trap Journal Article In: PHYSICAL REVIEW LETTERS, 108 (2), 2012, ISSN: 0031-9007. |
Modifying Chemical Landscapes by Coupling to Vacuum Fields Journal Article In: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 51 (7), pp. 1592–1596, 2012, ISSN: 1433-7851. |
Extraordinary optical transmission with tapered slits: effect of higher diffraction and slit resonance orders Journal Article In: JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 29 (1), pp. 130–137, 2012, ISSN: 0740-3224. |
2011 |
Optically switchable molecular device using microsphere based junctions Journal Article In: APPLIED PHYSICS LETTERS, 99 (23), 2011, ISSN: 0003-6951. |
Transition metal-templated synthesis of catenanes and rotaxanes Journal Article In: SCIENCE CHINA-CHEMISTRY, 54 (12), pp. 2028–2031, 2011, ISSN: 1674-7291. |
Formation of copper(I)-templated [2]rotaxanes using “click” methodology: influence of the base, the thread and the catalyst Journal Article In: JOURNAL OF INCLUSION PHENOMENA AND MACROCYCLIC CHEMISTRY, 71 (3-4, SI), pp. 507–515, 2011, ISSN: 1388-3127. |