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31.
Rational Topological Design for Fluorescence Enhancement upon Aggregation of Distyrylfuran Derivatives
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Dr. Charlotte Mallet Dr. Chady Moussallem Alexandre Faurie Magali Allain Dr. Frédéric Gohier Prof. William G. Skene Prof. Pierre Frère 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(21):7944-7953
A series of 2,5‐distyrylfuran derivatives bearing pentafluorophenyl‐ and cyanovinyl units have been synthesized for aggregation‐induced emission (AIE). The effect of the type and extent of the supramolecular connections on the AIE of the furan derivatives were examined and correlated with their X‐ray crystal structures. It was found that the simultaneous presence of cyano and perfluorophenyl units strongly enhances the fluorescence upon aggregation. Single‐crystal X‐ray diffraction analysis confirmed that C?H???F, F???F, C?H???nitrile, Ar???ArF (Ar=aryl, ArF=fluoroaryl), and nitrile???ArF intra‐ and intermolecular interactions drive the topology of the molecule and that solid‐state supramolecular contacts favor AIE of the furan derivatives. 相似文献
32.
Andreu R Cerdán MA Franco S Garín J Marco AB Orduna J Palomas D Villacampa B Alicante R Allain M 《Organic letters》2008,10(21):4963-4966
Replacement of the tricyanofuran (TCF) acceptor by its stronger analogue CF 3-TCF results in decreased second-order optical nonlinearities in merocyanines bearing a proaromatic 1,3-dithiole donor. The TCF-containing derivatives display exceptionally high mu beta values up to 31,000 x 10(-48) esu, unprecedented for 1,3-dithiole-based NLO-phores. 相似文献
33.
Alías S Andreu R Blesa MJ Cerdán MA Franco S Garín J López C Orduna J Sanz J Alicante R Villacampa B Allain M 《The Journal of organic chemistry》2008,73(15):5890-5898
A short, high-yielding route to omega-dithiafulvenylpolyenals (1) via the corresponding iminium salts (2) and starting from trimethyl-1,3-dithiolium tetrafluoroborate is reported. The Knoevenagel reactions of either 1 or 2 with isoxazolone-containing acceptors afford merocyanines 7 and 9, in a process that is often accompanied by a vinylene-shortening side reaction. Experimental and theoretical studies reveal that compounds 7 and 9, featuring two proaromatic end groups, are strongly polarized and show good second-order nonlinear optical responses. 相似文献
34.
Vuagnoux-d'Augustin M Alexakis A 《Chemistry (Weinheim an der Bergstrasse, Germany)》2007,13(34):9647-9662
Me3Al, Et3Al, and vinylalane species undergo enantioselective conjugate addition to a wide range of 2- or 3-substituted enones (cyclopent-2-enones, cyclohex-2-enones, 3-methyl cyclohept-2-enone) in the presence of catalytic amount of copper salt (copper thiophene carboxylate, [Cu(CH3CN)4]BF4 or [CuOTf]2C6H6) and tropos-phosphoramidite-based ligand. Thus, chiral quaternary centers can be built, with up to 98% ee after rigorous optimization of experimental conditions. It was shown that the main important parameter was the order of the introduction of the reagents. Then, the generated enantioenriched aluminium enolates and the chiral conjugate adducts were functionalized and used for subsequent reactions. 相似文献
35.
Duvail M Souaille M Spezia R Cartailler T Vitorge P 《The Journal of chemical physics》2007,127(3):034503
Pair interaction potentials (IPs) were defined to describe the La(3+)-OH(2) interaction for simulating the La(3+) hydration in aqueous solution. La(3+)-OH(2) IPs are taken from the literature or parametrized essentially to reproduce ab initio calculations at the second-order Moller-Plesset level of theory on La(H(2)O)(8) (3+). The IPs are compared and used with molecular dynamics (MD) including explicit polarization, periodic boundary conditions of La(H(2)O)(216) (3+) boxes, and TIP3P water model modified to include explicit polarization. As expected, explicit polarization is crucial for obtaining both correct La-O distances (r(La-O)) and La(3+) coordination number (CN). Including polarization also modifies hydration structure up to the second hydration shell and decreases the number of water exchanges between the La(3+) first and second hydration shells. r(La-O) ((1))=2.52 A and CN((1))=9.02 are obtained here for our best potential. These values are in good agreement with experimental data. The tested La-O IPs appear to essentially account for the La-O short distance repulsion. As a consequence, we propose that most of the multibody effects are correctly described by the explicit polarization contributions even in the first La(3+) hydration shell. The MD simulation results are slightly improved by adding a-typically negative 1r(6)-slightly attractive contribution to the-typically exponential-repulsive term of the La-O IP. Mean residence times are obtained from MD simulations for a water molecule in the first (1082 ps) and second (7.6 ps) hydration shells of La(3+). The corresponding water exchange is a concerted mechanism: a water molecule leaving La(H(2)O)(9) (3+) in the opposite direction to the incoming water molecule. La(H(2)O)(9) (3+) has a slightly distorded "6+3" tricapped trigonal prism D(3h) structure, and the weakest bonding is in the medium triangle, where water exchanges take place. 相似文献
36.
Brasseur R Braun N El Kirat K Deleu M Mingeot-Leclercq MP Dufrêne YF 《Langmuir : the ACS journal of surfaces and colloids》2007,23(19):9769-9772
Under specific conditions, lipid membranes form ripple phases with intriguing nanoscale undulations. Here, we show using in situ atomic force microscopy (AFM) that the biologically important surfactin lipopeptide induces nanoripples of 30 nm periodicity in dipalmitoyl phosphatidylcholine (DPPC) bilayers at 25 degrees (i.e. well below the pretransition temperature of DPPC). Whereas most undulations formed the classical straight orientation with characteristic angle changes of 120 degrees , some of them also displayed unusual circular orientations. Strikingly, ripple structures were formed at 15% surfactin but were rarely or never observed at 5 and 30% surfactin, emphasizing the important role played by the surfactin concentration. Theoretical simulations corroborated the AFM data by revealing the formation of stable surfactin/lipid assemblies with positive curvature. 相似文献
37.
Magali Cassebras Sagrario Pascual Alain Polton Michel Tardi Jean‐Pierre Vairon 《Macromolecular rapid communications》1999,20(5):261-264
Di‐ and triblock copolymers of styrene and butyl acrylate with controlled molar masses (Mn up to ≈ 105) were sequentially prepared by radical atom transfer polymerization in a homogeneous medium using chlorine end capped polymers as initiators and the copper(I) chloride/bipyridine complex as catalyst, in the presence of dimethylformamide. Random poly(styrene‐co‐butyl acrylate) was synthesized and the cross‐over reactions between Cl end capped polystyrene and poly(butyl acrylate) to the opposite monomers were examined. 相似文献
38.
Magali Asquier Philippe Colomban Vronique Milande 《Journal of Raman spectroscopy : JRS》2009,40(11):1641-1644
The conservation of ceramics and glass involves the repair or the restoration of broken and fragmented artefacts with polymer adhesives and gap fillers. In the past, many different adhesives had been used. Re‐restoration is often required and the fast identification of adhesive residues on objects would be very useful to define the best of way to remove them, in particular to avoid the use of noxious chemicals. Sixteen pottery artefacts restored during the 19th and 20th centuries at the Musée National de Céramique in Sèvres have been analysed by non‐destructive Raman microspectroscopy. For comparison purposes, the artefacts were also sampled in order to acquire infrared (IR) absorption spectra in KBr pellets. Modern adhesives (methyl metacrylate/acrylate, vinyl acetate, polychloroprene, methyl 2‐cyanoacrylate and diglycidylether biphenol) were also characterised with the same methods. IR and Raman spectra were obtained for all ancient glue residues, but among the 16 analysed items, only 7 adhesives have been identified unambiguously, and an assignment proposed for 4 others solely on the basis of the Raman signature. Copyright © 2009 John Wiley & Sons, Ltd. 相似文献
39.
Katherine Nott Michel Paquot Samuel Dufour Marc Eeman Magali Deleu 《Colloids and surfaces. B, Biointerfaces》2009,69(2):268-275
Three kinds of derivatives of the M1 factor of virginiamycin have been synthesised: esters with long chain fatty acids, oximes with modified polar amino acids and bis-derivatives with both the ester and oxime function. The study of the surface tension time dependence of M1 and its derivatives has shown that it is necessary to enhance simultaneously the hydrophobicity and the hydrophilicity of M1 to render M1 surface-active. A structure/function relationship study of the surface-active bis-derivatives has shown that enhancing the hydrophobicity of the molecule led to slower adsorption kinetics, higher stability of the monolayers formed and a better capacity to penetrate a membrane model. The repulsive electrostatic forces due to the presence of charges on the amino acids linked to M1 lead to higher surface tensions, a greater molecular area at the interface and lower penetration into a membrane model.This study has demonstrated that modifying systematically the hydrophobicity and hydrophilicity of a non surface-active molecule allows the production of surface-active derivatives. 相似文献
40.
Magali Mercier 《Journal of Mathematical Analysis and Applications》2009,350(1):369-383
Motivated by the modelling of a roundabout, we are led to study the traffic on a road with points of entry and exit. In this note, we would like to describe the modellisation of a junction and solve the Riemann problem for such a model. More precisely, between each point of discontinuity we use a multi-class extension of the LWR model to describe the evolution of the density of the vehicles, the ‘multi-class’ approach being used in order to distinguish the vehicles after their origin and destination. Then, we treat the points of entry and exit thanks to special boundary conditions that give bounds on the flows of the different types of vehicles. In the case of the one-T road we obtain a result of existence and uniqueness. This first step allows us to obtain a similar result for the n-T road. We describe these results and also some properties of the obtained solutions, in order to see how long this model is valid. 相似文献