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1. A zinc(II) tetraphenylporphyrin peripherally functionalized with redox-active 'trans-[(η5-C5H5)Fe(η5-C5H4)C C](κ2-dppe)2Ru(C C)-' substituents: Linear electrochromism and third-order nonlinear optics

Author

Frédéric Paul, Marie P. Cifuentes, Mark G. Humphrey, Areej Merhi, Guillaume Grelaud, Adam Barlow, Nicolas Ripoche, Christine O. Paul-Roth, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Research School of Chemistry, Australian National University (ANU), Organométalliques: Matériaux et Catalyse, Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR), F.P. and C.O. P.-R. thank the 'Université Européenne de Bretagne' (UEB), the CNRS (PICS program N° 5676), and FEDER via an EPT grant in the 'MITTSI' program from RTR BRESMAT for financial support. M.G.H. and M.P.C. thank the Australian Research Council for financial support, an Australian Professorial Fellowship (M.G.H.) and an Australian Research Fellowship (M.P.C.), A.M., N.R. and G.G thank the 'Région Bretagne' (ARED) for financial support., Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Institut des Sciences Chimiques de Rennes (ISCR), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Rennes (UR)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Electrochromism, Chemistry, chemistry.chemical_element, [CHIM.MATE]Chemical Sciences/Material chemistry, Zinc, Chromophore, Photochemistry, Porphyrin, Redox, Inorganic Chemistry, Metal, chemistry.chemical_compound, Ferrocene, π-Conjugation, visual_art, Alkynyl complex, Tetraphenylporphyrin, Polymer chemistry, Materials Chemistry, visual_art.visual_art_medium, Physical and Theoretical Chemistry
Abstract

Dedicated to Dr. Claude Lapinte on the occasion of his retirement, in memory of the good times spent together in France and Australia.; International audience; A nonametallic organometallic-coordination complex (4), assembled from redox-active ferrocenyl (Fc) and Ru(κ2-dppe)2 fragments (dppe = 1,2-bis(diphenylphosphino)ethane) as peripheral donor groups and a central Zn(II) tetraphenylporphyrin (ZnTPP) core, has been prepared and characterized. Complex 4 is obtained in one step from a pentametallic organometallic porphyrin precursor following substitution of the peripheral chloride ligands by ferrocenylalkynyl moieties (Ctriple bond; length of mdashCFc). The spectroelectrochemistry of 4, and that of previously reported porphyrins featuring related peripheral electron-rich d6-transition metal alkynyl units, has been investigated; the optical and redox properties of 4 are briefly discussed, and its potential, and that of a related pentanuclear tetraferrocenyl ZnTPP complex, to function as redox-switchable chromophores is examined. Preliminary studies of the cubic NLO properties of 4 have been undertaken by Z-scan studies at 560 nm and 630 nm, the results from which are also reported.

Published
2015
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2. Cubic nonlinear optical properties of new zinc tetraphenyl porphyrins peripherally functionalized with electron-rich Ru(II) alkynyl substituents

Author

Marek Samoc, Areej Merhi, Katarzyna Matczyszyn, Małgorzata Wielgus, Christine O. Paul-Roth, Samuel Drouet, Frédéric Paul, Marie P. Cifuentes, Joanna Olesiak-Banska, Mark G. Humphrey, Dandan Yao, Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Australian National University (ANU), Institute of Physical and Theoretical Chemistry, Wroclaw University of Science and Technology, Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES), Université Européenne de Bretagne (UEB), FEDER, RTR BRESMAT, CNRS [5676], Ministère National de la Recherche et de la Technologie (MNERT), Région Bretagne, China Scholarship Council (CSC), Foundation for Polish Science Welcome grant, Polish Ministry of Science and Higher Education, Australian Research Council, ARC, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)

Subjects
Nonlinear optics, ORGANIC MATERIALS, Stereochemistry, chemistry.chemical_element, Zinc, Electron, 010402 general chemistry, 01 natural sciences, Biochemistry, Chemical reaction, Porphyrin, RUTHENIUM COMPLEXES, chemistry.chemical_compound, ORGANOMETALLIC COMPLEXES, Polarizability, ARYL GROUP, FLUORENONE PENDANT ARMS, Drug Discovery, Tetraphenylporphyrin, DENDRIMERS, Pi-conjugation, [CHIM.ORGA]Chemical Sciences/Organic chemistry, 010405 organic chemistry, Organic Chemistry, Organometallics, Block (periodic table), DIMERS, 3. Good health, 0104 chemical sciences, Crystallography, 2-PHOTON ABSORPTION, chemistry, METAL-COMPLEXES, 3RD-ORDER, Acetylide complex
Abstract

We report the synthesis and characterization of new organometallic assemblies consisting of a central Zn(II) tetraphenylporphyrin (ZnTPP) core surrounded by four Ru(II) alkynyl complexes ( trans -Ru(dppe) 2 R) appended at the para phenyl positions and acting as peripheral donor groups. The synthesis of the tetra-chlorido derivative 2 (R=Cl) is reported first, followed by that of three extended homologues ( 3 –X) obtained from this building block by substitution of the chlorido ligands by functionalized arylacetylenes (R=C C(4-C 6 H 4 X); X=NO 2 , H, OMe). Measurement of the nonlinear absorption properties of the pentametallic derivatives 3 –X reveals that these extended π-networks incorporating polarizable organometallic units behave as good two-photon absorbers in the visible and near-IR range.

Published
2012
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3. Spectrin-like repeats 11-15 of human dystrophin show adaptations to a lipidic environment

Author

Joe Sarkis, Elisabeth Le Rumeur, Julien Jardin, Estelle Robert, Jean-François Hubert, Angélique Chéron, Véronique Vié, Eric Hitti, Baptiste Legrand, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Interactions cellulaires et moléculaires (ICM), Université européenne de Bretagne - European University of Brittany (UEB), Science et Technologie du Lait et de l'Oeuf (STLO), Institut National de la Recherche Agronomique (INRA)-AGROCAMPUS OUEST, Institut national d'enseignement supérieur pour l'agriculture, l'alimentation et l'environnement (Institut Agro)-Institut national d'enseignement supérieur pour l'agriculture, l'alimentation et l'environnement (Institut Agro), Laboratoire Traitement du Signal et de l'Image (LTSI), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National de la Santé et de la Recherche Médicale (INSERM), This work was supported by the 'Association Française contre les Myopathies'and by RTR-BRESMAT (Université Européenne de Bretagne)., De Villemeur, Hervé, Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Université de Rennes (UR)-Institut National de la Santé et de la Recherche Médicale (INSERM), Centre National de la Recherche Scientifique (CNRS)-IFR140-Université de Rennes 1 (UR1), and Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)

Subjects
Models, Molecular, myopathie de duchenne, muscle, homology modeling, Molecular Conformation, MESH: Trypsin, MESH: Protein Structure, Secondary, Microscopy, Atomic Force, Biochemistry, Protein Structure, Secondary, Dystrophin, MESH: Protein Structure, Tertiary, 0302 clinical medicine, Protein structure, Spectrin, Trypsin, Cytoskeleton, membrane, Phospholipids, MESH: Microscopy, Atomic Force, 0303 health sciences, Liposome, atomic force microscopy, [PHYS.PHYS.PHYS-BIO-PH] Physics [physics]/Physics [physics]/Biological Physics [physics.bio-ph], Vesicle, monocouche, MESH: Spectrin, MESH: Gene Expression Regulation, Lipids, medicine.anatomical_structure, lipidic environment, MESH: Models, Molecular, muscular dystrophy, spectrométrie infrarouge, Surface Properties, [PHYS.PHYS.PHYS-BIO-PH]Physics [physics]/Physics [physics]/Biological Physics [physics.bio-ph], interaction, MEMBRANE, DYSTROPHIN, spectrin-like repeat, label-free quantification, interfacial properties, dystrophin, phospholipid, lipid-binding protein, Biology, 03 medical and health sciences, MESH: Dystrophin, Membrane Biology, medicine, [SDV.BBM] Life Sciences [q-bio]/Biochemistry, Molecular Biology, Humans, [SDV.BBM]Life Sciences [q-bio]/Biochemistry, Molecular Biology, Molecular Biology, 030304 developmental biology, MESH: Surface Properties, MESH: Phospholipids, MESH: Molecular Conformation, Sarcolemma, MESH: Humans, Skeletal muscle, Cell Biology, MESH: Lipids, Protein Structure, Tertiary, Gene Expression Regulation, Liposomes, Biophysics, biology.protein, MESH: Liposomes, 030217 neurology & neurosurgery
Abstract

International audience; Dystrophin is essential to skeletal muscle function and confers resistance to the sarcolemma by interacting with cytoskeleton and membrane. In the present work, we characterized the behavior of dystrophin 11-15 (DYS R11-15), five spectrin-like repeats from the central domain of human dystrophin, with lipids. DYS R11-15 displays an amphiphilic character at the liquid/air interface while maintaining its secondary α-helical structure. The interaction of DYS R11-15 with small unilamellar vesicles (SUVs) depends on the lipid nature, which is not the case with large unilamellar vesicles (LUVs). In addition, switching from anionic SUVs to anionic LUVs suggests the lipid packing as a crucial factor for the interaction of protein and lipid. The monolayer model and the modulation of surface pressure aim to mimic the muscle at work (i.e. dynamic changes of muscle membrane during contraction and relaxation) (high and low surface pressure). Strikingly, the lateral pressure modifies the protein organization. Increasing the lateral pressure leads the proteins to be organized in a regular network. Nevertheless, a different protein conformation after its binding to monolayer is revealed by trypsin proteolysis. Label-free quantification by nano-LC/MS/MS allowed identification of the helices in repeats 12 and 13 involved in the interaction with anionic SUVs. These results, combined with our previous studies, indicate that DYS R11-15 constitutes the only part of dystrophin that interacts with anionic as well as zwitterionic lipids and adapts its interaction and organization depending on lipid packing and lipid nature. We provide strong experimental evidence for a physiological role of the central domain of dystrophin in sarcolemma scaffolding through modulation of lipid-protein interactions.

Published
2011
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