This work demonstrates the possibility of modulating the spin state of the FeII sites and subsequently the magnetic properties of a [2×2] FeII grid-like complex by variation of the degree of deprotonation of the hydrazine-based N-H sites of the ligand in the complex. Evidence has been provided, both in the solid state and in solution, towards understanding the strong influence of the spin-crossover process on the pKas of the grid ligands, which exhibit a unique deprotonation pattern. The present study provides a demonstration of the effect of spin state switching of a chemical property, here on ligand pKa in a metallosupramolecular grid.
Sébastien Dhers, Abhishake Mondal, David Aguilà, Juan Ramírez, Sergi Vela, Pierre Dechambenoit, Mathieu Rouzières, Jonathan R. Nitschke, Rodolphe Clérac & Jean-Marie Lehn. Spin State Chemistry: Modulation of Ligand pKa by Spin State Switching in a [2×2] Iron(II) Grid-Type Complex J. Am. Chem. Soc. 2018, 140 (26), pp 8218–8227 DOI : 10.1021/jacs.8b03735
Incorporating functional molecules into sensor devices is an emerging area in molecular electronics that aims at exploiting the sensitivity of different molecules to their environment and turning it into an electrical signal. Among the emergent and integrated sensors, microelectromechanical systems (MEMS) are promising for their extreme sensitivity to mechanical events. However, to bring new functions to these devices, the functionalization of their surface with molecules is required. Herein, we present original electronic devices made of an organic microelectromechanical resonator functionalized with switchable magnetic molecules. The change of their mechanical properties and geometry induced by the switching of their magnetic state at a molecular level alters the device’s dynamical behavior, resulting in a change of the resonance frequency. We demonstrate that these devices can be operated to sense light or thermal excitation. Moreover, thanks to the collective interaction of the switchable molecules, the device behaves as a non-volatile memory. Our results open up broad prospects of new flexible photo- and thermo-active hybrid devices for molecule-based data storage and sensors.
Matias Urdampilleta, Cedric Ayela,
Pierre-Henri Ducrot, Daniel Rosario-Amorin, Abhishake Mondal, Mathieu
Rouzières, Pierre Dechambenoit, Corine Mathonière, Fabrice Mathieu, Isabelle
Dufour et Rodolphe Clérac Molecule-based microelectromechanical sensors Scientific Reports – Mai 2018 DOI: 10.1038/s41598-018-26076-2
A new multi-switchable complex has been
rationally assembled using a redox-active and strongly complexing
bridging ligand. By simple oxidation/reduction, its magnetic properties
can be tuned from a spin-crossover complex, to a single-molecule magnet
with an S = 5/2 spin ground state (when once reduced) and to
diamagnetic species when twice reduced. This work illustrates
experimentally and theoretically how successive redox processes can
increase the spin delocalization, and thus promote a dramatic
enhancement of the intramolecular magnetic coupling through a bridging
ligand, not only in its radical form. This general synthetic approach
should help for the intentional design of new high-spin complexes and
SMMs, but it could also be extended to systems with higher nuclearities
and dimension- alities, for example to obtain high-temperature molecule-
Xiaozhou Ma, Elizaveta A. Suturina, Siddhartha De, Philippe Négrier, Mathieu Rouzières, Rodolphe Clérac et Pierre Dechambenoit Redox-Active Bridging Ligand as a Tool to Promote Spin Delocalization, High Spin Complexes and Magnetic Multi-Switchability Angewandte Chemie International Edition – Avril 2018 DOI: 10.1002/anie.201803842
Maître de Conférences / Associate professor, University of Bordeaux – IUT HSE (EH&S)
Place and date of Birth: Mulhouse (Haut Rhin, France) 25 Mars 1982 Institutional address: Centre de Recherche Paul Pascal CRPP – CNRS UMR5031 Research team M3 115, avenue du Dr. A. Schweitzer 33600 Pessac, France
Ph. D. at the University Louis Pasteur in Strasbourg, Prof. M. W. Hosseini and Dr. S. Ferlay
DEA of Transition Metal Chemistry and Molecular Engineering, Mention Bien (Strasbourg)
2003 – 2004
Licence and Maitrise of Chemistry (Strasbourg)
2001 – 2002
DEUG in Science of the matter, Mention Très Bien (1st) (Strasbourg)
2009 – 2010
Post-doctoral Research Associate at the University of California Berkeley, (USA), Prof J. R. Long
Author or co-author of 52 research papers published in refereed journals (h factor = 22).
. X. Ma, E. A. Suturina, M. Rouzières, F. Wilhelm, A. Rogalev, R. Clérac and P. Dechambenoit,“A heteroleptic diradical Cr(III) complex with extended spin delocalization and large intramolecular magnetic exchange”, Chem. Commun., 56, 4906-4909, (2020) – 10.1039/d0cc00548g
. X. Ma, E. A. Suturina, M. Rouzières, M. Platunov, F. Wilhelm, A. Rogalev, R. Clérac, P. Dechambenoit, “Using Redox-Active π Bridging Ligand as a Control Switch of Intramolecular Magnetic Interactions”, J. Am. Chem. Soc., 141, 7721-7725 (2019) – 10.1021/jacs.9b03044
. X. Ma, E. A. Suturina, S. De, P. Négrier, M. Rouzières, R. Clérac, P. Dechambenoit, “A Redox-Active Bridging Ligand to Promote Spin Delocalization, High-Spin Complexes, and Magnetic Multi-Switchability”, Angew. Chem. Int. Ed., 57, 7841-7845 (2018) – 10.1002/anie.201803842
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