BERTONI, Roman; LORENC, Maciej; LAISNEY, Jerome; TISSOT, Antoine; MORÉAC, Alain; MATAR, Samir F.; BOILLOT, Marie-Laure; COLLET, Eric

doi:10.1039/C5TC00854A

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BERTONI, Roman
Institut de Physique de Rennes [IPR]

LORENC, Maciej
Institut de Physique de Rennes [IPR]

LAISNEY, Jerome
Institut de Chimie Moléculaire et des Matériaux d'Orsay [ICMMO]

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Journal of Materials Chemistry C. 2015-05-05, vol. 3, n° 30, p. 7792-7801

Royal Society of Chemistry

Resumen en inglés

We investigate light-induced excited spin-state trapping (LIESST) dynamics of an FeIII spin-crossover material from low (S=1/2) to high (S=5/2) spin states. Our results show that this process occurs only at the molecular level as evidenced by the linear dependence of the fraction of photo-switched molecules with the excitation density as well as with the initial fraction of low spin molecules. The inter-system crossing from photoexcited LS (S=1/2) to HS (S=5/2) occurs within 200 fs and is accompanied by coherent non-equilibrium vibrational relaxation in the photo-induced HS state. These results reveal similar dynamical features to those already reported for LIESST in FeII systems. The activation of coherent molecular vibrations is essential for reaching rapidly the HS potential on the timescale of molecular motions, whereas their fast damping allows an efficient trapping in the HS potential. The observed coherent oscillations are attributed to photoinduced molecules in the HS states, as supported by Raman spectroscopy at thermal equilibrium, and DFT analyses of molecular vibrations and TD-DFT calculations of optical absorption.< Leer menos

DOI

http://dx.doi.org/10.1039/C5TC00854A

Proyecto ANR

Etude femtoseconde rayons X et optique de la dynamique ultrarapide de photocommutation de matériaux moléculaires magnétiques - ANR-13-BS04-0002

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Centros de investigación

Institut de Chimie de la Matière Condensée de Bordeaux (ICMCB) - UMR 5026