Probing Charge-Transfer Excited States in a Quasi-Nonluminescent Electron-Rich Fe(II)-Acetylide Complex by Femtosecond Optical Spectroscopy - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of Physical Chemistry C Année : 2012

Probing Charge-Transfer Excited States in a Quasi-Nonluminescent Electron-Rich Fe(II)-Acetylide Complex by Femtosecond Optical Spectroscopy

Résumé

Molecules with photoswitchable nonlinear optical (NLO) properties on the nanosecond time scale are attracting considerable attention as potential solid-state components of photonic devices, downsizeable at will, for ultrafast information encoding. In this context, we present here the study of an electron-rich Fe(II) 4-nitrophenylalkynyl complex which possesses a high hyperpolarizability in its singlet ground state and a negative (and presumably much decreased) NLO activity in its first excited MLCT state(s). On the basis of an ensemble of spectroscopic and time-resolved measurements we investigate the ultrafast dynamics for deactivation of the initially populated MLCT singlet state(s) of this particular organometallic complex, which are shown to decay into a metastable triplet state. The purported mechanism is rationalized with DFT calculations. We show that this triplet state, which should also exhibit a strongly diminished hyperpolarizability, is fully formed with a very high quantum yield within 15 ps.
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Dates et versions

hal-00753756 , version 1 (19-11-2012)

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Ciro d'Amico, Maciej Lorenc, Eric Collet, Katy A. Green, Karine Costuas, et al.. Probing Charge-Transfer Excited States in a Quasi-Nonluminescent Electron-Rich Fe(II)-Acetylide Complex by Femtosecond Optical Spectroscopy. Journal of Physical Chemistry C, 2012, 116 (5), pp.3719-3727. ⟨10.1021/jp208522w⟩. ⟨hal-00753756⟩
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