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Optically Controlled Electron Transfer in a ReI Complex.

ABSTRACT: Ultrafast optical control of intramolecular charge flow was demonstrated, which paves the way for photocurrent modulation and switching with a highly wavelength-selective ON/OFF ratio. The system that was explored is a fac-[Re(CO)3 (TTF-DPPZ)Cl] complex, where TTF-DPPZ=4',5'-bis(propylthio)tetrathiafulvenyl[i]dipyrido[3,2-a:2',3'-c]phenazine. DFT calculations and AC-Stark spectroscopy confirmed the presence of two distinct optically active charge-transfer processes, namely a metal-to-ligand charge transfer (MLCT) and an intra-ligand charge transfer (ILCT). Ultrafast transient absorption measurements showed that the ILCT state decays in the ps regime. Upon excitation to the MLCT state, only a long-lived 3 MLCT state was observed after 80 ps. Remarkably, however, the bleaching of the ILCT absorption band remained as a result of the effective inhibition of the HOMO-LUMO transition.

SUBMITTER: Rohwer EJ 

PROVIDER: S-EPMC8719466 | biostudies-literature | 2021 Mar

REPOSITORIES: biostudies-literature

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Optically Controlled Electron Transfer in a Re<sup>I</sup> Complex.

Rohwer Egmont J EJ   Geng Yan Y   Akbarimoosavi Maryam M   Daku Latévi M Lawson LML   Aleveque Olivier O   Levillain Eric E   Hauser Jürg J   Cannizzo Andrea A   Häner Robert R   Decurtins Silvio S   Stanley Robert J RJ   Feurer Thomas T   Liu Shi-Xia SX  

Chemistry (Weinheim an der Bergstrasse, Germany) 20210224 17

Ultrafast optical control of intramolecular charge flow was demonstrated, which paves the way for photocurrent modulation and switching with a highly wavelength-selective ON/OFF ratio. The system that was explored is a fac-[Re(CO)<sub>3</sub> (TTF-DPPZ)Cl] complex, where TTF-DPPZ=4',5'-bis(propylthio)tetrathiafulvenyl[i]dipyrido[3,2-a:2',3'-c]phenazine. DFT calculations and AC-Stark spectroscopy confirmed the presence of two distinct optically active charge-transfer processes, namely a metal-to-  ...[more]

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