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Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses.

Abstract：

:Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor-acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.

journal_name

Nat Commun

journal_title

Nature communications

authors

Canton SE,Kjær KS,Vankó G,van Driel TB,Adachi S,Bordage A,Bressler C,Chabera P,Christensen M,Dohn AO,Galler A,Gawelda W,Gosztola D,Haldrup K,Harlang T,Liu Y,Møller KB,Németh Z,Nozawa S,Pápai M,Sato T,Sato T,Su

doi

10.1038/ncomms7359

subject

Has Abstract

pub_date

2015-03-02 00:00:00

pages

6359

issn

2041-1723

pii

ncomms7359

journal_volume

6

pub_type

杂志文章

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