Attosecond Dynamics of Molecular Electronic Ring Currents

Ultrafast charge migration is of fundamental importance to photoinduced chemical reactions. However, exploring such a quantum dynamical process requires demanding spatial and temporal resolutions. We show how electronic coherence dynamics induced in molecules by a circularly polarized UV pulse can b...

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Bibliographic Details
Published in:The journal of physical chemistry letters 2017-05, Vol.8 (10), p.2229-2235
Main Authors: Yuan, Kai-Jun, Shu, Chuan-Cun, Dong, Daoyi, Bandrauk, André D
Format: Article
Language:English
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Summary:Ultrafast charge migration is of fundamental importance to photoinduced chemical reactions. However, exploring such a quantum dynamical process requires demanding spatial and temporal resolutions. We show how electronic coherence dynamics induced in molecules by a circularly polarized UV pulse can be tracked by using a time-delayed circularly polarized attosecond X-ray pulse. The X-ray probe spectra retrieve an image at different time delays, encoding instantaneous pump-induced circular charge migration information on an attosecond time scale. A time-dependent ultrafast electronic coherence associated with the periodical circular ring currents shows a strong dependence on the helicity of the UV pulse, which may provide a direct approach to access and control the electronic quantum coherence dynamics in photophysical and photochemical reactions in real time.
ISSN:1948-7185
1948-7185
DOI:10.1021/acs.jpclett.7b00877