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Exploring Coherent Electron Excitation and Migration Dynamics by Electron Diffraction with Ultrashort X-Ray Pulses

Abstract

Exploring ultrafast charge migration is of great importance in biological and chemical reactions. We present a scheme to monitor attosecond charge migration in molecules by electron diffraction with spatial and temporal resolutions from \textit{ab initio} numerical simulations. An ultraviolet pulse creates a coherent superposition of electronic states, after which a time-delayed attosecond X-ray pulse is used to ionize the molecule. It is found that diffraction patterns in the X-ray photoelectron spectra show an asymmetric structure, which is dependent on the time delay between the pump-probe pulses, encoding the information of molecular orbital symmetry and chemical bonding. We describe these phenomena by developing an electronic time-dependent ultrafast molecular photoionization model of a coherent superposition state. The periodical distortion of electron diffraction patterns illustrates the evolution of the electronic coherence, providing a tool for attosecond imaging of ultrafast molecular reaction processes.

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Publication details

The article was received on 26 Jul 2017, accepted on 14 Sep 2017 and first published on 14 Sep 2017


Article type: Communication
DOI: 10.1039/C7CP05067D
Citation: Phys. Chem. Chem. Phys., 2017, Accepted Manuscript
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    Exploring Coherent Electron Excitation and Migration Dynamics by Electron Diffraction with Ultrashort X-Ray Pulses

    K. Yuan and A. D. Bandrauk, Phys. Chem. Chem. Phys., 2017, Accepted Manuscript , DOI: 10.1039/C7CP05067D

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