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Issue 38, 2017
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Exploring coherent electron excitation and migration dynamics by electron diffraction with ultrashort X-ray pulses

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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 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.

Graphical abstract: Exploring coherent electron excitation and migration dynamics by electron diffraction with ultrashort X-ray pulses

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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., 2017,19, 25846-25852
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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, 19, 25846
    DOI: 10.1039/C7CP05067D

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