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Title: Simulation of X-ray transient absorption for following vibrations in coherently ionized F2 molecules

Abstract

We report femtosecond and attosecond X-ray transient absorption experiments are becoming increasingly sophisticated tools for probing nuclear dynamics. In this work, we explore and develop theoretical tools needed for interpretation of such spectra,in order to characterize the vibrational coherences that result from ionizing a molecule in a strong IR field. Ab initio data for F2 is combined with simulations of nuclear dynamics, in order to simulate time-resolved X-ray absorption spectra for vibrational wavepackets after coherent ionization at 0 K and at finite temperature. Dihalogens pose rather difficult electronic structure problems, and the issues encountered in this work will be reflective of those encountered with any core–valence excitation simulation when a bond is breaking. The simulations reveal a strong dependence of the X-ray absorption maximum on the locations of the vibrational wave packets. A Fourier transform of the simulated signal shows features at the overtone frequencies of both the neutral and the cation, which reflect spatial interferences of the vibrational eigenstates. This provides a direct path for implementing ultrafast X-ray spectroscopic methods to visualize coherent nuclear dynamics.

Authors:
 [1];  [2]
+ Show Author Affiliations
  1. University of the Pacific, Stockton, CA (United States)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF)
OSTI Identifier:
1532223
Alternate Identifier(s):
OSTI ID: 1419141
Grant/Contract Number:  
AC02-05CH11231; CHE-1361226
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Physics
Additional Journal Information:
Journal Volume: 482; Journal Issue: C; Journal ID: ISSN 0301-0104
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Dutoi, Anthony D., and Leone, Stephen R. Simulation of X-ray transient absorption for following vibrations in coherently ionized F2 molecules. United States: N. p., 2016. Web. doi:10.1016/j.chemphys.2016.10.006.
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Dutoi, Anthony D., & Leone, Stephen R. Simulation of X-ray transient absorption for following vibrations in coherently ionized F2 molecules. United States. https://doi.org/10.1016/j.chemphys.2016.10.006
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Dutoi, Anthony D., and Leone, Stephen R. Thu . "Simulation of X-ray transient absorption for following vibrations in coherently ionized F2 molecules". United States. https://doi.org/10.1016/j.chemphys.2016.10.006. https://www.osti.gov/servlets/purl/1532223.
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@article{osti_1532223,
title = {Simulation of X-ray transient absorption for following vibrations in coherently ionized F2 molecules},
author = {Dutoi, Anthony D. and Leone, Stephen R.},
abstractNote = {We report femtosecond and attosecond X-ray transient absorption experiments are becoming increasingly sophisticated tools for probing nuclear dynamics. In this work, we explore and develop theoretical tools needed for interpretation of such spectra,in order to characterize the vibrational coherences that result from ionizing a molecule in a strong IR field. Ab initio data for F2 is combined with simulations of nuclear dynamics, in order to simulate time-resolved X-ray absorption spectra for vibrational wavepackets after coherent ionization at 0 K and at finite temperature. Dihalogens pose rather difficult electronic structure problems, and the issues encountered in this work will be reflective of those encountered with any core–valence excitation simulation when a bond is breaking. The simulations reveal a strong dependence of the X-ray absorption maximum on the locations of the vibrational wave packets. A Fourier transform of the simulated signal shows features at the overtone frequencies of both the neutral and the cation, which reflect spatial interferences of the vibrational eigenstates. This provides a direct path for implementing ultrafast X-ray spectroscopic methods to visualize coherent nuclear dynamics.},
doi = {10.1016/j.chemphys.2016.10.006},
journal = {Chemical Physics},
number = C,
volume = 482,
place = {United States},
year = {Thu Oct 06 00:00:00 EDT 2016},
month = {Thu Oct 06 00:00:00 EDT 2016}
}
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https://doi.org/10.1016/j.chemphys.2016.10.006
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    Works referencing / citing this record:

    Ab initio investigation of Br-3 d core-excited states in HBr and HBr + toward XUV probing of photochemical dynamics
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