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Title: Detecting coherent core-hole wave-packet dynamics in N2 by time- and angle-resolved inner-shell photoelectron spectroscopy

Abstract

Here, we introduce an imaging technique to follow core-hole wave-packet oscillations in the nitrogen molecule. In this scheme, an attosecond x-ray pulse core-ionizes the nitrogen molecule and a subsequent attosecond x-ray pulse probes the evolution of the electron dynamics. We can image the oscillation of the core-hole between the two atomic sites by measuring the angular correlation between photoelectrons. Analytical relations for the angular correlation are derived based on the plane-wave approximation for the photoelectron wave function. We confirm these results with a scattering calculation for the photoelectron wave function. The feasibility of the experimental realization of this scheme is discussed in light of current and future capabilities of x-ray free-electron lasers.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [2]; ORCiD logo [3]
+ Show Author Affiliations
  1. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  2. Kansas State Univ., Manhattan, KS (United States)
  3. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States); Kansas State Univ., Manhattan, KS (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1577603
Alternate Identifier(s):
OSTI ID: 1546866
Grant/Contract Number:  
AC02-05CH11231; SC0019451; SC0019461
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 5; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Inhester, Ludger, Greenman, Loren, Rudenko, Artem, Rolles, Daniel, and Santra, Robin. Detecting coherent core-hole wave-packet dynamics in N2 by time- and angle-resolved inner-shell photoelectron spectroscopy. United States: N. p., 2019. Web. doi:10.1063/1.5109867.
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Inhester, Ludger, Greenman, Loren, Rudenko, Artem, Rolles, Daniel, & Santra, Robin. Detecting coherent core-hole wave-packet dynamics in N2 by time- and angle-resolved inner-shell photoelectron spectroscopy. United States. https://doi.org/10.1063/1.5109867
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Inhester, Ludger, Greenman, Loren, Rudenko, Artem, Rolles, Daniel, and Santra, Robin. Mon . "Detecting coherent core-hole wave-packet dynamics in N2 by time- and angle-resolved inner-shell photoelectron spectroscopy". United States. https://doi.org/10.1063/1.5109867. https://www.osti.gov/servlets/purl/1577603.
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@article{osti_1577603,
title = {Detecting coherent core-hole wave-packet dynamics in N2 by time- and angle-resolved inner-shell photoelectron spectroscopy},
author = {Inhester, Ludger and Greenman, Loren and Rudenko, Artem and Rolles, Daniel and Santra, Robin},
abstractNote = {Here, we introduce an imaging technique to follow core-hole wave-packet oscillations in the nitrogen molecule. In this scheme, an attosecond x-ray pulse core-ionizes the nitrogen molecule and a subsequent attosecond x-ray pulse probes the evolution of the electron dynamics. We can image the oscillation of the core-hole between the two atomic sites by measuring the angular correlation between photoelectrons. Analytical relations for the angular correlation are derived based on the plane-wave approximation for the photoelectron wave function. We confirm these results with a scattering calculation for the photoelectron wave function. The feasibility of the experimental realization of this scheme is discussed in light of current and future capabilities of x-ray free-electron lasers.},
doi = {10.1063/1.5109867},
journal = {Journal of Chemical Physics},
number = 5,
volume = 151,
place = {United States},
year = {Mon Aug 05 00:00:00 EDT 2019},
month = {Mon Aug 05 00:00:00 EDT 2019}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1063/1.5109867
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Cited by: 7 works
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Figures / Tables:

FIG. 1 FIG. 1: Intensity of the second photoelectron as a function of emission angle for selected delay times td and fixed emission angle of the first photoelectron and averaged over the orientation of the molecule with respect to the polarization axis. The left panel shows the angular dependence in the molecularmore » frame. The solid line shows the angular dependence when the first photoelectron has been emitted along the molecular axis (θ1 = 0). The dashed line shows the constant angular dependence when the first electron has been emitted perpendicular to the molecular axis (θ1 = π/2). The right panel shows the angular dependence in the lab frame, where the first photoelectron has been emitted along the polarization axis (Θ1 = 0). T is the core-hole oscillation period of 44.2 fs. The oscillation of the hole density from the left to the right atom is sketched in each subplot with the filled circle representing presence of the hole.« less
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