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Title: Detecting coherent core-hole wave-packet dynamics in N 2 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]
  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) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE
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.
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. doi:10.1063/1.5109867.
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. doi:10.1063/1.5109867.
@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 = {2019},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
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Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses
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Auger-induced charge migration
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Vibrationally Resolved O 1 s Photoelectron Spectrum of CO 2 : Vibronic Coupling and Dynamic Core-Hole Localization
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Watching energy transfer in metalloporphyrin heterodimers using stimulated X-ray Raman spectroscopy
journal, September 2013

  • Biggs, J. D.; Zhang, Y.; Healion, D.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 39
  • DOI: 10.1073/pnas.1308604110

Exploring coherent electron excitation and migration dynamics by electron diffraction with ultrashort X-ray pulses
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Attosecond Hole Migration in Benzene Molecules Surviving Nuclear Motion
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    Works referencing / citing this record:

    Molpro: a general-purpose quantum chemistry program package: Molpro
    journal, July 2011

    • Werner, Hans-Joachim; Knowles, Peter J.; Knizia, Gerald
    • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 2
    • DOI: 10.1002/wcms.82

    Vibronic coupling and symmetry breaking in core electron ionization
    journal, October 1977


    Ultrafast charge migration in 2-phenylethyl-N,N-dimethylamine
    journal, January 2008

    • Lünnemann, Siegfried; Kuleff, Alexander I.; Cederbaum, Lorenz S.
    • Chemical Physics Letters, Vol. 450, Issue 4-6
    • DOI: 10.1016/j.cplett.2007.11.031

    Double core–hole correlation satellite spectra of N2 and CO molecules
    journal, January 2012


    Time-Resolved Photoelectron Imaging of Molecular Coherent Excitation and Charge Migration by Ultrashort Laser Pulses
    journal, February 2018

    • Yuan, Kai-Jun; Bandrauk, André D.
    • The Journal of Physical Chemistry A, Vol. 122, Issue 8
    • DOI: 10.1021/acs.jpca.7b11669

    Ultrafast X-ray Photoelectron Imaging of Attosecond Electron Dynamics in Molecular Coherent Excitation
    journal, November 2018

    • Yuan, Kai-Jun; Bandrauk, André D.
    • The Journal of Physical Chemistry A, Vol. 123, Issue 7
    • DOI: 10.1021/acs.jpca.8b12313

    Symmetry-Selective Observation of the N 1s Shape Resonance in N 2
    journal, June 2001

    • Hergenhahn, U.; Kugeler, O.; Rüdel, A.
    • The Journal of Physical Chemistry A, Vol. 105, Issue 23
    • DOI: 10.1021/jp0038456

    Symmetry Breaking and Hole Localization in Multiple Core Electron Ionization
    journal, July 2013

    • Carravetta, V.; Ågren, H.
    • The Journal of Physical Chemistry A, Vol. 117, Issue 31
    • DOI: 10.1021/jp406602y

    Attosecond Hole Migration in Benzene Molecules Surviving Nuclear Motion
    journal, January 2015

    • Despré, V.; Marciniak, A.; Loriot, V.
    • The Journal of Physical Chemistry Letters, Vol. 6, Issue 3
    • DOI: 10.1021/jz502493j

    Isotope-induced partial localization of core electrons in the homonuclear molecule N2
    journal, September 2005

    • Rolles, Daniel; Braune, Markus; Cvejanović, Slobodan
    • Nature, Vol. 437, Issue 7059
    • DOI: 10.1038/nature04040

    High harmonic interferometry of multi-electron dynamics in molecules
    journal, July 2009

    • Smirnova, Olga; Mairesse, Yann; Patchkovskii, Serguei
    • Nature, Vol. 460, Issue 7258
    • DOI: 10.1038/nature08253

    Electron localization following attosecond molecular photoionization
    journal, June 2010

    • Sansone, G.; Kelkensberg, F.; Pérez-Torres, J. F.
    • Nature, Vol. 465, Issue 7299
    • DOI: 10.1038/nature09084

    Real-time observation of valence electron motion
    journal, August 2010

    • Goulielmakis, Eleftherios; Loh, Zhi-Heng; Wirth, Adrian
    • Nature, Vol. 466, Issue 7307
    • DOI: 10.1038/nature09212

    Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics
    journal, May 2016

    • Picón, A.; Lehmann, C. S.; Bostedt, C.
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms11652

    Attosecond imaging of molecular electronic wavepackets
    journal, January 2010

    • Haessler, S.; Caillat, J.; Boutu, W.
    • Nature Physics, Vol. 6, Issue 3
    • DOI: 10.1038/nphys1511

    Extreme-ultraviolet pump–probe studies of one-femtosecond-scale electron dynamics
    journal, July 2011

    • Tzallas, P.; Skantzakis, E.; Nikolopoulos, L. A. A.
    • Nature Physics, Vol. 7, Issue 10
    • DOI: 10.1038/nphys2033

    Attosecond science
    journal, June 2007

    • Corkum, P. B.; Krausz, Ferenc
    • Nature Physics, Vol. 3, Issue 6
    • DOI: 10.1038/nphys620

    (Sub-)femtosecond control of molecular reactions via tailoring the electric field of light
    journal, January 2013

    • Kling, Matthias F.; von den Hoff, Philipp; Znakovskaya, Irina
    • Physical Chemistry Chemical Physics, Vol. 15, Issue 24
    • DOI: 10.1039/c3cp50591j

    Analysis of a measurement scheme for ultrafast hole dynamics by few femtosecond resolution X-ray pump–probe Auger spectroscopy
    journal, January 2014

    • Cooper, Bridgette; Kolorenč, Přemysl; Frasinski, Leszek J.
    • Faraday Discuss., Vol. 171
    • DOI: 10.1039/c4fd00051j

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

    • Yuan, Kai-Jun; Bandrauk, André D.
    • Physical Chemistry Chemical Physics, Vol. 19, Issue 38
    • DOI: 10.1039/c7cp05067d

    Migration of holes: Formalism, mechanisms, and illustrative applications
    journal, March 2003

    • Breidbach, J.; Cederbaum, L. S.
    • The Journal of Chemical Physics, Vol. 118, Issue 9
    • DOI: 10.1063/1.1540618

    Multielectron wave-packet propagation: General theory and application
    journal, July 2005

    • Kuleff, Alexander I.; Breidbach, Jörg; Cederbaum, Lorenz S.
    • The Journal of Chemical Physics, Vol. 123, Issue 4
    • DOI: 10.1063/1.1961341

    Symmetry-dependent vibrational excitation in N 1s photoionization of N2: Experiment and theory
    journal, March 2006

    • Ehara, M.; Nakatsuji, H.; Matsumoto, M.
    • The Journal of Chemical Physics, Vol. 124, Issue 12
    • DOI: 10.1063/1.2181144

    Partial photoionization cross section and photoelectron angular distribution for the X2 Σ g + state of N 2 + in the static‐exchange approximation
    journal, May 1980

    • Raseev, G.; Le Rouzo, H.; Lefebvre‐Brion, H.
    • The Journal of Chemical Physics, Vol. 72, Issue 10
    • DOI: 10.1063/1.438988

    Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen
    journal, January 1989

    • Dunning, Thom H.
    • The Journal of Chemical Physics, Vol. 90, Issue 2
    • DOI: 10.1063/1.456153

    Calculation of low‐energy elastic cross sections for electron‐CF 4 scattering
    journal, May 1994

    • Gianturco, F. A.; Lucchese, R. R.; Sanna, N.
    • The Journal of Chemical Physics, Vol. 100, Issue 9
    • DOI: 10.1063/1.467237

    Cross section and asymmetry parameter calculation for sulfur 1s photoionization of SF6
    journal, September 1999

    • Natalense, Alexandra P. P.; Lucchese, Robert R.
    • The Journal of Chemical Physics, Vol. 111, Issue 12
    • DOI: 10.1063/1.479794

    An electronic time scale in chemistry
    journal, April 2006

    • Remacle, F.; Levine, R. D.
    • Proceedings of the National Academy of Sciences, Vol. 103, Issue 18
    • DOI: 10.1073/pnas.0601855103

    Imaging electronic quantum motion with light
    journal, July 2012

    • Dixit, G.; Vendrell, O.; Santra, R.
    • Proceedings of the National Academy of Sciences, Vol. 109, Issue 29
    • DOI: 10.1073/pnas.1202226109

    Watching energy transfer in metalloporphyrin heterodimers using stimulated X-ray Raman spectroscopy
    journal, September 2013

    • Biggs, J. D.; Zhang, Y.; Healion, D.
    • Proceedings of the National Academy of Sciences, Vol. 110, Issue 39
    • DOI: 10.1073/pnas.1308604110

    Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction
    journal, December 2018

    • Ye, Lyuzhou; Rouxel, Jérémy R.; Cho, Daeheum
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 2
    • DOI: 10.1073/pnas.1816730116

    K-shell photoionization of CO and N 2 : is there a link between the photoelectron angular distribution and the molecular decay dynamics?
    journal, September 2001

    • Weber, Th; Jagutzki, O.; Hattass, M.
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 34, Issue 18
    • DOI: 10.1088/0953-4075/34/18/305

    State-dependent gerade/ungerade intensity ratios in the Auger spectrum of N 2
    journal, July 2008

    • Püttner, R.; Fukuzawa, H.; Liu, X-J
    • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 41, Issue 14
    • DOI: 10.1088/0953-4075/41/14/141001

    On the Interpretation of Neutron-Proton Scattering Data by the Schwinger Variational Method
    journal, July 1949


    Low-energy electron scattering by silane ( SiH 4 )
    journal, November 1990


    Theory of time-resolved nonresonant x-ray scattering for imaging ultrafast coherent electron motion
    journal, April 2014


    Tracking hole localization in K -shell and core-valence-excited acetylene photoionization via body-frame photoelectron angular distributions
    journal, February 2015


    Attosecond x-ray scattering from a particle-hole wave packet
    journal, June 2017


    Auger-induced charge migration
    journal, October 2018


    Ultrafast nuclear dynamics in the doubly-core-ionized water molecule observed via Auger spectroscopy
    journal, December 2018


    Double-Core-Hole States in Neon: Lifetime, Post-Collision Interaction, and Spectral Assignment
    journal, September 2016


    Electronic Coherence in Ultrafast X-Ray Scattering from Molecular Wave Packets
    journal, February 2019


    Vibrationally Resolved O 1 s Photoelectron Spectrum of CO 2 : Vibronic Coupling and Dynamic Core-Hole Localization
    journal, August 1997


    Ultrafast Probing of Core Hole Localization in N2
    journal, May 2008


    Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses
    journal, October 2014


    Measurement and laser control of attosecond charge migration in ionized iodoacetylene
    journal, October 2015


    Multidimensional Attosecond Resonant X-Ray Spectroscopy of Molecules: Lessons from the Optical Regime
    journal, April 2013


    Detecting coherent core-hole wave-packet dynamics in N$_2$ by time- and angle-resolved inner-shell photoelectron spectroscopy
    text, January 2019

    • Inhester, Ludger; Greenman, Loren; Rudenko, Artem
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2019-02925