skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Laser control over the ultrafast Coulomb explosion of N 2 2 + after Auger decay: A quantum-dynamics investigation

Abstract

By theoretical calculation, we show the possibility to control and partially suppress the Coulomb explosion of N 2 molecules after core-level photoionization by an x-ray laser and subsequent Auger decay. This is achieved by means of a femtosecond infrared laser pulse interacting with the N 2 2 + dication produced by the x-ray pulse. Suppression of molecular fragmentation requires few-femtosecond IR pulses interacting with the system either during or shortly after the arrival of the x-ray pulse. The IR pulse suppresses fragmentation mostly by optically coupling the electronic routes to ultrafast molecular dissociation with electronic channels able to support long-lived vibrational resonances. The effect is strongly dependent on the orientation of the molecule with respect to the polarization axis of the IR field. These calculations are motivated by x-ray pump–IR probe experiments performed at an x-ray free-electron laser [J. M. Glownia et al., Opt. Express 18, 17620 (2010)], where only enhancement of N 2 2 + fragmentation as a function of the pump-probe delay time was reported. The opposite effect reported here becomes apparent when the various electronic channels are considered separately. In practice, this corresponds to a coincident measurement of the energy of the ejected Auger electron

Authors:
 [1];  [2];  [3];  [4]
  1. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany)
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Hamburg Centre for Ultrafast Imaging (Germany); Aarhus Univ. (Denmark)
  3. Univ. of Wisconsin, Milwaukee, WI (United States)
  4. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany); Hamburg Centre for Ultrafast Imaging (Germany)
Publication Date:
Research Org.:
Univ. of Wisconsin, Milwaukee, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1598189
Alternate Identifier(s):
OSTI ID: 1352965
Grant/Contract Number:  
SC0002164
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review A
Additional Journal Information:
Journal Volume: 95; Journal Issue: 4; Journal ID: ISSN 2469-9926
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Hanna, Athiya Mahmud, Vendrell, Oriol, Ourmazd, Abbas, and Santra, Robin. Laser control over the ultrafast Coulomb explosion of N22+ after Auger decay: A quantum-dynamics investigation. United States: N. p., 2017. Web. doi:10.1103/PhysRevA.95.043419.
Hanna, Athiya Mahmud, Vendrell, Oriol, Ourmazd, Abbas, & Santra, Robin. Laser control over the ultrafast Coulomb explosion of N22+ after Auger decay: A quantum-dynamics investigation. United States. doi:10.1103/PhysRevA.95.043419.
Hanna, Athiya Mahmud, Vendrell, Oriol, Ourmazd, Abbas, and Santra, Robin. Mon . "Laser control over the ultrafast Coulomb explosion of N22+ after Auger decay: A quantum-dynamics investigation". United States. doi:10.1103/PhysRevA.95.043419. https://www.osti.gov/servlets/purl/1598189.
@article{osti_1598189,
title = {Laser control over the ultrafast Coulomb explosion of N22+ after Auger decay: A quantum-dynamics investigation},
author = {Hanna, Athiya Mahmud and Vendrell, Oriol and Ourmazd, Abbas and Santra, Robin},
abstractNote = {By theoretical calculation, we show the possibility to control and partially suppress the Coulomb explosion of N2 molecules after core-level photoionization by an x-ray laser and subsequent Auger decay. This is achieved by means of a femtosecond infrared laser pulse interacting with the N22+ dication produced by the x-ray pulse. Suppression of molecular fragmentation requires few-femtosecond IR pulses interacting with the system either during or shortly after the arrival of the x-ray pulse. The IR pulse suppresses fragmentation mostly by optically coupling the electronic routes to ultrafast molecular dissociation with electronic channels able to support long-lived vibrational resonances. The effect is strongly dependent on the orientation of the molecule with respect to the polarization axis of the IR field. These calculations are motivated by x-ray pump–IR probe experiments performed at an x-ray free-electron laser [J. M. Glownia et al., Opt. Express 18, 17620 (2010)], where only enhancement of N22+ fragmentation as a function of the pump-probe delay time was reported. The opposite effect reported here becomes apparent when the various electronic channels are considered separately. In practice, this corresponds to a coincident measurement of the energy of the ejected Auger electron},
doi = {10.1103/PhysRevA.95.043419},
journal = {Physical Review A},
number = 4,
volume = 95,
place = {United States},
year = {2017},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Save / Share:

Works referenced in this record:

The multi-configurational time-dependent Hartree approach
journal, January 1990


2MOLCAS as a development platform for quantum chemistry software: MOLCAS: Software Development Platform
journal, January 2004

  • Veryazov, Valera; Widmark, Per-Olof; Serrano-Andrés, Luis
  • International Journal of Quantum Chemistry, Vol. 100, Issue 4
  • DOI: 10.1002/qua.20166

The N 1s core electron shake-up and the shake-up Auger satellite spectrum of the N 2 molecule
journal, January 1992

  • Svensson, S.; Brito, A. Naves de; Keane, M. P.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 25, Issue 1
  • DOI: 10.1088/0953-4075/25/1/017

Experimental and theoretical studies of the radiative properties of the N 2+ 2 D1 Σ + u state
journal, June 1988

  • Olsson, B. J.; Kindvall, G.; Larsson, M.
  • The Journal of Chemical Physics, Vol. 88, Issue 12
  • DOI: 10.1063/1.454314

On the theory of fast photoionization processes
journal, January 1977


MOLCAS 7: The Next Generation
journal, January 2010

  • Aquilante, Francesco; De Vico, Luca; Ferré, Nicolas
  • Journal of Computational Chemistry, Vol. 31, Issue 1
  • DOI: 10.1002/jcc.21318

Rates of exponential decay in systems of discrete energy levels by Stieltjes imaging
journal, July 2014

  • Craigie, Jacob; Hammad, Ali; Cooper, Bridgette
  • The Journal of Chemical Physics, Vol. 141, Issue 1
  • DOI: 10.1063/1.4884785

A high-resolution N 1s photoionization study of the molecule in the near-threshold region
journal, November 1996

  • Kempgens, B.; Kivimäki, A.; Neeb, M.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 29, Issue 22
  • DOI: 10.1088/0953-4075/29/22/016

MOLCAS: a program package for computational chemistry
journal, October 2003


Dissociation of doubly and triply charged N 2 in strong laser fields
journal, October 2011


Time-resolved pump-probe experiments at the LCLS
journal, January 2010

  • Glownia, James M.; Cryan, J.; Andreasson, J.
  • Optics Express, Vol. 18, Issue 17
  • DOI: 10.1364/OE.18.017620

Light-induced potentials ignite dissociation of N 2 2 +
journal, April 2006


On the interpretation of molecular valence Auger spectra
journal, August 1981

  • Ågren, Hans
  • The Journal of Chemical Physics, Vol. 75, Issue 3
  • DOI: 10.1063/1.442176

Ion momentum spectroscopy of N 2 and O 2 molecules irradiated by EUV free-electron laser pulses
journal, September 2009

  • Fukuzawa, H.; Motomura, K.; Liu, X-J
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 42, Issue 18
  • DOI: 10.1088/0953-4075/42/18/181001

Photofragment spectroscopy and dissociation dynamics of N 2+ 2 : A1 Π u X1 Σ + g
journal, April 1994

  • Martin, P. A.; Bennett, F. R.; Maier, J. P.
  • The Journal of Chemical Physics, Vol. 100, Issue 7
  • DOI: 10.1063/1.466267

Dynamics from noisy data with extreme timing uncertainty
journal, April 2016


Tracing nuclear-wave-packet dynamics in singly and doubly charged states of N 2 and O 2 with XUV-pump–XUV-probe experiments
journal, July 2012


Ultrafast X-ray Auger probing of photoexcited molecular dynamics
journal, June 2014

  • McFarland, B. K.; Farrell, J. P.; Miyabe, S.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5235

High-brilliance free-electron-laser photoionization of N 2 : Ground-state depletion and radiation-field-induced modifications
journal, July 2007


The influence of the σ resonance on the Auger decay of core-ionized molecular nitrogen
journal, April 2008


Competition between excitation and electronic decay of short-lived molecular states
journal, October 1996

  • Pahl, E.; Meyer, H. -D.; Cederbaum, L. S.
  • Zeitschrift f�r Physik D Atoms, Molecules and Clusters, Vol. 38, Issue 3
  • DOI: 10.1007/s004600050086

Softening of the H 2 + molecular bond in intense laser fields
journal, April 1990


Theoretical study of electronic states of N22+ in an intense radiation field
journal, October 2007

  • Jiang, Wanyi; Khait, Yuriy G.; Hoffmann, Mark R.
  • The Journal of Chemical Physics, Vol. 127, Issue 16
  • DOI: 10.1063/1.2790439

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

Threshold photoelectrons coincidence spectroscopy of doubly-charged ions of nitrogen, carbon monoxide, nitric oxide and oxygen
journal, June 1994

  • Dawber, G.; McConkey, A. G.; Avaldi, L.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 27, Issue 11
  • DOI: 10.1088/0953-4075/27/11/014

Time-resolved studies with FELs
journal, October 2015


Comparison of quantum and semiclassical radiation theories with application to the beam maser
journal, January 1963


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

High-resolution laser photofragment spectrum of N2+2( 1 π u1 Σ+g)
journal, January 1990

  • Masters, Tim E.; Sarre, Peter J.
  • J. Chem. Soc., Faraday Trans., Vol. 86, Issue 11
  • DOI: 10.1039/FT9908602005

Photofragment spectroscopy of N 2 2 +
journal, August 1983


Determination of the K—LL Auger Spectra of N 2 , O 2 , CO, NO, H 2 O, and CO 2
journal, September 1971

  • Moddeman, W. E.; Carlson, Thomas A.; Krause, Manfred O.
  • The Journal of Chemical Physics, Vol. 55, Issue 5
  • DOI: 10.1063/1.1676411

Quantum molecular dynamics: propagating wavepackets and density operators using the multiconfiguration time-dependent Hartree method
journal, June 2003


Theoretical investigation of the dication of molecular nitrogen
journal, October 1986

  • Wetmore, R. W.; Boyd, R. K.
  • The Journal of Physical Chemistry, Vol. 90, Issue 22
  • DOI: 10.1021/j100280a013

Multi-photon ionization of molecular nitrogen by femtosecond soft x-ray FEL pulses
journal, June 2006

  • Sorokin, A. A.; Bobashev, S. V.; Tiedtke, K.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 39, Issue 14
  • DOI: 10.1088/0953-4075/39/14/L04

Theoretical determination of the ground state of nitrogen molecule dication (N22+)
journal, November 1987

  • Taylor, Peter R.; Partridge, Harry.
  • The Journal of Physical Chemistry, Vol. 91, Issue 24
  • DOI: 10.1021/j100308a018

Molecular frame Auger electron energy spectrum from N 2
journal, February 2012

  • Cryan, J. P.; Glownia, J. M.; Andreasson, J.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 45, Issue 5
  • DOI: 10.1088/0953-4075/45/5/055601

Potential energy curves for N2, NO, O2 and corresponding ions
journal, March 1965


Angular distribution of N2 KVV Auger electrons induced by 1.5 and 2 MeV protons
journal, April 1997

  • Víkor, Gy.; Ricz, S.; Tóth, L.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 124, Issue 2-3
  • DOI: 10.1016/S0168-583X(96)00870-1

    Works referencing / citing this record:

    Laser control over the ultrafast Coulomb explosion of N$_{2}$$^{2+}$ after Auger decay: A quantum-dynamics investigation
    text, January 2017

    • Hanna, Athiya Mahmud; Vendrell, Oriol; Ourmazd, Abbas
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2017-01875

    Time-resolved x-ray/optical pump-probe simulations on N 2 molecules
    journal, March 2019

    • Hanna, Athiya Mahmud; Vendrell, Oriol; Santra, Robin
    • Structural Dynamics, Vol. 6, Issue 2
    • DOI: 10.1063/1.5053995