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

Title: Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

Abstract

New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Specifically, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. In this paper, we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF 2 molecules following X-ray absorption at the Xe site.

Authors:
 [1];  [1];  [2];  [3];  [4];  [4];  [5];  [6];  [7];  [8];  [1];  [7];  [4];  [4];  [1];  [1];  [1];  [4];  [4];  [1] more »;  [1];  [9];  [1];  [1];  [1] « less
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  3. Kansas State Univ., Manhattan, KS (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Kansas State Univ., Manhattan, KS (United States); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  6. Univ. of Connecticut, Storrs, CT (United States)
  7. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  8. Argonne National Lab. (ANL), Argonne, IL (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  9. SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1272409
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Picón, A., Lehmann, C. S., Bostedt, C., Rudenko, A., Marinelli, A., Osipov, T., Rolles, D., Berrah, N., Bomme, C., Bucher, M., Doumy, G., Erk, B., Ferguson, K. R., Gorkhover, T., Ho, P. J., Kanter, E. P., Krässig, B., Krzywinski, J., Lutman, A. A., March, A. M., Moonshiram, D., Ray, D., Young, L., Pratt, S. T., and Southworth, S. H. Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics. United States: N. p., 2016. Web. doi:10.1038/ncomms11652.
Picón, A., Lehmann, C. S., Bostedt, C., Rudenko, A., Marinelli, A., Osipov, T., Rolles, D., Berrah, N., Bomme, C., Bucher, M., Doumy, G., Erk, B., Ferguson, K. R., Gorkhover, T., Ho, P. J., Kanter, E. P., Krässig, B., Krzywinski, J., Lutman, A. A., March, A. M., Moonshiram, D., Ray, D., Young, L., Pratt, S. T., & Southworth, S. H. Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics. United States. doi:10.1038/ncomms11652.
Picón, A., Lehmann, C. S., Bostedt, C., Rudenko, A., Marinelli, A., Osipov, T., Rolles, D., Berrah, N., Bomme, C., Bucher, M., Doumy, G., Erk, B., Ferguson, K. R., Gorkhover, T., Ho, P. J., Kanter, E. P., Krässig, B., Krzywinski, J., Lutman, A. A., March, A. M., Moonshiram, D., Ray, D., Young, L., Pratt, S. T., and Southworth, S. H. Mon . "Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics". United States. doi:10.1038/ncomms11652. https://www.osti.gov/servlets/purl/1272409.
@article{osti_1272409,
title = {Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics},
author = {Picón, A. and Lehmann, C. S. and Bostedt, C. and Rudenko, A. and Marinelli, A. and Osipov, T. and Rolles, D. and Berrah, N. and Bomme, C. and Bucher, M. and Doumy, G. and Erk, B. and Ferguson, K. R. and Gorkhover, T. and Ho, P. J. and Kanter, E. P. and Krässig, B. and Krzywinski, J. and Lutman, A. A. and March, A. M. and Moonshiram, D. and Ray, D. and Young, L. and Pratt, S. T. and Southworth, S. H.},
abstractNote = {New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Specifically, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. In this paper, we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site.},
doi = {10.1038/ncomms11652},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {5}
}

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

Citation Metrics:
Cited by: 18 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: Hetero-site X-ray pump-probe scheme. Sketch of a two-colour X-ray-pump/X-ray-probe experiment. The X-ray absorbed by B induces

Save / Share:

Works referenced in this record:

Linac Coherent Light Source soft x-ray materials science instrument optical design and monochromator commissioning
journal, September 2011

  • Heimann, Philip; Krupin, Oleg; Schlotter, William F.
  • Review of Scientific Instruments, Vol. 82, Issue 9
  • DOI: 10.1063/1.3633947

Inner-shell photoionization and core-hole decay of Xe and XeF2
journal, June 2015

  • Southworth, Stephen H.; Wehlitz, Ralf; Picón, Antonio
  • The Journal of Chemical Physics, Vol. 142, Issue 22
  • DOI: 10.1063/1.4922208

Attosecond molecular dynamics: fact or fiction?
journal, February 2014

  • Lépine, Franck; Ivanov, Misha Y.; Vrakking, Marc J. J.
  • Nature Photonics, Vol. 8, Issue 3
  • DOI: 10.1038/nphoton.2014.25

Observation of femtosecond X-ray interactions with matter using an X-ray–X-ray pump–probe scheme
journal, January 2016

  • Inoue, Ichiro; Inubushi, Yuichi; Sato, Takahiro
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 6
  • DOI: 10.1073/pnas.1516426113

Distal Charge Transport in Peptides
journal, April 2007

  • Schlag, Edward W.; Sheu, Sheh-Yi; Yang, Dah-Yen
  • Angewandte Chemie International Edition, Vol. 46, Issue 18
  • DOI: 10.1002/anie.200601623

Few-femtosecond time-resolved measurements of X-ray free-electron lasers
journal, April 2014

  • Behrens, C.; Decker, F. -J.; Ding, Y.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4762

Evidence for interatomic Coulombic decay in Xe K -shell-vacancy decay of XeF 2
journal, September 2012


Femtobiology
journal, May 2008


Ultrafast isomerization initiated by X-ray core ionization
journal, September 2015

  • Liekhus-Schmaltz, Chelsea E.; Tenney, Ian; Osipov, Timur
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9199

Indications of radiation damage in ferredoxin microcrystals using high-intensity X-FEL beams
journal, February 2015

  • Nass, Karol; Foucar, Lutz; Barends, Thomas R. M.
  • Journal of Synchrotron Radiation, Vol. 22, Issue 2
  • DOI: 10.1107/S1600577515002349

Experimental Demonstration of Femtosecond Two-Color X-Ray Free-Electron Lasers
journal, March 2013


Imaging charge transfer in iodomethane upon x-ray photoabsorption
journal, July 2014


The Atomic, Molecular and Optical Science instrument at the Linac Coherent Light Source
journal, April 2015

  • Ferguson, Ken R.; Bucher, Maximilian; Bozek, John D.
  • Journal of Synchrotron Radiation, Vol. 22, Issue 3
  • DOI: 10.1107/S1600577515004646

When X-rays modify the protein structure: radiation damage at work
journal, April 2005


Dynamics of Light Harvesting in Photosynthesis
journal, May 2009


Auger cascade satellites following 3d ionization in xenon
journal, October 2003

  • Jonauskas, V.; Partanen, L.; Ku as, S.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 36, Issue 22
  • DOI: 10.1088/0953-4075/36/22/003

Absolute cross sections for photoionization of Xe q + ions ( 1 ⩽ q ⩽ 5 ) at the 3d ionization threshold
journal, May 2014

  • Schippers, S.; Ricz, S.; Buhr, T.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 47, Issue 11
  • DOI: 10.1088/0953-4075/47/11/115602

Charge Transport in Proteins Probed by Resonant Photoemission
journal, March 2009


Biomolecular imaging and electronic damage using X-ray free-electron lasers
journal, December 2010

  • Quiney, Harry M.; Nugent, Keith A.
  • Nature Physics, Vol. 7, Issue 2
  • DOI: 10.1038/nphys1859

Femtochemistry:  Atomic-Scale Dynamics of the Chemical Bond
journal, June 2000

  • Zewail, Ahmed H.
  • The Journal of Physical Chemistry A, Vol. 104, Issue 24
  • DOI: 10.1021/jp001460h

Transient lattice contraction in the solid-to-plasma transition
journal, January 2016

  • Ferguson, Ken R.; Bucher, Maximilian; Gorkhover, Tais
  • Science Advances, Vol. 2, Issue 1
  • DOI: 10.1126/sciadv.1500837

Recoil-ion and electron momentum spectroscopy: reaction-microscopes
journal, August 2003


Decay of τ Mesons of Known Charge
journal, May 1954


Potential for biomolecular imaging with femtosecond X-ray pulses
journal, August 2000

  • Neutze, Richard; Wouts, Remco; van der Spoel, David
  • Nature, Vol. 406, Issue 6797
  • DOI: 10.1038/35021099

Femtosecond dynamics of DNA-mediated electron transfer
journal, May 1999

  • Wan, C.; Fiebig, T.; Kelley, S. O.
  • Proceedings of the National Academy of Sciences, Vol. 96, Issue 11
  • DOI: 10.1073/pnas.96.11.6014

Ultralong-range energy transfer by interatomic Coulombic decay in an extreme quantum system
journal, June 2010

  • Sisourat, Nicolas; Kryzhevoi, Nikolai V.; Kolorenč, Přemysl
  • Nature Physics, Vol. 6, Issue 7
  • DOI: 10.1038/nphys1685

Visualizing electron rearrangement in space and time during the transition from a molecule to atoms
journal, November 2010

  • Li, W.; Jaron-Becker, A. A.; Hogle, C. W.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 47
  • DOI: 10.1073/pnas.1014723107

Femtosecond and Subfemtosecond X-Ray Pulses from a Self-Amplified Spontaneous-Emission–Based Free-Electron Laser
journal, February 2004


Multiple ionization of Xe—comparison of de-excitation pathways following 3d 5/2 ionization and 3d 5/2 → 6p resonance excitation
journal, June 2005

  • Partanen, L.; Sankari, R.; Osmekhin, S.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 38, Issue 12
  • DOI: 10.1088/0953-4075/38/12/005

Selecting core-hole localization or delocalization in CS2 by photofragmentation dynamics
journal, January 2015

  • Guillemin, R.; Decleva, P.; Stener, M.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7166

    Works referencing / citing this record:

    Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics
    text, January 2016


    Symmetry breakdown of electron emission in extreme ultraviolet photoionization of argon
    journal, November 2018


    Alignment, orientation, and Coulomb explosion of difluoroiodobenzene studied with the pixel imaging mass spectrometry (PImMS) camera
    journal, July 2017

    • Amini, Kasra; Boll, Rebecca; Lauer, Alexandra
    • The Journal of Chemical Physics, Vol. 147, Issue 1
    • DOI: 10.1063/1.4982220

    Detecting coherent core-hole wave-packet dynamics in N 2 by time- and angle-resolved inner-shell photoelectron spectroscopy
    journal, August 2019

    • Inhester, Ludger; Greenman, Loren; Rudenko, Artem
    • The Journal of Chemical Physics, Vol. 151, Issue 5
    • DOI: 10.1063/1.5109867

    Ultrashort Free-Electron Laser X-ray Pulses
    journal, September 2017

    • Helml, Wolfram; Grguraš, Ivanka; Juranić, Pavle
    • Applied Sciences, Vol. 7, Issue 9
    • DOI: 10.3390/app7090915

    Symmetry breakdown of electron emission in extreme ultraviolet photoionization of argon
    journal, November 2018


    Alignment, orientation, and Coulomb explosion of difluoroiodobenzene studied with the pixel imaging mass spectrometry (PImMS) camera
    journal, July 2017

    • Amini, Kasra; Boll, Rebecca; Lauer, Alexandra
    • The Journal of Chemical Physics, Vol. 147, Issue 1
    • DOI: 10.1063/1.4982220

    Detecting coherent core-hole wave-packet dynamics in N 2 by time- and angle-resolved inner-shell photoelectron spectroscopy
    journal, August 2019

    • Inhester, Ludger; Greenman, Loren; Rudenko, Artem
    • The Journal of Chemical Physics, Vol. 151, Issue 5
    • DOI: 10.1063/1.5109867

    Ultrashort Free-Electron Laser X-ray Pulses
    journal, September 2017

    • Helml, Wolfram; Grguraš, Ivanka; Juranić, Pavle
    • Applied Sciences, Vol. 7, Issue 9
    • DOI: 10.3390/app7090915

      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.