Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump–x-ray-probe spectroscopy

C. S. Lehmann, A. Picón, C. Bostedt, A. Rudenko, A. Marinelli, D. Moonshiram, T. Osipov, D. Rolles, N. Berrah, C. Bomme, M. Bucher, G. Doumy, B. Erk, K. R. Ferguson, T. Gorkhover, P. J. Ho, E. P. Kanter, B. Krässig, J. Krzywinski, A. A. Lutman, A. M. March, D. Ray, L. Young, S. T. Pratt, and S. H. Southworth
Phys. Rev. A 94, 013426 – Published 26 July 2016

Abstract

The capability of generating two intense, femtosecond x-ray pulses with a controlled time delay opens the possibility of performing time-resolved experiments for x-ray-induced phenomena. We have applied this capability to study the photoinduced dynamics in diatomic molecules. In molecules composed of low-Z elements, K-shell ionization creates a core-hole state in which the main decay mode is an Auger process involving two electrons in the valence shell. After Auger decay, the nuclear wave packets of the transient two-valence-hole states continue evolving on the femtosecond time scale, leading either to separated atomic ions or long-lived quasibound states. By using an x-ray pump and an x-ray probe pulse tuned above the K-shell ionization threshold of the nitrogen molecule, we are able to observe ion dissociation in progress by measuring the time-dependent kinetic energy releases of different breakup channels. We simulated the measurements on N2 with a molecular dynamics model that accounts for K-shell ionization, Auger decay, and the time evolution of the nuclear wave packets. In addition to explaining the time-dependent feature in the measured kinetic energy release distributions from the dissociative states, the simulation also reveals the contributions of quasibound states.

  • Figure
  • Figure
  • Figure
  • Figure
  • Received 10 May 2016

DOI:https://doi.org/10.1103/PhysRevA.94.013426

©2016 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

C. S. Lehmann1,*, A. Picón1,†, C. Bostedt1,2, A. Rudenko3, A. Marinelli4, D. Moonshiram1, T. Osipov4, D. Rolles3,5, N. Berrah6, C. Bomme5, M. Bucher1,4, G. Doumy1, B. Erk5, K. R. Ferguson4, T. Gorkhover4, P. J. Ho1, E. P. Kanter1, B. Krässig1, J. Krzywinski4, A. A. Lutman4, A. M. March1, D. Ray4, L. Young1,7, S. T. Pratt1, and S. H. Southworth1

  • 1Argonne National Laboratory, Argonne, Illinois 60439, USA
  • 2Department of Physics and Astronomy, Northwestern University, Evanston, Illinois 60208, USA
  • 3J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, Kansas 66506, USA
  • 4SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
  • 5Deutsches Elektronen-Synchrotron (DESY), 22607 Hamburg, Germany
  • 6Department of Physics, University of Connecticut, Storrs, Connecticut 06269, USA
  • 7The James Franck Institute and Department of Physics, The University of Chicago, Chicago, Illinois 60637, USA

  • *Present address: Fachbereich Chemie, Philipps-Universität Marburg, Marburg, Germany.
  • antonio.picon.alvarez@gmail.com

Article Text (Subscription Required)

Click to Expand

References (Subscription Required)

Click to Expand
Issue

Vol. 94, Iss. 1 — July 2016

Reuse & Permissions
Access Options
CHORUS

Article Available via CHORUS

Download Accepted Manuscript
Author publication services for translation and copyediting assistance advertisement

Authorization Required


×
×

Images

×

Sign up to receive regular email alerts from Physical Review A

Log In

Cancel
×

Search


Article Lookup

Paste a citation or DOI

Enter a citation
×