Bulletin of the American Physical Society
55th Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics
Monday–Friday, June 3–7, 2024; Fort Worth, Texas
Session C05: Ultrafast Dynamics in Complex Systems
2:00 PM–4:00 PM,
Tuesday, June 4, 2024
Room: 202AB
Chair: Michael Zuerch, University of California, Berkeley
Abstract: C05.00002 : Impulsive Stimulated X-ray Raman Scattering in the condensed phase with Attosecond XFEL Pulses*
2:30 PM–2:42 PM
Presenter:
Felix Egun
(Imperial College London)
Authors:
Felix Egun
(Imperial College London)
Oliver G Alexander
(Imperial College London)
Jonathan P Marangos
(Imperial College London)
Laura Rego
(IMDEA Nanociencia)
Antonio Picon
(Universidad Autónoma de Madrid)
Ana M Gutierrez
(Universidad Autónoma de Madrid)
James P Cryan
(SLAC National Accelerator Laboratory)
Agostino Marinelli
(SLAC National Accelerator Laboratory)
Douglas Garratt
(SLAC National Accelarator Laboratory)
Stefan P Moeller
(SLAC National Accelerator Laboratory)
Ming-Fu Lin
(SLAC National Accelerator Laboratory)
Georgi Dakovski
(SLAC National Accelerator Laboratory)
Collaboration:
LX52 Collaboration
Impulsive stimulated X-ray Raman scattering (ISXRS) is predicted to generate and allow detection of spatially-localised valence-excited wavepackets in a site selective manner - allowing for CM to be measured between specific atomic sites in heteroatomic systems. We present the first evidence for ISXRS in the condensed-phase, by focusing isolated attosecond soft x-ray pulses at the chemRIXS endstation at the Linac Coherent Light Source X-ray Free Electron Laser with power densities up to 1017 Wcm-2 on a water jet. Our observable is given by an enhancement of scattered modes of the x-ray field consistent with stimulated Stokes emission into the valence electronic excited states of the water molecules in the liquid phase.
We present calculations for the polarisation response of a water dimer following interaction with the x-ray field; hence allowing for the modelling of hydrogen bond interactions in bulk solvation environment. This results in good agreement with the experiment and offers insight into the dynamic populations of the core and valence-excited states during the process. We anticipate this work can serve as a building block for future time-resolved ISXRS pump-probe schemes, enabling characterization of CM in neutral condensed phase systems.
*We acknowledge support from research grants, EP/X026094/1, EP/V026690/1 and EP/T006943/1, PID2021-126560NB-I00, CNS2022-135803. The Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.
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