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Title: X-ray scattering signatures of early-time accelerations in iodine dissociation

Abstract

Ultrafast time-resolved x-ray scattering (TRXS) from a photoexcited molecular ensemble measures a distribution $S(Q, τ)$ of the x-ray momentum transfer Q and pump-probe delay τ in which all modes of motion induced by the excitation overlap. Frequency-resolved x-ray scattering (FRXS) based on $$\tilde {S}\left(Q,\omega \right)$$ separates each oscillation and dissociation channel in the TRXS data, enabling measurements of vibrational frequencies and phases, and dissociation velocities and time shifts. In this work, we extend FRXS analysis to study early-time accelerations as well. We show how these appear as diffuse scattering patterns with characteristic phase evolution in FXRS and we develop a set of transformations that isolate individual channels to measure the early-time accelerated motion. This procedure is used to analyze diatomic iodine x-ray scattering data with multiple dissociations, and the ability of this technique to characterize early-time accelerations of one dissociation channel even in the presence of another dissociation is demonstrated.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States). Dept. of Physics
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1767948
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics. B, Atomic, Molecular and Optical Physics
Additional Journal Information:
Journal Volume: 53; Journal Issue: 24; Journal ID: ISSN 0953-4075
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; ultrafast X-ray scattering; ultrafast molecular dynamics; molecular structure

Citation Formats

Gabalski, Ian, Ware, Matthew R., and Bucksbaum, Philip H. X-ray scattering signatures of early-time accelerations in iodine dissociation. United States: N. p., 2020. Web. doi:10.1088/1361-6455/abc22a.
Gabalski, Ian, Ware, Matthew R., & Bucksbaum, Philip H. X-ray scattering signatures of early-time accelerations in iodine dissociation. United States. https://doi.org/10.1088/1361-6455/abc22a
Gabalski, Ian, Ware, Matthew R., and Bucksbaum, Philip H. Fri . "X-ray scattering signatures of early-time accelerations in iodine dissociation". United States. https://doi.org/10.1088/1361-6455/abc22a. https://www.osti.gov/servlets/purl/1767948.
@article{osti_1767948,
title = {X-ray scattering signatures of early-time accelerations in iodine dissociation},
author = {Gabalski, Ian and Ware, Matthew R. and Bucksbaum, Philip H.},
abstractNote = {Ultrafast time-resolved x-ray scattering (TRXS) from a photoexcited molecular ensemble measures a distribution $S(Q, τ)$ of the x-ray momentum transfer Q and pump-probe delay τ in which all modes of motion induced by the excitation overlap. Frequency-resolved x-ray scattering (FRXS) based on $\tilde {S}\left(Q,\omega \right)$ separates each oscillation and dissociation channel in the TRXS data, enabling measurements of vibrational frequencies and phases, and dissociation velocities and time shifts. In this work, we extend FRXS analysis to study early-time accelerations as well. We show how these appear as diffuse scattering patterns with characteristic phase evolution in FXRS and we develop a set of transformations that isolate individual channels to measure the early-time accelerated motion. This procedure is used to analyze diatomic iodine x-ray scattering data with multiple dissociations, and the ability of this technique to characterize early-time accelerations of one dissociation channel even in the presence of another dissociation is demonstrated.},
doi = {10.1088/1361-6455/abc22a},
journal = {Journal of Physics. B, Atomic, Molecular and Optical Physics},
number = 24,
volume = 53,
place = {United States},
year = {Fri Nov 20 00:00:00 EST 2020},
month = {Fri Nov 20 00:00:00 EST 2020}
}

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