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:
-
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States). Dept. of Physics
- 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}
}
Works referenced in this record:
Mapping the emergence of molecular vibrations mediating bond formation
journal, June 2020
- Kim, Jong Goo; Nozawa, Shunsuke; Kim, Hanui
- Nature, Vol. 582, Issue 7813
Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule
journal, February 2019
- Haldrup, Kristoffer; Levi, Gianluca; Biasin, Elisa
- Physical Review Letters, Vol. 122, Issue 6
Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering
journal, October 2018
- Yong, Haiwang; Zotev, Nikola; Stankus, Brian
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 22
Pump–probe experimental methodology at the Linac Coherent Light Source
journal, April 2019
- Glownia, James M.; Gumerlock, Karl; Lemke, Henrik T.
- Journal of Synchrotron Radiation, Vol. 26, Issue 3
Observing Solvation Dynamics with Simultaneous Femtosecond X-ray Emission Spectroscopy and X-ray Scattering
journal, February 2016
- Haldrup, Kristoffer; Gawelda, Wojciech; Abela, Rafael
- The Journal of Physical Chemistry B, Vol. 120, Issue 6
On the limits of observing motion in time-resolved X-ray scattering
journal, April 2019
- Ware, Matthew R.; Glownia, James M.; Natan, Adi
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145
Analytic signal generation-tips and traps
journal, January 1994
- Reilly, A.; Frazer, G.; Boashash, B.
- IEEE Transactions on Signal Processing, Vol. 42, Issue 11
Classical motion of a Morse oscillator
journal, July 1978
- DeMarcus, W. C.
- American Journal of Physics, Vol. 46, Issue 7
Characterizing dissociative motion in time-resolved x-ray scattering from gas-phase diatomic molecules
journal, September 2019
- Ware, Matthew R.; Glownia, James M.; Al-Sayyad, Noor
- Physical Review A, Vol. 100, Issue 3
Ab initio studies of ultrafast x-ray scattering of the photodissociation of iodine
journal, September 2010
- Debnarova, Andrea; Techert, Simone; Schmatz, Stefan
- The Journal of Chemical Physics, Vol. 133, Issue 12
Direct observation of bond formation in solution with femtosecond X-ray scattering
journal, February 2015
- Kim, Kyung Hwan; Kim, Jong Goo; Nozawa, Shunsuke
- Nature, Vol. 518, Issue 7539
Iodine Revisited
journal, July 1971
- Mulliken, Robert S.
- The Journal of Chemical Physics, Vol. 55, Issue 1
On the interpretation of time-resolved anisotropic diffraction patterns
journal, November 2010
- Lorenz, U.; Møller, K. B.; Henriksen, N. E.
- New Journal of Physics, Vol. 12, Issue 11
Glownia et al. Reply:
journal, August 2017
- Glownia, J. M.; Natan, A.; Cryan, J. P.
- Physical Review Letters, Vol. 119, Issue 6
Characterizing Multiphoton Excitation Using Time-Resolved X-ray Scattering
journal, March 2020
- Bucksbaum, Philip H.; Ware, Matthew R.; Natan, Adi
- Physical Review X, Vol. 10, Issue 1
X-Ray Diffraction from Isolated and Strongly Aligned Gas-Phase Molecules with a Free-Electron Laser
journal, February 2014
- Küpper, Jochen; Stern, Stephan; Holmegaard, Lotte
- Physical Review Letters, Vol. 112, Issue 8
Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering
journal, January 2020
- Kunnus, Kristjan; Vacher, Morgane; Harlang, Tobias C. B.
- Nature Communications, Vol. 11, Issue 1
Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated
journal, June 2016
- Biasin, Elisa; van Driel, Tim Brandt; Kjær, Kasper S.
- Physical Review Letters, Vol. 117, Issue 1
Ultrafast X-ray Diffraction Theory
journal, November 1998
- Cao, Jianshu; Wilson, Kent R.
- The Journal of Physical Chemistry A, Vol. 102, Issue 47
Ultrafast myoglobin structural dynamics observed with an X-ray free-electron laser
journal, April 2015
- Levantino, Matteo; Schirò, Giorgio; Lemke, Henrik Till
- Nature Communications, Vol. 6, Issue 1