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Title: Ultrafast x-ray and electron scattering of free molecules: A comparative evaluation

Abstract

Resolving gas phase molecular motions with simultaneous spatial and temporal resolution is rapidly coming within the reach of x-ray Free Electron Lasers (XFELs) and Mega-electron-Volt (MeV) electron beams. These two methods enable scattering experiments that have yielded fascinating new results, and while both are important methods for determining transient molecular structures in photochemical reactions, it is important to understand their relative merits. In the present study, we evaluate the respective scattering cross sections of the two methods and simulate their ability to determine excited state molecular structures in light of currently existing XFEL and MeV source parameters. Using the example of optically excited N-methyl morpholine and simulating the scattering patterns with shot noise, we find that the currently achievable signals are superior with x-ray scattering for equal samples and on a per-shot basis and that x-ray scattering requires fewer detected signal counts for an equal fidelity structure determination. Importantly, within the independent atom model, excellent structure determinations can be achieved for scattering vectors only to about 5Å–1, leaving larger scattering vector ranges for investigating vibrational motions and wavepackets. Electron scattering has a comparatively higher sensitivity toward hydrogen atoms, which may point to applications where electron scattering is inherently the preferredmore » choice, provided that excellent signals can be achieved at large scattering angles that are currently difficult to access.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [1]
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  1. Brown Univ., Providence, RI (United States)
Publication Date:
Research Org.:
Brown Univ., Providence, RI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE
OSTI Identifier:
1660746
Alternate Identifier(s):
OSTI ID: 1634249
Grant/Contract Number:  
SC0017995; SC0020276
Resource Type:
Accepted Manuscript
Journal Name:
Structural Dynamics
Additional Journal Information:
Journal Volume: 7; Journal Issue: 3; Conference: 5.International Conference on Ultrafast Structural Dynamics (ICUSD 2019), Daejeon (South Korea), 25-28 Jun 2019; Journal ID: ISSN 2329-7778
Publisher:
American Crystallographic Association/AIP
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; X-ray scattering; Electron scattering; Ultrafast X-rays; Scattering theory; Free electron lasers; Gas phase; Photochemical reactions

Citation Formats

Ma, Lingyu, Yong, Haiwang, Geiser, Joseph D., Moreno Carrascosa, Andrés, Goff, Nathan, and Weber, Peter M. Ultrafast x-ray and electron scattering of free molecules: A comparative evaluation. United States: N. p., 2020. Web. doi:10.1063/4.0000010.
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Ma, Lingyu, Yong, Haiwang, Geiser, Joseph D., Moreno Carrascosa, Andrés, Goff, Nathan, & Weber, Peter M. Ultrafast x-ray and electron scattering of free molecules: A comparative evaluation. United States. https://doi.org/10.1063/4.0000010
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Ma, Lingyu, Yong, Haiwang, Geiser, Joseph D., Moreno Carrascosa, Andrés, Goff, Nathan, and Weber, Peter M. Tue . "Ultrafast x-ray and electron scattering of free molecules: A comparative evaluation". United States. https://doi.org/10.1063/4.0000010. https://www.osti.gov/servlets/purl/1660746.
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@article{osti_1660746,
title = {Ultrafast x-ray and electron scattering of free molecules: A comparative evaluation},
author = {Ma, Lingyu and Yong, Haiwang and Geiser, Joseph D. and Moreno Carrascosa, Andrés and Goff, Nathan and Weber, Peter M.},
abstractNote = {Resolving gas phase molecular motions with simultaneous spatial and temporal resolution is rapidly coming within the reach of x-ray Free Electron Lasers (XFELs) and Mega-electron-Volt (MeV) electron beams. These two methods enable scattering experiments that have yielded fascinating new results, and while both are important methods for determining transient molecular structures in photochemical reactions, it is important to understand their relative merits. In the present study, we evaluate the respective scattering cross sections of the two methods and simulate their ability to determine excited state molecular structures in light of currently existing XFEL and MeV source parameters. Using the example of optically excited N-methyl morpholine and simulating the scattering patterns with shot noise, we find that the currently achievable signals are superior with x-ray scattering for equal samples and on a per-shot basis and that x-ray scattering requires fewer detected signal counts for an equal fidelity structure determination. Importantly, within the independent atom model, excellent structure determinations can be achieved for scattering vectors only to about 5Å–1, leaving larger scattering vector ranges for investigating vibrational motions and wavepackets. Electron scattering has a comparatively higher sensitivity toward hydrogen atoms, which may point to applications where electron scattering is inherently the preferred choice, provided that excellent signals can be achieved at large scattering angles that are currently difficult to access.},
doi = {10.1063/4.0000010},
journal = {Structural Dynamics},
number = 3,
volume = 7,
place = {United States},
year = {Tue Jun 23 00:00:00 EDT 2020},
month = {Tue Jun 23 00:00:00 EDT 2020}
}
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https://doi.org/10.1063/4.0000010
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