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Title: Feasibility of Valence-to-Core X-ray Emission Spectroscopy for Tracking Transient Species

Abstract

X-ray spectroscopies, when combined in laser-pump, X-ray-probe measurement schemes, can be powerful tools for tracking the electronic and geometric structural changes that occur during the course of a photoinitiated chemical reaction. X-ray absorption spectroscopy (XAS) is considered an established technique for such measurements, and X-ray emission spectroscopy (XES) of the strongest core-to-core emission lines (Kα and Kβ) is now being utilized. Flux demanding valence-to-core XES promises to be an important addition to the time-resolved spectroscopic toolkit. Here In this paper we present measurements and density functional theory calculations on laser-excited, solution-phase ferrocyanide that demonstrate the feasibility of valence-to-core XES for time-resolved experiments. Lastly, we discuss technical improvements that will make valence-to-core XES a practical pump–probe technique.

Authors:
 [1];  [2];  [3];  [1];  [2];  [2];  [1];  [4];  [4];  [1];  [1];  [4]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  2. European x-ray free electron laser (XFEL), Hamburg (Germany)
  3. European x-ray free electron laser (XFEL), Hamburg (Germany); Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
  4. Hungarian Academy Sciences, Budapest (Hungary). Wigner Research Centre for Physics
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); European Research Council (ERC)
OSTI Identifier:
1225106
Alternate Identifier(s):
OSTI ID: 1261143
Grant/Contract Number:
ERC-tG-259709; SFB925; AC02-06CH11357
Resource Type:
Journal Article: Published Article
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 119; Journal Issue: 26; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

March, Anne Marie, Assefa, Tadesse A., Bressler, Christian, Doumy, Gilles, Galler, Andreas, Gawelda, Wojciech, Kanter, Elliot P., Németh, Zoltán, Pápai, Mátyás, Southworth, Stephen H., Young, Linda, and Vankó, György. Feasibility of Valence-to-Core X-ray Emission Spectroscopy for Tracking Transient Species. United States: N. p., 2015. Web. doi:10.1021/jp511838q.
March, Anne Marie, Assefa, Tadesse A., Bressler, Christian, Doumy, Gilles, Galler, Andreas, Gawelda, Wojciech, Kanter, Elliot P., Németh, Zoltán, Pápai, Mátyás, Southworth, Stephen H., Young, Linda, & Vankó, György. Feasibility of Valence-to-Core X-ray Emission Spectroscopy for Tracking Transient Species. United States. doi:10.1021/jp511838q.
March, Anne Marie, Assefa, Tadesse A., Bressler, Christian, Doumy, Gilles, Galler, Andreas, Gawelda, Wojciech, Kanter, Elliot P., Németh, Zoltán, Pápai, Mátyás, Southworth, Stephen H., Young, Linda, and Vankó, György. Mon . "Feasibility of Valence-to-Core X-ray Emission Spectroscopy for Tracking Transient Species". United States. doi:10.1021/jp511838q.
@article{osti_1225106,
title = {Feasibility of Valence-to-Core X-ray Emission Spectroscopy for Tracking Transient Species},
author = {March, Anne Marie and Assefa, Tadesse A. and Bressler, Christian and Doumy, Gilles and Galler, Andreas and Gawelda, Wojciech and Kanter, Elliot P. and Németh, Zoltán and Pápai, Mátyás and Southworth, Stephen H. and Young, Linda and Vankó, György},
abstractNote = {X-ray spectroscopies, when combined in laser-pump, X-ray-probe measurement schemes, can be powerful tools for tracking the electronic and geometric structural changes that occur during the course of a photoinitiated chemical reaction. X-ray absorption spectroscopy (XAS) is considered an established technique for such measurements, and X-ray emission spectroscopy (XES) of the strongest core-to-core emission lines (Kα and Kβ) is now being utilized. Flux demanding valence-to-core XES promises to be an important addition to the time-resolved spectroscopic toolkit. Here In this paper we present measurements and density functional theory calculations on laser-excited, solution-phase ferrocyanide that demonstrate the feasibility of valence-to-core XES for time-resolved experiments. Lastly, we discuss technical improvements that will make valence-to-core XES a practical pump–probe technique.},
doi = {10.1021/jp511838q},
journal = {Journal of Physical Chemistry. C},
number = 26,
volume = 119,
place = {United States},
year = {Mon Feb 09 00:00:00 EST 2015},
month = {Mon Feb 09 00:00:00 EST 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/jp511838q

Citation Metrics:
Cited by: 15 works
Citation information provided by
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