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Title: Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS

Abstract

Femtosecond-resolved Extended X-ray Absorption Fine Structure (EXAFS) measurements of solvated transition metal complexes are successfully implemented at the X-ray Free Electron Laser LCLS. Benchmark experiments on [Fe(terpy)2]2+ in solution show a signal-to-noise ratio on the order of 500, comparable to typical 100 ps-resolution synchrotron measurements. In the few femtoseconds after photoexcitation, we observe the EXAFS fingerprints of a short-lived (B100 fs) intermediate as well as those of a vibrationally hot long-lived (Bns) excited state.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [5]; ORCiD logo [6];  [4];  [4];  [4];  [3];  [6];  [4]
+ Show Author Affiliations
  1. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, USA, Linac Coherent Light Source
  2. Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, USA, Stanford Synchrotron Radiation Lightsource
  3. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, USA
  4. Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, USA
  5. SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, USA
  6. Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, USA
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1558679
Alternate Identifier(s):
OSTI ID: 1546779
Grant/Contract Number:  
AC02-76SF00515; SC0014607
Resource Type:
Published Article
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print) Journal Volume: 22 Journal Issue: 5; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Britz, Alexander, Abraham, Baxter, Biasin, Elisa, van Driel, Tim Brandt, Gallo, Alessandro, Garcia-Esparza, Angel T., Glownia, James, Loukianov, Anton, Nelson, Silke, Reinhard, Marco, Sokaras, Dimosthenis, and Alonso-Mori, Roberto. Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS. United Kingdom: N. p., 2020. Web. doi:10.1039/C9CP03483H.
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Britz, Alexander, Abraham, Baxter, Biasin, Elisa, van Driel, Tim Brandt, Gallo, Alessandro, Garcia-Esparza, Angel T., Glownia, James, Loukianov, Anton, Nelson, Silke, Reinhard, Marco, Sokaras, Dimosthenis, & Alonso-Mori, Roberto. Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS. United Kingdom. doi:https://doi.org/10.1039/C9CP03483H
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Britz, Alexander, Abraham, Baxter, Biasin, Elisa, van Driel, Tim Brandt, Gallo, Alessandro, Garcia-Esparza, Angel T., Glownia, James, Loukianov, Anton, Nelson, Silke, Reinhard, Marco, Sokaras, Dimosthenis, and Alonso-Mori, Roberto. Wed . "Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS". United Kingdom. doi:https://doi.org/10.1039/C9CP03483H.
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@article{osti_1558679,
title = {Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS},
author = {Britz, Alexander and Abraham, Baxter and Biasin, Elisa and van Driel, Tim Brandt and Gallo, Alessandro and Garcia-Esparza, Angel T. and Glownia, James and Loukianov, Anton and Nelson, Silke and Reinhard, Marco and Sokaras, Dimosthenis and Alonso-Mori, Roberto},
abstractNote = {Femtosecond-resolved Extended X-ray Absorption Fine Structure (EXAFS) measurements of solvated transition metal complexes are successfully implemented at the X-ray Free Electron Laser LCLS. Benchmark experiments on [Fe(terpy)2]2+ in solution show a signal-to-noise ratio on the order of 500, comparable to typical 100 ps-resolution synchrotron measurements. In the few femtoseconds after photoexcitation, we observe the EXAFS fingerprints of a short-lived (B100 fs) intermediate as well as those of a vibrationally hot long-lived (Bns) excited state.},
doi = {10.1039/C9CP03483H},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 5,
volume = 22,
place = {United Kingdom},
year = {2020},
month = {2}
}
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DOI: https://doi.org/10.1039/C9CP03483H
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