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Ultrafast Time-Resolved X-ray Absorption Spectroscopy of Ferrioxalate Photolysis with a Laser Plasma X-ray Source and Microcalorimeter Array

O’Neil, Galen C.; Miaja Avila, Luis; Joe, Young Il; Alpert, Bradley K.; Balasubramanian, Mahalingam; Sagar, D. M.; Doriese, William; Fowler, Joseph W.; Fullagar, Wilfred K. LU and Chen, Zhi Ning, et al. (2017) In The Journal of Physical Chemistry Letters 8(5). p.1099-1104
Abstract

The detailed pathways of photoactivity on ultrafast time scales are a topic of contemporary interest. Using a tabletop apparatus based on a laser plasma X-ray source and an array of cryogenic microcalorimeter X-ray detectors, we measured a transient X-ray absorption spectrum during the ferrioxalate photoreduction reaction. With these high-efficiency detectors, we observe the Fe K edge move to lower energies and the amplitude of the extended X-ray absorption fine structure reduce, consistent with a photoreduction mechanism in which electron transfer precedes disassociation. These results are compared to previously published transient X-ray absorption measurements on the same reaction and found to be consistent with the results from Ogi... (More)

The detailed pathways of photoactivity on ultrafast time scales are a topic of contemporary interest. Using a tabletop apparatus based on a laser plasma X-ray source and an array of cryogenic microcalorimeter X-ray detectors, we measured a transient X-ray absorption spectrum during the ferrioxalate photoreduction reaction. With these high-efficiency detectors, we observe the Fe K edge move to lower energies and the amplitude of the extended X-ray absorption fine structure reduce, consistent with a photoreduction mechanism in which electron transfer precedes disassociation. These results are compared to previously published transient X-ray absorption measurements on the same reaction and found to be consistent with the results from Ogi et al. and inconsistent with the results of Chen et al. (Ogi, Y.; et al. Struct. Dyn. 2015, 2, 034901; Chen, J.; Zhang, H.; Tomov, I. V.; Ding, X.; Rentzepis, P. M. Chem. Phys. Lett. 2007, 437, 50-55). We provide quantitative limits on the Fe-O bond length change. Finally, we review potential improvements to our measurement technique, highlighting the future potential of tabletop X-ray science using microcalorimeter sensors.

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The Journal of Physical Chemistry Letters
volume
8
issue
5
pages
6 pages
publisher
The American Chemical Society
external identifiers
  • scopus:85014377934
  • wos:000395619100033
ISSN
1948-7185
DOI
10.1021/acs.jpclett.7b00078
language
English
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yes
id
34a93080-e96b-44e0-b86c-9dd5c23e25e8
date added to LUP
2017-03-14 13:54:22
date last changed
2018-01-07 11:55:14
@article{34a93080-e96b-44e0-b86c-9dd5c23e25e8,
  abstract     = {<p>The detailed pathways of photoactivity on ultrafast time scales are a topic of contemporary interest. Using a tabletop apparatus based on a laser plasma X-ray source and an array of cryogenic microcalorimeter X-ray detectors, we measured a transient X-ray absorption spectrum during the ferrioxalate photoreduction reaction. With these high-efficiency detectors, we observe the Fe K edge move to lower energies and the amplitude of the extended X-ray absorption fine structure reduce, consistent with a photoreduction mechanism in which electron transfer precedes disassociation. These results are compared to previously published transient X-ray absorption measurements on the same reaction and found to be consistent with the results from Ogi et al. and inconsistent with the results of Chen et al. (Ogi, Y.; et al. Struct. Dyn. 2015, 2, 034901; Chen, J.; Zhang, H.; Tomov, I. V.; Ding, X.; Rentzepis, P. M. Chem. Phys. Lett. 2007, 437, 50-55). We provide quantitative limits on the Fe-O bond length change. Finally, we review potential improvements to our measurement technique, highlighting the future potential of tabletop X-ray science using microcalorimeter sensors.</p>},
  author       = {O’Neil, Galen C. and Miaja Avila, Luis and Joe, Young Il and Alpert, Bradley K. and Balasubramanian, Mahalingam and Sagar, D. M. and Doriese, William and Fowler, Joseph W. and Fullagar, Wilfred K. and Chen, Zhi Ning and Hilton, Gene C. and Jimenez, Ralph and Ravel, Bruce and Reintsema, Carl D. and Schmidt, Dan R. and Silverman, Kevin L. and Swetz, Daniel S. and Uhlig, Jens and Ullom, Joel N.},
  issn         = {1948-7185},
  language     = {eng},
  month        = {03},
  number       = {5},
  pages        = {1099--1104},
  publisher    = {The American Chemical Society},
  series       = {The Journal of Physical Chemistry Letters},
  title        = {Ultrafast Time-Resolved X-ray Absorption Spectroscopy of Ferrioxalate Photolysis with a Laser Plasma X-ray Source and Microcalorimeter Array},
  url          = {http://dx.doi.org/10.1021/acs.jpclett.7b00078},
  volume       = {8},
  year         = {2017},
}