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Jens Uhlig. Portrait.

Jens Uhlig

Senior lecturer

Jens Uhlig. Portrait.

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

Author

  • Galen C. O’Neil
  • Luis Miaja Avila
  • Young Il Joe
  • Bradley K. Alpert
  • Mahalingam Balasubramanian
  • D. M. Sagar
  • William Doriese
  • Joseph W. Fowler
  • Wilfred K. Fullagar
  • Zhi Ning Chen
  • Gene C. Hilton
  • Ralph Jimenez
  • Bruce Ravel
  • Carl D. Reintsema
  • Dan R. Schmidt
  • Kevin L. Silverman
  • Daniel S. Swetz
  • Jens Uhlig
  • Joel N. Ullom
Show all

Summary, in English

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.

Department/s

  • Chemical Physics

Publishing year

2017-03-02

Language

English

Pages

1099-1104

Publication/Series

The Journal of Physical Chemistry Letters

Volume

8

Issue

5

Document type

Journal article (letter)

Publisher

The American Chemical Society (ACS)

Topic

  • Physical Chemistry (including Surface- and Colloid Chemistry)

Status

Published

ISBN/ISSN/Other

  • ISSN: 1948-7185