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

Forskningsoutput: TidskriftsbidragLetter

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 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.

Detaljer

Författare
  • 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
Enheter & grupper
Externa organisationer
  • National Institute of Standards and Technology (NIST)
  • Argonne National Laboratory
  • University of Colorado
  • Canadian Light Source
Forskningsområden

Ämnesklassifikation (UKÄ) – OBLIGATORISK

  • Fysikalisk kemi
Originalspråkengelska
Sidor (från-till)1099-1104
Antal sidor6
TidskriftThe Journal of Physical Chemistry Letters
Volym8
Utgåva nummer5
StatusPublished - 2017 mar 2
PublikationskategoriForskning
Peer review utfördJa