Ultrafast time-resolved X-ray absorption spectroscopy of ferrioxalate photolysis with a laser plasma X-ray source and microcalorimeter array
Journal Article
·
· Journal of Physical Chemistry Letters
- National Institute of Standards and Technology, Boulder, CO (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- National Institute of Standards and Technology and Univ. of Colorado, Boulder, CO (United States)
- Lund Univ., Lund (Sweden)
- Canadian Light Source, Saskatoon, SK (Canada)
- National Institute of Standards and Technology, Gaithersburg, MD (United States)
- National Institute of Standards and Technology, Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States)
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. We provide quantitative limits on the Fe–O bond length change. Lastly, we review potential improvements to our measurement technique, highlighting the future potential of tabletop X-ray science using microcalorimeter sensors.
- Research Organization:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
- Grant/Contract Number:
- AC02-06CH11357
- OSTI ID:
- 1344424
- Journal Information:
- Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Vol. 8; ISSN 1948-7185
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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