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

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

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22 Citeringar (SciVal)

Sammanfattning

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.

Originalspråkengelska
Sidor (från-till)1099-1104
Antal sidor6
TidskriftThe Journal of Physical Chemistry Letters
Volym8
Utgåva5
DOI
StatusPublished - 2017 mar 2

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