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Title: Ultrafast time-resolved X-ray absorption spectroscopy of ferrioxalate photolysis with a laser plasma X-ray source and microcalorimeter array

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. 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.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [2];  [3];  [1];  [1];  [4];  [5];  [1]; ORCiD logo [3];  [6];  [1];  [1];  [1];  [1];  [4];  [7]
  1. National Institute of Standards and Technology, Boulder, CO (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. National Institute of Standards and Technology and Univ. of Colorado, Boulder, CO (United States)
  4. Lund Univ., Lund (Sweden)
  5. Canadian Light Source, Saskatoon, SK (Canada)
  6. National Institute of Standards and Technology, Gaithersburg, MD (United States)
  7. National Institute of Standards and Technology, Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1344424
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
47 OTHER INSTRUMENTATION; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

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., Chen, Ning, Hilton, Gene C., Jimenez, Ralph, Ravel, Bruce, Reintsema, Carl D., Schmidt, Dan R., Silverman, Kevin L., Swetz, Daniel S., Uhlig, Jens, and Ullom, Joel N. Ultrafast time-resolved X-ray absorption spectroscopy of ferrioxalate photolysis with a laser plasma X-ray source and microcalorimeter array. United States: N. p., 2017. Web. doi:10.1021/acs.jpclett.7b00078.
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., Chen, Ning, Hilton, Gene C., Jimenez, Ralph, Ravel, Bruce, Reintsema, Carl D., Schmidt, Dan R., Silverman, Kevin L., Swetz, Daniel S., Uhlig, Jens, & Ullom, Joel N. Ultrafast time-resolved X-ray absorption spectroscopy of ferrioxalate photolysis with a laser plasma X-ray source and microcalorimeter array. United States. doi:10.1021/acs.jpclett.7b00078.
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., Chen, Ning, Hilton, Gene C., Jimenez, Ralph, Ravel, Bruce, Reintsema, Carl D., Schmidt, Dan R., Silverman, Kevin L., Swetz, Daniel S., Uhlig, Jens, and Ullom, Joel N. Fri . "Ultrafast time-resolved X-ray absorption spectroscopy of ferrioxalate photolysis with a laser plasma X-ray source and microcalorimeter array". United States. doi:10.1021/acs.jpclett.7b00078. https://www.osti.gov/servlets/purl/1344424.
@article{osti_1344424,
title = {Ultrafast time-resolved X-ray absorption spectroscopy of ferrioxalate photolysis with a laser plasma X-ray source and microcalorimeter array},
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, 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.},
abstractNote = {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.},
doi = {10.1021/acs.jpclett.7b00078},
journal = {Journal of Physical Chemistry Letters},
number = ,
volume = 8,
place = {United States},
year = {Fri Feb 17 00:00:00 EST 2017},
month = {Fri Feb 17 00:00:00 EST 2017}
}

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