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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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Cited by: 4works
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  • We describe a laser-driven x-ray plasma source designed for ultrafast x-ray absorption spectroscopy. The source is comprised of a 1 kHz, 20 W, femtosecond pulsed infrared laser and a water target. We present the x-ray spectra as a function of laser energy and pulse duration. Additionally, we investigate the plasma temperature and photon flux as we vary the laser energy. We obtain a 75 μm FWHM x-ray spot size, containing ~10 6 photons/s, by focusing the produced x-rays with a polycapillary optic. Since the acquisition of x-ray absorption spectra requires the averaging of measurements from >10 7 laser pulses, wemore » also present data on the source stability, including single pulse measurements of the x-ray yield and the x-ray spectral shape. In single pulse measurements, the x-ray flux has a measured standard deviation of 8%, where the laser pointing is the main cause of variability. Further, we show that the variability in x-ray spectral shape from single pulses is low, thus justifying the combining of x-rays obtained from different laser pulses into a single spectrum. Finally, we show a static x-ray absorption spectrum of a ferrioxalate solution as detected by a microcalorimeter array. Altogether, our results demonstrate that this water-jet based plasma source is a suitable candidate for laboratory-based time-resolved x-ray absorption spectroscopy experiments.« less
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  • No abstract prepared.
  • The dynamics of the laser ablation plume expansion of aluminum was investigated by using space- and time-resolved soft x-ray absorption spectroscopy. Blueshifts of the Al L-shell photoabsorption edge indicating the state of aluminum were observed in the plumes, which were generated by irradiating an aluminum target with 120 fs near-infrared pulses at an intensity of 10{sup 14} W/cm{sup 2}. The spatiotemporal evolution of the plumes exhibited a multilayer structure consisting of vaporized aluminum and condensed aluminum particles, following the expansion of plasma, with expansion velocities of 10{sup 4} m/s for the atomic state and 10{sup 3} m/s for the condensedmore » state.« less