Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource

Reinhard, Marco; Skoien, Dean; Spies, Jacob A.; Garcia-Esparza, Angel T.; Matson, Benjamin D.; Corbett, Jeff; Tian, Kai; Safranek, James; Granados, Eduardo; Strader, Matthew; Gaffney, Kelly J.; Alonso-Mori, Roberto; Kroll, Thomas; Sokaras, Dimosthenis

doi:10.1063/4.0000207

Title: Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource

Journal Article · Fri Oct 27 00:00:00 EDT 2023 · Structural Dynamics

DOI:https://doi.org/10.1063/4.0000207· OSTI ID:2202664

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SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Yale University, New Haven, CT (United States)

We present a dedicated end-station for solution phase high repetition rate (MHz) picosecond hard x-ray spectroscopy at beamline 15-2 of the Stanford Synchrotron Radiation Lightsource. A high-power ultrafast ytterbium-doped fiber laser is used to photoexcite the samples at a repetition rate of 640 kHz, while the data acquisition operates at the 1.28 MHz repetition rate of the storage ring recording data in an alternating on-off mode. The time-resolved x-ray measurements are enabled via gating the x-ray detectors with the 20 mA/70 ps camshaft bunch of SPEAR3, a mode available during the routine operations of the Stanford Synchrotron Radiation Lightsource. As a benchmark study, aiming to demonstrate the advantageous capabilities of this end-station, we have conducted picosecond Fe K-edge x-ray absorption spectroscopy on aqueous [Fe^II(phen)₃]²⁺, a prototypical spin crossover complex that undergoes light-induced excited spin state trapping forming an electronic excited state with a 0.6–0.7 ns lifetime. In addition, we report transient Fe Kβ main line and valence-to-core x-ray emission spectra, showing a unique detection sensitivity and an excellent agreement with model spectra and density functional theory calculations, respectively. Notably, the achieved signal-to-noise ratio, the overall performance, and the routine availability of the developed end-station have enabled a systematic time-resolved science program using the monochromatic beam at the Stanford Synchrotron Radiation Lightsource.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER); National Institutes of Health (NIH); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS)

Contributing Organization:: SS

Grant/Contract Number:: AC02-76SF00515; P30GM133894; AC02-05CH11231; SC0014664

OSTI ID:: 2202664

Journal Information:: Structural Dynamics, Vol. 10, Issue 5; ISSN 2329-7778

Publisher:: American Crystallographic Association/AIPCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource

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