A Flat Analyzer Polycapillary Spectrometer for X-ray Absorption Spectroscopy of Dilute Transition Metals at X-ray-Free Electron Lasers

Garcia-Esparza, Angel T.; Lim, Jinkyu; Britz, Alexander; Reinhard, Marco; Ribson, Ryan D.; Babicz, Jeffrey T.; Antolini, Cali; Gee, Leland B.; Claussen, Quinn; Boiadjieva, Nina A.; Hsiao, Leslie; Defever, Jim; Oppermann, Patrick; Esposito, Vincent; Yavas, Hasan; Skoien, Dean; Chollet, Matthieu; van Driel, Tim B.; Song, Sanghoon; Zhu, Diling; Sokaras, Dimosthenis; Alonso-Mori, Roberto

doi:10.1021/photonsci.5c00024

A Flat Analyzer Polycapillary Spectrometer for X-ray Absorption Spectroscopy of Dilute Transition Metals at X-ray-Free Electron Lasers

Journal Article · Sun Dec 14 00:00:00 EST 2025 · Photon Science

DOI:https://doi.org/10.1021/photonsci.5c00024· OSTI ID:3024710

^[1]; ^[2]; ^[1]; ^[1]; ^[1]; Babicz, Jeffrey T. ^[1]; Antolini, Cali ^[1]; ^[1]; Claussen, Quinn ^[1]; Boiadjieva, Nina A. ^[1]; Hsiao, Leslie ^[1]; Defever, Jim ^[1]; Oppermann, Patrick ^[1]; Esposito, Vincent ^[1]; Yavas, Hasan ^[1]; Skoien, Dean ^[1]; ^[1]; ^[1]; Song, Sanghoon ^[1]; Zhu, Diling ^[1] more »

SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Hanbat National Univ. (Korea, Republic of)

X-ray absorption spectroscopy (XAS) coupled with highly intense pulses from an X-ray-free electron laser (XFEL) can be used to track ultrafast chemical dynamics. Nonetheless, measurements for dilute samples (≤1 mM) have been exceptionally challenging, as scattering background signals dominate over the sample’s X-ray fluorescence. We show that femtosecond time-resolved XAS measurements of sub-millimolar transition metal solutions are now possible at the Linac Coherent Light Source (LCLS) using a high-throughput polycapillary XAS spectrometer, designed, developed, and commissioned at LCLS and the Stanford Synchrotron Radiation Lightsource (SSRL). The instrument integrates three polycapillary optics that collect and collimate X-ray fluorescence emitted from the interaction point with a high solid angle. X-ray collimated fluorescence is then selectively diffracted by coupled graphite analyzer crystals. As a result, the contribution of scattered photons is suppressed. Experiments at the Pt L₃-edge on 0.1 mM aqueous K₂PtCl₆ (delivered via a 100 μm liquid jet) were successfully performed in the laser pump X-ray probe configuration at the LCLS XCS and XPP instruments. We report the transient spectra of hexachloroplatinate within the first 10 ps after a 266 nm photoexcitation. We observed a short-lived reduced intermediate (≈2 ps). The polycapillary X-ray spectrometer at LCLS now enables the efficient study of the dynamics of ultradilute transition metals in solution. This capability opens the door to investigating plasmonic systems, photocatalysts, enzymes, and other scarce and dilute samples.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

Other Award/Contract Number:: P41GM139687

OSTI ID:: 3024710

Journal Information:: Photon Science, Journal Name: Photon Science Journal Issue: 2 Vol. 1; ISSN 2998-8799

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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SSRL
polycapillary optics
time-resolved
ultrafast spectroscopy
x-ray absorption spectroscopy
x-ray free electron laser

A Flat Analyzer Polycapillary Spectrometer for X-ray Absorption Spectroscopy of Dilute Transition Metals at X-ray-Free Electron Lasers

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