Ferricyanide photo-aquation pathway revealed by combined femtosecond Kβ main line and valence-to-core x-ray emission spectroscopy

Reinhard, Marco; Gallo, Alessandro; Guo, Meiyuan; Garcia-Esparza, Angel T.; Biasin, Elisa; Qureshi, Muhammad; Britz, Alexander; Ledbetter, Kathryn; Kunnus, Kristjan; Weninger, Clemens; van Driel, Tim; Robinson, Joseph; Glownia, James M.; Gaffney, Kelly J.; Kroll, Thomas; Weng, Tsu-Chien; Alonso-Mori, Roberto; Sokaras, Dimosthenis

doi:10.1038/s41467-023-37922-x

Title: Ferricyanide photo-aquation pathway revealed by combined femtosecond Kβ main line and valence-to-core x-ray emission spectroscopy

Journal Article · 04 May 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-37922-x · OSTI ID:1972199

^[1];

^[2];

^[3]; Qureshi, Muhammad ^[2]; Britz, Alexander ^[2];

^[4]; Kunnus, Kristjan ^[2]; Weninger, Clemens ^[2]; van Driel, Tim ^[2]; Robinson, Joseph ^[2]; Glownia, James M. ^[2];

^[2]; Kroll, Thomas ^[2]; Weng, Tsu-Chien ^[5];

^[2];

^[2]

SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); SLAC National Accelerator Laboratory
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Stanford University, CA (United States)
Shanghai Technical University (China)

Reliably identifying short-lived chemical reaction intermediates is crucial to elucidate reaction mechanisms but becomes particularly challenging when multiple transient species occur simultaneously. Here, we report a femtosecond x-ray emission spectroscopy and scattering study of the aqueous ferricyanide photochemistry, utilizing the combined Fe Kβ main and valence-to-core emission lines. Following UV-excitation, we observe a ligand-to-metal charge transfer excited state that decays within 0.5 ps. On this timescale, we also detect a hitherto unobserved short-lived species that we assign to a ferric penta-coordinate intermediate of the photo-aquation reaction. We provide evidence that bond photolysis occurs from reactive metal-centered excited states that are populated through relaxation of the charge transfer excited state. Beyond illuminating the elusive ferricyanide photochemistry, these results show how current limitations of Kβ main line analysis in assigning ultrafast reaction intermediates can be circumvented by simultaneously using the valence-to-core spectral range.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Institutes of Health (NIH); USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

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

OSTI ID:: 1972199

Alternate ID(s):: OSTI ID: 2007384

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Ferricyanide photo-aquation pathway revealed by combined femtosecond Kβ main line and valence-to-core x-ray emission spectroscopy

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