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Ferricyanide photo-...
Ferricyanide photo-aquation pathway revealed by combined femtosecond Kβ main line and valence-to-core x-ray emission spectroscopy
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- Reinhard, Marco (author)
- Stanford Linear Accelerator Center (SLAC)
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- Gallo, Alessandro (author)
- Stanford Linear Accelerator Center (SLAC)
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- Guo, Meiyuan (author)
- Stanford Linear Accelerator Center (SLAC)
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- Garcia-Esparza, Angel T. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Biasin, Elisa (author)
- Pacific Northwest National Laboratory
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- Qureshi, Muhammad (author)
- Stanford Linear Accelerator Center (SLAC)
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- Britz, Alexander (author)
- Stanford Linear Accelerator Center (SLAC)
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- Ledbetter, Kathryn (author)
- Harvard University,Stanford University
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- Kunnus, Kristjan (author)
- Stanford Linear Accelerator Center (SLAC)
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- Weninger, Clemens (author)
- Lund University,Lunds universitet,MAX IV, Vetenskaplig Data,MAX IV, Tekniska divisionen,MAX IV-laboratoriet,MAX IV, Scientific Data,MAX IV, Technical division,MAX IV Laboratory,Stanford Linear Accelerator Center (SLAC)
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- van Driel, Tim (author)
- Stanford Linear Accelerator Center (SLAC)
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- Robinson, Joseph (author)
- Stanford Linear Accelerator Center (SLAC)
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- Glownia, James M. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Gaffney, Kelly J. (author)
- Stanford Linear Accelerator Center (SLAC)
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- Kroll, Thomas (author)
- Stanford Linear Accelerator Center (SLAC)
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- Weng, Tsu Chien (author)
- ShanghaiTech University
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- Alonso-Mori, Roberto (author)
- Stanford Linear Accelerator Center (SLAC)
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- Sokaras, Dimosthenis (author)
- Stanford Linear Accelerator Center (SLAC)
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(creator_code:org_t)
- 2023
- 2023
- English.
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In: Nature Communications. - 2041-1723. ; 14:1
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http://dx.doi.org/10... (free)
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https://lup.lub.lu.s...
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https://doi.org/10.1...
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Abstract
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- 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.
Subject headings
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
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- art (subject category)
- ref (subject category)
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- By the author/editor
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Reinhard, Marco
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Gallo, Alessandr ...
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Guo, Meiyuan
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Garcia-Esparza, ...
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Biasin, Elisa
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Qureshi, Muhamma ...
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show more...
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Britz, Alexander
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Ledbetter, Kathr ...
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Kunnus, Kristjan
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Weninger, Clemen ...
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van Driel, Tim
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Robinson, Joseph
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Glownia, James M ...
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Gaffney, Kelly J ...
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Kroll, Thomas
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Weng, Tsu Chien
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Alonso-Mori, Rob ...
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Sokaras, Dimosth ...
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- About the subject
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Physical Chemist ...
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Nature Communica ...
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Lund University