Ultraviolet photochemical reaction of [Fe(III)(C2O4)3](3-) in aqueous solutions studied by femtosecond time-resolved X-ray absorption spectroscopy using an X-ray free electron laser

Structural Dynamics
Yoshihiro OgiToshinori Suzuki

Abstract

Time-resolved X-ray absorption spectroscopy was performed for aqueous ammonium iron(III) oxalate trihydrate solutions using an X-ray free electron laser and a synchronized ultraviolet laser. The spectral and time resolutions of the experiment were 1.3 eV and 200 fs, respectively. A femtosecond 268 nm pulse was employed to excite [Fe(III)(C2O4)3](3-) in solution from the high-spin ground electronic state to ligand-to-metal charge transfer state(s), and the subsequent dynamics were studied by observing the time-evolution of the X-ray absorption spectrum near the Fe K-edge. Upon 268 nm photoexcitation, the Fe K-edge underwent a red-shift by more than 4 eV within 140 fs; however, the magnitude of the redshift subsequently diminished within 3 ps. The Fe K-edge of the photoproduct remained lower in energy than that of [Fe(III)(C2O4)3](3-). The observed red-shift of the Fe K-edge and the spectral feature of the product indicate that Fe(III) is upon excitation immediately photoreduced to Fe(II), followed by ligand dissociation from Fe(II). Based on a comparison of the X-ray absorption spectra with density functional theory calculations, we propose that the dissociation proceeds in two steps, forming first [(CO2 (•))Fe(II)(C2O4)2](3-) a...Continue Reading

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Citations

Mar 24, 2016·Journal of the American Chemical Society·Barry K CarpenterAndrew J Orr-Ewing
Oct 24, 2017·Reports on Progress in Physics·E A SeddonW Wurth
Aug 15, 2018·Physical Chemistry Chemical Physics : PCCP·Steffen StraubPeter Vöhringer
Mar 12, 2019·Journal of Synchrotron Radiation·Tetsuo KatayamaMakina Yabashi
Dec 4, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Peter Vöhringer
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May 10, 2017·Chemical Communications : Chem Comm·Yohei UemuraKiyotaka Asakura
Dec 14, 2018·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Eva Muchová, Petr Slavíček
Jan 30, 2018·Structural Dynamics·Rafael AbelaLuc Patthey
Oct 20, 2019·Nature Communications·Yves KayserJakub Szlachetko
Oct 30, 2019·Physical Chemistry Chemical Physics : PCCP·Frank Hendrik PilzPeter Vöhringer
Jun 15, 2021·Photochemistry and Photobiology·Joseph RabaniJames R Bolton
Sep 6, 2017·Journal of Chemical Theory and Computation·Martina RubešováPetr Slavíček
Nov 9, 2021·Physical Chemistry Chemical Physics : PCCP·L LongettiM Chergui
Dec 17, 2021·The Journal of Physical Chemistry Letters·Yujin KimTae Kyu Kim

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Methods Mentioned

BETA
X-ray
profiler

Software Mentioned

Gaussian09
FEFF6
ORCA
TDDFT

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