Photooxidation and photoaquation of iron hexacyanide in aqueous solution: A picosecond X-ray absorption study

Structural Dynamics
M ReinhardMajed Chergui

Abstract

We present a picosecond Fe K-edge absorption study of photoexcited ferrous and ferric hexacyanide in water under 355 and 266 nm excitation. Following 355 nm excitation, the transient spectra for the ferrous and ferric complexes exhibit a red shift of the edge reflecting an increased electron density at the Fe atom. For the former, an enhanced pre-edge transition is also observed. These observations are attributed to the aquated [Fe(CN)5OH2](3-) species, based on quantum chemical calculations which also provide structural parameters. Upon 266 nm excitation of the ferric complex, a transient reminiscent of the aquated species is observed (appearance of a pre-edge feature and red shift of the edge) but it is different from that obtained under 355 nm excitation. This points to a new reaction channel occurring through an intermediate state lying between these two excitation energies. Finally, 266 nm excitation of the ferrous species is dominated by the photooxidation channel with formation of the ferric complex as main photoproduct. However, we observe an additional minor photoproduct, which is identical to the 266 nm generated photoproduct of the ferric species, suggesting that under our experimental conditions, the pump pulse phot...Continue Reading

References

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Jan 10, 2013·The Journal of Chemical Physics·T J PenfoldM Chergui
Jul 4, 2013·Nature Communications·Fabrizio MessinaMajed Chergui

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Citations

Apr 9, 2020·Chemical Record : an Official Publication of the Chemical Society of Japan ... [et Al.]·Julien Eng, Thomas J Penfold
Jan 25, 2018·Physical Chemistry Chemical Physics : PCCP·Kasper S KjærKelly J Gaffney
Oct 7, 2015·Proceedings of the National Academy of Sciences of the United States of America·Mahsa SilataniMajed Chergui
Jan 16, 2018·Structural Dynamics·Hans Jakob WörnerOliver Wenger
May 24, 2017·Physical Chemistry Chemical Physics : PCCP·Nicholas EngelEmad F Aziz
May 22, 2019·Faraday Discussions·Majed Chergui
Feb 24, 2019·The Journal of Chemical Physics·Majed Chergui
Aug 28, 2020·Proceedings of the National Academy of Sciences of the United States of America·Camila BacellarMajed Chergui
Jun 18, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Marwah M M MadkhaliThomas J Penfold
Mar 18, 2021·The Journal of Physical Chemistry. a·C D Rankine, T J Penfold
Oct 29, 2015·The Journal of Physical Chemistry Letters·Fabrizio MessinaMajed Chergui
Jun 13, 2015·The Journal of Physical Chemistry. a·G CapanoT J Penfold
Nov 17, 2015·The Journal of Physical Chemistry. C, Nanomaterials and Interfaces·Anne Marie MarchGyörgy Vankó
May 10, 2017·Journal of the American Chemical Society·Marco ReinhardMajed Chergui
Sep 17, 2014·The Journal of Physical Chemistry. a·T J PenfoldM Chergui
Sep 10, 2019·The Journal of Physical Chemistry Letters·Meixin ChengGermán Sciaini
Oct 31, 2017·Journal of the American Chemical Society·Aditi BhattacherjeeStephen R Leone
Jan 17, 2020·Ultrasonics Sonochemistry·Paulina Rajchel-MieldzioćPiotr Fita

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Methods Mentioned

BETA
X-ray

Software Mentioned

ORCA
COSMO
Finite Difference Method Near Edge Structure ( FDMNES )

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