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Title:OBSERVATION OF TRANSIENT HIGH-VALENT STATES IN THE WATER OXIDATION CATALYST CoIII4O4 CUBANE VIA EXTREME ULTRAVIOLET SPECTROSCOPY
Author(s):Shari'ati, Yusef A.
Contributor(s):Vura-Weis, Josh
Subject(s):Mini-symposium: High-Harmonic Generation and XUV Spectroscopy
Abstract:\begin{wrapfigure}{r}{0pt} \includegraphics[scale=0.35]{CubanePET.eps} \end{wrapfigure} The tetranuclear metal-oxo complex [Co$^{III}$$_{4}$O$_{4}$](OAc)$_{4}$(py)$_{4}$ is a homogeneous water oxidation catalyst and structural mimic of the oxygen evolving complex in photosynthetic organisms. The catalytic cycle involves a highly-oxidized intermediate the nature of which is controversial: leading formulations argue for either [Co$^{IV}$$_{2}$Co$^{III}$$_{2}$O$_{4}$] or [Co$^{V}$Co$^{III}$$_{3}$O$_{4}$]. We report the sensitization of the [Co$^{III}$$_{4}$O$_{4}$] cubane with a perylene bisimide dye thus enabling photoinduced electron transfer upon green light illumination and effecting a transient oxidation of the cobalt center(s). The resultant high-valent states and their dynamics are probed by ultrafast transient absorption and extreme ultraviolet (XUV) spectroscopies. XUV spectroscopy, by dint of its oxidation-state specificity, has the potential to reveal the true distribution of holes among cobalt centers within the oxidized cluster.
Issue Date:2019-06-19
Publisher:International Symposium on Molecular Spectroscopy
Genre:Conference Paper / Presentation
Type:Text
Language:English
URI:http://hdl.handle.net/2142/104340
DOI:10.15278/isms.2019.WE04
Rights Information:Copyright 2019 Yusef A. Shari'ati
Date Available in IDEALS:2019-07-15
2020-01-25


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