FN Thomson Reuters Web of Science™
VR 1.0
PT J
AU Smolentsev, Grigory
   Guda, Alexander A.
   Janousch, Markus
   Frieh, Cristophe
   Jud, Gaudenz
   Zamponi, Flavio
   Chavarot-Kerlidou, Murielle
   Artero, Vincent
   van Bokhoven, Jeroen A.
   Nachtegaal, Maarten
TI X-ray absorption spectroscopy with time-tagged photon counting:
   application to study the structure of a Co(I) intermediate of H-2
   evolving photo-catalyst
SO FARADAY DISCUSSIONS
VL 171
BP 259
EP 273
DI 10.1039/c4fd00035h
PD 2014
PY 2014
AB In order to probe the structure of reaction intermediates of
   photochemical reactions a new setup for laser-initiated time-resolved
   X-ray absorption (XAS) measurements has been developed. With this
   approach the arrival time of each photon in respect to the laser pulse
   is measured and therefore full kinetic information is obtained. All
   X-rays that reach the detector are used to measure this kinetic
   information and therefore the detection efficiency of this method is
   high. The newly developed setup is optimized for timeresolved
   experiments in the microsecond range for samples with relatively low
   metal concentration (similar to 1mM). This setup has been applied to
   study a multicomponent photocatalytic system with a Co(dmgBF(2))(2)
   catalyst (dmg2(-) = dimethylglyoximato dianion), [Ru(bpy)(3)](2+)
   chromophore (bpy = 2,2'-bipyridine) and methyl viologen as the electron
   relay. On the basis of the analysis of hundreds of Co K-edge XAS spectra
   corresponding to different delay times after the laser excitation of the
   chromophore, the presence of a Co(I) intermediate is confirmed. The
   calculated X-ray transient signal for a model of Co(I) state with a 0.14
   angstrom displacement of Co out of the dmg ligand plane and with the
   closest solvent molecule at a distance of 2.06 angstrom gives reasonable
   agreement with the experimental data.
RI Guda, Alexander/A-3671-2015
OI Guda, Alexander/0000-0002-6941-4987
ZB 0
Z8 0
ZR 0
ZS 0
TC 7
Z9 7
SN 1359-6640
EI 1364-5498
UT WOS:000345529900014
PM 25415460
ER

EF