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- W2322736054 abstract "The average molecular orientation of several rheniumbipyridyl CO2-reduction catalysts adsorbed onto rutile singlecrystalline TiO2 surfaces has been determined using vibrational sumfrequency generation spectroscopy (VSFGS). The vibrationalrelaxation dynamics of two such catalysts were also investigated ontwo model electrode surfaces using time-resolved VSFGS techniques.Polarization-resolved VSFGS was used to determine the averagemolecular orientation of ReC0A on TiO2 (001), which was found to bewithin 0 - 22° from the surface normal. These results weresupported by Density Functional Theory (DFT) calculations ofoptimized adsorption geometries. The influence of the substrate onthe molecular organization was investigated by monitoring thedegree of surface-induced ordering for ReC0A on TiO2 (110). ReC0Aexhibited a well-defined anisotropic arrangement following the C2vsymmetry of the TiO2 (110) surface, in contrast to an isotropicdistribution on the more symmetric (C4) TiO2 (001) surface. Anaverage orientation angle of 28° was determined for the ReC0A/TiO2(110) system. The influence of lengthening the molecular linkers ina similar system was determined by investigating the adsorptiongeometries for the series ReCnA (n = 0 - 4) on TiO2 (001) usingphase-sensitive VSFGS and DFT calculations. The orientation angleswere found to be closely correlated with the average lengths of thetwo linking anchoring groups, with the molecules tilting moretowards the TiO2 surface with increasing linker length.Time-resolved VSFGS was used to investigate the vibrationalrelaxation dynamics of the totally symmetric CO stretch of ReC0A onTiO2 (110) and ReC0-Au. Both systems exhibited bi-exponentialrelaxation from the I� = 1 state consisting of an ultrafast(sub-picosecond) initial relaxation followed by complete recoveryof the ground vibrational state within tens of picoseconds. Theultrafast decay is assigned to rapid I�-I� coupling between thethree CO stretching modes, and the slower decay is assigned tovibrational population relaxation from the coupled CO modes.Although both systems exhibited similar ultrafast decay rates ofthe excited state, the excited a'(1) mode persisted forsignificantly longer in ReC0A on TiO2 compared to ReC0-Au (I�2 =30.35 and 14.8 ps, respectively). This is attributed to electronicinteractions between ReC0A and TiO2 not present in the ReC0-Ausystem." @default.
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- W2322736054 date "2012-01-01" @default.
- W2322736054 modified "2023-09-24" @default.
- W2322736054 title "Orientation and Vibrational Dynamics of Rhenium BipyridylCO2-Reduction Catalysts on Model Electrode Surfaces" @default.
- W2322736054 hasPublicationYear "2012" @default.
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