Proceedings of nanoGe September Meeting 2017 (NFM17)
Publication date: 20th June 2016
I will address the role of charge carrier dynamics in determining the efficiency of solar driven fuel synthesis, focusing on photoelectrodes for water oxidation and reduction. Experimentally, these studies will be based around transient absorption spectroscopy on timescales from femtoseconds to seconds, which will be correlated with the results of photoelectrochemical analyses of device efficiency. These studies will address the dynamics of charge separation and recombination, as well as the kinetics of water oxidation / reduction at semiconductor / liquid interfaces. Issues which will be addressed will include the underlying photochemistry of oxides, the role of the space charge layers at electrochemical junctions in spatially separating charges, and the role of heterojunctions and catalysts layers in enhancing system efficiency. Particular consideration will be placed on analysis of the mechanism of water oxidation / reduction, and the extent to which oxide surfaces function as heterogeneous catalysts for this reaction. These studies will be based on rate law analysis of water oxidation reduction for different photoelectrodes, and as a function of temperature, pH and kinetic isotope exchange, and correlated with TD-DFT calculations of catalytic mechanism