Abstract
In order to utilize solar power for the production of solar electricity and solar fuels on a global scale, it is necessary to develop solar photon conversion systems that have an appropriate combination of very high efficiency (delivered watts/m2) and low capital cost ($/m2). One potential promising approach to attain high conversion efficiencies well above the Shockley-Queisser limit of 33% is to utilize the unique properties of semiconductor nanostructures (viz., quantum dots/rods/films) and singlet fission chromophores to control the relaxation dynamics of photogenerated carriers and photochemical excited states, respectively. The former process creates enhanced photocurrent through efficient photogenerated electron-hole pair multiplication (electron-hole pairs exist as excitons in size-quantized nanostructures), or enhanced photopotential through hot carrier transport, transfer, and extraction processes. The latter process of singlet fission generates two triplets from an excited singlet state. These fundamental dynamics in various bulk and nanoscale semiconductors and in molecular chromophores have been studied using transient absorption, photoluminescence, photocurrent and THz spectroscopy with fs to ns time resolution. The predictions that the generation of more than one electron-hole pair or exciton per absorbed photon would be an efficient process in nanostructures, and via singlet fission, have been confirmed in different classes of materials, molecules, and their architectures in photon conversion devices. Selected aspects of this work will be summarized and recent advances will be discussed, including the very remarkable and beneficial theoretical effects of combining MEG or singlet fission with solar concentration and controlling the thicknesses of the photoactive layers in a two-photon photoelectrosynthesis cell structure for solar fuels.
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