Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.084
Publication date: 6th July 2018
Generating multiple excitons by a single high-energy photon is a promising third generation solar energy conversion strategy. I will discuss recent progress within the Center for Advanced Solar Photophysics (CASP) on both improving the multple exciton generation (MEG) efficiency in heterostructured nanostructures as well as in the using MEG in the production of solar fuels. We are exploring MEG in PbE|CdE (E = S, Se) Janus-like hetero-nanostructures and find that MEG is enhanced over that of single-component and core/shell nanocrystal architectures. The enhanced MEG arrises due to the asymmetric nature of the hetero-nanostructure that results in an increase in the effective Coulomb interaction that drives MEG and a reduction of the competing hot exciton cooling rate. We find that slowed cooling occurs through effective trapping of hot-holes by a manifold of valence band interfacial states having character of both PbS and CdS. The Janus-like NCs retain their symmetric structure and thus can be easily incorporated as the main absorber layer in functional solid-state solar cell architectures. Finally, based upon our analysis, we provide design rules for the next generation of engineered nanocrystals to further improve the MEG characteristics. In addition, we have developed a PbS QD photoelectrochemical cell that is able to drive a hydrogen evolution reaction with a peak external quantum efficiency (EQE) of over 100%, with the highest EQE at 114±1.3%. Our results show that the extra carriers produced via MEG can be used to drive a chemical reaction with above unity quantum efficiency thus demonstrating a new direction in exploring high efficiency approaches for solar fuels. I will discuss the potential for using MEG to drive a photochemical reaction as opposed to use in a solar cell.
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