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Challenges in Using Quantum Dot-Molecule Complexes for Production of Solar Fuels and Strategies to Address Them

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This thesis describes fundamental photophysical studies of quantum dot (QD)-molecule complexes, aimed at discovering strategies for enhancing the efficiency of QD-photocatalyzed and QD-sensitized multi-electron catalytic reactions, for the purpose of solar fuels production. Photosensitization of molecular catalysts that are active for reactions such as the reduction of carbon dioxide or protons and oxidation of water is a sustainable route to storable solar fuels. As photosensitizers, QDs provide many unique advantages over traditional organic chromophores because of their (i) high absorptivity across the UV, visible and near-infrared spectral regions, (ii) large surface-area-to-volume ratio, and (iii) tunable absorption spectra and redox potentials. Currently, there are two major challenges that limit the photocatalytic efficiency of QD-molecule catalyst complexes for the production of solar fuels: (i) the mismatch between fast electron delivery from the QD to the catalyst and slow hole extraction from the QD; and (ii) the slow rate of creation of excitons in QD sensitizers. The projects that I outlined in this thesis are designed to address these two challenges.

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