Ultrafast Carrier Dynamics in Nanostructures for Solar Fuels

Sunlight can be used to drive chemical reactions to produce fuels that store energy in chemical bonds. These fuels, such as hydrogen from splitting water, have much larger energy density than do electrical storage devices. The efficient conversion of clean, sustainable solar energy using photoelectrochemical and photocatalytic systems requires precise control over the thermodynamics, kinetics, and structural aspects of materials and molecules. Generation, thermalization, trapping, interfacial transfer, and recombination of photoexcited charge carriers often occur on femtosecond to picosecond timescales. These short timescales limit the transport of photoexcited carriers to nanometer-scale distances, but nanostructures with high surface-to-volume ratios can enable both significant light absorption and high quantum efficiency. This review highlights the importance of understanding ultrafast carrier dynamics for the generation of solar fuels, including case studies on colloidal nanostructures, nanostructured photoelectrodes, and photoelectrodes sensitized with molecular chromophores and catalysts.