Ultrafast photoinduced dynamics in quantum dot-based systems for light harvesting

Colloidal semiconductor nanocrystals, referred to as quantum dots, offer simple low-temperature solution-based methods for constructing optoelectronic devices such as light emitting diodes and solar cells. We review recent progress in the understanding of photoinduced processes in key components of a certain type of quantum dot solar cells where the dots sensitize a suitable metal oxide, such as ZnO or TiO₂, for electron injection, and NiO for hole injection. The electron and hole injection dynamics are discussed in detail as a function of the quantum dot size and core-shell structure, the linker molecule type, and the morphology of the accepting metal oxide. Hole trapping is identified as a major factor limiting the performance of quantum dot-based devices. We review possible strategies for improvement that use core-shell structures and directed excitation energy transfer between quantum dots. Finally, the generation and injection of multiple excitons are revisited. We show that the assumption of a linear relationship between the intensity of transient absorption signal and the number of excitons does not generally hold, and this observation can partially explain highly disparate results for the efficiency of generating multiple excitons. A consistent calculation procedure for studies of multiple exciton generation is provided. Finally, we offer a brief personal outlook on the topic.