Nanoscale Photoinduced Charge Transfer with Individual Quantum Dots: Tunability through Synthesis, Interface Design, and Interaction with Charge Traps.

Semiconducting colloidal quantum dots (QDs) provide an excellent platform for nanoscale charge-transfer studies. Because of their size-dependent optoelectronic properties, which can be tuned via chemical synthesis and of their versatility in surface ligand exchange, QDs can be coupled with various types of acceptors to create hybrids with controlled type (electron or hole), direction, and rate of charge flow, depending on the foreseen application, either solar harvesting, light emitting, or biosensing. This perspective highlights several examples of QD-based hybrids with controllable (tunable) rate of charge transfer obtained by various approaches, including by changing the QD core size and shell thickness by colloidal synthesis, by the insertion of molecular linkers or dielectric spacers between donor and acceptor components. We also show that subjecting QDs to external factors such as electric fields and alternate optical excitation energy is another approach to bias the internal charge transfer between charges photogenerated in the QD core and QD's surface charge traps. The perspective also provides the reader with various examples of how single nanoparticle spectroscopic studies can help in understanding and quantifying nanoscale charge transfer with QDs.