Photoluminescence Decay of Colloidal Quantum Dots: Reversible Trapping and the Nature of the Relevant Trap States

摘要： Interfaces are crucial factors in shaping the properties of colloidal quantum dots (QDs), in particular the size-dependent optical properties that are a hallmark of these materials. However, the role played by the interfaces associated with QDs on the kinetics of photoluminescence (PL) decay of these nanocrystals is not fully understood even for the most extensively investigated II-VI QDs. In particular, interfaces are a hotbed of trapping sites over which control is essential for efficient performance of QD-based devices, because traps condition PL lifetimes and may be related to PL intermittency. In this work, we analyze the room-temperature PL decay of drop-cast films of CdSe/ZnS QDs varying a number of factors (casting solvent, capping ligands, core/shell interface character). We show how the use of a function that accounts for reversible trapping of photogenerated charge carriers with physically meaningful parameters (time constant, trapping and detrapping rate constants, and average number of traps per QD) can provide valuable information concerning the relevant interfaces, and therefore the nature of the trap states, involved in the recombination of those charge carriers. This approach should be applicable to QDs of a variety of compositions as well as materials beyond inorganic semiconductors.