Multicarrier dynamics in colloidal quantum dots (QDs) are normally controlled by nonradiative Auger recombination wherein the energy of an electron-hole pair is converted not into a photon but instead transferred to a third carrier (an electron or a hole). Auger decay is extremely fast in QDs (time scales of tens-to-hundreds of picoseconds) due to both close proximity between interacting charges and elimination of restrictions imposed by translational momentum conservation. Photoluminescence (PL) quenching by nonradiative Auger processes complicates realization of applications that require high emissivity of multicarrier states such as light-emitting diodes (LEDs) and lasers. Therefore, the development of “Auger-recombination-free” QDs is an important current challenge in the field of colloidal nanostructures.
Previous single-dot spectroscopic studies have indicated a significant spread in Auger lifetimes across an ensemble of nominally identical QDs. It has been speculated that in addition to dot-to-dot variation in physical dimensions, this spread is contributed to by variations in the structure of the QD interface, which controls the shape of the confinement potential. Here we directly evaluate the effect of the composition of the core-shell interface on single- and multi-exciton dynamics via side-by-side measurements of individual core-shell CdSe/CdS nanocrystals with a sharp vs. smooth (graded) interface. We observe that while having essentially no effect on single-exciton decay, the interfacial alloy layer leads to a systematic increase in the biexciton lifetime indicating suppression of Auger recombination. We demonstrate that using QDs with “engineered interfaces” we can considerably improve the performance of QD LEDs and lasers.
Victor I. Klimov, "Auger-decay engineering in quantum dots in relation to applications in LEDs and lasers (Presentation Recording)," Proc. SPIE 9546, Active Photonic Materials VII, 954612 (Presented at SPIE Nanoscience + Engineering: August 11, 2015; Published: 5 October 2015); https://doi.org/10.1117/12.2190074.4519370261001.
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