Formation of PbSe/CdSe Core/Shell Nanocrystals for Stable Near-Infrared High Photoluminescence Emission

PbSe/CdSe core/shell nanocrystals with quantum yield of 70% were obtained by the “successive ion layer adsorption and reaction” technology in solution. The thickness of the CdSe shell was exactly controlled. A series of spectral red shifts with the CdSe shell growth were observed, which was attributed to the combined effect of the surface polarization and the expansion of carriers’ wavefunctions. The stability of PbSe nanocrystals was tremendously improved with CdSe shells

Quantum coherence of multiple excitons governs absorption cross-sections of PbS/CdS core/shell nanocrystals

半導体ナノ粒子の光吸収効率の増加メカニズムを解明 --高効率な太陽電池や光検出器へ期待--. 京都大学プレスリリース. 2018-08-22.Multiple excitons in semiconductor nanocrystals have been extensively studied with respect to unique carrier dynamics including quantized Auger recombination and implementation in optoelectronic devices such as solar cells and photodetectors. However, the generation mechanism of multiple excitons still remains unclear. Here, we study instantaneous and delayed multiple exciton generation processes in PbS/CdS core/shell nanocrystals. The absorption cross-sections of biexcitons and triexcitons are identical to that of single excitons under instantaneous excitation with a single pulse. In contrast, the delayed excitation using double pulses shows a reduction of the biexciton and triexciton absorption cross-sections. Our theoretical analysis reveals that the excitonic coherence assists the generation of multiple excitons and that the reduction of multiple exciton absorption cross-sections is caused by the reduction of coherent excitation pathways. We clarify that exciton coherences play a key role in multiple exciton generation processes and seamlessly connect the identical and reduced multiple exciton absorption cross-sections

Controlling the influence of Auger recombination on the performance of quantum-dot light-emitting diodes

Development of light-emitting diodes (LEDs) based on colloidal quantum dots is driven by attractive properties of these fluorophores such as spectrally narrow, tunable emission and facile processibility via solution-based methods. A current obstacle towards improved LED performance is an incomplete understanding of the roles of extrinsic factors, such as non-radiative recombination at surface defects, versus intrinsic processes, such as multicarrier Auger recombination or electron-hole separation due to applied electric field. Here we address this problem with studies that correlate the excited state dynamics of structurally engineered quantum dots with their emissive performance within LEDs. We find that because of significant charging of quantum dots with extra electrons, Auger recombination greatly impacts both LED efficiency and the onset of efficiency roll-off at high currents. Further, we demonstrate two specific approaches for mitigating this problem using heterostructured quantum dots, either by suppressing Auger decay through the introduction of an intermediate alloyed layer, or by using an additional shell that impedes electron transfer into the quantum dot to help balance electron and hole injection.4Chemical Sciences, Biosciences and Geosciences Division of Office of Science, Office of Basic Energy Sciences, US Department of Energ