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

Ultra Long-Lived Radiative Trap States in CdSe Quantum Dots

Surface states and traps play an important role in the photophysics of colloidal quantum dots. These states typically lead to large red-shifted photoluminescence. We have used steady-state and time-resolved spectroscopic techniques to investigate the nature of the traps and their lifetimes in colloidal CdSe quantum dots. We conclude that at least two different types of traps contribute to the photoluminescence. The trapping is more pronounced at higher excitation energies compared to the band edge excitation. Hole trapping is dominant in CdSe quantum dots. The time-resolved photoluminescence and pump–probe measurements show that the trapped holes live for longer than tens of microseconds at room temperature