Ultrafast biexciton spectroscopy in semiconductor quantum dots: Evidence for early emergence of multiple-exciton generation

Younghwan Choi, Sangwan Sim, Seong Chu Lim, Young Hee Lee, Hyunyong Choi

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

Understanding multiple-exciton generation (MEG) in quantum dots (QDs) requires in-depth measurements of transient exciton dynamics. Because MEG typically faces competing ultrafast energy-loss intra-band relaxation, it is of central importance to investigate the emerging time-scale of the MEG kinetics. Here, we present ultrafast spectroscopic measurements of the MEG in PbS QDs via probing the ground-state biexciton transients. Specifically, we directly compare the biexciton spectra with the single-exciton ones before and after the intra-band relaxation. Early emergence of MEG is evidenced by observing transient Stark shift and quasi-instantaneous linewidth broadening, both of which take place before the intra-band relaxation. Photon-density-dependent study shows that the broadened biexciton linewidth strongly depends on the MEG-induced extra-exciton generation. Long after the intra-band relaxation, the biexciton broadening is small and the single-exciton state filling is dominant.

Original languageEnglish
Article number3206
JournalScientific reports
Volume3
DOIs
Publication statusPublished - 2013 Nov 21

All Science Journal Classification (ASJC) codes

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