Ultrafast biexciton spectroscopy in semiconductor quantum dots: evidence for early emergence of multiple-exciton generation
- Authors
- Choi, Younghwan; Sim, Sangwan; Lim, Seong Chu; Lee, Young Hee; Choi, Hyunyong
- Issue Date
- Nov-2013
- Publisher
- Nature Publishing Group
- Citation
- Scientific Reports, v.3, pp.1 - 6
- Indexed
- SCIE
SCOPUS
- Journal Title
- Scientific Reports
- Volume
- 3
- Start Page
- 1
- End Page
- 6
- URI
- https://scholarworks.bwise.kr/erica/handle/2021.sw.erica/26312
- DOI
- 10.1038/srep03206
- ISSN
- 2045-2322
- 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.
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