Optical Gain from Biexcitons in CsPbBr3 Nanocrystals Revealed by Two-dimensional Electronic Spectroscopy

The Journal of Physical Chemistry Letters
Wei ZhaoMin Xiao

Abstract

Perovskite semiconductor nanocrystals (NCs) exhibit highly efficient optical gain, which is promising for laser applications. However, the intrinsic mechanism of optical gain in perovskite NCs, particularly whether more than one exciton per NCs is required, remains poorly understood. Here, we use two-dimensional electronic spectroscopy to resonantly probe the interplay between near-band-edge transitions during the buildup of optical gain in CsPbBr3 NCs. We find compelling evidence to conclude that optical gain in CsPbBr3 NCs is generated through stimulated emission from strongly interacting biexcitons. The threshold is largely determined by the competition between stimulated emission from biexcitons and excited-state absorption from single exciton to biexciton states. The findings in this work may guide future explorations of NC materials with low-threshold optical gain.

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Citations

Mar 3, 2021·The Review of Scientific Instruments·Gang-Hua DengYi Rao
Jun 18, 2021·ACS Nano·Amrita DeyLakshminarayana Polavarapu
Apr 23, 2019·The Journal of Physical Chemistry Letters·Chunyi ZhaoShengye Jin
Feb 12, 2020·The Journal of Physical Chemistry Letters·Ganghua DengYi Rao
Sep 24, 2019·The Journal of Physical Chemistry Letters·Juan Navarro-ArenasJuan Martínez-Pastor

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