Abstract
Lead halide perovskites are emerging as an excellent material platform for optoelectronic processes. There have been extensive discussions on lasing, polariton formation, and nonlinear processes in this material system, but the underlying mechanism remains unknown. Here we probe lasing from CsPbBr3 perovskite nanowires with picosecond (ps) time resolution and show that lasing originates from stimulated emission of an electron-hole plasma. We observe an anomalous blue-shifting of the lasing gain profile with time up to 25 ps, and assign this as a signature for lasing involving plasmon emission. The time domain view provides an ultra-sensitive probe of many-body physics which was obscured in previous time-integrated measurements of lasing from lead halide perovskite nanowires.
Highlights
Lead halide perovskites are emerging as an excellent material platform for optoelectronic processes
Photophysical studies in the past few years have established that charge carrier properties in Lead halide perovskites (LHPs) are distinct from those in conventional semiconductors; those in the former are exemplified by exceptional defect tolerance, slow hot carrier cooling, and efficient dynamic screening[6]
While exciton-polaritons may exist at low excitation density and continuous wave (CW) conditions, lasing under pulsed excitation may occur above the exciton Mott density from stimulated emission from a non-degenerate electron hole plasma (n-EHP, referred to as a Coulomb-correlated EHP)[24,25,26,27]
Summary
Lead halide perovskites are emerging as an excellent material platform for optoelectronic processes. There have been extensive discussions on lasing, polariton formation, and nonlinear processes in this material system, but the underlying mechanism remains unknown. We probe lasing from CsPbBr3 perovskite nanowires with picosecond (ps) time resolution and show that lasing originates from stimulated emission of an electron-hole plasma. The time domain view provides an ultra-sensitive probe of many-body physics which was obscured in previous time-integrated measurements of lasing from lead halide perovskite nanowires. The lasing spectrum under pulsed excitation is a strongly time-dependent function, which consists of red-shifting cavity modes concurrent with blueshifting laser gain profiles. The latter is unprecedented, and is strong evidence for stimulated emission from an n-EHP coupled with plasmon emission
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