Stable, Ultralow Threshold Amplified Spontaneous Emission from CsPbBr₃ Nanoparticles Exhibiting Trion Gain

Abstract

Wet-chemically synthesized cesium lead halide nanoparticles have many attractive properties that make them promising as optical gain media, but generally suffer from poor stability under ambient conditions and an optical gain threshold that is widely believed to be dictated by the need for biexcitons. These conditions make it impractical for such particles to be utilized as gain media given the need to undergo repeated stimulated emission processes at above-threshold pump intensities over long periods of time. We demonstrate that the surface treatment of CsPbBr nanoparticles with a mixture of PbBr, oleic acid, and oleylamine not only raises their fluorescence quantum yield to nearly unity and prolongs their stability in air from days to months, but it also dramatically increases their trion photoluminescence lifetime from ∼0.9 to ∼1.6 ns. Via a combination of time-resolved photoluminescence and transient absorption spectroscopy, we provide evidence for trion gain at sufficiently low pump intensities in which the likelihood of predominantly biexciton-based gain is small. We then show that, in line with theoretical prediction, the amplified spontaneous emission (ASE) threshold of a thin film of surface-treated CsPbBr nanoparticles reduces to a record low of ∼1.2 μJ/cm with a corresponding average exciton occupancy per nanoparticle of 0.62. The ultralow pump threshold and increased stability allow for stable ASE over millions of laser shots, paving the way for the deployment of these nanoparticles as viable solution-processed optical gain media.

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Recent Progress in Metal Halide Perovskite Micro‐ and Nanolasers

“…The insets are the corresponding PL spectra for pump fluences above and below the ASE threshold F th . Reproduced with permission . Copyright 2018, American Chemical Society.…”

Ultrastable CsPbBr3 Perovskite Quantum Dot and Their Enhanced Amplified Spontaneous Emission by Surface Ligand Modification

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