Single-Exciton Amplified Spontaneous Emission in Thin Films of CsPbX3 (X = Br, I) Perovskite Nanocrystals.

Abstract

CsPbX3 perovskite nanocrystals (PNCs) have emerged as an excellent material for stimulated emission purposes, with even more prospective applications than conventional colloidal quantum dots. However, a better understanding of the physical mechanisms responsible for amplified spontaneous emission (ASE) is required to achieve more ambitious targets (lasing under continuous wave optical or electrical excitation). Here, we establish the intrinsic mechanisms underlying ASE in PNCs of three different band gaps (CsPbBr3, CsPbBr1.5I1.5, and CsPbI3). Our characterization at cryogenic temperatures does not reveal any evidence of the biexciton mechanism in the formation of ASE. Instead, the measured shift toward long wavelengths of the ASE band is easily explained by the reabsorption in the PNC layer, which becomes stronger for thicker layers. In this way, the threshold of ASE is determined only by optical losses at a given geometry, which is the single-exciton mechanism responsible for ASE. Experimental results are properly reproduced by a physical model.