Semi-empirical approach to assess externally-induced photoluminescence linewidth broadening of halide perovskite nanocrystals with particle-size distribution

Abstract

Colloidal nanocrystals (NCs) can be used to prepare high-color-purity metal halide perovskites (MHPs) for light-emitting displays. However, the NCs have a finite particle-size distribution, which broadens the linewidth of photoluminescence spectra under strong quantum confinement, and thereby degrades the color purity of the MHPs. This paper presents a simple method to quantify this externally-introduced broadening of linewidth Gamma(SD) by combining experimental size-distribution histogram with size-dependent photoluminescence-wavelength (Pl-lambda) curve. We develop a semi-empirical method to estimate the other three contributions to the experimentally-measured full-width at half-maximum, Gamma(EXP). Namely: the intrinsic linewidth Gamma(LO) caused by exciton-longitudinal optical (LO) phonon Frohlich coupling; the inhomogeneous linewidth Gamma(o) caused by imperfections-related scattering, and the broadening Gamma(QC) due to the quantum-confinement effect. We show that Gamma(LO) of a nanocrystal decreases together with the particle size, disappearing at 1.6 nm radius. Finally, we show that Gamma(LO) is correlated with the degree of Frohlich-polaron formation, hence proportional to the long-range LO-phonon-electron coupling.