Metal Coordination Sphere Deformation Induced Highly Stokes-Shifted, Ultra Broadband Emission in 2D Hybrid Lead-Bromide Perovskites and Investigation of Its Origin

Angew Chem Int Ed Engl. 2020 Jun 26;59(27):10791-10796. doi: 10.1002/anie.201915708. Epub 2020 May 7.

Abstract

Published studies of layered (2D) (100)-oriented hybrid lead-bromide perovskites evidence a correlation between increased inter-octahedral (Pb-Br-Pb) distortions and the appearance of broadband white light emission. However, the impact of distortions within their constituent [PbBr6 ]4- octahedra has yet to be assessed. Herein, we report two new (100)-oriented 2D Pb-Br perovskites, whose structures display unusually high intra-octahedral distortions, whilst retaining minimal inter-octahedral distortions. Using a combination of temperature-dependent, power-dependent and time-resolved photoluminescence spectroscopic measurements, we show that increased intra-octahedral distortion induces exciton localization processes and leads to formation of multiple photoinduced emissive colour centres. Ultimately, this leads to highly Stokes-shifted, ultrabroad white light emission at room temperature.

Keywords: crystal engineering; intra-octahedral distortion; lead-bromide perovskites; photophysics; white-light emission.