Photophysics and Carrier Dynamics of Lasing in Quasi-2D Lead Halide Perovskites

Quasi-2D perovskites have recently been extensively studied due to their narrow-bandwidth-tunable emission, solution processability, and applicability as optical gain media. Quasi-2D perovskites are composed of inorganic perovskite crystal layers encapsulated with a bulky organic ligand such as phenylethylammonium, endowing the perovskite with a quantum-well structure and improved stability. In this article, we explore the photophysics of a quasi-2D metal halide perovskite as a promising light-harvesting and emitting medium. We find it exhibits high optical absorption (~10⁵ cm^-1) and an optically pumped amplified spontaneous emission threshold at 623 μJ/cm². We study charge transfer processes in the complex mixed quantum wells of these perovskites through transient absorption and time-resolved photoluminescence measurements and develop a phenomenological model that incorporates optical gain for lasing. Further, while both free carriers and excitons are observed, we show surprisingly that photoluminescence is dominated by excitons despite the relatively small binding energy (~16 meV) of the low-energy band edge. Additionally, we extract the rates of exciton relaxation pathways, revealing a relatively large radiative term of 4.6 x 10⁸ s^-1 as well as an exciton-exciton annihilation term of 3.6 x 10^-13 cm³ s^-1 that is 3 orders of magnitude smaller than in similar quasi-2D perovskites.. Authors: Chowdhury, Sarah N. [Purdue Univ., West Lafayette, IN (United States)]; Fruhling, Colton [Purdue Univ., West Lafayette, IN (United States)]; Diroll, Benjamin T. [Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)]; Wang, Kang [Purdue Univ., West Lafayette, IN (United States); Chinese Academy of Sciences (CAS), Beijing (China)]; Prokopeva, Ludmila J. [Purdue Univ., West Lafayette, IN (United States)]. DOE Contract: AC02-06CH11357; SC0017717. Subjects: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Perovskites; Recombination rates; Ruddlesden–Popper