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

Chowdhury, Sarah N.; Fruhling, Colton; Diroll, Benjamin T.; Wang, Kang; Prokopeva, Ludmila J.; Marinova, Miroslava M.; Dou, Letian; Schaller, Richard D.; Kildishev, Alexander V.; Boltasseva, Alexandra; Shalaev, Vladimir M.

doi:10.1021/acsphotonics.3c01791

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

Journal Article · 12 May 2024 · ACS Photonics

DOI: https://doi.org/10.1021/acsphotonics.3c01791 · OSTI ID:2514398

Chowdhury, Sarah N. ^[1]; Fruhling, Colton ^[1]; Diroll, Benjamin T. ^[2]; Wang, Kang ^[3]; Prokopeva, Ludmila J. ^[1]; Marinova, Miroslava M. ^[1]; Dou, Letian ^[1]; Schaller, Richard D. ^[2]; Kildishev, Alexander V. ^[1]; Boltasseva, Alexandra ^[1]; Shalaev, Vladimir M. ^[1]

Purdue Univ., West Lafayette, IN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Purdue Univ., West Lafayette, IN (United States); Chinese Academy of Sciences (CAS), Beijing (China)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: US Air Force Office of Scientific Research (AFOSR); US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0017717

OSTI ID:: 2514398

Journal Information:: ACS Photonics, Journal Name: ACS Photonics Journal Issue: 6 Vol. 11; ISSN 2330-4022

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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