Monitoring Electron–Phonon Interactions in Lead Halide Perovskites Using Time-Resolved THz Spectroscopy

Zhao, Daming; Hu, Hongwei; Haselsberger, Reinhard; Marcus, Rudolph A.; Michel-Beyerle, Maria-Elisabeth; Lam, Yeng Ming; Zhu, Jian-Xin; La-o-vorakiat, Chan; Beard, Matthew C.; Chia, Elbert E.  M.

doi:10.1021/acsnano.9b02049

Monitoring Electron–Phonon Interactions in Lead Halide Perovskites Using Time-Resolved THz Spectroscopy

Journal Article · Fri Jul 26 00:00:00 EDT 2019 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.9b02049· OSTI ID:1550786

Zhao, Daming ^[1]; Hu, Hongwei ^[1]; Haselsberger, Reinhard ^[1]; Marcus, Rudolph A. ^[2]; Michel-Beyerle, Maria-Elisabeth ^[1]; ^[1]; ^[3]; La-o-vorakiat, Chan ^[4]; ^[5]; ^[1]

Nanyang Technological Univ. (Singapore)
Nanyang Technological Univ. (Singapore); California Inst. of Technology (CalTech), Pasadena, CA (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
King Mongkut’s Univ. of Technology Thonburi (KMUTT), Bangkok (Thailand)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

Lead halide perovskite semiconductors have low-frequency phonon modes within the lead halide sublattice and thus are considered to be soft. The soft lattice is considered to be important in defining their interesting optoelectronic properties. Electron-phonon coupling governs hot-carrier relaxation, carrier mobilities, carrier lifetimes, among other important electronic characteristics. Directly observing the interplay between free charge carriers and phonons can provide details on how phonons impact these properties (e.g., exciton populations and other collective modes). Here, we observe a delicate interplay among carriers, phonons, and excitons in mixed-cation and mixed-halide perovskite films by simultaneously resolving the contribution of charge carriers and phonons in time-resolved terahertz photoconductivity spectra. We are able to observe directly the increase in phonon population during carrier cooling and discuss how thermal equilibrium populations of carriers and phonons modulate the carrier transport properties, as well as reduce the population of carriers within band tails. We are also able to observe directly the formation of free charge carriers when excitons interact with phonons and dissociate and to describe how free carriers and exciton populations exchange through phonon interactions. Finally, we also time-resolve how the carriers are screened via the Coulomb interaction at low and room temperatures. Our studies shed light on how charge carriers interact with the low-energy phonons and discuss implications.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC). Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: 89233218CNA000001; AC36-08GO28308

OSTI ID:: 1550786

Alternate ID(s):: OSTI ID: 1726158

Report Number(s):: LA-UR--18-21691; NREL/JA--5900-72381

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 8 Vol. 13; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Monitoring Electron–Phonon Interactions in Lead Halide Perovskites Using Time-Resolved THz Spectroscopy

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