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

Zhao, Daming and Hu, Hongwei and Haselsberger, Reinhard and Marcus, Rudolph A. and Michel-Beyerle, Maria-Elisabeth and Lam, Yeng Ming and Zhu, Jian-Xin and La-o-vorakiat, Chan and Beard, Matthew C. and Chia, Elbert E. M. (2019) Monitoring Electron–Phonon Interactions in Lead-Halide Perovskites Using Time-Resolved THz Spectroscopy. ACS Nano, 13 (8). pp. 8826-8835. ISSN 1936-0851.

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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.

Item Type:Article
Related URLs:
URLURL TypeDescription
Zhao, Daming0000-0001-5046-2199
Marcus, Rudolph A.0000-0001-6547-1469
Lam, Yeng Ming0000-0001-9390-8074
Zhu, Jian-Xin0000-0001-7991-3918
La-o-vorakiat, Chan0000-0002-0231-8499
Beard, Matthew C.0000-0002-2711-1355
Chia, Elbert E. M.0000-0003-2066-0834
Additional Information:© 2019 American Chemical Society. Received: March 15, 2019; Accepted: July 26, 2019; Published: July 26, 2019. E.E.M.C. acknowledges support from the Singapore Ministry of Education AcRF Tier 2 (MOE2015-T2-2-065 and MOE2016-T2-1-054). C.L. is grateful for the support from the Theoretical and Computational Science (TaCS) Center, Thailand Research Fund (MRG6080264), and KMUTT 55th Anniversary Commemorative Fund. M.C.B. acknowledges funding from the Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE) an Energy Frontier Research Center funded by the Office of Science of the U.S. Department of Energy. Part of this work was authored in part by Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Eenrgy (ODE) under Contract No. DE-AC36-08GO28308. Y.M.L. acknowledges financial support from a Ministry of Education, Singapore, Tier 1 Funding (RG105/18). R.A.M. thanks the ONR and ARO for their support. M.-E.M.-B. is grateful to the Nanyang Technological University for supporting the Biophysics Center. The work was supported in part by the Center for Integrated Nanotechnologies, a U.S. DOE BES user facility. The authors declare no competing financial interest.
Funding AgencyGrant Number
Ministry of Education (Singapore)MOE2015-T2-2-065
Ministry of Education (Singapore)MOE2016-T2-1-054
Thailand Research FundMRG6080264
King Mongkut’s University of Technology ThonburiUNSPECIFIED
Department of Energy (DOE)DE-AC36-08GO28308
Ministry of Education (Singapore)RG105/18
Office of Naval Research (ONR)UNSPECIFIED
Army Research Office (ARO)UNSPECIFIED
Nanyang Technological UniversityUNSPECIFIED
Subject Keywords:perovskite, time-resolved terahertz spectroscopy, phonon, free carrier, exciton
Issue or Number:8
Record Number:CaltechAUTHORS:20190729-101612764
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Official Citation:Monitoring Electron–Phonon Interactions in Lead Halide Perovskites Using Time-Resolved THz Spectroscopy. Daming Zhao, Hongwei Hu, Reinhard Haselsberger, Rudolph A. Marcus, Maria-Elisabeth Michel-Beyerle, Yeng Ming Lam, Jian-Xin Zhu, Chan La-o-vorakiat, Matthew C. Beard, and Elbert E. M. Chia. ACS Nano 2019 13 (8), 8826-8835. DOI: 10.1021/acsnano.9b02049
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:97484
Deposited By: Tony Diaz
Deposited On:29 Jul 2019 17:31
Last Modified:03 Oct 2019 21:32

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