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Title: Hot carrier cooling mechanisms in halide perovskites
Authors: Fu, Jianhui
Xu, Qiang
Han, Guifang
Wu, Bo
Huan, Cheng Hon Alfred
Leek, Meng Lee
Sum, Tze Chien
Keywords: Methylammonium Lead Triiodide
Atomic Absorption Spectroscopy
Issue Date: 2017
Source: Fu, J., Xu, Q., Han, G., Wu, B., Huan, C. H. A., Leek, M. L.,et al. (2017). Hot carrier cooling mechanisms in halide perovskites. Nature Communications, 8(1), 1300-.
Series/Report no.: Nature Communications
Abstract: Halide perovskites exhibit unique slow hot-carrier cooling properties capable of unlocking disruptive perovskite photon–electron conversion technologies (e.g., high-efficiency hot-carrier photovoltaics, photo-catalysis, and photodetectors). Presently, the origins and mechanisms of this retardation remain highly contentious (e.g., large polarons, hot-phonon bottleneck, acoustical–optical phonon upconversion etc.). Here, we investigate the fluence-dependent hot-carrier dynamics in methylammonium lead triiodide using transient absorption spectroscopy, and correlate with theoretical modeling and first-principles calculations. At moderate carrier concentrations (around 1018 cm−3), carrier cooling is mediated by polar Fröhlich electron–phonon interactions through zone-center delayed longitudinal optical phonon emissions (i.e., with phonon lifetime τ LO around 0.6 ± 0.1 ps) induced by the hot-phonon bottleneck. The hot-phonon effect arises from the suppression of the Klemens relaxation pathway essential for longitudinal optical phonon decay. At high carrier concentrations (around 1019 cm−3), Auger heating further reduces the cooling rates. Our study unravels the intricate interplay between the hot-phonon bottleneck and Auger heating effects on carrier cooling, which will resolve the existing controversy.
ISSN: 2041-1723
DOI: 10.1038/s41467-017-01360-3
Rights: © 2017 The Author(s). This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit licenses/by/4.0/.
Fulltext Permission: open
Fulltext Availability: With Fulltext
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