Hot carrier cooling mechanisms in halide perovskites

Jianhui Fu, Qiang Xu, Guifang Han, Bo Wu, Cheng Hon Alfred Huan, Meng Lee Leek and Tze Chien Sum ()
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Jianhui Fu: Nanyang Technological University
Qiang Xu: Nanyang Technological University
Guifang Han: Energy Research Institute @NTU (ERI@N), Research Techno Plaza
Bo Wu: Nanyang Technological University
Cheng Hon Alfred Huan: Nanyang Technological University
Meng Lee Leek: Nanyang Technological University
Tze Chien Sum: Nanyang Technological University

Nature Communications, 2017, vol. 8, issue 1, 1-9

Abstract: 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.

Date: 2017
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DOI: 10.1038/s41467-017-01360-3

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