Hot carrier cooling mechanisms in halide perovskites.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 29101381.
- Also identified by DOI 10.1038/s41467-017-01360-3 and PMC identifier 5670184.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
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.