%0 Journal Article %1 fu2017carrier %A Fu, Jianhui %A Xu, Qiang %A Han, Guifang %A Wu, Bo %A Huan, Cheng Hon Alfred %A Leek, Meng Lee %A Sum, Tze Chien %D 2017 %J Nature Communications %K hot_carrier perovskite %N 1 %P 1300-- %R 10.1038/s41467-017-01360-3 %T Hot carrier cooling mechanisms in halide perovskites %U https://doi.org/10.1038/s41467-017-01360-3 %V 8 %X 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.

@article{fu2017carrier, 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.}, added-at = {2018-01-17T16:21:08.000+0100}, author = {Fu, Jianhui and Xu, Qiang and Han, Guifang and Wu, Bo and Huan, Cheng Hon Alfred and Leek, Meng Lee and Sum, Tze Chien}, biburl = {https://www.bibsonomy.org/bibtex/249194667204a4ef7ab0ec84a3e27ca94/bretschneider_m}, doi = {10.1038/s41467-017-01360-3}, interhash = {efbcc4c943d9d1b762c10a8408e9646d}, intrahash = {49194667204a4ef7ab0ec84a3e27ca94}, issn = {20411723}, journal = {Nature Communications}, keywords = {hot_carrier perovskite}, number = 1, pages = {1300--}, refid = {Fu2017}, timestamp = {2018-01-17T16:21:08.000+0100}, title = {Hot carrier cooling mechanisms in halide perovskites}, url = {https://doi.org/10.1038/s41467-017-01360-3}, volume = 8, year = 2017 }