TY - JOUR
T1 - Enhanced Hot-Phonon Bottleneck Effect on Slowing Hot Carrier Cooling in Metal Halide Perovskite Quantum Dots with Alloyed A-Site
AU - Li, Hua
AU - Wang, Qing
AU - Oteki, Yusuke
AU - Ding, Chao
AU - Liu, Dong
AU - Guo, Yao
AU - Li, Yusheng
AU - Wei, Yuyao
AU - Wang, Dandan
AU - Yang, Yongge
AU - Masuda, Taizo
AU - Chen, Mengmeng
AU - Zhang, Zheng
AU - Sogabe, Tomah
AU - Hayase, Shuzi
AU - Okada, Yoshitaka
AU - Iikubo, Satoshi
AU - Shen, Qing
N1 - Publisher Copyright:
© 2023 Wiley-VCH GmbH.
PY - 2023/9/21
Y1 - 2023/9/21
N2 - A deep understanding of the effect of the A-site cation cross-exchange on the hot-carrier relaxation dynamics in perovskite quantum dots (PQDs) has profound implications on the further development of disruptive photovoltaic technologies. In this study, the hot carrier cooling kinetics of pure FAPbI3 (FA+, CH(NH2)2+), MAPbI3 (MA+, CH3NH3++), CsPbI3 (Cs+, Cesium) and alloyed FA0.5MA0.5PbI3, FA0.5Cs0.5PbI3, and MA0.5Cs0.5PbI3 QDs are investigated using ultrafast transient absorption (TA) spectroscopy. The lifetimes of the initial fast cooling stage (<1 ps) of all the organic cation-containing PQDs are shorter than those of the CsPbI3 QDs, as verified by the electron-phonon coupling strength extracted from the temperature-dependent photoluminescence spectra. The lifetimes of the slow cooling stage of the alloyed PQDs are longer under illumination greater than 1 sun, which is ascribed to the introduction of co-vibrational optical phonon modes in the alloyed PQDs. This facilitated efficient acoustic phonon upconversion and enhanced the hot-phonon bottleneck effect, as demonstrated by first-principles calculations.
AB - A deep understanding of the effect of the A-site cation cross-exchange on the hot-carrier relaxation dynamics in perovskite quantum dots (PQDs) has profound implications on the further development of disruptive photovoltaic technologies. In this study, the hot carrier cooling kinetics of pure FAPbI3 (FA+, CH(NH2)2+), MAPbI3 (MA+, CH3NH3++), CsPbI3 (Cs+, Cesium) and alloyed FA0.5MA0.5PbI3, FA0.5Cs0.5PbI3, and MA0.5Cs0.5PbI3 QDs are investigated using ultrafast transient absorption (TA) spectroscopy. The lifetimes of the initial fast cooling stage (<1 ps) of all the organic cation-containing PQDs are shorter than those of the CsPbI3 QDs, as verified by the electron-phonon coupling strength extracted from the temperature-dependent photoluminescence spectra. The lifetimes of the slow cooling stage of the alloyed PQDs are longer under illumination greater than 1 sun, which is ascribed to the introduction of co-vibrational optical phonon modes in the alloyed PQDs. This facilitated efficient acoustic phonon upconversion and enhanced the hot-phonon bottleneck effect, as demonstrated by first-principles calculations.
KW - A-site cation cross-exchange
KW - electron-phonon coupling
KW - hot carrier
KW - hot-phonon bottleneck effect
KW - perovskites
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U2 - 10.1002/adma.202301834
DO - 10.1002/adma.202301834
M3 - Article
C2 - 37311157
AN - SCOPUS:85165870434
SN - 0935-9648
VL - 35
JO - Advanced Materials
JF - Advanced Materials
IS - 38
M1 - 2301834
ER -