Enhanced Hot-Phonon Bottleneck Effect on Slowing Hot Carrier Cooling in Metal Halide Perovskite Quantum Dots with Alloyed A-Site

Hua Li; Qing Wang; Yusuke Oteki; Chao Ding; Dong Liu; Yao Guo; Yusheng Li; Yuyao Wei; Dandan Wang; Yongge Yang; Taizo Masuda; Mengmeng Chen; Zheng Zhang; Tomah Sogabe; Shuzi Hayase; Yoshitaka Okada; Satoshi Iikubo; Qing Shen

doi:10.1002/adma.202301834

Enhanced Hot-Phonon Bottleneck Effect on Slowing Hot Carrier Cooling in Metal Halide Perovskite Quantum Dots with Alloyed A-Site

Adv Mater. 2023 Sep;35(38):e2301834. doi: 10.1002/adma.202301834. Epub 2023 Jul 27.

Authors

Hua Li¹, Qing Wang², Yusuke Oteki³, Chao Ding^{1

4}, Dong Liu¹, Yao Guo⁵, Yusheng Li¹, Yuyao Wei¹, Dandan Wang¹, Yongge Yang¹, Taizo Masuda^{1

6}, Mengmeng Chen¹, Zheng Zhang¹, Tomah Sogabe¹, Shuzi Hayase¹, Yoshitaka Okada³, Satoshi Iikubo², Qing Shen¹

Affiliations

¹ Faculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo, 182-8585, Japan.
² Department of Advanced Materials Science and Engineering, Faculty of Engineering Sciences, Kyushu University, Kasuga, Fukuoka, 816-8580, Japan.
³ Research Center for Advanced Science and Technology (RCAST), The University of Tokyo, 4-6-1 Komaba, Meguro, Tokyo, 153-8904, Japan.
⁴ Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu, 610065, China.
⁵ Department of Materials Science and Engineering, Anyang Institute of Technology, Anyang, 455000, China.
⁶ CN development division, Toyota Motor Corporation, Susono, Shizuoka, 410-1193, Japan.

PMID: 37311157
DOI: 10.1002/adma.202301834

Abstract

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⁺ , CH₃ NH₃ ⁺ ₊ ), CsPbI₃ (Cs⁺ , Cesium) and alloyed FA_0.5 MA_0.5 PbI₃ , FA_0.5 Cs_0.5 PbI₃ , and MA_0.5 Cs_0.5 PbI₃ 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.

Keywords: A-site cation cross-exchange; electron-phonon coupling; hot carrier; hot-phonon bottleneck effect; perovskites.

Abstract

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