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阳离子动力学控制卤化铅钙钛矿纳米线的热性能。

Cation Dynamics Governed Thermal Properties of Lead Halide Perovskite Nanowires.

机构信息

National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, and Collaborative Innovation Center of Advanced Microstructures , Nanjing University , Nanjing 210093 , People's Republic of China.

Department of Mechanical Engineering , Vanderbilt University , Nashville , Tennessee 37212 , United States.

出版信息

Nano Lett. 2018 May 9;18(5):2772-2779. doi: 10.1021/acs.nanolett.7b04437. Epub 2018 Apr 9.

Abstract

Metal halide perovskite (MHP) nanowires such as hybrid organic-inorganic CHNHPbX (X = Cl, Br, I) have drawn significant attention as promising building blocks for high-performance solar cells, light-emitting devices, and semiconductor lasers. However, the physics of thermal transport in MHP nanowires is still elusive even though it is highly relevant to the device thermal stability and optoelectronic performance. Through combined experimental measurements and theoretical analyses, here we disclose the underlying mechanisms governing thermal transport in three different kinds of lead halide perovskite nanowires (CHNHPbI, CHNHPbBr and CsPbBr). It is shown that the thermal conductivity of CHNHPbBr nanowires is significantly suppressed as compared to that of CsPbBr nanowires, which is attributed to the cation dynamic disorder. Furthermore, we observed different temperature-dependent thermal conductivities of hybrid perovskites CHNHPbBr and CHNHPbI, which can be attributed to accelerated cation dynamics in CHNHPbBr at low temperature and the combined effects of lower phonon group velocity and higher Umklapp scattering rate in CHNHPbI at high temperature. These data and understanding should shed light on the design of high-performance MHP based thermal and optoelectronic devices.

摘要

金属卤化物钙钛矿(MHP)纳米线,如混合有机-无机 CHNHPbX(X = Cl、Br、I),作为高性能太阳能电池、发光器件和半导体激光器的有前途的构建块引起了极大的关注。然而,尽管热输运对于器件热稳定性和光电性能至关重要,但 MHP 纳米线中的热输运物理仍然难以捉摸。通过结合实验测量和理论分析,我们揭示了三种不同类型的卤化铅钙钛矿纳米线(CHNHPbI、CHNHPbBr 和 CsPbBr)中热输运的基本机制。结果表明,与 CsPbBr 纳米线相比,CHNHPbBr 纳米线的热导率显著降低,这归因于阳离子动态无序。此外,我们观察到混合钙钛矿 CHNHPbBr 和 CHNHPbI 的不同温度依赖性热导率,这可以归因于 CHNHPbBr 在低温下阳离子动力学的加速以及 CHNHPbI 在高温下较低的声子群速度和较高的 Umklapp 散射率的综合影响。这些数据和理解应该为设计高性能基于 MHP 的热和光电设备提供启示。

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