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卤化铅钙钛矿中的极化子电荷载流子-晶格相互作用

Polaronic Charge Carrier-Lattice Interactions in Lead Halide Perovskites.

作者信息

Wolf Christoph, Cho Himchan, Kim Young-Hoon, Lee Tae-Woo

机构信息

Department of Materials Science and Engineering, Research Institute of Advanced Materials, BK21 PLUS SNU Materials Division for Educating Creative Global Leaders, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826, Republic of Korea.

Department of Materials Science and Engineering, Pohang University of Science and Technology, Pohang, Gyungbuk, 790-784, Republic of Korea Republic of Korea.

出版信息

ChemSusChem. 2017 Oct 9;10(19):3705-3711. doi: 10.1002/cssc.201701284. Epub 2017 Sep 21.

Abstract

Almost ten years after the renaissance of the popular perovskite-type semiconductors based on lead salts with the general formula AMX (A=organic or inorganic cation; M=divalent metal; X=halide), many facets of photophysics continue to puzzle researchers. In this Minireview, light is shed on the low mobilities of charge carriers in lead halide perovskites with special focus on the lattice properties at non-zero temperature. The polar and soft lattice leads to pronounced electron-phonon coupling, limiting carrier mobility and retarding recombination. We propose that the proper picture of excited charge carriers at temperature ranges that are relevant for device operations is that of a polaron, with Fröhlich coupling constants between 1<α<3. Under the aspect of light-emitting diode application, APbX perovskite show moderate second order (bimolecular) recombination rates and high third-order (Auger) rate constants. It has become apparent that this is a direct consequence of the anisotropic polar A-site cation in organic-inorganic hybrid perovskites and might be alleviated by replacing the organic moiety with an isotropic cation.

摘要

在基于通式为AMX(A = 有机或无机阳离子;M = 二价金属;X = 卤化物)的铅盐的流行钙钛矿型半导体复兴近十年后,光物理的许多方面仍然困扰着研究人员。在这篇小型综述中,我们特别关注非零温度下的晶格性质,揭示了卤化铅钙钛矿中载流子迁移率较低的问题。极性和软晶格导致明显的电子 - 声子耦合,限制了载流子迁移率并延缓了复合。我们提出,在与器件操作相关的温度范围内,激发电荷载流子的恰当图像是极化子,其弗罗利希耦合常数在1 < α < 3之间。从发光二极管应用的角度来看,APbX钙钛矿显示出适度的二阶(双分子)复合速率和高三阶(俄歇)速率常数。很明显,这是有机 - 无机杂化钙钛矿中各向异性极性A位阳离子的直接结果,并且通过用各向同性阳离子取代有机部分可能会得到缓解。

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