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正电子湮没光谱法对甲基碘化铅铵钙钛矿中温度依赖电响应起源的研究

Positron Annihilation Spectroscopic Investigation on the Origin of Temperature-Dependent Electrical Response in Methylammonium Lead Iodide Perovskite.

作者信息

Dhar Joydeep, Sil Sayantan, Dey Arka, Ray Partha Pratim, Sanyal Dirtha

机构信息

Department of Physics, Jadavpur University , Kolkata 700032, India.

Variable Energy Cyclotron Centre , 1/AF, Bidhannagar, Kolkata 700064, India.

出版信息

J Phys Chem Lett. 2017 Apr 20;8(8):1745-1751. doi: 10.1021/acs.jpclett.7b00446. Epub 2017 Apr 5.

Abstract

Organic-inorganic hybrid perovskite has appeared as one of the leading materials for realizing solution-based high-performing optoelectronic devices. The charge transport properties in this class of material are quite intriguing and still need to be carefully investigated. The temperature-dependent electrical property of methylammonium lead iodide (CHNHPbI) has been investigated by employing positron annihilation spectroscopy (PAS), which unambiguously reveals the gradual formation of open volume defects with the enhancement in temperature. The high-temperature ionic conductivity is due to the generation of both cationic (CHNH) and anionic (I) vacancies, possibly because of the elimination of methylammonium iodide (CHNHI) as identified from the coincidence Doppler broadening (CDB) of the positron annihilation spectroscopy. Further, the evolution of temperature-dependent defect density and corresponding electrical responses has been correlated with the structural phase transitions of CHNHPbI. This is the first ever report of temperature-dependent PAS measurement on hybrid lead halide perovskites to understand the nature and the origin of its electrical characteristics arising due to the variation in temperature.

摘要

有机-无机杂化钙钛矿已成为实现基于溶液的高性能光电器件的主要材料之一。这类材料中的电荷传输特性十分有趣,仍需仔细研究。通过正电子湮没光谱(PAS)研究了甲基碘化铅铵(CH₃NH₃PbI₃)的温度依赖性电学性质,该研究明确揭示了随着温度升高,开放体积缺陷逐渐形成。高温离子电导率归因于阳离子(CH₃NH₃⁺)和阴离子(I⁻)空位的产生,这可能是由于从正电子湮没光谱的符合多普勒展宽(CDB)中确定的碘化甲铵(CH₃NH₃I)的消除。此外,温度依赖性缺陷密度的演变及其相应的电响应已与CH₃NH₃PbI₃的结构相变相关联。这是首次关于混合卤化铅钙钛矿的温度依赖性PAS测量的报告,以了解其因温度变化而产生的电学特性的本质和起源。

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