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Polaron transport in hybrid CH3NH3PbI3 perovskite thin films.
Nanoscale ( IF 6.7 ) Pub Date : 2020-06-09 , DOI: 10.1039/d0nr03432k
Anusit Thongnum 1 , Udomsilp Pinsook 2
Affiliation  

A comprehensive study of the transport properties of a prototypical CH3NH3PbI3 thin film is presented. The polaron–longitudinal optical (LO) phonon scattering mechanism, based on Low-Pines's polaron mobility, was studied to elucidate the charge-carrier mobility. We found that the calculated mobilities showed very good quantitative agreement with the experimental data measured in thin film samples using photoconductivity techniques. In THz mobility, the calculated results yielded room-temperature (RT) mobilities of ∼650 cm2 V−1 s−1 (single crystal) and ∼220 cm2 V−1 s−1 (disordered thin film) at a low quantum yield (ϕ) and 32 cm2 V−1 s−1 (high-quality thin film) at ϕ = 1. The dynamic disorder due to organic reorientation was included in the calculations. Its effect provided a power law mobility of μTm and satisfactorily supported temperature-dependent mobility over the temperature range of 80–370 K. In the orthorhombic and tetragonal phases, the charge-carrier mobilities with dynamic disorder were approximately 47% and 22% lower than those obtained from phases without dynamic disorder. The RT mobility was 26 cm2 V−1 s−1 at ϕ = 1. In the low-temperature orthorhombic phase, the structural phase transition was considered. The mobility followed a power law with m = −1.7. In the tetragonal and cubic phases, the mobility also followed a power law, but with m = −1.1, which is an intermediate range in optical phonon scattering. When combined with recent theoretical analysis, we also found three limitations of power law mobility with exponents between −0.46 and −1.1 for polaron–LO phonon scattering, −1.2 and −1.6 for bare carrier–LO phonon scattering, and −1.7 and −2.0 for carrier scattering off optical phonons and lattice fluctuations. This work not only provides a description of temperature-dependent mobility in CH3NH3PbI3 thin films, but also gives new insights into THz photoconductivity and the relationship between LO phonon scattering and power law mobility.

中文翻译:

极化CH3NH3PbI3钙钛矿薄膜中的极化子传输。

提出了一种典型的CH 3 NH 3 PbI 3薄膜的传输性能的综合研究。研究了基于低松的极化子迁移率的极化子-纵向光学(LO)声子散射机制,以阐明电荷-载流子迁移率。我们发现,计算出的迁移率与使用光电导技术在薄膜样品中测得的实验数据显示出非常好的定量一致性。在太赫兹迁移率下,计算结果得出室温(RT)迁移率约为650 cm 2 V -1 s -1(单晶),约为220 cm 2 V -1 s -1(无序薄膜)以低量子产率(φ)和32厘米2 V -1小号-1处(高品质的薄膜)φ = 1的动态紊乱由于有机重新取向被包括在计算中。其效果提供的幂定律迁移率μ α Ť并且令人满意地支撑在温度范围80-370 K的在斜方晶和四方晶相依赖于温度的流动性,具有动态病症电荷流子迁移率分别约为47%和22比从没有动态紊乱的相获得的那些低%。所述RT迁移率为26厘米2 V -1小号-1ϕ= 1。在低温正交相中,考虑了结构相变。迁移率遵循幂定律,其中m = -1.7。在四方相和立方相中,迁移率也遵循幂定律,但是m = -1.1,这是光声子散射的中间范围。当与最新的理论分析结合时,我们还发现了幂律迁移率的三个局限性,极化子-LO声子散射的指数在-0.46至-1.1之间,裸载子-LO声子散射的指数在-1.2和-1.6之间,以及-1.7和-2.0用于从声子和光子涨落中散射出载流子。这项工作不仅描述了CH 3 NH 3 PbI 3中依赖温度的迁移率 薄膜,但也为THz光电导以及LO声子散射与幂律迁移率之间的关系提供了新的见解。
更新日期:2020-07-09
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