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arXiv 2407.02809cond-mat.mtrl-sci
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利用超快光谱与数值模拟区分钙钛矿-传输层界面处的载流子输运与界面复合

Distinguishing Carrier Transport and Interfacial Recombination at Perovskite-Transport Layer Interfaces Using Ultrafast Spectroscopy and Numerical Simulation

Edward Butler-Caddle, K. D. G. Imalka Jayawardena, Anjana Wijesekara, Rebecca L Milot, James Lloyd-Hughes

AI总结:

本文利用超快太赫兹光谱、光学测量和数值模拟,研究钙钛矿与C60、PCBM、Spiro-OMeTAD三种传输层界面的载流子提取与复合,确定了提取速度和双极扩散系数,并据此提出改进器件性能的明确方向。

摘要:

在钙钛矿太阳能电池中,光伏作用由光吸收金属卤化物钙钛矿半导体两侧的电荷传输层(CTLs)产生。因此,钙钛矿-CTL界面处期望的电荷提取速率与不期望的界面复合速率对器件效率起着关键作用。本文通过脉冲光激发后载流子动力学的超快太赫兹和光学研究,结合包含选择性电荷提取进入CTL后产生的显著库仑力以及跨界面复合的载流子输运物理模型,获得了钙钛矿-CTL双层异质结构的电学性质。利用三种性能最高的CTL,即C$_{60}$、PCBM和Spiro-OMeTAD,所构成异质结构的实验衰减曲线,确定了界面处的电荷提取速度以及钙钛矿内的双极扩散系数。由此推导出进一步改进器件的明确目标:富勒烯提供快速的电子提取,但存在较大的跨界面复合或空穴提取速率常数。相反,Spiro-OMeTAD表现出较慢的空穴提取,但不会增加钙钛矿的表面复合速率,这可能是其在太阳能电池器件中取得成功的原因之一。

英文摘要:

In perovskite solar cells, photovoltaic action is created by charge transport layers (CTLs) either side of the light-absorbing metal halide perovskite semiconductor. Hence, the rates for desirable charge extraction and unwanted interfacial recombination at the perovskite-CTL interfaces play a critical role for device efficiency. Here, the electrical properties of perovskite-CTL bilayer heterostructures are obtained using ultrafast THz and optical studies of the charge carrier dynamics after pulsed photoexcitation, combined with a physical model of charge carrier transport that includes the prominent Coulombic forces that arise after selective charge extraction into a CTL, and cross-interfacial recombination. The charge extraction velocity at the interface and the ambipolar diffusion coefficient within the perovskite are determined from the experimental decay profiles for heterostructures with three of the highest performing CTLs, namely C$_{60}$, PCBM and Spiro-OMeTAD. Definitive targets for the further improvement of devices are deduced: fullerenes deliver fast electron extraction, but suffer from a large rate constant for cross-interface recombination or hole extraction. Conversely, Spiro-OMeTAD exhibits slow hole extraction but does not increase the perovskite's surface recombination rate, likely contributing to its success in solar cell devices.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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