通过时间分辨光致发光揭示卤化铅包晶中双星对的潜力

Hannes Hempel, Martin Stolterfoht, Orestis Karalis, Thomas Unold
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引用次数: 0

摘要

连续照明下的光致发光(PL)通常用于评估太阳能转换材料中的电压损耗。然而,人们对这些损耗的早期时间演变仍然知之甚少。因此,我们将这一方法扩展到时间分辨型聚光,引入了基质聚光、掺杂聚光和同胞聚光的概念,以量化光生电子-空穴对的瞬态化学势和关键光电特性。通过分析初始聚光幅值,可以发现 100 纳米左右的热电荷载流子分离,这可能受到三阳离子包晶的晶粒尺寸的限制。随后的聚光衰减是由非骤变宝石对的扩散分离引起的,并通过增加熵来解决一个基本但却经常被忽视的能量损失问题。对于三阳离子卤代磷灰石,我们测得的 "宝石相关能 "高达 90 meV,可持续约十纳秒。这种能量在标准太阳电池中未被利用,在肖克利-奎塞尔模型中被认为是损失的。因此,这种相关能量可以大大提高设备的效率,尤其是在最大功率点和低照度条件下。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
The Potential of Geminate Pairs in Lead Halide Perovskite revealed via Time-resolved Photoluminescence
Photoluminescence (PL) under continuous illumination is commonly employed to assess voltage losses in solar energy conversion materials. However, the early temporal evolution of these losses remains poorly understood. Therefore, we extend the methodology to time-resolved PL, introducing the concepts of geminate PL, doping PL, and sibling PL to quantify the transient chemical potential of photogenerated electron-hole pairs and key optoelectronic properties. Analyzing the initial PL amplitudes reveals hot charge carrier separation for around 100 nm and is likely limited by the grain size of the triple cation perovskite. The following PL decay is caused by the diffusive separation of non-excitonic geminate pairs and time-resolves a fundamental yet often overlooked energy loss by increasing entropy. For triple-cation halide perovskite, we measure a "geminate correlation energy" of up to 90 meV, persisting for ~ten nanoseconds. This energy is unutilized in standard solar cells and is considered lost in the Shockley-Queisser model. Therefore, this geminate energy could substantially enhance the device's efficiency, particularly under maximum power point and low-illumination conditions.
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