Long-Lived Hot Carriers in Two-Dimensional Perovskites: The Role of Alternating Cations in Interlayer Space,ACS Energy Letters

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Long-Lived Hot Carriers in Two-Dimensional Perovskites: The Role of Alternating Cations in Interlayer Space
ACS Energy Letters ( IF 19.3 ) Pub Date : 2023-09-22 , DOI: 10.1021/acsenergylett.3c01691
Qi Wei ₁ , Hui Ren ₁ , Jinjie Liu ₁ , Qi Liu ₁ , Chenhao Wang ₁ , Ting Wai Lau ₁ , Luwei Zhou ₁ , Tieyuan Bian ₁ , Yifan Zhou ₁ , Pengzhi Wang ₁ , Qiong Lei ₁ , Omar F. Mohammed ₂ , Mingjie Li _{1,

3} , Jun Yin ₁

Affiliation

Solar absorbers featuring prolonged hot-carrier (HC) cooling are highly desired for the development of HC solar cells. Two-dimensional (2D) hybrid perovskites are known for their exceptional stability and tunable optoelectronic properties. Nevertheless, their hot-carrier dynamics have been inadequately investigated. Here, we demonstrate ultraslow hot-carrier cooling with a lifetime >2 ns and long HC diffusion length in 2D (ACA)(MA)PbI₄ (ACA = acetamidinium) with alternating cations in the interlayer space (ACI), surpassing those of 3D MAPbBr₃ and 2D Ruddlesden–Popper (PEA)₂PbI₄. Our nonadiabatic molecular dynamics simulations with spin–orbit coupling show that the enhanced HC cooling in the ACI-phase 2D perovskite is due to multiple split-off bands and reduced electron–phonon coupling. Furthermore, the hot electrons can be efficiently extracted from (ACA)(MA)PbI₄ and then transferred to the electron-transporting layer. These new insights highlight the benefit of manipulating interlayer cations in 2D perovskites as an advantageous approach to control long-lived hot carriers, thus potentially enhancing photovoltaic device performance.

中文翻译：

二维钙钛矿中的长寿命热载流子：交替阳离子在层间空间中的作用

HC太阳能电池的开发非常需要具有长时间热载流子（HC）冷却功能的太阳能吸收器。二维（2D）杂化钙钛矿以其卓越的稳定性和可调谐的光电特性而闻名。然而，它们的热载流子动力学尚未得到充分研究。_{在这里，我们展示了 2D (ACA)(MA)PbI 4} (ACA = 乙脒) 中具有交替阳离子的层间空间 (ACI) 的超慢热载流子冷却，其寿命 >2 ns 和长 HC 扩散长度，超过了 3D MAPbBr ₃和 2D Ruddlesden-Popper (PEA) ₂ PbI ₄。我们利用自旋轨道耦合进行的非绝热分子动力学模拟表明，ACI 相二维钙钛矿中 HC 冷却的增强是由于多个分裂能带和减少的电子声子耦合。此外，热电子可以有效地从(ACA)(MA)PbI ₄中提取，然后转移到电子传输层。这些新见解强调了操纵二维钙钛矿中层间阳离子的好处，作为控制长寿命热载流子的有利方法，从而有可能提高光伏器件的性能。

更新日期：2023-09-22

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