Organic–inorganic lead-halide perovskites have received a revival of interest in the past few years as a promising class of materials for photovoltaic applications. Despite recent extensive research, the role of cations in defining the high photovoltaic performance of these materials is not fully understood. Here, we conduct nonadiabatic molecular dynamics simulations to study and compare nonradiative hot carrier relaxation in three lead-halide perovskite materials: CH₃NH₃PbI₃, HC(NH₂)₂PbI₃, and CsPbI₃. It is found that the relaxation of hot carriers to the band edges occurs on the ultrafast time scale and displays a strong quantitative dependence on the nature of the cations. The obtained results are explained in terms of electron–phonon couplings, which are strongly affected by the atomic displacements in the Pb–I framework triggered by the cation dynamics.

中文翻译：

---

阳离子对卤化物钙钛矿材料热载体冷却的影响

在过去的几年中，有机-无机卤化铅钙钛矿受到了人们的关注，作为一种有前途的光伏应用材料。尽管最近进行了广泛的研究，但阳离子在定义这些材料的高光伏性能方面的作用尚未完全了解。在这里，我们进行非绝热分子动力学模拟，以研究和三个引卤化物钙钛矿材料比较无辐射热载流子弛豫：CH ₃ NH ₃碘化铅₃，HC（NH ₂）₂碘化铅₃，和CsPbI ₃。发现热载流子向能带边缘的弛豫发生在超快的时间尺度上，并且表现出对阳离子性质的强烈定量依赖性。所获得的结果用电子-声子耦合来解释，电子-声子耦合受阳离子动力学触发的Pb-I框架中原子位移的强烈影响。