The hot phonon bottleneck (HPB) effect has been proposed as one of the main phenomena behind the slow cooling in metal halide perovskites. Even though consensus has been reached regarding its existence, open questions remain concerning the HPB’s specific applicability and potential regarding hot carrier solar cell (HCSC) applications. We present a full investigation using ensemble Monte Carlo simulations of the HPB effect in metal halide perovskites (MHP). After describing the HPB effect in detail, we quantify how the HPB effect can extend carrier cooling times by orders of magnitude. We show how the HPB effect depends on carrier concentration, longitudinal optical (LO) phonon lifetime, and LO phonon frequency and connect these findings to how MHPs should be tuned concretely. Using ensemble Monte Carlo simulations, we can accurately model the interplay between carrier–phonon and carrier–carrier interactions up to high carrier density, yielding precise predictions regarding the HPB effect. This study provides important insights into the governing dynamics behind the HPB effect and shows how cooling times can be extended far beyond the phonon lifetime. Furthermore, it contributes to the discussion on cooling times in MHPs and their suitability for HCSC applications.

中文翻译：

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金属卤化物钙钛矿中的热声子瓶颈效应


热声子瓶颈 （HPB） 效应被认为是金属卤化物钙钛矿缓慢冷却的主要现象之一。尽管已经就其存在达成了共识，但关于 HPB 在热载流子太阳能电池 （HCSC） 应用方面的具体适用性和潜力仍然存在悬而未决的问题。我们使用集成蒙特卡洛模拟对金属卤化物钙钛矿 （MHP） 中的 HPB 效应进行了全面研究。在详细描述了 HPB 效应之后，我们量化了 HPB 效应如何将载流子冷却时间延长几个数量级。我们展示了 HPB 效应如何取决于载流子浓度、纵向光学 （LO） 声子寿命和 LO 声子频率，并将这些发现与 MHP 的具体调谐方式联系起来。使用集成蒙特卡洛模拟，我们可以准确地模拟载流子-声子和载流子-载流子相互作用之间的相互作用，直至高载流子密度，从而对 HPB 效应产生精确预测。这项研究为 HPB 效应背后的控制动力学提供了重要的见解，并展示了如何将冷却时间延长到远远超过声子寿命。此外，它还有助于讨论 MHP 的冷却时间及其对 HCSC 应用的适用性。