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Slow thermal equilibration in methylammonium lead iodide revealed by transient mid-infrared spectroscopy

机译:瞬态中红外光谱显示甲基铵碘化铅中的缓慢热平衡

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摘要

Hybrid organic–inorganic perovskites are emerging semiconductors for cheap and efficient photovoltaics and light-emitting devices. Different from conventional inorganic semiconductors, hybrid perovskites consist of coexisting organic and inorganic sub-lattices, which present disparate atomic masses and bond strengths. The nanoscopic interpenetration of these disparate components, which lack strong electronic and vibrational coupling, presents fundamental challenges to the understanding of charge and heat dissipation. Here we study phonon population and equilibration processes in methylammonium lead iodide (MAPbI3) by transiently probing the vibrational modes of the organic sub-lattice following above-bandgap optical excitation. We observe inter-sub-lattice thermal equilibration on timescales ranging from hundreds of picoseconds to a couple of nanoseconds. As supported by a two-temperature model based on first-principles calculations, the slow thermal equilibration is attributable to the sequential phonon populations of the inorganic and organic sub-lattices, respectively. The observed long-lasting thermal non-equilibrium offers insights into thermal transport and heat management of the emergent hybrid material class.
机译:有机-无机杂化钙钛矿是新兴的半导体,可用于廉价,高效的光伏和发光器件。与传统的无机半导体不同,杂化钙钛矿由共存的有机和无机亚晶格组成,这些亚晶格具有不同的原子质量和键强度。这些分散的组件之间的纳米级互穿缺乏牢固的电子和振动耦合,这对理解电荷和散热提出了根本性的挑战。在这里,我们通过在带隙以上的光激发之后瞬态探测有机亚晶格的振动模式来研究甲基铵碘化铅(MAPbI3)中的声子填充和平衡过程。我们在几百皮秒到几纳秒的时间尺度上观察到亚晶格间的热平衡。在基于第一性原理计算的双温度模型的支持下,缓慢的热平衡分别归因于无机和有机亚晶格的连续声子群。观察到的持久热不平衡为新兴杂化材料类别的热传输和热管理提供了见解。

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