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Electron–phonon coupling in hybrid lead halide perovskites

机译:混合卤化钙钛矿中的电子-声子耦合

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摘要

Phonon scattering limits charge-carrier mobilities and governs emission line broadening in hybrid metal halide perovskites. Establishing how charge carriers interact with phonons in these materials is therefore essential for the development of high-efficiency perovskite photovoltaics and low-cost lasers. Here we investigate the temperature dependence of emission line broadening in the four commonly studied formamidinium and methylammonium perovskites, HC(NH2)2PbI3, HC(NH2)2PbBr3, CH3NH3PbI3 and CH3NH3PbBr3, and discover that scattering from longitudinal optical phonons via the Fröhlich interaction is the dominant source of electron–phonon coupling near room temperature, with scattering off acoustic phonons negligible. We determine energies for the interacting longitudinal optical phonon modes to be 11.5 and 15.3 meV, and Fröhlich coupling constants of ∼40 and 60 meV for the lead iodide and bromide perovskites, respectively. Our findings correlate well with first-principles calculations based on many-body perturbation theory, which underlines the suitability of an electronic band-structure picture for describing charge carriers in hybrid perovskites.
机译:声子散射限制了载流子迁移率,并控制了混合金属卤化物钙钛矿中的发射线加宽。因此,建立电荷载流子如何与这些材料中的声子相互作用对于开发高效钙钛矿光伏电池和低成本激光器至关重要。在这里,我们研究了四种常用的钙钛矿型甲铵和甲基铵钙钛矿,HC(NH2)2PbI3,HC(NH2)2PbBr3,CH3NH3PbI3和CH3NH3PbBr3中发射线展宽的温度依赖性,并发现通过Fröhlich相互作用从纵向光子产生的散射是室温附近电子-声子耦合的主要来源,声子的散射可以忽略不计。我们确定相互作用的纵向光学声子模式的能量分别为11.5和15.3idemeV,碘化铅和溴化钙钛矿的Fröhlich耦合常数分别为40和60 meV。我们的发现与基于多体扰动理论的第一性原理计算很好地相关,这强调了电子能带结构图片用于描述混合钙钛矿中电荷载体的适用性。

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