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arXiv 2606.02460cond-mat.mes-hall
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外延CsPbBr3单晶中的非平衡输运

Nonequilibrium transport in epitaxial CsPbBr3 single crystals

Massachusetts Institute of Technology(麻省理工学院);Philipps Universität Marburg(马尔堡菲利普斯大学);Rutgers University(罗格斯大学)

Seryio Saris, Roberto Rosati, Vladimir Bruevich, Thomas J. Sheehan, Maksim Roman, Vitaly Podzorov, Ermin Malic, William A. Tisdale

AI总结:

通过瞬态显微镜研究外延CsPbBr3钙钛矿单晶中光激发载流子的输运,发现近室温下符合准平衡图像,但在低温(<60 K)下平衡模型失效,观察到热激子气体和准局域态两种耦合布居,表明输运与热化不可分离。

摘要:

半导体中光激发载流子的输运通常用准平衡图像描述,其中能量由具有明确输运系数的单一热化准粒子布居携带。这里,我们证明在外延CsPbBr3钙钛矿单晶中,该图像在室温附近成立,但在低温下显著失效。利用瞬态显微镜,我们展示了光学测量的载流子迁移率在宽温度范围内与器件级霍尔效应和场效应晶体管测量结果一致,解决了报道的差异,并验证了自由载流子区域中的平衡框架。然而,在约60 K以下,当激子效应变得显著时,平衡模型开始失效。我们观察到两个耦合布居:一个瞬态(<100 ps)热激子气体,其扩散率约为25-30 cm²/s,远超热化激子的预期扩散率;以及一个准局域态,由热激子气体的冷却提供。这些结果表明,在CsPbBr3中,输运和热化不是可分离的过程:载流子在移动的同时仍在内部自由度之间重新分布,打破了传统半导体中平衡输运理论所依赖的时间尺度分离。通过在布居水平上解析输运,我们可以直接访问激子形成、相互转换和冷却的竞争动力学,为控制钙钛矿材料及其光子应用中的能量流提供了新的空间。

英文摘要:

Transport of optically excited carriers in semiconductors is typically described within a quasi-equilibrium picture, where energy is carried by a single thermalized quasiparticle population characterized by well-defined transport coefficients. Here, we demonstrate that in epitaxial CsPbBr3 perovskite single crystals, this picture holds near room temperature - but breaks down dramatically at low temperature. Using transient microscopy, we show that optically measured carrier mobilities match device-scale Hall-effect and field-effect transistor measurements across a broad temperature range, resolving reported discrepancies and validating the equilibrium framework in the free-carrier regime. Below ~60 K, however, when excitonic effects become significant, equilibrium models begin to fail. We observe two coupled populations: a transient (<100 ps) hot-exciton gas with a diffusivity ~25-30 cm<sup>2</sup>/s - greatly exceeding the diffusivity expected for thermalized excitons - and a quasi-localized state that is fed by the cooling of the hot-exciton gas. These results reveal that in CsPbBr3, transport and thermalization are not separable processes: carriers move while still redistributing among internal degrees of freedom, breaking the timescale separation that underpins equilibrium transport theory in conventional semiconductors. By resolving transport at the population level, we can directly access the competing kinetics of exciton formation, interconversion, and cooling, offering a new space for controlling energy flow in perovskite materials and their photonic applications.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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