Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites

Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites
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DOI:
10.1103/physrevresearch.1.032032
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发表时间:
2019-04
影响因子:
4.2
通讯作者:
F. Thouin;D. Cortecchia;A. Petrozza;A. R. Srimath Kandada;Carlos Silva
F. Thouin;D. Cortecchia;A. Petrozza;A. R. Srimath Kandada;Carlos Silva
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文献类型:
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作者:
F. Thouin;D. Cortecchia;A. Petrozza;A. R. Srimath Kandada;Carlos Silva

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在二维混合有机-无机金属卤化物钙钛矿中,固有光学线形反射具有不同结合能的多个激子,每个激子通过混合晶格被不同地修饰。考虑到这种复杂性,一个根本上意义深远的问题是如何库仑介导的多体相互作用-弹性散射,如激发诱导的退相,非弹性激子双分子散射,和多激子绑定-取决于特定的激子晶格耦合。我们报告的内在和密度依赖的激子纯退相率和它们的依赖于温度的相干非线性光谱。我们发现,相对于其他二维单原子层半导体,多激子散射具有非常强的屏蔽效应。重要的是,不同激子的退相速率的激子密度依赖性明显不同。这些研究结果建立了特定的晶格敷料上激子多体量子动力学的后果,严格定义基本的光学特性,支持相关激子密度制度的光子学和量子光电子学。
In two-dimensional hybrid organic-inorganic metal-halide perovskites, the intrinsic optical lineshape reflects multiple excitons with distinct binding energies, each dressed differently by the hybrid lattice. Given this complexity, a fundamentally far-reaching issue is how Coulomb-mediated many-body interactions --- elastic scattering such as excitation-induced dephasing, inelastic exciton bimolecular scattering, and multi-exciton binding --- depend upon the specific exciton-lattice coupling. We report the intrinsic and density-dependent exciton pure dephasing rates and their dependence on temperature by means of a coherent nonlinear spectroscopy. We find exceptionally strong screening effects on multi-exciton scattering relative to other two-dimensional single-atomic-layer semiconductors. Importantly, the exciton-density dependence of the dephasing rates is markedly different for distinct excitons. These findings establish the consequences of particular lattice dressing on exciton many-body quantum dynamics, which critically define fundamental optical properties that underpin photonics and quantum optoelectronics in relevant exciton density regimes.