Los Alamos National Laboratory, Los Alamos, NM, 87545, USA.
Department of Materials Science and Nanoengineering, Rice University, Houston, TX, 77005, USA.
Nat Commun. 2018 Jun 8;9(1):2254. doi: 10.1038/s41467-018-04659-x.
Ruddlesden-Popper halide perovskites are 2D solution-processed quantum wells with a general formula AA'M X, where optoelectronic properties can be tuned by varying the perovskite layer thickness (n-value), and have recently emerged as efficient semiconductors with technologically relevant stability. However, fundamental questions concerning the nature of optical resonances (excitons or free carriers) and the exciton reduced mass, and their scaling with quantum well thickness, which are critical for designing efficient optoelectronic devices, remain unresolved. Here, using optical spectroscopy and 60-Tesla magneto-absorption supported by modeling, we unambiguously demonstrate that the optical resonances arise from tightly bound excitons with both exciton reduced masses and binding energies decreasing, respectively, from 0.221 m to 0.186 m and from 470 meV to 125 meV with increasing thickness from n equals 1 to 5. Based on this study we propose a general scaling law to determine the binding energy of excitons in perovskite quantum wells of any layer thickness.
Ruddlesden-Popper 卤化物钙钛矿是二维溶液处理量子阱,其通式为 AA'MX,通过改变钙钛矿层厚度(n 值)可以调节光电性能,最近作为具有技术相关稳定性的高效半导体而出现。然而,关于光学共振(激子或自由载流子)的本质以及激子有效质量及其与量子阱厚度的关系的基本问题,对于设计高效的光电设备至关重要,仍未得到解决。在这里,我们使用光学光谱学和 60 特斯拉磁吸收,并通过建模进行支持,明确证明了光学共振是由紧密束缚的激子引起的,激子有效质量和结合能分别从 0.221m 减小到 0.186m,从 470meV 减小到 125meV,厚度从 n 等于 1 增加到 5。基于这项研究,我们提出了一个通用的标度定律来确定任何层厚的钙钛矿量子阱中激子的结合能。