论文标题

使用Van der waals钝化,在2D钙钛矿中揭示了巨大的激子精细结构分裂

Revealing giant exciton fine-structure splitting in 2D perovskites using van der Waals passivation

论文作者

Canet-Albiach, Rodolfo, Krecmarova, Marie, Bailach, José Bosch, Gualdrón-Reyes, Andrés F., Rodríguez-Romero, Jesús, Gorji, Setatira, Pashaei-Adl, Hamid, Mora-Seró, Iván, Pastor, Juan Martínez, Sánchez-Royo, Juan Francisco, Matutano, Guillermo Muñoz

论文摘要

在过去的十年中,二维(2D)范德华材料的研究一直是新的光电子和光子应用开发的积极研究领域。有机无机分层的钙钛矿目前是一些最有前途的2D范德华材料,因为它们具有出色的光学亮度和增强的兴奋型效应。然而,低晶体质量和光谱扩散通常会扩大激子宽度,从而掩盖了传统的光致发光实验中激子的精细结构。在这里,我们提出了一种机械方法,用于通过HBN限制对具有不同厚度的分层钙晶质的含量来降低光谱扩散的影响,从而揭示了激子细胞的结构。我们使用随机模型将光谱线宽的降低与有机隔离器中存在的活跃电荷波动中心的种群联系起来,参与了动态较为鲜明的变化。当我们根据直接光谱测量值包括HBN限制时,主动波动中心减少了3.7至7.1。该速率与对平方钙钛矿晶格与六角形HBN晶格之间重叠的分析非常吻合。两个晶格之间的范德华力会导致钙钛矿有机间隔分子的部分夹紧,因此,光谱扩散效应的动力学鲜明偏移特性的幅度降低了。我们的工作为访问重要的精细结构激子信息信息的问题提供了一种简单且低成本的解决方案,并解释了有机间隔者中存在的重要载体动力学,从而影响光学发射的质量。

The study of two-dimensional (2D) van der Waals materials has been an active field of research in the development of new optoelectronics and photonic applications over the last decade. Organic-inorganic layered perovskites are currently some of the most promising 2D van der Waals materials, due to their exceptional optical brightness and enhanced excitonic effects. However, low crystal quality and spectral diffusion usually broaden the exciton linewidth, obscuring the fine structure of the exciton in conventional photoluminescence experiments. Here, we propose a mechanical approach for reducing the effect of spectral diffusion by means of hBN-capping on layered perovskites with different thicknesses, revealing the exciton fine structure. We used a stochastic model to link the reduction of the spectral linewidth with the population of active charge fluctuation centres present in the organic spacer taking part in the dynamical Stark shift. Active fluctuation centres are reduced by a factor of 3.7 to 7.1 when we include hBN-capping according to our direct spectral measurements. This rate is in good agreement with the analysis of the overlap between the squared perovskite lattice and the hexagonal hBN lattice. Van der Waals forces between both lattices cause the partial clamping of the perovskite organic spacer molecules, and hence, the amplitude of the dynamical Stark shift characteristic of the spectral diffusion effect is reduced. Our work provides an easy and low-cost solution to the problem of accessing important fine-structure excitonic state information, along with an explanation of the important carrier dynamics present in the organic spacer that affect the quality of the optical emission.

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