Room-Temperature Spin Splitting Enabled by Thermally Activated Symmetry Breaking in Two-Dimensional Hybrid Perovskites

IF 8.6 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-03 DOI:10.1021/acsmaterialslett.6c00650

Aowen Ma, Yumeng Song, Qi Wei, Qiong Lei, Mingjie Li, Philip C. Y. Chow, Jun Yin

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Abstract

We report a combined computational−experimental study that identifies and explains the enhanced spin splitting in single-layered (n = 1) two-dimensional (2D) lead−iodide hybrid perovskites. We develop a high-throughput screening workflow for experimentally synthesized 2D hybrid perovskites and identify 12 compounds with spin splitting, among which (2-BrPEA)₂PbI₄ exhibits the largest splitting energy. To establish a unified structure-splitting relationship, we introduce a root-mean-square deviation (RMSD)-based descriptor defined as the deviation between a structure and its inverted counterpart, which correlates with spin-splitting energy more strongly than conventional bond-angle metrics. Notably, although the reported room-temperature structure of (2-BrPEA)₂PbI₄ is nominally centrosymmetric, it shows strong circularly polarized luminescence (CPL) at room temperature, comparable to the benchmark (4AMP)PbI₄. Ab initio molecular dynamics (AIMD) simulations further reveal thermally activated dynamical distortions that transiently break inversion symmetry and amplify spin splitting, establishing lattice dynamics as a key driver of room-temperature spin functionality in 2D hybrid perovskites.

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二维杂化钙钛矿中热激活对称破缺的室温自旋分裂

我们报告了一项计算-实验相结合的研究，该研究确定并解释了单层（n = 1）二维（2D）铅-碘化杂化钙钛矿中增强的自旋分裂。我们建立了实验合成的二维杂化钙钛矿的高通量筛选流程，并鉴定出12种具有自旋分裂的化合物，其中（2-BrPEA）2PbI4具有最大的分裂能。为了建立统一的结构分裂关系，我们引入了一个基于均方根偏差（RMSD）的描述符，它被定义为一个结构与其反向对应结构之间的偏差，它与自旋分裂能的相关性比传统的键角指标更强。值得注意的是，尽管报道的（2-BrPEA）2PbI4的室温结构名义上是中心对称的，但它在室温下表现出很强的圆偏振发光（CPL），与基准（4AMP）PbI4相当。从头算分子动力学（AIMD）模拟进一步揭示了热激活的动态扭曲，这些扭曲会瞬间打破反转对称并放大自旋分裂，从而确立了晶格动力学是二维杂化钙钛矿室温自旋功能的关键驱动因素。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.