Intra- and Interlayer Excitonic Fine Structure of the Two-Dimensional Perovskite (PEA)2PbI4

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2026-10-21 DOI:10.1021/acs.nanolett.6c01957

Patrick Grenzer,Fabian Lie,Klaus H. Eckstein,Tobias Hertel,Linn Leppert

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Abstract

Two-dimensional halide perovskites host strongly bound excitons whose fine structure governs polarization selection rules and radiative recombination, yet spectral features in phenethylammonium lead iodide ((PEA)2PbI4) remain controversially assigned. Here, polarization-resolved low-temperature photoluminescence (PL) combined with first-principles G0W0+BSE calculations probes the intralayer and interlayer excitonic fine structure of this Ruddlesden–Popper perovskite. The low-energy multiplet is consistent with the intralayer excitonic fine structure governed by electron–hole exchange, crystal symmetry, and layer inequivalence in the two-layer unit cell, without requiring Rashba effects or exciton–polaron mechanisms as its primary origin. The weak doublet about 40 meV higher is best accounted for by interlayer excitons based on its energetics, splitting, and real-space character. Distortion-induced mixing of interlayer excitons with bright intralayer excitons provides a plausible explanation for the observed interlayer PL intensities and nearly orthogonal polarizations. These results support a layer-resolved excitonic picture encompassing both intralayer and interlayer states in (PEA)2PbI4.

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二维钙钛矿（PEA）2PbI4的层内和层间激子精细结构

二维卤化物钙钛矿具有强束缚激子，其精细结构决定了极化选择规则和辐射复合，但苯乙基碘化铅铵（PEA）2PbI4)的光谱特征仍然存在争议。在这里，偏振分辨低温光致发光（PL）结合第一性原理G0W0+BSE计算探索了Ruddlesden-Popper钙钛矿的层内和层间激子精细结构。低能多重体与两层单元电池中由电子-空穴交换、晶体对称性和层不对称性控制的层内激子精细结构一致，而不需要Rashba效应或激子-极化子机制作为其主要来源。基于其能量学、分裂和实空间特性，用层间激子来解释高约40 meV的弱重态是最好的。扭曲诱导的层间激子与明亮的层内激子混合为观察到的层间PL强度和近正交极化提供了合理的解释。这些结果支持在（PEA）2PbI4中包含层内和层间态的层分辨激子图像。

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

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

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