Nano Letters· 2026Q1
Intra- and Interlayer Excitonic Fine Structure of the Two-Dimensional Perovskite (PEA)2PbI4
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- Q1SCImago
- 2026year
Short summary
Polarization-resolved photoluminescence and first-principles calculations reveal that the fine structure of excitons in the 2D perovskite (PEA)2PbI4 is primarily governed by intralayer electron-hole exchange and crystal symmetry, with a distinct interlayer exciton component.
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Key points
- The low-energy excitonic multiplet in (PEA)2PbI4 is primarily due to intralayer excitonic fine structure.
- Electron-hole exchange, crystal symmetry, and layer inequivalence are the main drivers of this intralayer structure.
- A weaker, higher-energy doublet is attributed to interlayer excitons.
- Distortion-induced mixing between interlayer and intralayer excitons explains the observed interlayer PL intensities and polarizations.
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Abstract
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.
The authors' abstract, as published at the source. Nano Letters, 2026 · DOI ↗
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Field: Electrical and Electronic Engineering
Electrical and Electronic EngineeringEngineering