Surface Exciton Polariton in Cesium Lead Halide Perovskites

In this article, we developed a theory describing surface exciton polaritons (SEPs) that accounts for the spatial dispersion of the dielectric constant connected with exciton momentum. Due to strong coupling between light and bulk excitons in the frequency separation, ℏωLT, between the longitudinal and transverse excitons, the SEP is formed and behaves as partially light and partially matter. The dispersion of the SEP was found through a combined solution of Maxwell’s and Thomas-Hopfield’s equations. The analytical theory describes SEPs at any bulk exciton/vacuum interface and provides its complete dispersion if one knows ℏωLT, the exciton effective mass, M, and the high-frequency dielectric constant, κ∞. The presented theory is in excellent agreement with the only numerical modeling of this problem, which was conducted for SEPs at a ZnO/vacuum interface. Calculations show the spatial dispersion of the dielectric constant leads to rather small broadening of the photon-like quasi-particle and suggest using SEPs for long-range coherence transfer. The theory was used to describe SEP dispersion in CsPbCl3 and CsPbBr3 perovskites.

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Publication Details

Journal
Chemistry of Materials
Published
2025-03-07
DOI
https://doi.org/10.1021/acs.chemmater.4c03262
Primary Topic
Perovskite Materials and Applications
Type
article
Field-Weighted Citation Impact
0.00

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Surface Exciton Polariton in Cesium Lead Halide Perovskites

Daniel Ratchford, Alexander L. Efros, Jeffrey C. Owrutsky, J. Hao et al.
Chemistry of Materials
Perovskite Materials and Applications
article

Surface Exciton Polariton in Cesium Lead Halide Perovskites

Daniel Ratchford, Alexander L. Efros, Jeffrey C. Owrutsky, J. Hao, Blake S. Simpkins
article en

Abstract

In this article, we developed a theory describing surface exciton polaritons (SEPs) that accounts for the spatial dispersion of the dielectric constant connected with exciton momentum. Due to strong coupling between light and bulk excitons in the frequency separation, ℏωLT, between the longitudinal and transverse excitons, the SEP is formed and behaves as partially light and partially matter. The dispersion of the SEP was found through a combined solution of Maxwell’s and Thomas-Hopfield’s equations. The analytical theory describes SEPs at any bulk exciton/vacuum interface and provides its complete dispersion if one knows ℏωLT, the exciton effective mass, M, and the high-frequency dielectric constant, κ∞. The presented theory is in excellent agreement with the only numerical modeling of this problem, which was conducted for SEPs at a ZnO/vacuum interface. Calculations show the spatial dispersion of the dielectric constant leads to rather small broadening of the photon-like quasi-particle and suggest using SEPs for long-range coherence transfer. The theory was used to describe SEP dispersion in CsPbCl3 and CsPbBr3 perovskites.

Chemistry of MaterialsVol. 37(6)
United States Naval Research Laboratory (US), Thomas Jefferson School of Law (US), Precise (India) (IN), PRG S&Tech (South Korea), United States Navy (US)
U.S. Navy, Office of Naval Research
Openalex Percentile: Top 97%
Perovskite Materials and Applications
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Surface Exciton Polariton in Cesium Lead Halide Perovskites — Daniel Ratchford, Alexander L. Efros, et al. · Chemistry of Materials (2025) | TGRS Research Map | TGRS