Quantitative Modeling of Polaritonic Emission Using the Source Term Method

Strong exciton-photon coupling leads to the formation of hybrid states, polaritons, with properties different from those of their constituents, making it a valuable tool for modifying the physical and chemical properties of organic and inorganic materials. Despite its potential, the field lacks a fu...

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Bibliographic Details
Authors: Bhuyan, Rahul; Lednev, Maksim; Schäfer, Clara; Feist, Johannes Maximilian; Börjesson, Karl
Format: Article
Publication date:2025
Country:España
Institution:Universidad Autónoma de Madrid
Repository:Biblos-e Archivo. Repositorio Institucional de la UAM
Language:English
OAI Identifier:oai:repositorio.uam.es:10486/752760
Online Access:https://hdl.handle.net/10486/752760
https://dx.doi.org/10.1021/acs.jpclett.5c01213
Access Level:Open access
Keyword:Cavities
energy
molecules
polaritons
polarization
Física
Description
Summary:Strong exciton-photon coupling leads to the formation of hybrid states, polaritons, with properties different from those of their constituents, making it a valuable tool for modifying the physical and chemical properties of organic and inorganic materials. Despite its potential, the field lacks a fundamental understanding of the photophysics involved and the ability to model experimental data effectively. In this study, we quantitatively simulate polaritonic emission using the source term method. This model assumes that each molecular dipole in the exciton reservoir emits as it would in free space, into the optical environment formed by the polaritons. To benchmark theory with experiments, a BODIPY derivative containing a suitable amount of steric bulk was synthesized. Neat films of this molecule exhibited close to unperturbed absorption and emission envelopes compared to dilute solution. When placed in an optical cavity, the ultrastrong coupling regime was reached, and a collapse of the polaritonic line width was observed. Such a collapse is an indication of an ideal polariton, and it allowed for the emission in the transverse electric and magnetic polarizations to be spectrally resolved and thus successfully compared to the simulated emission. This work hence describes an effective model that fits experimental data, which is crucial for advancing the field and for optimizing applications