Microscopic Theory of Multimode Polariton Dispersion in Multilayered Materials.

Nano Lett

Department of Chemistry, Columbia University, 3000 Broadway, New York, New York 10027, United States.

Published: May 2023

We develop a microscopic theory for the multimode polariton dispersion in materials coupled to cavity radiation modes. Starting from a microscopic light-matter Hamiltonian, we devise a general strategy for obtaining simple matrix models of polariton dispersion curves based on the structure and spatial location of multilayered 2D materials inside the optical cavity. Our theory exposes the connections between seemingly distinct models that have been employed in the literature and resolves an ambiguity that has arisen concerning the experimental description of the polaritonic band structure. We demonstrate the applicability of our theoretical formalism by fabricating various geometries of multilayered perovskite materials coupled to cavities and demonstrating that our theoretical predictions agree with the experimental results presented here.

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http://dx.doi.org/10.1021/acs.nanolett.3c01017DOI Listing

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