Microscopic theory of phonon polaritons and long wavelength dielectric response

Fuente: arXiv
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Autores principales: Hellman, Olle, Kronik, Leeor
Formato: Preprint
Publicado: 2025
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author Hellman, Olle
Kronik, Leeor
author_facet Hellman, Olle
Kronik, Leeor
contents We present a first-principles approach for calculating phonon-polariton dispersion relations. In this approach, phonon-photon interaction is described by quantization of a Hamiltonian that describes harmonic lattice vibrations coupled with the electromagnetic field inside the material. All Hamiltonian parameters are obtained from first-principles calculations, with diagonalization leading to non-interacting polariton quasiparticles. This method naturally includes retardation effects and resolves non-analytical behavior and ambiguities in phonon frequencies at the Brillouin zone center, especially in non-cubic and optically anisotropic materials. Furthermore, by incorporating higher-order terms in the Hamiltonian, we also account for quasiparticle interactions and spectral broadening. Specifically, we show how anharmonic effects in phonon polaritons lead to a dielectric response that challenges traditional models. The accuracy and consequences of the approach are demonstrated on GaP and GaN as harmonic test systems and PbTe and $β$-Ga$_2$O$_3$ as anharmonic test systems.
format Preprint
id arxiv_https___arxiv_org_abs_2505_03915
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Microscopic theory of phonon polaritons and long wavelength dielectric response
Hellman, Olle
Kronik, Leeor
Materials Science
We present a first-principles approach for calculating phonon-polariton dispersion relations. In this approach, phonon-photon interaction is described by quantization of a Hamiltonian that describes harmonic lattice vibrations coupled with the electromagnetic field inside the material. All Hamiltonian parameters are obtained from first-principles calculations, with diagonalization leading to non-interacting polariton quasiparticles. This method naturally includes retardation effects and resolves non-analytical behavior and ambiguities in phonon frequencies at the Brillouin zone center, especially in non-cubic and optically anisotropic materials. Furthermore, by incorporating higher-order terms in the Hamiltonian, we also account for quasiparticle interactions and spectral broadening. Specifically, we show how anharmonic effects in phonon polaritons lead to a dielectric response that challenges traditional models. The accuracy and consequences of the approach are demonstrated on GaP and GaN as harmonic test systems and PbTe and $β$-Ga$_2$O$_3$ as anharmonic test systems.
title Microscopic theory of phonon polaritons and long wavelength dielectric response
topic Materials Science
url https://arxiv.org/abs/2505.03915