Raman resonances mediated by excitonic polarons in BiVO$_4$

Fuente: arXiv
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Autores principales: Gordeev, Georgy, Hill, Christina, Gudima, Angelina, Reich, Stephanie, Guennou, Mael
Formato: Preprint
Publicado: 2024
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author Gordeev, Georgy
Hill, Christina
Gudima, Angelina
Reich, Stephanie
Guennou, Mael
author_facet Gordeev, Georgy
Hill, Christina
Gudima, Angelina
Reich, Stephanie
Guennou, Mael
contents Excitonic polarons are quasiparticles formed by a Coulomb-bound electron-hole pair with strong coupling to lattice vibrations. Despite high fundamental interest in excitonic polarons, the experimental investigation of these particles remains challenging. In this work, we exploit the resonant Raman effect to probe the excitonic polarons in bismuth vanadate. We track enhancement of Raman modes as a function of excitation energy and reveal two optical resonances: one inside the band gap at 1.94 eV and another one near the optical absorption edge at 2.45 eV. The high-energy resonance originates from free excitons, which exhibit a characteristic 40 meV anisotropy between polarizations parallel and perpendicular to the c axis. Remarkably, the low-energy resonance shows no contrast in the optical absorption spectra. We attribute this resonance to an excitonic polaron formed through strong exciton-phonon coupling, making excitonic and excitonic polaron Raman resonances similar in strength. We probe the energy level of the excitonic polaron and compare its coupling strength to the different vibrational modes. Our results establish resonant Raman spectroscopy as a unique and powerful tool for probing quasiparticles of polaronic and excitonic nature in oxide materials.
format Preprint
id arxiv_https___arxiv_org_abs_2404_04112
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Raman resonances mediated by excitonic polarons in BiVO$_4$
Gordeev, Georgy
Hill, Christina
Gudima, Angelina
Reich, Stephanie
Guennou, Mael
Materials Science
Excitonic polarons are quasiparticles formed by a Coulomb-bound electron-hole pair with strong coupling to lattice vibrations. Despite high fundamental interest in excitonic polarons, the experimental investigation of these particles remains challenging. In this work, we exploit the resonant Raman effect to probe the excitonic polarons in bismuth vanadate. We track enhancement of Raman modes as a function of excitation energy and reveal two optical resonances: one inside the band gap at 1.94 eV and another one near the optical absorption edge at 2.45 eV. The high-energy resonance originates from free excitons, which exhibit a characteristic 40 meV anisotropy between polarizations parallel and perpendicular to the c axis. Remarkably, the low-energy resonance shows no contrast in the optical absorption spectra. We attribute this resonance to an excitonic polaron formed through strong exciton-phonon coupling, making excitonic and excitonic polaron Raman resonances similar in strength. We probe the energy level of the excitonic polaron and compare its coupling strength to the different vibrational modes. Our results establish resonant Raman spectroscopy as a unique and powerful tool for probing quasiparticles of polaronic and excitonic nature in oxide materials.
title Raman resonances mediated by excitonic polarons in BiVO$_4$
topic Materials Science
url https://arxiv.org/abs/2404.04112