Phonon-Polaritons in Non-Centrosymmetric Systems: Theory of Terahertz Pump-Optical Probe Spectroscopy

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Main Authors: Sellati, Niccolò, Fiore, Jacopo, Villani, Stefano Paolo, Benfatto, Lara, Udina, Mattia
Format: Preprint
Published: 2024
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author Sellati, Niccolò
Fiore, Jacopo
Villani, Stefano Paolo
Benfatto, Lara
Udina, Mattia
author_facet Sellati, Niccolò
Fiore, Jacopo
Villani, Stefano Paolo
Benfatto, Lara
Udina, Mattia
contents Hybrid lattice-light modes, known as phonon-polaritons, represent the backbone of advanced protocols based on THz pumping of infrared modes. Here we provide a theoretical framework able to capture the different roles played by phonon-polaritons in experimental protocols based either on Raman-like pump and probe schemes, typical of four-wave-mixing processes, or on THz pump-visible probe three-wave mixing protocols. By using a many-body description of the nonlinear optical kernel, along with a perturbative solution of nonlinear Maxwell's equations, we highlight the advantages of exploiting broadband THz pumps to enlarge the phase space of the phonon-polariton dispersion accessible in a single experiment. Besides providing a quantitative description of existing and future experiments, our results offer a general framework for the theoretical modeling of the hybridization between light and lattice degrees of freedom in time-resolved experiments.
format Preprint
id arxiv_https___arxiv_org_abs_2411_10160
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Phonon-Polaritons in Non-Centrosymmetric Systems: Theory of Terahertz Pump-Optical Probe Spectroscopy
Sellati, Niccolò
Fiore, Jacopo
Villani, Stefano Paolo
Benfatto, Lara
Udina, Mattia
Materials Science
Hybrid lattice-light modes, known as phonon-polaritons, represent the backbone of advanced protocols based on THz pumping of infrared modes. Here we provide a theoretical framework able to capture the different roles played by phonon-polaritons in experimental protocols based either on Raman-like pump and probe schemes, typical of four-wave-mixing processes, or on THz pump-visible probe three-wave mixing protocols. By using a many-body description of the nonlinear optical kernel, along with a perturbative solution of nonlinear Maxwell's equations, we highlight the advantages of exploiting broadband THz pumps to enlarge the phase space of the phonon-polariton dispersion accessible in a single experiment. Besides providing a quantitative description of existing and future experiments, our results offer a general framework for the theoretical modeling of the hybridization between light and lattice degrees of freedom in time-resolved experiments.
title Phonon-Polaritons in Non-Centrosymmetric Systems: Theory of Terahertz Pump-Optical Probe Spectroscopy
topic Materials Science
url https://arxiv.org/abs/2411.10160