Theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systems.

Niccolò Sellati, Jacopo Fiore, Stefano Paolo Villani, Lara Benfatto, Mattia Udina

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Article in npj quantum materials, 2025. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.

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5 authors.

Niccolò SellatiDepartment of Physics, Sapienza University of Rome, P.le A. Moro 5, 00185 Rome, Italy.

Jacopo FioreDepartment of Physics, Sapienza University of Rome, P.le A. Moro 5, 00185 Rome, Italy.

Stefano Paolo VillaniDepartment of Physics, Sapienza University of Rome, P.le A. Moro 5, 00185 Rome, Italy.

Lara BenfattoDepartment of Physics, Sapienza University of Rome, P.le A. Moro 5, 00185 Rome, Italy.

Mattia UdinaDepartment of Physics, Sapienza University of Rome, P.le A. Moro 5, 00185 Rome, Italy.

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Abstract

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 discuss the limitations of all-optical four-wave mixing protocols and we highlight the advantages of exploiting broadband THz pumps to enlarge the phase space of the phonon polariton dispersion at low momenta 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.

Indexed as

Condensed-matter physicsNonlinear opticsPolaritonsTerahertz opticsUltrafast photonics

Identifiers

PMID40322594

DOI10.1038/s41535-025-00761-8

PMCPMC12045802

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