Theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systems
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 Rama...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-05-01
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| Series: | npj Quantum Materials |
| Online Access: | https://doi.org/10.1038/s41535-025-00761-8 |
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| author | Niccolò Sellati Jacopo Fiore Stefano Paolo Villani Lara Benfatto Mattia Udina |
| author_facet | Niccolò Sellati Jacopo Fiore Stefano Paolo Villani Lara Benfatto Mattia Udina |
| author_sort | Niccolò Sellati |
| collection | DOAJ |
| description | 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. |
| format | Article |
| id | doaj-art-0fb4ad1b820d4ea1987d5955eab4aac6 |
| institution | OA Journals |
| issn | 2397-4648 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | npj Quantum Materials |
| spelling | doaj-art-0fb4ad1b820d4ea1987d5955eab4aac62025-08-20T02:10:48ZengNature Portfolionpj Quantum Materials2397-46482025-05-011011610.1038/s41535-025-00761-8Theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systemsNiccolò Sellati0Jacopo Fiore1Stefano Paolo Villani2Lara Benfatto3Mattia Udina4Department of Physics, Sapienza University of RomeDepartment of Physics, Sapienza University of RomeDepartment of Physics, Sapienza University of RomeDepartment of Physics, Sapienza University of RomeDepartment of Physics, Sapienza University of RomeAbstract 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.https://doi.org/10.1038/s41535-025-00761-8 |
| spellingShingle | Niccolò Sellati Jacopo Fiore Stefano Paolo Villani Lara Benfatto Mattia Udina Theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systems npj Quantum Materials |
| title | Theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systems |
| title_full | Theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systems |
| title_fullStr | Theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systems |
| title_full_unstemmed | Theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systems |
| title_short | Theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systems |
| title_sort | theory of terahertz pump optical probe spectroscopy of phonon polaritons in noncentrosymmetric systems |
| url | https://doi.org/10.1038/s41535-025-00761-8 |
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