Phonon-Polaritons in Non-Centrosymmetric Systems: Theory of Terahertz Pump-Optical Probe Spectroscopy
arXiv:2411.10160 · doi:10.1038/s41535-025-00761-8
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 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.
References in corpus (13)
- Nonlinear phononics: A new ultrafast route to lattice control
- An effective magnetic field from optically driven phonons
- Ultrafast reversal of the ferroelectric polarization
- Cherenkov radiation emitted by ultrafast laser pulses and the generation of coherent polaritons
- Theory of coherent oscillations detection in THz pump-probe spectroscopy: from phonons to electronic collective modes
- Femtosecond Photophysics of Molecular Polaritons
- Hamiltonian optics of hyperbolic polaritons in nanogranules
- Probing Hyperbolic and Surface Phonon-Polaritons in 2D materials using Raman Spectroscopy
- Terahertz ionic Kerr effect: Two-phonon contribution to the nonlinear optical response in insulators
- Infrared super-resolution wide-field microscopy using sum-frequency generation
- Ultrafast tunable modulation of light polarization at terahertz frequencies
- Time-domain study of coupled collective excitations in quantum materials
- Raman-phonon-polariton condensation in a transversely pumped cavity