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We introduce a new theoretical approach for analyzing pump and probe experiments in non-linear systems of optical phonons. In our approach, the effect of coherently pumped polaritons is modeled as providing time-periodic modulation of the system parameters. Within this framework, propagation of the probe pulse is described by the Floquet version of Maxwell’s equations and leads to phenomena such as frequency mixing and resonant parametric production of polariton pairs. We analyze light reflection from a slab of insulating material with a strongly excited phonon-polariton mode and obtain analytic expressions for the frequency-dependent reflection coefficient for the probe pulse. Our results are in agreement with recent experiments by Cartella et al. [Proc. Natl. Acad. Sci. U. S. A. 115, 12148 (2018)], which demonstrated light amplification in a resonantly excited SiC insulator. We show that, beyond a critical pumping strength, such systems should exhibit Floquet parametric instability, which corresponds to resonant scattering of pump polaritons into pairs of finite momentum polaritons. We find that the parametric instability should be achievable in SiC using current experimental techniques and discuss its signatures, including the non-analytic frequency dependence of the reflection coefficient and the probe pulse afterglow. We discuss possible applications of the parametric instability phenomenon and suggest that similar types of instabilities can be present in other photoexcited non-linear systems.
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This content will become publicly available on March 1, 2026
Effective Polarizability in Near-Field Microscopy of Phonon-Polariton Resonances
We investigate the resonant characteristics of planar surfaces and distinct edges of structures with the excitation of phonon-polaritons. We analyze two materials supporting phonon-polariton excitations in the mid-infrared spectrum: silicon carbide, characterized by an almost isotropic dielectric constant, and hexagonal boron nitride, notable for its pronounced anisotropy in a spectral region exhibiting hyperbolic dispersion. We formulate a theoretical framework that accurately captures the excitations of the structure involving phonon-polaritons, predicts the response in scattering-type near-field optical microscopy, and is effective for complex resonant geometries where the locations of hot spots are uncertain. We account for the tapping motion of the probe, perform analysis for different heights of the probe, and demodulate the signal using a fast Fourier transform. Using this Fourier demodulation analysis, we show that light enhancement across the entire apex is the most accurate characteristic for describing the response of all resonant excitations and hot spots. We demonstrate that computing the demodulation orders of light enhancement in the microscope probe accurately predicts its imaging.
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- Award ID(s):
- 2418519
- PAR ID:
- 10577981
- Publisher / Repository:
- MDPI
- Date Published:
- Journal Name:
- Nanomaterials
- Volume:
- 15
- Issue:
- 6
- ISSN:
- 2079-4991
- Page Range / eLocation ID:
- 458
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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