Phonon polaritons enable waveguiding and localization of infrared light with extreme confinement and low losses. The spatial propagation and spectral resonances of such polaritons are usually probed with complementary techniques such as near-field optical microscopy and far-field reflection spectroscopy. Here, infrared-visible sum-frequency spectro-microscopy is introduced as a tool for spectroscopic imaging of phonon polaritons. The technique simultaneously provides sub-wavelength spatial resolution and highly-resolved spectral resonance information. This is implemented by resonantly exciting polaritons using a tunable infrared laser and wide-field microscopic detection of the upconverted light. The technique is employed to image hybridization and strong coupling of localized and propagating surface phonon polaritons in a metasurface of SiC micropillars. Spectro-microscopy allows to measure the polariton dispersion simultaneously in momentum space by angle-dependent resonance imaging, and in real space by polariton interferometry. Notably, it is possible to directly image how strong coupling affects the spatial localization of polaritons, inaccessible with conventional spectroscopic techniques. The formation of edge states is observed at excitation frequencies where strong coupling prevents polariton propagation into the metasurface. The technique is applicable to the wide range of polaritonic materials with broken inversion symmetry and can be used as a fast and non-perturbative tool to image polariton hybridization and propagation.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1002/adma.202312507 | DOI Listing |
Nano Lett
January 2025
Department of Physics, University of Oviedo, Oviedo 33006, Spain.
Polaritons are central to the development of nanophotonics, as they provide mechanisms for manipulating light at the nanoscale. A key advancement has been the demonstration of polariton canalization in which the energy flow is directed along a single direction. An intriguing case is the canalization of ray polaritons, characterized by an enhanced density of optical states.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Department of Chemistry, Columbia University, New York, New York 10027, USA.
In this work, we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of light-matter interactions, where spatially localized cavity radiation modes couple to localized vibrations. Within this theoretical framework, we employ self-consistent phonon theory and vibrational dynamical mean-field theory to efficiently simulate momentum-resolved vibrational-polariton spectra, including effects of anharmonicity.
View Article and Find Full Text PDFACS Nano
December 2024
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.
Ultrafast thermal switches are pivotal for managing heat generated in advanced solid-state applications, including high-speed chiplets, thermo-optical modulators, and on-chip lasers. However, conventional phonon-based switches cannot meet the demand for picosecond-level response times, and existing near-field radiative thermal switches face challenges in efficiently modulating heat transfer across vacuum gaps. To overcome these limitations, we propose an ultrafast thermal switch design based on pump-driven transient polaritons in asymmetric terminals.
View Article and Find Full Text PDFACS Photonics
December 2024
SUPA, School of Physics and Astronomy, University of St Andrews, St Andrews KY16 9SS, U.K.
We derive the transition rates, dephasing rates, and Lamb shifts for a system consisting of many molecules collectively coupled to a resonant cavity mode. Using a variational polaron master equation, we show that strong vibrational interactions inherent to molecules give rise to multi-phonon processes and suppress the light-matter coupling. In the strong light-matter coupling limit, multiphonon contributions to the transition and dephasing rates strongly dominate over single-phonon contributions for typical molecular parameters.
View Article and Find Full Text PDFNanophotonics
June 2024
Vienna Center for Quantum Science and Technology (VCQ), Faculty of Physics, University of Vienna, Boltzmanngasse 5, 1090 Vienna, Austria.
Polariton thermalization is a key process in achieving light-matter Bose-Einstein condensation, spanning from solid-state semiconductor microcavities at cryogenic temperatures to surface plasmon nanocavities with molecules at room temperature. Originated from the matter component of polariton states, the microscopic mechanisms of thermalization are closely tied to specific material properties. In this work, we investigate polariton thermalization in strongly-coupled molecular systems.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!