We demonstrate the generation of a spatiotemporal optical continuum in a highly nonlinear exciton-polariton waveguide using extremely low excitation powers (2-ps, 100-W peak power pulses) and a submillimeter device suitable for integrated optics applications. We observe contributions from several mechanisms over a range of powers and demonstrate that the strong light-matter coupling significantly modifies the physics involved in all of them. The experimental data are well understood in combination with theoretical modeling. The results are applicable to a wide range of systems with linear coupling between nonlinear oscillators and particularly to emerging polariton devices that incorporate materials, such as gallium nitride and transition metal dichalcogenide monolayers that exhibit large light-matter coupling at room temperature. These open the door to low-power experimental studies of spatiotemporal nonlinear optics in submillimeter waveguide devices.
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http://dx.doi.org/10.1038/s41377-019-0120-7 | DOI Listing |
Nano Lett
January 2025
State Key Laboratory for Mesoscopic Physics and Frontiers Science Center for Nano-optoelectronics, School of Physics, Peking University, 100871 Beijing, China.
Nano Lett
January 2025
Key Laboratory of Light Field Manipulation and Information Acquisition, Ministry of Industry and Information Technology, School of Physical Science and Technology, Northwestern Polytechnical University, Xi'an 710129, China.
Tip-enhanced Raman spectroscopy (TERS) has been extensively employed to investigate the light-matter interaction at the nanoscale. However, the current TERS strategies lack the ability to excite the low-background inhomogeneous electromagnetic field with significant enhancement of electric field, electric field gradient, and optomagnetic field, simultaneously. To overcome this, we developed a fiber vector light-field-based TERS strategy aimed at exploring the multipole Raman scattering processes of molecules.
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 PDFJ Phys Chem Lett
December 2024
Department of Chemistry and Department of Physics, Westlake University, Hangzhou, Zhejiang 310030, China.
Collective strong light-matter coupling provides a versatile means to manipulate physicochemical properties of molecules and materials. Understanding collective polaritonic dynamics is hindered by the macroscopic number of molecules interacting collectively with photonic modes. We develop a many-body theory to investigate the spectroscopy and dynamics of a molecular ensemble embedded in an optical cavity in the collective strong coupling regime.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Department of Physics, Stockholm University, AlbaNova University Center, SE-10691 Stockholm, Sweden.
Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. Experiments have demonstrated that vibrational strong coupling can change molecular properties and even affect chemical reactivity. However, the interactions in a molecular ensemble are complex, and the exact mechanisms that lead to modifications are not fully understood yet.
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