A polariton is a fundamental quasiparticle that arises from strong light-matter interaction and as such has attracted wide scientific and practical interest. When light is strongly coupled to the crystal lattice, it gives rise to phonon-polaritons (PPs), which have been proven useful in the dynamical manipulation of quantum materials and the advancement of terahertz technologies. Yet, current detection and characterization methods of polaritons are still limited. Traditional techniques such as Raman or transient grating either rely on fine-tuning of external parameters or complex phase extraction techniques. To overcome these inherent limitations, we propose and demonstrate a technique based on a time-of-flight measurement of PPs. We resonantly launch broadband PPs with intense terahertz fields and measure the time-of-flight of each spectral component with time-resolved second harmonic generation. The time-of-flight information, combined with the PP attenuation, enables us to resolve the real and imaginary parts of the PP dispersion relation. We demonstrate this technique in the van der Waals magnets NiI and MnPS and reveal a hidden magnon-phonon interaction. We believe that this approach will unlock new opportunities for studying polaritons across diverse material systems and enhance our understanding of strong light-matter interaction.
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http://dx.doi.org/10.1038/s41467-024-46515-1 | DOI Listing |
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January 2025
CNR NANOTEC Institute of Nanotechnology, Via Monteroni, 73100, Lecce, Italy.
Photonics bound states in the continuum (BICs) are peculiar localized states in the continuum of free-space waves, unaffected by far-field radiation loss. Although plasmonic nano-antennas squeeze the optical field to nanoscale volumes, engineering the emergence of quasi-BICs with plasmonic hotspots remains challenging. Here, the origin of symmetry-protected (SP) quasi-BICs in a 2D system of silver-filled dimers, quasi-embedded in a high-index dielectric waveguide, is investigated through the strong coupling between photonic and plasmonic modes.
View Article and Find Full Text PDFNanophotonics
January 2025
Institute of Physics, Swiss Federal Institute of Technology Lausanne (EPFL), CH-1015 Lausanne, Switzerland.
Sum-frequency generation (SFG) enables the coherent upconversion of electromagnetic signals and plays a significant role in mid-infrared vibrational spectroscopy for molecular analysis. Recent research indicates that plasmonic nanocavities, which confine light to extremely small volumes, can facilitate the detection of vibrational SFG signals from individual molecules by leveraging surface-enhanced Raman scattering combined with mid-infrared laser excitation. In this article, we compute the degree of second order coherence ( (0)) of the upconverted mid-infrared field under realistic parameters and accounting for the anharmonic potential that characterizes vibrational modes of individual molecules.
View Article and Find Full Text PDFNanoscale
January 2025
State Key Laboratory of Electrical Insulation and Power Equipment, Xi'an Jiaotong University, Xi'an, 710049, China.
Two-dimensional (2D) organic-inorganic halide perovskites are promising sensitive materials for optoelectronic applications due to their strong light-matter interactions, layered structure, long carrier lifetime and diffusion length. However, a high gate bias is indispensable for perovskite-based phototransistors to optimize detection performances, since ion migration seriously screens the gate electric field and the deposition process introduces intrinsic defects, which induces severe leakages and large power dissipation. In this work, an ultrasensitive phototransistor based on the (PEA)SnI perovskite and the Al:HfO ferroelectric layer is meticulously studied, working without an external gate voltage.
View Article and Find Full Text PDFNat Chem
January 2025
Department of Chemistry, University of California Irvine, Irvine, CA, USA.
Controlling reaction outcomes through external influences is a central goal in chemistry. Vibrational coupling between molecular vibrations and cavity modes is rapidly emerging as a distinct strategy compared with conventional thermochemical and photochemical methods; however, insight into the fundamental mechanisms remains limited. Here we investigate how vibrational weak and strong coupling in plasmonic nanocavities modifies the thermal dehydration of copper sulfate pentahydrate.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan.
The quantum-electrodynamic non-adiabatic emission (QED-NAE) is a type of radiatively assisted vibronic de-excitation due to electromagnetic vacuum fluctuations on non-adiabatic processes. Building on our previous work [Tsai et al., J.
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