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Award ID contains: 2033454

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  1. Abstract Polaritons—confined light–matter waves—in van der Waals (vdW) materials are a research frontier in light–matter interactions with demonstrated advances in nanophotonics. Reflection, as a fundamental phenomenon involving waves, is particularly important for vdW polaritons, predominantly because it enables the investigation of polariton standing waves using the scanning probe technique. While previous works demonstrate a rigid phase ≈π/4 for the polariton reflection, herein is reported the altering of the polariton reflection phase by varying the geometry of polaritonic microstructures for the case study of hyperbolic surface polaritons (HSPs) in hexagonal boron nitride (hBN). Specifically, it is demonstrated that the polariton reflection phase can be systematically altered by varying the corner angle of the hBN microstructures, and that it experiences a π jump around a specific angle. This behavior, which is a consequence of the mathematical nature of the reflection coefficient, is therefore expected in other physical phenomena. 
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  2. The mid‐infrared with a characteristic wavelength of 3–20 μm is important for a wealth of technologies. In particular, mid‐infrared spectroscopy can reveal material composition and structure information by fingerprinting chemical bonds’ infrared resonances. Despite these merits, state‐of‐the‐art mid‐infrared techniques are spatially limited above tens of micrometers due to the fundamental diffraction law. Herein, recent progress in the scanning probe nanoscale infrared characterization of biochemical materials and natural specimens beyond this spatial limitation is reviewed. By leveraging the strong tip–sample local interactions, scanning probe nano‐infrared methods probe nanoscale optical and mechanical responses to disclose material composition, heterogeneity, orientation, fine structure, and phase transitions at unprecedented length scales. These advances, therefore, revolutionize the understanding of a broad range of biochemical and natural materials and offer new material manipulation and engineering opportunities close to the ultimate length scales of fundamental physical, chemical, and biological processes. 
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    Free, publicly-accessible full text available November 1, 2025
  3. Polar van der Waals (vdW) crystals, composed of atomic layers held together by vdW forces, can host phonon polaritons—quasiparticles arising from the interaction between photons in free-space light and lattice vibrations in polar materials. These crystals offer advantages such as easy fabrication, low Ohmic loss, and optical confinement. Recently, hexagonal boron nitride (hBN), known for having hyperbolicity in the mid-infrared range, has been used to explore multiple modes with high optical confinement. This opens possibilities for practical polaritonic nanodevices with subdiffractional resolution. However, polariton waves still face exposure to the surrounding environment, leading to significant energy losses. In this work, we propose a simple approach to inducing a hyperbolic phonon polariton (HPhP) waveguide in hBN by incorporating a low dielectric medium, ZrS2. The low dielectric medium serves a dual purpose—it acts as a pathway for polariton propagation, while inducing high optical confinement. We establish the criteria for the HPhP waveguide in vdW heterostructures with various thicknesses of ZrS2 through scattering-type scanning near-field optical microscopy (s-SNOM) and by conducting numerical electromagnetic simulations. Our work presents a feasible and straightforward method for developing practical nanophotonic devices with low optical loss and high confinement, with potential applications such as energy transfer, nano-optical integrated circuits, light trapping, etc. 
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  4. Charge transfer is a fundamental interface process that can be harnessed for light detection, photovoltaics, and photosynthesis. Recently, charge transfer was exploited in nanophotonics to alter plasmon polaritons by involving additional non-polaritonic materials to activate the charge transfer. Yet, direct charge transfer between polaritonic materials has not been demonstrated. We report the direct charge transfer in pure polaritonic van der Waals (vdW) heterostructures of α-MoO3/graphene. We extracted the Fermi energy of 0.6 eV for graphene by infrared nano-imaging of charge transfer hyperbolic polaritons in the vdW heterostructure. This unusually high Fermi energy is attributed to the charge transfer between graphene and α-MoO3. Moreover, we have observed charge transfer hyperbolic polaritons in multiple energy–momentum dispersion branches with a wavelength elongation of up to 150%. With the support from the density functional theory calculation, we find that the charge transfer between graphene and α-MoO3, absent in mechanically assembled vdW heterostructures, is attributed to the relatively pristine heterointerface preserved in the epitaxially grown vdW heterostructure. The direct charge transfer and charge transfer hyperbolic polaritons demonstrated in our work hold great promise for developing nano-optical circuits, computational devices, communication systems, and light and energy manipulation devices. 
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  5. Sample suspension is a valuable method to improve the mechanical, thermal, electronic, and optical properties of low-dimensional materials. In terms of confined light-matter waves—the polaritons, sample suspension can elongate the wavelength of polaritons with a positive phase velocity. Previous work demonstrates a wavelength elongation of ∼10% for hyperbolic phonon polaritons (HPPs) in uniaxial crystals of hexagonal boron nitride (hBN). In this work, we report the alteration of HPPs in biaxial α-phase molybdenum trioxide (α-MoO3) by sample suspension. Our combined infrared nano-imaging experiments and electromagnetic theory reveal a wavelength elongation > 60% and a propagation length increase > 140%, due to the simultaneous wavelength elongation and dissipation elimination in the suspended specimen. We have also examined HPPs in α-MoO3with a negative phase velocity. The sample suspension shortens the HPP wavelength and simultaneously reduces the dissipation due to the unique permittivity tensor. The HPPs with improved figures of merits in the suspended specimen may be developed for nano-polaritonic circuits, biochemical sensing, emission engineering, and energy transfer. 
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