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Phonons are important lattice vibrations that affect the thermal, electronic, and optical properties of materials. In this work, we studied infrared phonon resonance in a prototype van der Waals (vdW) material—hexagonal boron nitride (hBN)—with the thickness ranging from monolayers to bulk, especially on ultra-thin crystals with atomic layers smaller than 20. Our combined experimental and modeling results show a systematic increase in the intensity of in-plane phonon resonance at the increasing number of layers in hBN, with a sensitivity down to one atomic layer. While the thickness-dependence of the phonon resonance reveals the antenna nature of our nanoscope, the linear thickness-scaling of the phonon polariton wavelength indicates the preservation of electromagnetic hyperbolicity in ultra-thin hBN layers. Our conclusions should be generic for fundamental resonances in vdW materials and heterostructures where the number of constituent layers can be conveniently controlled. The thickness-dependent phonon resonance and phonon polaritons revealed in our work also suggest vdW engineering opportunities for desired thermal and nanophotonic functionalities. 

Polaritons enable subwavelength confinement and highly anisotropic flows of light over a wide spectral range, holding the promise for applications in modern nanophotonic and optoelectronic devices. However, to fully realize their practical application potential, facile methods enabling nanoscale active control of polaritons are needed. Here, we introduce a hybrid polaritonic-oxide heterostructure platform consisting of van der Waals crystals, such as hexagonal boron nitride (hBN) or alpha-phase molybdenum trioxide (α-MoO₃), transferred on nanoscale oxygen vacancy patterns on the surface of prototypical correlated perovskite oxide, samarium nickel oxide, SmNiO₃(SNO). Using a combination of scanning probe microscopy and infrared nanoimaging techniques, we demonstrate nanoscale reconfigurability of complex hyperbolic phonon polaritons patterned at the nanoscale with high resolution. Hydrogenation and temperature modulation allow spatially localized conductivity modulation of SNO nanoscale patterns, enabling robust real-time modulation and nanoscale reconfiguration of hyperbolic polaritons. Our work paves the way towards nanoscale programmable metasurface engineering for reconfigurable nanophotonic applications.

 

Hexagonal boron nitride (h-BN) has been predicted to exhibit an in-plane thermal conductivity as high as ~ 550 W m⁻¹K⁻¹at room temperature, making it a promising thermal management material. However, current experimental results (220–420 W m⁻¹K⁻¹) have been well below the prediction. Here, we report on the modulation of h-BN thermal conductivity by controlling the B isotope concentration. For monoisotopic¹⁰B h-BN, an in-plane thermal conductivity as high as 585 W m⁻¹K⁻¹is measured at room temperature, ~ 80% higher than that of h-BN with a disordered isotope concentration (52%:48% mixture of¹⁰B and¹¹B). The temperature-dependent thermal conductivities of monoisotopic h-BN agree well with first principles calculations including only intrinsic phonon-phonon scattering. Our results illustrate the potential to achieve high thermal conductivity in h-BN and control its thermal conductivity, opening avenues for the wide application of h-BN as a next-generation thin-film material for thermal management, metamaterials and metadevices.

 

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.

 

Probing of polaritons in 2D materials is facilitated by spectroscopic imaging with nanometer spatial resolution. The combination of atomic force microscopy and infrared laser sources provides access for in situ mappings of phonon polaritons. Here, it is demonstrated that the photothermal‐based peak force infrared microscopy is capable of revealing phonon polaritons with high spatial resolution in isotopically pure hexagonal boron nitride microstructures without damaging the sample. To further improve the sensitivity, peak force infrared microscopy is enhanced with a scheme of multiple laser pulse excitation. The resulting method of multipulse peak force infrared microscopy can detect phonon polaritons with high sensitivity, which is particularly useful for probing polaritons in 2D materials with high damping characteristics.

 

Coherent optical excitations in two-dimensional (2D) materials, 2D polaritons, can generate a plethora of optical phenomena that arise from the extraordinary dispersion relations that do not exist in regular materials. Probing of the dynamical phenomena of 2D polaritons requires simultaneous spatial and temporal imaging capabilities and could reveal unknown coherent optical phenomena in 2D materials. Here, we present a spatiotemporal measurement of 2D wave packet dynamics, from its formation to its decay, using an ultrafast transmission electron microscope driven by femtosecond midinfrared pulses. The ability to coherently excite phonon-polariton wave packets and probe their evolution in a nondestructive manner reveals intriguing dispersion-dependent dynamics that includes splitting of multibranch wave packets and, unexpectedly, wave packet deceleration and acceleration. Having access to the full spatiotemporal dynamics of 2D wave packets can be used to illuminate puzzles in topological polaritons and discover exotic nonlinear optical phenomena in 2D materials.