An official website of the United States government
Abstract Electromagnetic hyperbolicity has driven key functionalities in nanophotonics, including super-resolution imaging, efficient energy control, and extreme light manipulation. Central to these advances are hyperbolic polaritons—nanometer-scale light-matter waves—spanning multiple energy-momentum dispersion orders with distinct mode profiles and incrementally high optical momenta. In this work, we report the mode conversion of hyperbolic polaritons across different dispersion orders by breaking the structure symmetry in engineered step-shape van der Waals (vdW) terraces. The mode conversion from the fundamental to high-order hyperbolic polaritons is imaged using scattering-type scanning near-field optical microscopy (s-SNOM) on both hexagonal boron nitride (hBN) and alpha-phase molybdenum trioxide (α-MoO3) vdW terraces. Our s-SNOM data, augmented with electromagnetics simulations, further demonstrate the alteration of polariton mode conversion by varying the step size of vdW terraces. The mode conversion reported here offers a practical approach toward integrating previously independent different-order hyperbolic polaritons with ultra-high momenta, paving the way for promising applications in nano-optical circuits, sensing, computation, information processing, and super-resolution imaging.
more »
« less
Tunable Phonon Polariton Hybridization in a Van der Waals Hetero‐Bicrystal
Abstract Phonon polaritons, the hybrid quasiparticles resulting from the coupling of photons and lattice vibrations, have gained significant attention in the field of layered van der Waals heterostructures. Particular interest has been paid to hetero‐bicrystals composed of molybdenum oxide (MoO3) and hexagonal boron nitride (hBN), which feature polariton dispersion tailorable via avoided polariton mode crossings. In this work, the polariton eigenmodes in MoO3‐hBN hetero‐bicrystals self‐assembled on ultrasmooth gold are systematically studied using synchrotron infrared nanospectroscopy. It is experimentally demonstrated that the spectral gap in bicrystal dispersion and corresponding regimes of negative refraction can be tuned by material layer thickness, and these results are quantitatively matched with a simple analytic model. Polaritonic cavity modes and polariton propagation along “forbidden” directions are also investigated in microscale bicrystals, which arise from the finite in‐plane dimension of the synthesized MoO3micro‐ribbons. The findings shed light on the unique dispersion properties of polaritons in van der Waals heterostructures and pave the way for applications leveraging deeply sub‐wavelength mid‐infrared light‐matter interactions.
more »
« less
- Award ID(s):
- 1608525
- PAR ID:
- 10516525
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 36
- Issue:
- 33
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract One of the main bottlenecks in the development of terahertz (THz) and long-wave infrared (LWIR) technologies is the limited intrinsic response of traditional materials. Hyperbolic phonon polaritons (HPhPs) of van der Waals semiconductors couple strongly with THz and LWIR radiation. However, the mismatch of photon − polariton momentum makes far-field excitation of HPhPs challenging. Here, we propose an In-Plane Hyperbolic Polariton Tuner that is based on patterning van der Waals semiconductors, here α-MoO3, into ribbon arrays. We demonstrate that such tuners respond directly to far-field excitation and give rise to LWIR and THz resonances with high quality factors up to 300, which are strongly dependent on in-plane hyperbolic polariton of the patterned α-MoO3. We further show that with this tuner, intensity regulation of reflected and transmitted electromagnetic waves, as well as their wavelength and polarization selection can be achieved. Our results can help the development of THz and LWIR miniaturized devices.more » « less
-
Abstract Polar van der Waals (vdW) crystals that support phonon polaritons have recently attracted much attention because they can confine infrared and terahertz (THz) light to deeply subwavelength dimensions, allowing for the guiding and manipulation of light at the nanoscale. The practical applications of these crystals in devices rely strongly on deterministic engineering of their spatially localized electromagnetic field distributions, which has remained challenging. The polariton interference can be enhanced and tailored by patterning the vdW crystalα‐MoO3into microstructures that support highly in‐plane anisotropic phonon polaritons. The orientation of the polaritonic in‐plane isofrequency curve relative to the microstructure edges is a critical parameter governing the polariton interference, rendering the configuration of infrared electromagnetic field localizations by enabling the tuning of the microstructure size and shape and the excitation frequency. Thus, the study presents an effective rationale for engineering infrared light flow in planar photonic devices.more » « less
-
Abstract The biaxial van der Waals semiconductor α‐phase molybdenum trioxide (α‐MoO3) has recently received significant attention due to its ability to support highly anisotropic phonon polaritons (PhPs)—infrared (IR) light coupled to lattice vibrations—offering an unprecedented platform for controlling the flow of energy at the nanoscale. However, to fully exploit the extraordinary IR response of this material, an accurate dielectric function is required. Here, the accurate IR dielectric function of α‐MoO3is reported by modeling far‐field polarized IR reflectance spectra acquired on a single thick flake of this material. Unique to this work, the far‐field model is refined by contrasting the experimental dispersion and damping of PhPs, revealed by polariton interferometry using scattering‐type scanning near‐field optical microscopy (s‐SNOM) on thin flakes of α‐MoO3, with analytical and transfer‐matrix calculations, as well as full‐wave simulations. Through these correlative efforts, exceptional quantitative agreement is attained to both far‐ and near‐field properties for multiple flakes, thus providing strong verification of the accuracy of this model, while offering a novel approach to extracting dielectric functions of nanomaterials. In addition, by employing density functional theory (DFT), insights into the various vibrational states dictating the dielectric function model and the intriguing optical properties of α‐MoO3are provided.more » « less
-
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.more » « less
