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.
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.
more » « less- PAR ID:
- 10363949
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- Applied Physics Letters
- Volume:
- 120
- Issue:
- 11
- ISSN:
- 0003-6951
- Page Range / eLocation ID:
- Article No. 113101
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract In recent years, the excitation of surface phonon polaritons (SPhPs) in van der Waals materials received wide attention from the nanophotonics community. Alpha-phase Molybdenum trioxide (
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Abstract Hyperbolic phonon polaritons (HPhPs) are stimulated by coupling infrared (IR) photons with the polar lattice vibrations. Such HPhPs offer low‐loss, highly confined light propagation at subwavelength scales with out‐of‐plane or in‐plane hyperbolic wavefronts. For HPhPs, while a hyperbolic dispersion implies multiple propagating modes with a distribution of wavevectors at a given frequency, so far it has been challenging to experimentally launch and probe the higher‐order modes that offer stronger wavelength compression, especially for in‐plane HPhPs. In this work, the experimental observation of higher‐order in‐plane HPhP modes stimulated on a 3C‐SiC nanowire (NW)/α‐MoO3heterostructure is reported where leveraging both the low‐dimensionality and low‐loss nature of the polar NWs, higher‐order HPhPs modes within 2D α‐MoO3crystal are launched by the 1D 3C‐SiC NW. The launching mechanism is further studied and the requirements for efficiently launching of such higher‐order modes are determined. In addition, by altering the geometric orientation between the 3C‐SiC NW and α‐MoO3crystal, the manipulation of higher‐order HPhP dispersions as a method of tuning is demonstrated. This work illustrates an extremely anisotropic low dimensional heterostructure platform to confine and configure electromagnetic waves at the deep‐subwavelength scales for a range of IR applications including sensing, nano‐imaging, and on‐chip photonics.
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Abstract Polaritons in hyperbolic van der Waals materials—where principal axes have permittivities of opposite signs—are light-matter modes with unique properties and promising applications. Isofrequency contours of hyperbolic polaritons may undergo topological transitions from open hyperbolas to closed ellipse-like curves, prompting an abrupt change in physical properties. Electronically-tunable topological transitions are especially desirable for future integrated technologies but have yet to be demonstrated. In this work, we present a doping-induced topological transition effected by plasmon-phonon hybridization in graphene/α-MoO3heterostructures. Scanning near-field optical microscopy was used to image hybrid polaritons in graphene/α-MoO3. We demonstrate the topological transition and characterize hybrid modes, which can be tuned from surface waves to bulk waveguide modes, traversing an exceptional point arising from the anisotropic plasmon-phonon coupling. Graphene/α-MoO3heterostructures offer the possibility to explore dynamical topological transitions and directional coupling that could inspire new nanophotonic and quantum devices.
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Abstract Exploiting polaritons in natural vdW materials has been successful in achieving extreme light confinement and low-loss optical devices and enabling simplified device integration. Recently, α-MoO3has been reported as a semiconducting biaxial vdW material capable of sustaining naturally orthogonal in-plane phonon polariton modes in IR. In this study, we investigate the polarization-dependent optical characteristics of cavities formed using α-MoO3to extend the degrees of freedom in the design of IR photonic components exploiting the in-plane anisotropy of this material. Polarization-dependent absorption over 80% in a multilayer Fabry-Perot structure with α-MoO3is reported without the need for nanoscale fabrication on the α-MoO3. We observe coupling between the α-MoO3optical phonons and the Fabry-Perot cavity resonances. Using cross-polarized reflectance spectroscopy we show that the strong birefringence results in 15% of the total power converted into the orthogonal polarization with respect to incident wave. These findings can open new avenues in the quest for polarization filters and low-loss, integrated planar IR photonics and in dictating polarization control.
