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Infrared permittivity of the biaxial van der Waals semiconductor $alpha$-MoO$_3$ from near- and far-field correlative studies

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 Publication date 2019
  fields Physics
and research's language is English




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The biaxial van der Waals semiconductor $alpha$-phase molybdenum trioxide ($alpha$-MoO$_3$) has recently received significant attention due to its ability to support highly anisotropic phonon polaritons (PhPs) -infrared (IR) light coupled to lattice vibrations in polar materials-, 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, we report the accurate IR dielectric function of $alpha$-MoO$_3$ by modelling far-field, polarized IR reflectance spectra acquired on a single thick flake of this material. Unique to our 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 $alpha$-MoO$_3$, 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 our model, while offering a novel approach to extracting dielectric functions of nanomaterials, usually too small or inhomogeneous for establishing accurate models only from standard far-field methods. In addition, by employing density functional theory (DFT), we provide insights into the various vibrational states dictating our dielectric function model and the intriguing optical properties of $alpha$-MoO$_3$.



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Recently, in-plane biaxial hyperbolicity has been observed in $alpha$-MoO${_3}$ --a van der Waal crystal-- in the mid-infrared frequency regime. Here, we present a comprehensive theoretical analysis of thin film $alpha$-MoO${_3}$ for application to two mid-IR photonic devices -- a polarizer and a waveplate. We show the possibility of a significant reduction in the device footprint while maintaining an enormous extinction ratio from $alpha$-MoO${_3}$ based polarizers in comparison with that of conventional polarizers. Secondly, we carry out device optimization of $alpha$-MoO${_3}$ based waveplates with subwavelength thickness. We explain our results using natural in-plane hyperbolicity of $alpha$-MoO${_3}$ via analytical and full wave simulations. This work will build a foundation for miniaturization of mid-infrared photonic devices by exploiting the optical anisotropy of $alpha$-MoO${_3}$.
Hyperbolic media have attracted much attention in the photonics community, thanks to their ability to confine light to arbitrarily small volumes and to their use for super-resolution applications. The 2D counterpart of these media can be achieved with hyperbolic metasurfaces, which support in-plane hyperbolic guided modes thanks to nanopatterns which, however, pose significant fabrication challenges and limit the achievable confinement. We show that thin flakes of the van der Waals material {alpha}-MoO3 can support naturally in-plane hyperbolic polariton guided modes at mid-infrared frequencies without any patterning. This is possible because {alpha}-MoO3 is a biaxial hyperbolic crystal, with three different Restrahlen bands, each for a different crystal axis. Our findings can pave the way towards new paradigm to manipulate and confine light in planar photonic devices.
Light-emitting diodes (LEDs) based on III-V/II-VI materials have delivered a compelling performance in the mid-infrared (mid-IR) region, which enabled wide-ranging applications, including environmental monitoring, defense and medical diagnostics. Continued efforts are underway to realize on-chip sensors via heterogeneous integration of mid-IR emitters on a silicon photonic chip. But the uptake of such approach is limited by the high costs and interfacial strains, associated with the process of heterogeneous integrations. Here, the black phosphorus (BP)-based van der Waals (vdW) heterostructures are exploited as room temperature LEDs. The demonstrated devices can emit linearly polarized light, and their spectra cover the technologically important mid-IR atmospheric window (3-4 um). Additionally, the BP LEDs exhibit fast modulation speed as well as exceptional stability, and its peak extrinsic quantum efficiency (QE~0.9%) is comparable to the III-V/II-VI mid-IR LEDs. By leveraging the integrability of vdW heterostructures, we further demonstrate a silicon photonic waveguide-integrated BP LED. The reported hybrid platform holds great promise for mid-IR silicon photonics.
Van der Waals (vdW) semiconductors are attractive for highly scaled devices and heterogeneous integration since they can be isolated into self-passivated, two-dimensional (2D) layers that enable superior electrostatic control. These attributes have led to numerous demonstrations of field-effect devices ranging from transistors to triodes. By exploiting the controlled, substitutional doping schemes in covalently-bonded, three-dimensional (3D) semiconductors and the passivated surfaces of 2D semiconductors, one can construct devices that can exceed performance metrics of all-2D vdW heterojunctions. Here, we demonstrate, 2D/3D semiconductor heterojunctions using MoS2 as the prototypical 2D semiconductor laid upon Si and GaN as the 3D semiconductor layers. By tuning the Fermi levels in MoS2, we demonstrate devices that concurrently exhibit over seven orders of magnitude modulation in rectification ratios and conductance. Our results further suggest that the interface quality does not necessarily affect Fermi-level tuning at the junction opening up possibilities for novel 2D/3D heterojunction device architectures.
Two-dimensional van der Waals (vdW) crystals can sustain various types of polaritons with strong electromagnetic confinements, making them highly attractive for the nanoscale photonic and optoelectronic applications. While extensive experimental and numerical studies are devoted to the polaritons of the vdW crystals, analytical models are sparse. Particularly, applying such a model to describe the polariton behaviors visualized by state-of-art near-field optical microscopy requires further investigation. Herein, we develop an analytical waveguide model to describe the polariton propagations in vdW crystals. The dispersion contours, dispersion relations, and electromagnetic field distributions of different polariton waveguide modes are derived. The model is verified by near-field optical imaging and numerical simulation of phonon polaritons in the {alpha}-MoO3, a typical vdW biaxial crystals. The model can be extended to other types of polaritons in vdW crystals, thus allowing for describing and understanding their localized electromagnetic behaviors analytically.
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