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

Abstract

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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• Layer-Resolved Resonance Intensity of Evanescent Polariton Modes in Anisotropic Multilayers
• Canalization acoustic phonon polaritons in metal-MoO3-metal sandwiched structures for nano-light guiding and manipulation
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• Misalignment between the Directions of Propagation and Decay of Nanoscale-confined Polaritons
• Retrieving optical parameters of emerging van der Waals flakes
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• Rapid synthesis of dual-element isotope-enriched alpha-MoO3 crystals by reactive vapor transport
• Long-range mid-infrared energy transfer mediated by hyperbolic phonon polaritons
• Bloch phonon-polaritons with anomalous dispersion in polaritonic Fourier crystals
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