Large optical anisotropy observed in a broad spectral range is of paramount importance for efficient light manipulation in countless devices. Although a giant anisotropy has been recently observed in the mid-infrared wavelength range, for visible and near-infrared spectral intervals, the problem remains acute with the highest reported birefringence values of 0.8 in BaTiS₃ and h-BN crystals. This issue inspired an intensive search for giant optical anisotropy among natural and artificial materials. Here, we demonstrate that layered transition metal dichalcogenides (TMDCs) provide an answer to this quest owing to their fundamental differences between intralayer strong covalent bonding and weak interlayer van der Waals interaction. To do this, we made correlative far- and near-field characterizations validated by first-principle calculations that reveal a huge birefringence of 1.5 in the infrared and 3 in the visible light for MoS₂. Our findings demonstrate that this remarkable anisotropy allows for tackling the diffraction limit enabling an avenue for on-chip next-generation photonics.

Layered semiconductors such as transition metal dichalcogenides (TMDs) offer endless possibilities for designing modern photonic and optoelectronic components. However, their optical engineering is still a challenging task owing to multiple obstacles, including the absence of a rapid, contactless, and the reliable method to obtain their dielectric function as well as to evaluate in situ the changes in optical constants and exciton binding energies. Here, we present an advanced approach based on ellipsometry measurements for retrieval of dielectric functions and the excitonic properties of both monolayer and bulk TMDs. Using this method, we conduct a detailed study of monolayer MoS₂ and its bulk crystal in the broad spectral range (290–3300 nm). In the near- and mid-infrared ranges, both configurations appear to have no optical absorption and possess an extremely high dielectric permittivity making them favorable for lossless subwavelength photonics. In addition, the proposed approach opens a possibility to observe a previously unreported peak in the dielectric function of monolayer MoS₂ induced by the use of perylene-3,4,9,10-tetracarboxylic acid tetrapotassium salt (PTAS) seeding promoters for MoS₂ synthesis and thus enables its applications in chemical and biological sensing. Therefore, this technique as a whole offers a state-of-the-art metrological tool for next-generation TMD-based devices.

Atomically thin transition metal dichalcogenides (TMDCs) present a promising platform for numerous photonic applications due to excitonic spectral features, possibility to tune their constants by external gating, doping, or light, and mechanical stability. Utilization of such materials for sensing or optical modulation purposes would require a clever optical design, as by itself the 2D materials can offer only a small optical phase delay – consequence of the atomic thickness. To address this issue, we combine films of 2D semiconductors which exhibit excitonic lines with the Fabry-Perot resonators of the standard commercial SiO₂/Si substrate, in order to realize topological phase singularities in reflection. Around these singularities, reflection spectra demonstrate rapid phase changes while the structure behaves as a perfect absorber. Furthermore, we demonstrate that such topological phase singularities are ubiquitous for the entire class of atomically thin TMDCs and other high-refractive-index materials, making it a powerful tool for phase engineering in flat optics. As a practical demonstration, we employ PdSe₂ topological phase singularities for a refractive index sensor and demonstrate its superior phase sensitivity compared to typical surface plasmon resonance sensors.

Optical constants of monolayers MoS2 and WS2 were measured by spectroscopic ellipsometry in the spectral range 365–1700 nm. Analysis of ellipsometry spectra was carried out, taking into account the excitonic nature of dispersion. In the considered wavelength range, excitons originate from different interband transitions. As a result, they can be described via Tauc–Lorentz oscillators, one for each exciton. The scalability and universality of such an approach could be applied for the extended wavelength range and to the other transition metal dichalcogenides.