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 MoS 2 and its bulk crystal in the broad spectral range (290-3300 nm). In the near-and midinfrared 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 MoS 2 induced by the use of perylene-3,4,9,10-tetracarboxylic acid tetrapotassium salt (PTAS) seeding promoters for MoS 2 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.

Controlled and reliable field enhancement (FE) effects associated with the excitation of plasmons in resonant metal nanostructures constitute an essential prerequisite for the development of various sensing configurations, especially those utilizing surface-enhanced Raman scattering (SERS) spectroscopy techniques. Leveraging advantages of random nanostructures in providing strong collective resonances in a broad wavelength range with the design flexibility of individual gap plasmon resonators, we experimentally investigate fractal-shaped arrays of gap plasmon resonators and characterize the occurring FE effects by mapping SERS signals from uniformly spread Rhodamine 6G with high-resolution Raman microscopy. In such a geometry, the total FE is expected to benefit from both FE associated with gap plasmon excitation and FE due to constructive interference of the surface plasmon modes reflected and diffracted by fractal-shaped boundaries. Linear reflection imaging spectroscopy is used to verify that the fabricated nanostructures exhibit spatially distributed resonances (bright spots) close to the excitation wavelengths used for the Raman microscopy. The positions of bright spots are argued to be influenced by fractal-shaped boundaries, particle dimensions, polarization, and wavelength of the incident and scattered light. Experimentally obtained SERS images from similar fractal (gold) structures fabricated with different dielectric SiO 2 spacer thicknesses (0, 20, and 40 nm) featured diffraction-limited bright spots corresponding to local SERS enhancements of up to ∼10 7 (relative to Raman signals obtained with a glass substrate) for 40 nm thick SiO 2 layers. Our results indicate that the strategy of combining fractal array geometry with gap plasmon resonances is promising for the design of highly efficient SERS substrates for potential applications in surface-enhanced multichannel sensing, including single-molecule spectroscopy.

Graphene is a promising platform for surface-enhanced Raman spectroscopy (SERS)-active substrates, primarily due to the possibility of quenching photoluminescence and fluorescence. Here we study ultrathin gold films near the percolation threshold fabricated by electron-beam deposition on monolayer CVD graphene. The advantages of such hybrid graphene/gold substrates for surface-enhanced Raman spectroscopy are discussed in comparison with conventional substrates without the graphene layer. The percolation threshold is determined by independent measurements of the sheet resistance and effective dielectric constant by spectroscopic ellipsometry. The surface morphology of the ultrathin gold films is analyzed by the use of scanning electron microscopy (SEM) and atomic force microscopy (AFM), and the thicknesses of the films in addition to the quartz-crystal mass-thickness sensor are also measured by AFM. We experimentally demonstrate that the maximum SERS signal is observed near and slightly below the percolation threshold. In this case, the region of maximum enhancement of the SERS signal can be determined using the figure of merit (FOM), which is the ratio of the real and imaginary parts of the effective dielectric permittivity of the films. SERS measurements on hybrid graphene/gold substrates with the dye Crystal Violet show an enhancement factor of ~105 and also demonstrate the ability of graphene to quench photoluminescence by an average of ~60%.

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In present study, we develop an effective and universal technique for retrieving dispersion of bulk and monolayer TMDs from spectroscopic ellipsometry measurements. The basis of the method is excitonic nature of the dispersion. In addition, we demonstrate beneficial influence of annealing on optical properties of MoS2.