Optical amplification by surface-plasmon-resonant Au grating substrates: Monolayer MoS2 with 170-fold second harmonic generation and 3-fold (off-resonance) Raman scattering

Nanoplasmonics is a potential game-changer in the development of next-generation on-chip photonic devices and computers, owing to the geometrically controlled and amplified linear and nonlinear optical processes. For instance, it resolves the limited light-matter interaction of the unique two-dimensional (2D) crystalline materials like semiconducting monolayer molybdenum disulfide (1L-MoS2). Metal grating (MG) substrates excel at this because their surface plasmons (SPs) can lead to stark field confinement near the surface. This work studies optical amplification of 1L-MoS2 on the gold (Au) MG substrate, which was designed to operate in a glycerol environment with SP resonance (SPR) at 850 nm excitation wavelength. Its design was verified by simulated and experimental reflectances, and topographically inspected by atomic force microscopy (AFM). Two advanced imaging modalities, second harmonic generation (SHG) and confocal Raman microscopy (CRM) were used to evaluate its 170-fold SHG on- and 3-fold CRM offresonance optical amplifications, respectively. Some MoS2-to-grating adhesion issues due to trapped liquid showed as image nonuniformities. Possible improvements to limitations like surface roughness were also discussed. These Au MG substrates can boost conventional linear and nonlinear backscattering microscopies because they are tunable in the visible and near-infrared range by selecting geometry, metal, and environment.