Second-harmonic generation enhancement in monolayer transition-metal dichalcogenides by an epsilon-near-zero substrate

Abstract: Monolayer transition-metal dichalcogenides (TMDCs) present high second-order optical nonlinearity, which is extremely desirable for, e.g., frequency conversion in nonlinear photonic devices. On the other hand, the atomic thickness of 2D materials naturally leads to low frequency converted intensities, highlighting the importance to design structures that enhance the nonlinear response for practical applications. A number of methods to increase the pump electric field at the 2D material has been reported, relying on complex plasmonic and/or metasurface structures. Here, we take advantage of the fact that unstructured substrates with a low refractive index naturally maximize the pump field at a dielectric interface, offering a simple means to promote enhanced nonlinear optical effects. In particular, we measured second harmonic generation (SHG) in MoS2 and WS2 on fluorine tin oxide (FTO), which presents an epsilon-near-zero point near our 1550-nm pump wavelength. Polarized SHG measurements reveal an SHG intensity that is one order of magnitude higher on FTO than on a glass substrate.