Efficient Frequency Mixing of Guided Surface Waves by Atomically Thin Nonlinear Crystals.

Monolayer transition metal dichalcogenides possess considerable second-order nonlinear coefficients but a limited efficiency of frequency conversion due to the short interaction length with light under the typical direct illumination. Here, we demonstrate an efficient frequency mixing of the guided surface waves on a monolayer tungsten disulfide (WS2) by simultaneously lifting the temporal and spatial overlap of the guided wave and the nonlinear crystal. Three orders-of-magnitude enhancement of the conversion efficiency was achieved in the counter-propagating excitation configuration. Also, the frequency-mixing signals are highly collimated, with the emission direction and polarization controlled, respectively, by the pump frequencies and the rotation angle of WS2 relative to the propagation direction of the guided waves. These results indicate that the rules of nonlinear frequency conversion are applicable even when the crystal is scaled down to the ultimate single-layer limit. This study provides a versatile platform to enhance the nonlinear optical response of 2D materials and favor the scalable generation of a coherent light source and entangled photon pairs.