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The efficient optical second-harmonic generation (SHG) of two-dimensional(2D) crystals, coupled with their atomic thickness that circumvents thephase-match problem, has garnered considerable attention. While various 2Dheterostructures have shown promising applications in photodetectors, switchingelectronics, and photovoltaics, the modulation of nonlinear optical propertiesin such hetero-systems remains unexplored. In this study, we investigateexciton sensitized SHG in heterobilayers of transition metal dichalcogenides(TMDs), where photoexcitation of one donor layer enhances the SHG response ofthe other as an acceptor. We utilize polarization-resolved interferometry todetect the SHG intensity and phase of each individual layer, revealing theenergetic match between the excitonic resonances of donors and the SHGenhancement of acceptors for four TMD combinations. Our results also uncoverthe dynamic nature of interlayer coupling, as evidenced by the dependence ofsensitization on interlayer gap spacing and the average power of thefundamental beam. This work provides insights into how interlayer coupling oftwo different layers can modify nonlinear optical phenomena in 2Dheterostructures.

Exciton-Sensitized Second-Harmonic Generation in 2D Heterostructures