Second-harmonic generation (SHG) is a nonlinear optical process that converts two identical photons into a new one with doubled frequency. Two-dimensional semiconductors represented by transition-metal dichalcogenides are highly efficient SHG media because of their excitonic resonances. Using spectral phase interferometry, here we directly show that SHG in heterobilayers of MoS and WS is governed by optical interference between two coherent SH fields that are phase-delayed differently in each material. We also quantified the frequency-dependent phase difference between the two, which agreed with polarization-resolved data and first-principles calculations on complex susceptibility. The second-harmonic analogue of Young's double-slit interference shown in this work demonstrates the potential of custom-designed parametric generation by atom-thick nonlinear optical materials.
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