Dual Resonant Sum Frequency Generations from Two-Dimensional Materials

We propose dual resonant optical sum frequency generation (SFG), where the two most singular resonances could be selected, and report for the monolayer (1L-) WSe₂ when one (ω₁) of two excitation pulses is resonant to A exciton and their sum frequency (ω₁ + ω₂) to D exciton. The dual resonant SFG confirms that, under an irradiation of ω₁ and ω₂ pulses with the same fluence of ∼1.4 × 10¹⁰ W/m², its signal intensity could be enhanced about 20 times higher than the resonant SHG (i.e., 2ω₁ to the D excitonic absorption). Further, the dual resonant SFG intensity of 1L-WSe₂ is found to be 1 order of magnitude higher than the single resonant SFG intensity of 1L-WS₂ under the same condition of two-pulse irradiation. Finally, observations of the dual resonant SFG are thoroughly examined using real-time time-dependent density functional theory (rt-TDDFT), and the relevant nonlinear optical characteristics are scrutinized using the Greenwood-Kubo formalism.