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We investigate the coupling effects between a double-resonance split-ring resonators (SRRs) design and the epsilon-near-zero (ENZ) guided mode of ultrathin indium tin oxide (ITO) films on second-harmonic generation (SHG). The optimized SRRs with an aspect ratio of 0.3 support a magnetic dipole (MD) resonance within the ENZ regime of ITO and a higher-order resonance at the SH frequency to achieve mode matching under cross-polarized excitation. The SRR-ITO coupled system (as opposed to the nanorod-ITO coupled system) was found to perform constructive (destructive) polarization interference between the nonlinear polarization currents at the upper hybridized modes (ω + ) and the linear electric field at SH frequency (2ω + ), resulting in a 1218-fold SHG enhancement outperformed than that of the nanorod-ITO coupled system, as predicted by overlap integral analysis. The measured SHG conversion efficiency for the SRR-ITO coupled system exceeds 10 −7  at an excitation wavelength of 1,320 nm, corresponding to a one-order (two-order) of magnitude enhancement compared to the nanorod-ITO coupled system (Au/ITO film). These findings highlight the potential of the proposed hybrid metasurfaces for efficient cross-polarized nonlinear signal generation, paving the way for advanced applications such as light sources, modulators in integrated photonic circuits, and biological sensing.

Strong coupling of double resonance designs and epsilon-near-zero modes for mode-matching enhancement of second-harmonic generation