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Distinct broadband third-harmonic generation on a thin amorphous medium-air interface.

We achieve a series of distinct broadband third-harmonic generation (THG) signals at the amorphous glass-air interface attributed to third-order and cascaded third-order nonlinear processes. A novel THG laser sideband arises from cascaded interaction between fundamental pulses and the cascaded four-wave mixing signals. The spatially separated THG sidebands with distinct spectral profiles manifest femtosecond quantum beats. Using a versatile setup with two crossing near-IR pulses temporally delayed to each other, we design an incident pulse polarization control method on the THG sideband lasers and also acquire the low-frequency surface Raman spectrum of the amorphous medium.