We investigate generation of the third harmonic (TH; λ = 355 nm) signal by two-colour excitation (λ = 1064 nm and its second harmonic, λ = 532 nm) in argon gas, with emphasis on the influence of relative phases and intensities of the two-colour pump on the third-order nonlinear frequency conversion process. Perturbative nonlinear optics predicts that the TH signal will oscillate periodically with the relative phases of the two-colour driving laser fields due to the interference of TH signals from a direct third-harmonic-generation (THG) channel and a four-wave mixing (FWM) channel. For the first time, we show unequivocal experimental evidence of this effect. A modulation level as high as 0.35 is achieved by waveform control of the two-colour laser field. The modulation also offers a promising way to retrieve the relative phase value of the two-colour laser field.
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