Optical third-harmonic generation using ultrashort laser pulses

To better predict optical third-harmonic generation (THG) in transparent dielectrics, we model a typical ultrashort pulsed Gaussian beam, including both group velocity mismatch and phase mismatch of the fundamental and harmonic fields. We find that competition between the group velocity mismatch and phase mismatch leads to third-harmonic generation that is sensitive only to interfaces. In this case, the spatial resolution is determined by the group velocity walk-off length. THG of modern femtosecond lasers in optical solids is a bulk process, without a surface susceptibility, but bears the signature of a surface enhancement effect in z-scan measurements. We demonstrate the accuracy of the model, by showing the agreement between the predicted spectral intensity and the measured third-harmonic spectrum from a thin sapphire crystal.