Cascaded multi-harmonic generation in a β-BBO crystal reaching 133 nm from a single 800 nm pump beam

Abstract

Nonlinear crystals are widely used to efficiently generate the second or third harmonic, and also for frequency mixing. Generation of multiple cascaded harmonics simultaneously, however, appears much less studied, although supported by the usually large nonlinearity of these crystals. Here, we demonstrate the generation of multiple harmonics up to 6th order in a β-BBO crystal, extending into the vacuum ultraviolet spectral range. Phase matched generation of the second or the third harmonic is directly driven by a single 800 nm Ti:sapphire oscillator beam. Our study reveals that the harmonics are generated by χ(2):χ(2) and χ(2):χ(3) cascaded processes and intense signals are obtained even for the 5th and 6th harmonic, where the β-BBO crystal is mostly absorbing. While higher order harmonics cannot be phase matched simultaneously, limiting the harmonic amplitudes, even the weakest harmonics are more than three orders of magnitude above the measurement noise limit, making them suitable for many spectroscopic applications.