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High-harmonic generation (HHG) provides short-wavelength light that is useful for precision spectroscopy and probing ultrafast dynamics. We report efficient, phase-coherent harmonic generation up to the ninth order (333 nm) in chirped periodically poled lithium niobate waveguides driven by phase-stable$\le <\#comment/>12\mathrm{n}\mathrm{J}$, 100 fs pulses at 3 µm with 100 MHz repetition rate. A mid-infrared to ultraviolet-visible conversion efficiency as high as 10% is observed, among an overall 23% conversion of the fundamental to all harmonics. We verify the coherence of the harmonic frequency combs despite the complex highly nonlinear process. Accommodating the extreme spectral bandwidth, numerical simulations based on a single broadband envelope equation with only quadratic nonlinearity give estimates for the conversion efficiency within approximately 1 order of magnitude over a wide range of experimental parameters. From this comparison between theory and experiment, we identify a dimensionless parameter capturing the competition between three-wave mixing and group-velocity walk-off of the harmonics that governs the cascaded HHG physics. We also gain insights into spectral optimization via tuning the waveguide poling profile and pump pulse parameters. These results can inform cascaded HHG in a range of different platforms.

 

Broadband ultrafast optical spectroscopy methods, such as transient absorption spectroscopy and 2D spectroscopy, are widely used to study molecular dynamics. However, these techniques are typically restricted to optically thick samples, such as solids and liquid solutions. In this article we discuss a cavity-enhanced ultrafast transient absorption spectrometer covering almost the entire visible range with a detection limit of ΔOD < 1 × 10 −9 , extending broadband all-optical ultrafast spectroscopy techniques to dilute beams of gas-phase molecules and clusters. We describe the technical innovations behind the spectrometer and present transient absorption data on two archetypical molecular systems for excited-state intramolecular proton transfer, 1′-hydroxy-2′-acetonapthone and salicylideneaniline, under jet-cooled and Ar cluster conditions. 

We describe the cavity enhancement of frequency combs over a wide tuning range of 450–700 nm ($><\#comment/>7900{\mathrm{c}\mathrm{m}}^{-<\#comment/>1}$), covering nearly the entire visible spectrum. Tunable visible frequency combs from a synchronously pumped optical parametric oscillator are coupled into a four-mirror, dispersion-managed cavity with a finesse of 600–1400. An intracavity absorption path length enhancement greater than 190 is obtained over the entire tuning range, while preserving intracavity spectral bandwidths capable of supporting sub-200 fs pulse durations. These tunable cavity-enhanced frequency combs can find many applications in nonlinear optics and spectroscopy.

 

We report on the development of a high-power mid-infrared frequency comb with 100 MHz repetition rate and 100 fs pulse duration. Difference frequency generation is realized between two branches derived from an Er:fiber comb, amplified separately in Yb:fiber and Er:fiber amplifiers. Average powers of 6.7 W and 14.9 W are generated in the 2.9 µm idler and 1.6 µm signal, respectively. With high average power, excellent beam quality, and passive carrier-envelope phase stabilization, this light source is a promising platform for generating broadband frequency combs in the far infrared, visible, and deep ultraviolet.