We report a coherent mid-infrared (MIR) source with a combination of broad spectral coverage (6-18 μm), high repetition rate (50 MHz), and high average power (0.5 W). The waveform-stable pulses emerge via intrapulse differencefrequency generation (IPDFG) in a GaSe crystal, driven by a 30-W-average-power train of 32-fs pulses spectrally centered at 2 μm, delivered by a fiber-laser system. Electro-optic sampling (EOS) of the waveform-stable MIR waveforms reveals their single-cycle nature, confirming the excellent phase matching both of IPDFG and of EOS with 2-μm pulses in GaSe.

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We present a source of brilliant mid-infrared radiation, seamlessly covering the wavelength range between 1.33 and 18 μm (7500-555 cm −1 ) with three channels, employing broadband nonlinear conversion processes driven by the output of a thulium-fiber laser system. The high-average-power femtosecond frontend delivers a 50 MHz train of 250 fs pulses spectrally centered at 1.96 μm. The three parallel channels employ soliton self-compression in a fused-silica fiber, supercontinuum generation in a ZBLAN fiber, and difference-frequency generation in GaSe driven by soliton selfcompressed pulses. The total output enables spectral coverage from 1.33 to 2.4 μm, from 2.4 to 5.2 μm, and from 5.2 to 18 μm with 4.5 W, 0.22 W and 0.5 W, respectively. This spatially coherent source with a footprint of less than 4 m 2 exceeds the brilliance of 3rd-generation synchrotrons by more than three orders of magnitude over 90% of the bandwidth.

Femtosecond enhancement cavities1 are key to applications including high-sensitivity linear2–4 and nonlinear5,6 gas spectroscopy, as well as efficient nonlinear optical frequency conversion7–10. Yet, to date, the broadest simultaneously enhanced bandwidths amount to <20% of the central optical frequency8,9,11–15. Here, we present an ultrabroadband femtosecond enhancement cavity comprising gold-coated mirrors and a wedged-diamond-plate input coupler, with an average finesse of 55 for optical frequencies below 40 THz and exceeding 40 in the 120–300 THz range. Resonant enhancement of a 50-MHz-repetition-rate offset-free frequency comb spanning 22–40 THz results in a waveform-stable ultrashort circulating pulse with a spectrum supporting a Fourier limit of 1.6 cycles, enabling time-domain electric-field-resolved spectroscopy of molecular samples with temporally separated excitation and molecular response16. The contrast between the two is improved by taking advantage of destructive interference at the input coupler. At an effective interaction length with a gas of up to 81 m, this concept promises parts-per-trillion-level ultrabroadband electric-field-resolved linear and nonlinear spectroscopy of impulsively excited molecular vibrations.