In-line synthesis of multi-octave phase-stable infrared light

in: Optics Express (2023)
Kassab, Hadil; Gröbmeyer, Sebastian; Schweinberger, Wolfgang; Hofer, Christina; Steinleitner, Philipp; Högner, Maximilian; Amotchkina, Tatiana; Gerz, Daniel; Knorr, Matthias; Huber, Rupert; Karpowicz, Nicholas; Pupeza, Ioachim
Parametric downconversion driven by modern, high-power sources of 10-fs-scale near-infrared pulses, in particular intrapulse difference-frequency generation (IPDFG), affords combinations of properties desirable for molecular vibrational spectroscopy in the mid-infrared range: broad spectral coverage, high brilliance, and spatial and temporal coherence. Yet, unifying these in a robust and compact radiation source has remained a key challenge. Here, we address this need by employing IPDFG in a multi-crystal in-line geometry, driven by the 100-W-level, 10.6-fs pulses of a 10.6-MHz-repetition-rate, nonlinearly post-compressed Yb:YAG thin-disk oscillator. Polarization tailoring of the driving pulses using a bichromatic waveplate is followed by a sequence of two crystals, LiIO3 and LiGaS2, resulting in the simultaneous coverage of the 800-cm−1-to-3000-cm−1 spectral range (at -30-dB intensity) with 130mW of average power. We demonstrate that optical-phase coherence is maintained in this in-line geometry, in theory and experiment, the latter employing ultra-broadband electro-optic sampling. These results pave the way toward coherent spectroscopy schemes like field-resolved and frequency-comb spectroscopy, as well as nonlinear, ultrafast spectroscopy and optical-waveform synthesis across the entire infrared molecular fingerprint region.

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