Efficient generation of few-cycle pulses beyond 10 μm from an optical parametric amplifier pumped by a 1-µm laser system

Nonlinear vibrational spectroscopy profits from broadband sources emitting in the molecular fingerprint region. Yet, broadband lasers operating at wavelengths above 7 μm have been lacking, while traditional cascaded parametric frequency down-conversion schemes suffer from exceedingly low conversion efficiencies. Here we present efficient, direct frequency down-conversion of femtosecond 100-kHz, 1.03-μm pulses to the mid-infrared from 7.5 to 13.3 μm in a supercontinuum-seeded, tunable, single-stage optical parametric amplifier based on the wide-bandgap material Cd(0.65)Hg(0.35)Ga(2)S(4). The amplifier delivers near transform-limited, few-cycle pulses with an average power > 30 mW at center wavelengths between 8.8 and 10.6 μm, at conversion efficiencies far surpassing that of optical parametric amplification followed by difference-frequency generation or intrapulse difference-frequency generation. The pulse duration at 10.6 μm is 101 fs corresponding to 2.9 optical cycles with a spectral coverage of 760–1160 cm(−1). Cd(x)Hg(1−x)Ga(2)S(4) is an attractive alternative to LiGaS(2) and BaGa(4)S(7) in small-scale, Yb-laser-pumped, few-cycle mid-infrared optical parametric amplifiers and offers a much higher nonlinear figure of merit compared to those materials. Leveraging the inherent spatial variation of composition in Cd(x)Hg(1−x)Ga(2)S(4), an approach is proposed to give access to a significant fraction of the molecular fingerprint region using a single crystal at a fixed phase matching angle.