Mid-Infrared Frequency Comb Generation and Spectroscopy with Few-Cycle Pulses and χ^{(2)} Nonlinear Optics

The mid-infrared atmospheric window of 3-5.5  μm holds valuable information regarding molecular composition and function for fundamental and applied spectroscopy. Using a robust, mode-locked fiber-laser source of <11  fs pulses in the near infrared, we explore quadratic (χ^{(2)}) nonlinear optical processes leading to frequency comb generation across this entire mid-infrared atmospheric window. With experiments and modeling, we demonstrate intrapulse difference frequency generation that yields few-cycle mid-infrared pulses in a single pass through periodically poled lithium niobate. Harmonic and cascaded χ^{(2)} nonlinearities further provide direct access to the carrier-envelope offset frequency of the near infrared driving pulse train. The high frequency stability of the mid-infrared frequency comb is exploited for spectroscopy of acetone and carbonyl sulfide with simultaneous bandwidths exceeding 11 THz and with spectral resolution as high as 0.003  cm^{-1}. The combination of low noise and broad spectral coverage enables detection of trace gases with concentrations in the part-per-billion range.