Journal
PHYSICAL REVIEW LETTERS
Volume 124, Issue 13, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.124.133904
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Funding
- National Institute of Standards and Technology
- DARPA SCOUT Program
- National Science Foundation [1708743]
- Air Force Office of Scientific Research [FA9550-16-1-0016, FA9550-16-1-0164]
- Fapesp [2018/26673-5]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1708743] Funding Source: National Science Foundation
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The mid-infrared atmospheric window of 3-5.5 mu m holds valuable information regarding molecular composition and function for fundamental and applied spectroscopy. Using a robust, mode-locked fiberlaser source of < U fs pulses in the near infrared, we explore quadratic (chi((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 chi((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.
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