Mid-Infrared Frequency Comb Generation and Spectroscopy with Few-Cycle Pulses and χð2Þ Nonlinear Optics

Published

April 1, 2020

Author(s)

Alexander Lind, Abijith S. Kowligy, Henry R. Timmers, Flavio Caldas da Cruz, Nima Nader, Myles C. Silfies, Thomas K. Allison, Scott Papp, Scott Diddams

Abstract

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 fiberlaser source of < 11 fs pulses in the near infrared, we explore quadratic (χð2Þ ) 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 fewcycle mid-infrared pulses in a single pass through periodically poled lithium niobate. Harmonic and cascaded χð2Þ 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.

Citation

Physical Review Letters

Pub Type

Journals

Download Paper

https://doi.org/10.1103/PhysRevLett.124.133904

Local Download

Keywords

Mid-infrared, Spectroscopy

Citation

Lind, A. , Kowligy, A. , Timmers, H. , Caldas da Cruz, F. , Nader, N. , Silfies, M. , Allison, T. , Papp, S. and Diddams, S. (2020), Mid-Infrared Frequency Comb Generation and Spectroscopy with Few-Cycle Pulses and &#967;&#240;2&#222; Nonlinear Optics, Physical Review Letters, [online], https://doi.org/10.1103/PhysRevLett.124.133904, https://tsapps.nist.gov/publication/get_pdf.cfm?pub_id=926905 (Accessed October 9, 2025)