High-precision molecular interrogation by direct referencing of a quantum-cascade-laser to a near-infrared frequency comb.

This work presents a very simple yet effective way to obtain direct referencing of a quantum-cascade-laser at 4.3 µm to a near-IR frequency-comb. Precise tuning of the comb repetition-rate allows the quantum-cascade-laser to be scanned across absorption lines of a CO2 gaseous sample and line profiles to be acquired with extreme reproducibility and accuracy. By averaging over 50 acquisitions, line-centre frequencies are retrieved with an uncertainty of 30 kHz in a linear interaction regime. The extension of this methodology to other lines and molecules, by the use of widely tunable extended-cavity quantum-cascade-lasers, paves the way to a wide availability of high-quality and traceable spectroscopic data in the most crucial region for molecular detection and interrogation.