Measuring molecular frequencies in the 1-10 µm range at 11-digits accuracy.

High-resolution spectroscopy in the 1-10 µm region has never been fully tackled for the lack of widely-tunable and practical light sources. Indeed, all solutions proposed thus far suffer from at least one of three issues: they are feasible only in a narrow spectral range; the power available for spectroscopy is limited; the frequency accuracy is poor. Here, we present a setup for high-resolution spectroscopy, whose approach can be applied in the whole 1-10 µm range. It combines the power of quantum cascade lasers (QCLs) and the accuracy achievable by difference frequency generation using an orientation patterned GaP crystal. The frequency is measured against a primary frequency standard using the Italian metrological fibre link network. We demonstrate the performance of the setup by measuring a vibrational transition in a highly-excited metastable state of CO around 6 µm with 11 digits of precision.

Absolute frequency measurements of the 2(3)S1-->2(3)P 0,1,2 atomic helium transitions around 1083 nm.

We measure the frequency of the 2(3)S1-->2(3)P(0,1,2) transitions of helium in a metastable beam using an optical frequency comb synthesizer. The relative uncertainty of these measurements ranging from 5x10(-11) to 7x10(-12) is, to our knowledge, the most precise result for any optical helium transition. Considering existing accurate values of the 2(3)P fine structure, we measure a centroid value of the 2(3)S-2(3)P frequency of 276 736 495 624.6(2.4) kHz, improving the previous interferometric measurement by 30 times. New accurate values of the 2(3)S-2(3)P and 2(3)P Lamb-shift energies are obtained.