Absolute frequency metrology of buffer-gas-cooled molecular spectra at 1 kHz accuracy level.

Aiello, Roberto; Di Sarno, Valentina; Delli Santi, Maria Giulia; De Rosa, Maurizio; Ricciardi, Iolanda; De Natale, Paolo; Santamaria, Luigi; Giusfredi, Giovanni et al. · Nat Commun · 2022

basic_science · Level V

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Abstract

By reducing both the internal and translational temperature of any species down to a few kelvins, the buffer-gas-cooling (BGC) technique has the potential to dramatically improve the quality of ro-vibrational molecular spectra, thus offering unique opportunities for transition frequency measurements with unprecedented accuracy. However, the difficulty in integrating metrological-grade spectroscopic tools into bulky cryogenic equipment has hitherto prevented from approaching the kHz level even in the best cases. Here, we overcome this drawback by an original opto-mechanical scheme which, effectively coupling a Lamb-dip saturated-absorption cavity ring-down spectrometer to a BGC source, allows us to determine the absolute frequency of the acetylene (ν<sub>1</sub> + ν<sub>3</sub>) R(1)e transition at 6561.0941 cm<sup>-1</sup> with a fractional uncertainty as low as 6 × 10<sup>-12</sup>. By improving the previous record with buffer-gas-cooled molecules by one order of magnitude, our approach paves the way for a number of ultra-precise low-temperature spectroscopic studies, aimed at both fundamental Physics tests and optimized laser cooling strategies.