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Narrow optical resonances of atoms or molecules have immense significance in various precision measurements, such as testing fundamental physics and the generation of primary frequency standards. In these studies, accurate transition centers derived from fitting the measured spectra are demanded, which critically rely on the knowledge of spectral line profiles. Here, we propose a new mechanism of Fano-like resonance induced by distant discrete levels %in atoms or molecules and experimentally verify it with Doppler-free spectroscopy of vibration-rotational transitions of CO$_2$. The observed spectrum has an asymmetric profile and its amplitude increases quadratically with the probe laser power. Our results facilitate a broad range of topics based on narrow transitions. %, such as optical clocks, determination of fundamental physical constants, and quantum memory., 6 pages, 4 figures

We report on a two-fold increase of the $^{39}Ar$ loading rate in an atom trap by enhancing the generation of metastable atoms in a discharge source. Additional atoms in the metastable $1s_5$ level (Paschen notation) are obtained via optically pumping both the $1s_4$ - $2p_6$ transition at 801 nm and the $1s_2$ - $2p_6$ transition at 923 nm. By solving the master equation for the corresponding six-level system, we identify these two transitions to be the most suitable ones and encounter a transfer process between $1s_2$ and $1s_4$ when pumping both transitions simultaneously. We calculate the previously unknown frequency shifts of the two transitions in $^{39}Ar$ and confirm the results with trap loading measurements. The demonstrated increase in the loading rate enables a corresponding decrease in the required sample size, uncertainty and measurement time for $^{39}Ar$ dating, a significant improvement for applications such as dating of ocean water and alpine ice cores., arXiv admin note: text overlap with arXiv:2005.11056

Information about molecular collisions is encoded in the shapes of collision-perturbed molecular resonances. This connection between molecular interactions and line shapes is most clearly seen in simple systems, such as the molecular hydrogen perturbed by a noble gas atom. We study the H2–Ar system by means of highly accurate absorption spectroscopy and ab initio calculations. On the one hand, we use the cavity-ring-down-spectroscopy technique to record the shapes of the S(1) 3-0 line of molecular hydrogen perturbed by argon. On the other hand, we simulate the shapes of this line using ab initio quantum-scattering calculations performed on our accurate H2–Ar potential energy surface (PES). In order to validate the PES and the methodology of quantum-scattering calculations separately from the model of velocity-changing collisions, we measured the spectra in experimental conditions in which the influence of the latter is relatively minor. In these conditions, our theoretical collision-perturbed line shapes reproduce the raw experimental spectra at the percent level. However, the collisional shift, δ0, differs from the experimental value by 20%. Compared to other line-shape parameters, collisional shift displays much higher sensitivity to various technical aspects of the computational methodology. We identify the contributors to this large error and find the inaccuracies of the PES to be the dominant factor. With regard to the quantum scattering methodology, we demonstrate that treating the centrifugal distortion in a simple, approximate manner is sufficient to obtain the percent-level accuracy of collisional spectra.

The (30012) ← (00001) band of

Sub-Doppler saturated absorption spectroscopy of rovibrational transitions of carbon monoxide broadened by nitrogen was recorded at low pressures (1-24 Pa) near 1.56 µm with comb-locked cavity ring-down saturation spectroscopy. We found a nonlinear pressure dependence of the Lamb-dip width of the CO transition induced by elastic scattering. Analysis of the results allows us to characterize parameters of elastic- and nonelastic- scattering under collisions. The elastic scattering angle for nitrogen-induced collisions (CO-N2) was determined to be larger than 0.6 × 10−3 rad. The line broadening of the Lamb dip in the region of low pressures exceeds the broadening at high pressures by a factor of 4 and 5 for the self- and N2-broadening CO R(9) transition. Moreover, much smaller line shifts for both self- and N2-broaden Lamb dips were observed, which was also attributed to the decrease in the number of scattered molecules in the interaction and the increasing attracting forces.