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We make absolute frequency measurements of Cs Rydberg transitions, $\vert 6S_{1/2}, F=3 \rangle \rightarrow \vert nS_{1/2}~(n=23\rm{-}90)\rangle$ and $\vert nD_{3/2,5/2}~(n=21\rm{-}90)\rangle$, with an accuracy of less than $ 72\,\rm kHz$. The quantum defect parameters for the measured Rydberg series are the most precise obtained to date. The quantum defect series is terminated at $\delta_4$, showing that prior fits requiring higher order quantum defects reflect uncertainties in the observations. The precision of the measured quantum defects allow for the calculation of Rydberg electric-dipole transitions and fine-structure intervals extrapolated from high principal quantum numbers, to rival that of sophisticated many-body relativistic calculations carried out at low Rydberg principal quantum numbers. We quantitatively predict the contributions to the quantum defect parameters from core polarization and core penetration of Cs inner shell electrons. A new value for the ionization energy, consistent across the $ nS_{1/2}$ and $ nD_{3/2,5/2}$ Rydberg series, is reported at $31406.467 751 48 (14)~\rm{cm}^{-1}$., Comment: 15 pages, 7 figures, 7 tables

We calculate, via variational techniques, single- and two-photon Rydberg microwave transitions, as well as scalar and tensor polarizabilities of sodium atom using the parametric one-electron valence potential, including the spin-orbit coupling. The trial function is expanded in a basis set of optimized Slater-type orbitals, resulting in highly accurate and converged eigen-energies up to $n=60$. We focus our studies on the microwave band 90-150 GHz, due to its relevance to laser excitation in the Earth's upper-atmospheric sodium layer for wavelength-dependent radiometry and polarimetry, as precise microwave polarimetry in this band is an important source of systematic uncertainty in searches for signatures of primordial gravitational waves within the anisotropic polarization pattern of photons from the cosmic microwave background. We present the most efficient transition coefficients in this range, as well as the scalar and tensor polarizabilities compared with available experimental and theoretical data.

Partial wave resonances are quasi-bound states that are formed by tunneling through the centrifugal barrier. Such states are important to collisions that deviate from the Langevin limit where direct collision path is suppressed due to quantum symmetry or a potential barrier. In such a case, quantum resonances play a major role in the dynamics at low temperatures where scattering process can be described mainly by the resonance contribution. Here we present the first observation of the lowest-lying partial wave resonance in the Penning ionization collisions between metastable neon and rovibrationally ground state HD molecules. We observe the resonance at an energy of $k_B\times$22mK taking advantage of the phase space correlation similar to atomic delta kick cooling. We show that the $p$-wave resonance position is particularly sensitive to the leading term of the van der Waals interaction. We also measure shape resonance at a higher angular momentum state, $l=6$, allowing us to disentangle and probe the short and the long parts of the intermolecular interaction.

We compute the Rydberg spectrum of a single Ca$^+$ ion in a Paul trap by incorporating various internal and external coupling terms of the ion to the trap in the Hamiltonian. The coupling terms include spin-orbit coupling in Ca$^+$, charge (electron and ionic core) coupling to the radio frequency and static fields, ion-electron coupling in the Paul trap, and ion center-of-mass coupling. The electronic Rydberg states are precisely described by a one-electron model potential for e$^-$+Ca$^{2+}$, and accurate eigenenergies, quantum defect parameters, and static and tensor polarizabilities for a number of excited Rydberg states are obtained. The time-periodic rf Hamiltonian is expanded in the Floquet basis, and the trapping-field-broadened Rydberg lines are compared with recent observations of Ca$^+(23P)$ and Ca$^+(52F)$ Rydberg lines.

Cold collisions serve as a very sensitive probe of the interaction potential. In the recent study of Klein et al. (Nature Phys. 13, 35-38 (2017)) the one-parameter scaling of the interaction potential was necessary to obtain agreement between theoretical and observed patterns of the orbiting resonances for excited metastable helium atoms colliding with hydrogen molecules. Here we show that the effect of nonrigidity of the H$_2$ molecule on the resonant structure, absent in the previous study, is critical to predict correct positions of the resonances in that case. We have complemented the theoretical description of the interaction potential and revised reaction rate coefficients by proper inclusion of the flexibility of the molecule. The calculated reaction rate coefficients are in remarkable agreement with the experimental data without empirical adjustment of the interaction potential. We have shown that even state-of-the-art calculations of the interaction energy cannot ensure agreement with the experiment if such an important physical effect as flexibility of the interacting molecule is neglected. Our findings about the significance of the nonrigidity effects can be especially crucial in cold chemistry, where the quantum nature of molecules is pronounced.

The absorption spectra of the cold Na2 molecule dressed by a linearly polarized standing laser wave is investigated. In the studied scenario the rotational motion of the molecules is frozen while the vibrational and translational degrees of freedom are accounted for as dynamical variables. In such a situation a light-induced conical intersection (LICI) can be formed. To measure the spectra a weak field is used whose propagation direction is perpendicular to the direction of the dressing field but has identical polarization direction. Although LICIs are present in our model, the simulations demonstrate a very robust absorption spectrum, which is insensitive to the intensity and the wavelength of the dressing field and which does not reflect clear signatures of light-induced nonadiabatic phenomena related to the strong mixing between the electronic, vibration and translational motions. However, by widening artificially the very narrow translational energy level gaps, the fingerprint of the LICI appears to some extent in the spectrum.

Anisotropy is a fundamental property of particle interactions. It occupies a central role in cold and ultra-cold molecular processes, where long range forces have been found to significantly depend on orientation in ultra-cold polar molecule collisions. Recent experiments have demonstrated the emergence of quantum phenomena such as scattering resonances in the cold collisions regime due to quantization of the intermolecular degrees of freedom. Although these states have been shown to be sensitive to interaction details, the effect of anisotropy on quantum resonances has eluded experimental observation so far. Here, we directly measure the anisotropy in atom-molecule interactions via quantum resonances by changing the quantum state of the internal molecular rotor. We observe that a quantum scattering resonance at a collision energy of $k_B$ x 270 mK appears in the Penning ionization of molecular hydrogen with metastable helium only if the molecule is rotationally excited. We use state of the art ab initio and multichannel quantum molecular dynamics calculations to show that the anisotropy contributes to the effective interaction only for $H_2$ molecules in the first excited rotational state, whereas rotationally ground state $H_2$ interacts purely isotropically with metastable helium. Control over the quantum state of the internal molecular rotation allows us to switch the anisotropy on or off and thus disentangle the isotropic and anisotropic parts of the interaction. These quantum phenomena provide a challenging benchmark for even the most advanced theoretical descriptions, highlighting the advantage of using cold collisions to advance the microscopic understanding of particle interactions., Comment: 19 pages, 3 figures