We present a new method implemented in our new package \textit{FitAik}, to perform least-squares fitting of calculated and experimental atomic transition probabilities, by using the mono-electronic transition integrals $\langle n\ell |r| n'\ell' \rangle$ (with $r$ the electronic radial coordinate) as adjustable quantities. \textit{FitAik} is interfaced to the Cowan suite of codes, for which it automatically writes input files and reads output files. We illustrate our procedure with the example of Er$^{+}$ ion, for which the agreement between calculated and experimental Einstein coefficients is found to be very good. The source code of \emph{FitAik} can be found on GitLab, and the calculated Einstein coefficients are stored in our new database CaDDiACs. They are also used to calculate the dynamic dipole polarizability of Er$^+$.
We present a new method implemented in our new package \textit{FitAik}, to perform least-squares fitting of calculated and experimental atomic transition probabilities, by using the mono-electronic transition integrals ⟨nℓ∣r∣n′ℓ′⟩ (with r the electronic radial coordinate) as adjustable quantities. \textit{FitAik} is interfaced to the Cowan suite of codes, for which it automatically writes input files and reads output files. We illustrate our procedure with the example of Er+ ion, for which the agreement between calculated and experimental Einstein coefficients is found to be very good. The source code of \emph{FitAik} can be found on GitLab, and the calculated Einstein coefficients are stored in our new database CaDDiACs. They are also used to calculate the dynamic dipole polarizability of Er+.
The efficiency of laser cooling relies on the existence of an almost closed optical-transition cycle in the energy spectrum of the considered species. In this respect, rare-earth elements exhibit many transitions which are likely to induce noticeable leaks from the cooling cycle. In this work, to determine whether laser cooling of singly ionized erbium Er+ is feasible, we have performed accurate electronic-structure calculations of energies and spontaneous-emission Einstein coefficients of Er+, using a combination of ab initio and least-squares-fitting techniques. We identify five weak closed transitions suitable for laser cooling, the broadest of which is in the kilohertz range. For the strongest transitions, by simulating the cascade dynamics of spontaneous emission, we show that repumping is necessary, and we discuss possible repumping schemes. We expect our detailed study on Er+ to give good insight into the laser cooling of neighboring ions such as Dy+.
Étude théorique des spectres atomiques de lanthanides neutres et trivalents : Application aux gaz ultra-froids et aux solides dopés Le refroidissement laser et le piégeage des lanthanides ont ouvert la possibilité de réaliser de nouvelles expériences avec des gaz dipolaires ultra-froids, qui peuvent être utilisés, par exemple, pour la simulation quantique de la physique du solide. Pour identifier de nouveaux candidats au refroidissement laser, il est crucial de disposer d’une connaissance spectroscopique précise de l’atome considéré. La première grande orientation de ma thèse est la modélisation du spectre des lanthanides neutres, d'une part de l'erbium (Er), un élément de la partie droite de la rangée des lanthanides, particulièrement attractif en raison d'une transition très fine, reliant l'état fondamental et un état excité métastable, et d'autre part du néodyme (Nd), un élément de la partie gauche de la rangée, qui n'a pas encore été explorée pour le refroidissement laser. En utilisant la méthode semi-empirique implémentée dans les codes de Cowan, nous avons amélioré la description des niveaux de configurations impaires de Er.Nous avons aussi calculé des quantités telles que le facteur de Landé, la durée de vie et la polarisabilité de l'état excité cité plus haut, pour les comparer aux résultats expérimentaux obtenus par un groupe d'Innsbruck en Autriche.Ensuite, pour Nd, nous avons pu interpréter plus de 200 niveaux expérimentaux de la base de données du NIST appartenant aux deux parités, puis nous avons proposé de nouvelles transitions de refroidissement laser. La suite logique de ces travaux est le calcul des coefficients d'Einstein, nécessaires pour caractériser l'efficacité du refroidissement laser et du piégeage des atomes.La plupart des lanthanides existent généralement sous forme de cations trivalents. En raison de la présence d’électrons non appariés, les lanthanides présentent d'intéressantes propriétés électromagnétiques et lumineuses. Sous leur forme trivalente, ils sont largement utilisés à des fins industrielles, dans les lasers et comme (co-)dopants dans les amplificateurs optiques à fibres, par exemple dopée à l'erbium.La deuxième grande orientation de ma thèse est consacrée aux lanthanides trivalents, utilisés comme dopants dans un matériau hôte. Toutes les transitions intéressantes pour ces applications sont induites par le champ cristallin. La théorie de Judd-Ofelt est utilisée depuis des décennies pour décrire ces transitions, mais il existe certaines restrictions liées à la manière dont elle est formulée, en particulier pour l'europium (Eu3+). Dans cette thèse, nous avons effectué des calculs spectroscopiques, en utilisant la même méthodologie que pour les lanthanides neutres, pour trois éléments : Eu3+, Nd3+ et Er3+.Nous avons proposé une extension de la théorie de Judd-Ofelt dans laquelle nous incluons une description précise du spectre de l'ion dopant, et nous tenons compte de la variation de l'indice de réfraction du matériau hôte avec la longueur d'onde. Les résultats de notre modèle sont satisfaisants, car il nous donne un aperçu physique de toutes les transitions observées, y compris celles qui sont interdites par la version standard de la théorie. Par ailleurs, notre modèle reproduit quantitativement les forces d'oscillateurs d'absorption expérimentales. Le code utilisé pour effectuer les calculs est disponible sur GitLab.Comme perspective, nous prévoyons de traiter les transitions en lumière polarisée ou entre des sous-niveaux individuels des ions. Cela sera possible dans notre modèle, car les seuls paramètres ajustés sont ceux du champ cristallin. Cela ouvre la possibilité de modéliser les propriétés spectroscopiques de matériaux hôtes à l'échelle nanométrique.
Abstract Laser cooling and trapping of lanthanides has opened the possibility to carry out new experiments with ultracold dipolar gases, for example for quantum simulation of solid state physics. To identify new suitable candidates for laser-cooling, it is important to have a precise spectroscopic knowledge of the atom under consideration. Along this direction, we present here a detailed modeling of the energy levels of neutral neodymium (Nd), an element belonging to the left part of the lanthanide row, which has not yet been considered for laser-cooling. Using the semi-empirical method implemented in the Cowan suite of codes, we are in particular able to interpret more than 200 experimental levels of the NIST database belonging to both parities. The optimal set of atomic parameters obtained after the least-square fitting step can serve to calculate radiative transition probabilities in the future.
Apropos of the growing interest in the study of long-range interactions for their applications in cold-atom physics, we perform theoretical calculations for the two-dipole C6 and three-dipole C9 dispersion coefficients involving alkaline-earth-metal atoms with alkaline-earth-metal atoms and alkaline-earth-metal ions. The C6 and C9 coefficients are expressed in terms of the dynamic dipole polarizabilities, which are calculated using relativistic methods. Thereafter, the calculated C6 coefficients for the considered alkaline-earth-metal atoms are compared with previously reported values. Due to unavailability of any other earlier theoretical or experimental results, for the C6 coefficients for alkaline-earth-metal atoms with alkaline-earth-metal ions and the C9 coefficients we perform separate fitting calculations and compare the results. Our calculations match in an excellent manner with the fitting calculations. We also report the oscillator strengths for the leading transitions and static dipole polarizabilities for the ground states of the alkaline-earth-metal ions, i.e., Be+,Mg+,Ca+,Sr+, and Ba+, as well as the alkaline-earth-metal atoms, i.e., Be, Mg, Ca, Sr, and Ba. These show good agreement when compared with the available experimental results.
Alkaline-earth dimers are now been used, as new grounds for, testing fundamental physics laws, precision measurements and quantum computation. As a starting point for such experiments, one needs a very good knowledge of the electronic structure, energetics and long-range behavior of these molecular ions. We perform accurate ab initio calculations for the ground and low-lying excited states of Be2+, Mg2+, Ca2+ and Sr2+ molecular ions. We have also calculated the spectroscopic constants, electronic transition dipole moments, polarizabilities and long-range dispersion coefficients for the various alkaline-earth ionic dimers. We have extended our calculations to study heteronuclear species of alkaline-earth molecular ions, like BeCa+, and also mixed alkali alkaline-earth species like NaCa+. We calculated photoassociation (PA) pathways for formation of cold molecular ions and also studied corrections to the Born-Oppenheimer Hamiltonian: non-adiabatic couplings and hyperfine structure due to nuclear spins and electric quadrupoles. We believe, this work would lay foundation, not only for new experiments in ultracold physics and chemistry, but would also provide valuable starting point for theoretical calculations involving low temperature scattering and resonant charge transfer.
We present revised measurements of the static electric dipole polarizabilities of K, Rb, and Cs based on atom interferometer experiments presented in [Phys. Rev. A 2015, 92, 052513] but now re-analyzed with new calibrations for the magnitude and geometry of the applied electric field gradient. The resulting polarizability values did not change, but the uncertainties were significantly reduced. Then we interpret several measurements of alkali metal atomic polarizabilities in terms of atomic oscillator strengths fik, Einstein coefficients Aik, state lifetimes τk, transition dipole matrix elements Dik, line strengths Sik, and van der Waals C6 coefficients. Finally, we combine atom interferometer measurements of polarizabilities with independent measurements of lifetimes and C6 values in order to quantify the residual contribution to polarizability due to all atomic transitions other than the principal ns-npJ transitions for alkali metal atoms.