Search

We present high accuracy relativistic coupled cluster calculations of the first and second ionization potentials and the electron affinity of the heaviest element in the periodic table, Og. The results were extrapolated to the basis set limit and augmented with the higher order excitations (up to perturbative quadruples), the Breit contribution, and the QED self-energy and vacuum polarization corrections. We have performed an extensive investigation of the effect of the various computational parameters on the calculated properties, which allowed us to assign realistic uncertainties on our predictions. Similar study on the lighter homolog of Og, Rn, yields excellent agreement with experiment for the first ionization potential and a reliable prediction for the second ionization potential.

We investigate the merits of a measurement of the permanent electric dipole moment of the electron (eEDM) with barium monofluoride molecules, thereby searching for phenomena of CP violation beyond those incorporated in the standard model (SM) of particle physics. Although the BaF molecule has a smaller enhancement factor in terms of the effective electric field than other molecules used in current studies (YbF, ThO and ThF+), we show that a competitive measurement is possible by combining Stark-deceleration, laser-cooling and an intense primary cold source of BaF molecules. With the long coherent interaction times obtainable in a cold beam of BaF, a sensitivity of 5 × 10−30 e⋅cm for an eEDM is feasible. We describe the rationale, the challenges and the experimental methods envisioned to achieve this target. Graphical abstract: [Figure not available: see fulltext.].

The NL-eEDM collaboration is building an experimental setup to search for the permanent electric dipole moment of the electron in a slow beam of cold barium fluoride molecules [Eur. Phys. J. D, 72, 197 (2018)]. Knowledge of molecular properties of BaF is thus needed to plan the measurements and in particular to determine an optimal laser-cooling scheme. Accurate and reliable theoretical predictions of these properties require incorporation of both high-order correlation and relativistic effects in the calculations. In this work theoretical investigations of the ground and the lowest excited states of BaF and its lighter homologues, CaF and SrF, are carried out in the framework of the relativistic Fock-space coupled cluster (FSCC) and multireference configuration interaction (MRCI) methods. Using the calculated molecular properties, we determine the Franck-Condon factors (FCFs) for the $A^2\Pi_{1/2} \rightarrow X^2\Sigma^{+}_{1/2}$ transition, which was successfully used for cooling CaF and SrF and is now considered for BaF. For all three species, the FCFs are found to be highly diagonal. Calculations are also performed for the $B^2\Sigma^{+}_{1/2} \rightarrow X^2\Sigma^{+}_{1/2}$ transition recently exploited for laser-cooling of CaF; it is shown that this transition is not suitable for laser-cooling of BaF, due to the non-diagonal nature of the FCFs in this system. Special attention is given to the properties of the $A'^2\Delta$ state, which in the case of BaF causes a leak channel, in contrast to CaF and SrF species where this state is energetically above the excited states used in laser-cooling. We also present the dipole moments of the ground and the excited states of the three molecules and the transition dipole moments (TDMs) between the different states., Comment: Minor changes; The following article has been submitted to the Journal of Chemical Physics. After it is published, it will be found at https://publishing.aip.org/resources/librarians/products/journals/