45 research outputs found
High accuracy theoretical investigations of CaF, SrF, and BaF and implications for laser-cooling
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 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
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
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
Deceleration of a supersonic beam of SrF molecules to 120 m/s
We report on the deceleration of a beam of SrF molecules from 290 to 120~m/s.
Following supersonic expansion, the molecules in the (, )
low-field seeking states are trapped by the moving potential wells of a
traveling-wave Stark decelerator. With a deceleration strength of 9.6 km/s
we have demonstrated the removal of 85 % of the initial kinetic energy in a 4
meter long modular decelerator. The absolute amount of kinetic energy removed
is a factor 1.5 higher compared to previous Stark deceleration experiments. The
demonstrated decelerator provides a novel tool for the creation of highly
collimated and slow beams of heavy diatomic molecules, which serve as a good
starting point for high-precision tests of fundamental physics
Dynamics of molecular beams in a traveling-wave Stark decelerator
Physicists have observed all the elementary particles predicted by the Standard Model. These particles, however, account for only 5% of the total mass-energy of the Universe. In the quest to solve the mystery of missing matter and to extend our knowledge about nature, a large number of experimental research programs are devoted to find a glimpse of New Physics. Table-top high precision measurements on molecules can contribute to these efforts in a manner complementary to high-energy experiments at colliders. In this thesis, we describe the operation of a traveling-wave Stark decelerator. This device is designed and constructed in order to slow down heavy polar molecules for various future explorations. Deceleration is achieved by manipulation of the molecules in controllable electric fields. We demonstrate in an experiment the successful operation of the Stark decelerator by slowing down a beam of SrF molecules to one-third of their initial velocity, thus removing almost 90% of the initial kinetic energy. We also reveal limiting conditions for this process. These results are of importance for many exciting experiments using heavy molecules in the near future. One relevant and promising example of such experiments is the search for a permanent electric dipole moment of the electron