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An electrostatic hexapole lens is used to manipulate the transverse properties of a beam of barium fluoride molecules from a cryogenic buffer gas source. The spatial distribution of the beam is measured by recording state-selective laser-induced fluorescence on an emccd camera, providing insight into the intensity and transverse position spread of the molecular beam. Although the high mass and unfavorable Stark shift of barium fluoride pose a considerable challenge, the number of molecules in the low-field seeking component of the N=1 state that pass a 4 mm diameter aperture 712 mm behind the source is increased by a factor of 12. Furthermore, it is demonstrated that the molecular beam can be displaced by up to +/-5 mm by moving the hexapole lens. Our measurements agree well with numerical trajectory simulations. We discuss how electrostatic lenses may be used to increase the sensitivity of beam experiments such as the search for the electric dipole moment of the electron.

We demonstrate a novel method to determine the longitudinal phase-space distribution of a cryogenic buffer gas beam of barium-fluoride molecules based on a two-step laser excitation scheme. The spatial resolution is achieved by a transversely aligned laser beam that drives molecules from the ground state $X^2\Sigma^+$ to the $A^2\Pi_{1/2}$ state around 860 nm, while the velocity resolution is obtained by a laser beam that is aligned counter-propagating with respect to the molecular beam and that drives the Doppler shifted $A^2\Pi_{1/2}$ to $D^2\Sigma^+$ transition around 797 nm. Molecules in the $D$-state are detected virtually background-free by recording the fluorescence from the $D-X$ transition at 413 nm. As molecules in the ground state do not absorb light at 797 nm, problems due to due to optical pumping are avoided. Furthermore, as the first step uses a narrow transition, this method can also be applied to molecules with hyperfine structure. The measured phase-space distributions, reconstructed at the source exit, show that the average velocity and velocity spread vary significantly over the duration of the molecular beam pulse. Our method gives valuable insight into the dynamics in the source and helps to reduce the velocity and increase the intensity of cryogenic buffer gas beams. In addition, transition frequencies are reported for the $X-A$ and $X-D$ transitions in barium fluoride with an absolute accuracy below 0.3 MHz., Comment: 7 pages, 6 figures

The toolbox for material characterization has never been richer than today. Great progress with all kinds of particles and interaction methods provide access to nearly all properties of an object under study. However, a tomographic analysis of the subsurface region remains still a challenge today. In this regard, the Muon-Induced X-ray Emission (MIXE) technique has seen rebirth fueled by the availability of high intensity muon beams. We report here a study conducted at the Paul Scherrer Institute (PSI). It demonstrates that the absence of any beam time-structure leads to low pile-up events and a high signal-to-noise ratio (SNR) with less than one hour acquisition time per sample or data point. This performance creates the perspective to open this technique to a wider audience for the routine investigation of non-destructive and depth-sensitive elemental compositions, for example in rare and precious samples. Using a hetero-structured sample of known elements and thicknesses, we successfully detected the characteristic muonic X-rays, emitted during the capture of a negative muon by an atom, and the gamma-rays resulting from the nuclear capture of the muon, characterizing the capabilities of MIXE at PSI. This sample emphasizes the quality of a continuous beam, and the exceptional SNR at high rates. Such sensitivity will enable totally new statistically intense aspects in the field of MIXE, e.g. elemental 3D-tomography and chemical analysis. Therefore, we are currently advancing our proof-of-concept experiments with the goal of creating a full fledged permanently operated user station to make MIXE available to the wider scientific community as well as industry.

We present an investigation of the performance of the relativistic multi-reference Fock-space coupled cluster (FSCC) method for predicting molecular hyperfine structure (HFS) constants, including a thorough computational study to estimate the associated uncertainties. In particular, we considered the $^{19}$F HFS constant in the ground and excited states of BaF. Due to a larger basis set dependence, the uncertainties on the excited state results (16-85%) were found to be significantly larger than those on the ground state constants ($\sim$2%). The ab initio values were compared to the recent experimental results, and good overall agreement within the theoretical uncertainties was found. This work demonstrates the predictive power of the FSCC method and the reliability of the established uncertainty estimates, which can be crucial in cases where the calculated property cannot be directly compared to experiment.

A measurement of the magnitude of the electric dipole moment of the electron (eEDM) larger than that predicted by the Standard Model (SM) of particle physics is expected to have a huge impact on the search for physics beyond the SM. Polar diatomic molecules containing heavy elements experience enhanced sensitivity to parity ($P$) and time-reversal ($T$)-violating phenomena, such as the eEDM and the scalar-pseudoscalar (S-PS) interaction between the nucleons and the electrons, and are thus promising candidates for measurements. The NL-\textit{e}EDM collaboration is preparing an experiment to measure the eEDM and S-PS interaction in a slow beam of cold BaF molecules [Eur. Phys. J. D, 72, 197 (2018)]. Accurate knowledge of the electronic structure parameters, $W_d$ and $W_s$, connecting the eEDM and the S-PS interaction to the measurable energy shifts is crucial for the interpretation of these measurements. In this work we use the finite field relativistic coupled cluster approach to calculate the $W_d$ and $W_s$ parameters in the ground state of the BaF molecule. Special attention was paid to providing a reliable theoretical uncertainty estimate based on investigations of the basis set, electron correlation, relativistic effects and geometry. Our recommended values of the two parameters, including conservative uncertainty estimates, are 3.13 $\pm$ $0.12 \times 10^{24}\frac{\text{Hz}}{e\cdot \text{cm}}$ for $W_d$ and 8.29 $\pm$ 0.12 kHz for $W_s$.

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/

We investigate the merits of a measurement of the permanent electric dipole moment of the electron ($e$EDM) with barium monofluoride molecules, thereby searching for phenomena of CP violation beyond those incorporated in the Standard Model 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 $5\times10^{-30}$ e$\cdot$cm for an $e$EDM is feasible. We describe the rationale, the challenges and the experimental methods envisioned to achieve this target.

The apparent dominance of matter over antimatter in our universe is an obvious and puzzling fact which cannot be adequately explained in present physical frameworks that assume matter-antimatter symmetry at the big bang. However, our present knowledge of starting conditions and of known sources of CP violation are both insufficient to explain the observed asymmetry. Therefore ongoing research on matter-antimatter differences is strongly motivated as well as attempts to identify viable new mechanisms that could create the present asymmetry. Here we concentrate on possible precision experiments at low energies towards a resolution of this puzzle., Comment: 6 pages, 1 figure; accepted for publication in Annalen der Physik (2015)

The lifetime of the metastable 5d$^2$D$_{5/2}$ state has been measured for a single trapped Ba$^+$ ion in a Paul trap in Ultra High Vacuum (UHV) in the 10$^{-10}$ mbar pressure range. A total of 5046 individual periods when the ion was shelved in this state have been recorded. A preliminary value $\tau_{D_{5/2}} = 26.4(1.7)$~s is obtained through extrapolation to zero residual gas pressure., Comment: 6 pages, 6 figures, EXA 2014

We report the first detailed decay studies of trapped metastable (2S) hydrogen. By two-photon excitation of ultracold H samples, we have produced clouds of at least 5x10^7 magnetically trapped 2S atoms at densities greater than 4x10^10 cm^-3 and temperatures below 100 \muK. We derive experimental values for the total 2S-2S two-body loss rate constant in this temperature regime. Our results are in the range of recent theoretical calculations. We also find experimental upper limits on the rate constant for loss due to inelastic 1S-2S collisions., Comment: Submitted to Phys. Rev. A. Pre-print format: 21 pages, 8 figures

We have observed Bose-Einstein condensation (BEC) of trapped atomic hydrogen, and studied it by two-photon spectroscopy of the 1S-2S transition. In these lecture notes we briefly review the history of spin-polarized atomic hydrogen and describe the final steps to BEC. Laser spectroscopy, which probes the difference in mean field energy of the 1S and 2S states, is used to study the condensate, which has a peak density of 4.8e15 cm^-3 and population of 10^9., Comment: 24 pages, 11 figures, contribution to School of Physics "Enrico Fermi", session 140, 1998

We have observed the cold collision frequency shift of the 1S-2S transition in trapped spin-polarized atomic hydrogen. We find $\Delta \nu_{1S-2S} = -3.8(8)\times 10^{-10} n Hz cm^3$, where $n$ is the sample density. From this we derive the 1S-2S s-wave triplet scattering length, $a_{1S-2S}=-1.4(3)$ nm, which is in fair agreement with a recent calculation. The shift provides a valuable probe of the distribution of densities in a trapped sample., Comment: Accepted for publication in PRL, 9 pages, 4 PostScript figures, ReVTeX. Updated connection of our measurement to theoretical work

We report observation of Bose-Einstein condensation of a trapped, dilute gas of atomic hydrogen. The condensate and normal gas are studied by two-photon spectroscopy of the 1S-2S transition. Interactions among the atoms produce a shift of the resonance frequency proportional to density. The condensate is clearly distinguished by its large frequency shift. The peak condensate density is 4.8 +/- 1.1 \times 10^{15} cm^{-3}, corresponding to a condensate population of 10^9 atoms. The BEC transition occurs at about T=50 uK and n=1.8 \times 10^{14} cm^{-3}., Comment: Accepted for publication in PRL; 9 pages, 4 PostScript figures, ReVTeX. Updated discussion of degeneracy effects