Nuclear charge radius differences in the silver isotopic chain have been reported through different combinations of experiment and theory, exhibiting a tension of two combined standard errors. This study investigates this issue by combining high-accuracy calculations for six low-lying states of atomic silver with an improved measurement of the 5s2S1/2−5p2P3/2 transition optical isotope shift. Our calculations predict measured electronic transition energies in Ag at the 0.3% level, the highest accuracy achieved in this system so far. We calculate electronic isotope shift factors by employing analytical response relativistic coupled-cluster theory and find that a consistent charge radius difference between Ag107,109 is returned when combining our calculations with the available optical isotope shift measurements. We therefore recommend an improved value for the mean-squared charge radius difference between Ag107 and Ag109 as 0.207(6) fm2, within one combined error from the value derived from muonic Ag experiments, and an updated set of charge radii differences across the isotopic chain. Published by the American Physical Society 2024

The electron's electric dipole moment (eEDM) can be determined by polarizing the spin of an atom or a molecule and then measuring the spin precession frequency in an applied electric field. Radiation is used to polarize the spin and then analyze the precession angle, and the measurement is often sensitive to the polarization of this radiation. We show how systematic errors can arise when both the polarization of the radiation and the magnitude of the electric field are imperfectly controlled. We derive approximate analytical expressions for these errors, confirm their accuracy numerically, and show how they can be corrected empirically. We consider spin manipulation using single-photon pulses, Raman pulses, and stimulated Raman adiabatic passage (STIRAP), and we show that STIRAP provides better immunity to these systematic errors. An experimental study of these errors partly supports our findings but also reveals another potential error that is not captured by this analysis.

Cryogenic buffer gas beams are central to many cold molecule experiments. Here, we use absorption and fluorescence spectroscopy to directly compare molecular beams of AlF, CaF, MgF and YbF molecules, produced by chemical reaction of laser ablated atoms with fluorine rich reagents. The beam brightness for AlF is measured as 2×1012 molecules per steradian per pulse in a single rotational state, comparable to an Al atomic beam produced in the same setup. The CaF, MgF and YbF beams show an order of magnitude lower brightness than AlF and far below the brightness of Ca and Yb beams. The addition of either NF3 or SF6 to the cell extinguishes the Al atomic beam, but has a minimal effect on the Ca and Yb beams. NF3 reacts more efficiently than SF6, as a significantly lower flow rate is required to maximise the molecule production, which is particularly beneficial for long-term stability of the AlF beam. We use NO as a proxy for the reactant gas as it can be optically detected. We demonstrate that a cold, rotationally pure NO beam can be generated by laser desorption, thereby gaining insight into the dynamics of the reactant gas inside the buffer gas cell.

In this work, we explore the role of chemical reactions on the properties of buffer gas cooled molecular beams. In particular, we focus on scenarios relevant to the formation of AlF and CaF via chemical reactions between the Ca and Al atoms ablated from a solid target in an atmosphere of a fluorine-containing gas, in this case, SF6 and NF3. Reactions are studied following an ab initio molecular dynamics approach, and the results are rationalized following a tree-shaped reaction model based on Bayesian inference. We find that NF3 reacts more efficiently with hot metal atoms to form monofluoride molecules than SF6. In addition, when using NF3, the reaction products have lower kinetic energy, requiring fewer collisions to thermalize with the cryogenic helium. Furthermore, we find that the reaction probability for AlF formation is much higher than for CaF across a broad range of kinetic temperatures.

Isotope shifts (ISs) in atomic energy levels are sensitive probes of nuclear structure and new physics beyond the Standard Model. We present an analysis of the ISs of the cadmium atom (Cd I) and singly charged cadmium ion (Cd II). ISs of the 229 nm, 326 nm, 361 nm and 480 nm lines of Cd I are measured with a variety of techniques; buffer-gas-cooled beam spectroscopy, capturing atoms in a magneto-optic-trap, and optical pumping. IS constants for the D1 and D2 lines of Cd II are calculated with high accuracy by employing analytical response relativistic coupled-cluster theory in the singles, doubles and triples approximations. Combining the calculations for Cd II with experiments, we infer IS constants for all low-lying transitions in Cd I. We benchmark these constants as calculated via different many-body methods. Our calculations for Cd II enable nuclear charge radii of Cd isotopes to be extracted with unprecedented accuracy. The combination of our precise calculations and measurements shows that King Plots for Cd I can improve the state-of-theart sensitivity to a new heavy boson by up to two orders of magnitude.

We report on hyperfine-resolved laser spectroscopy of the A(2)Pi <- X-2 sigma(+) transition of magnesium monofluoride (MgF), relevant for laser cooling. We recorded 25 rotational transitions with an absolute accuracy of better than 20 MHz, assigned 56 hyperfine lines, and determined precise rotational, fine, and hyperfine structure parameters for the A(2)Pi state. The radiative lifetime of the A(2)Pi state was determined to be 7.2(3) ns, in good agreement with ab initio calculations. The transition isotope shift between bosonic isotopologues of the molecule is recorded and compared to predicted values within the Born-Oppenheimer approximation. We measured the Stark effect of selected rotational lines of the A(2)Pi <- X-2 sigma(+) transition by applying electric fields of up to 10.6 kV cm(-1) and determined the permanent electric dipole moments of (MgF)-Mg-24 in its ground X-2 sigma???????(+) and first excited A(2)Pi states to be mu(X) = 2.88(20) D and mu(A) = 3.20(22) D, respectively. Based on these measurements, we caution for potential losses from the optical cycling transition due to electric field induced parity mixing in the excited state. In order to scatter 10(4) photons, the electric field must be controlled to below 1 V cm(-1). (C) 2022 Author(s)& nbsp;

We report on hyperfine-resolved laser spectroscopy of the A2Π ← X2Σ+ transition of magnesium monofluoride (MgF), relevant for laser cooling. We recorded 25 rotational transitions with an absolute accuracy of better than 20 MHz, assigned 56 hyperfine lines, and determined precise rotational, fine, and hyperfine structure parameters for the A2Π state. The radiative lifetime of the A2Π state was determined to be 7.2(3) ns, in good agreement with ab initio calculations. The transition isotope shift between bosonic isotopologues of the molecule is recorded and compared to predicted values within the Born-Oppenheimer approximation. We measured the Stark effect of selected rotational lines of the A2Π ← X2Σ+ transition by applying electric fields of up to 10.6 kV cm-1 and determined the permanent electric dipole moments of 24MgF in its ground X2Σ+ and first excited A2Π states to be μX = 2.88(20) D and μA = 3.20(22) D, respectively. Based on these measurements, we caution for potential losses from the optical cycling transition due to electric field induced parity mixing in the excited state. In order to scatter 104 photons, the electric field must be controlled to below 1 V cm-1.

Aluminium monofluoride (AlF) is a promising candidate for laser cooling and trapping at high densities. We show efficient production of AlF in a bright, pulsed cryogenic buffer gas beam, and demonstrate rapid optical cycling on the Q rotational lines of the $A^1\Pi \leftrightarrow X^1\Sigma^+ $ transition. We measure the brightness of the molecular beam to be $>10^{12}$ molecules per steradian per pulse in a single rotational state and present a new method to determine its velocity distribution in a single shot. The photon scattering rate of the optical cycling scheme is measured using three different methods, and is compared to theoretical predictions of the optical Bloch equations and a simplified rate equation model. Despite the large number of Zeeman sublevels (up to 216 for the Q(4) transition) involved, a high scattering rate of at least $17(2)\times 10^6$ s$^{-1}$ can be sustained using a single, fixed-frequency laser without the need to modulate the polarisation. We deflect the molecular beam using the radiation pressure force and measure an acceleration of $8.7(1.5)\times 10^5$ m/s$^2$. We demonstrate that losses from the optical cycle due to vibrational branching to $X^1\Sigma^+, v''=1$ can be addressed efficiently with a single repump laser. Further, we investigate two other loss channels, parity mixing by stray electric fields and photo-ionisation. The upper bounds for these effects are sufficiently low to allow loading into a magneto optical trap.

The electric dipole moment of the electron (eEDM) can be measured with high precision using heavy polar molecules. In this paper, we report on a series of new techniques that have improved the statistical sensitivity of the YbF eEDM experiment. We increase the number of molecules participating in the experiment by an order of magnitude using a carefully designed optical pumping scheme. We also increase the detection efficiency of these molecules by another order of magnitude using an optical cycling scheme. In addition, we show how to destabilise dark states and reduce backgrounds that otherwise limit the efficiency of these techniques. Together, these improvements allow us to demonstrate a statistical sensitivity of 1.8 × 10 −28 e cm after one day of measurement, which is 1.2 times the shot-noise limit. The techniques presented here are applicable to other high-precision measurements using molecules.

We demonstrate a trap that confines polarizable particles around the antinode of a standing-wave microwave field. The trap relies only on the polarizability of the particles far from any resonances, so can trap a wide variety of atoms and molecules in a wide range of internal states, including the ground state. The trap has a volume of about 10 cm$^3$, and a depth approaching 1 K for many polar molecules. We measure the trap properties using $^{7}$Li atoms, showing that when the input microwave power is 610 W, the atoms remain trapped with a $1/e$ lifetime of 1.76(12) s, oscillating with an axial frequency of 28.55(5) Hz and a radial frequency of 8.81(8) Hz. The trap could be loaded with slow molecules from a range of available sources, and is particularly well suited to sympathetic cooling and evaporative cooling of molecules.

We present an experiment based on a fibered Mach-Zehnder interferometer, with the aim of familiarizing students with fibered optics and interferometry, and of improving their understanding of optical amplification. The laboratory project has two parts. In the first, students modulate the optical path of the interferometer to study the spectra of light sources via Fourier Transform Spectroscopy. In the second, an optical amplifier is placed in one or both arms of the interferometer. The set-up uses monomode, polarization-maintaining fibers that propagate light with a wavelength of 1.5 μm. Here, we describe the set-up and the analysis of the measurements, and we present results from student reports.