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We report lifetime measurements of the metastable $6d\, ^2\!D_{5/2}$ and $6d\, ^2\!D_{3/2}$ states of the radium ion. The measured lifetimes, $\tau_{5} = $ 303.8(1.5) ms and $\tau_{3} = $ 642(9) ms, are important for optical frequency standards and for benchmarking high-precision relativistic atomic theory. Independent of the reported measurements, the $D$ state lifetimes were calculated using the coupled-cluster single double triple method, in which the coupled-cluster equations for both core and valence triple excitations were solved iteratively. The method was designed for precise prediction of atomic properties, especially for heavy elements, where relativistic and correlation corrections become large, making their treatment more challenging. This work presents the first benchmark comparisons of the method for transition properties. Our prediction agrees with experimental values within the uncertainties. The ability to accurately predict the atomic properties of heavy elements is important for many applications, from tests of fundamental symmetries to the development of optical clocks., Comment: 11 pages, 8 figures

We report on spectroscopy of the low-lying electronic transitions in $^{224}$Ra$^+$. The ion's low charge to mass ratio and convenient wavelengths make $^{224}$Ra$^+$ a promising optical clock candidate. We measured the frequencies of the the $^2{S}_{1/2} \ $$\leftrightarrow$$\ ^2{P}_{1/2}$ cooling transition, the $^2{S}_{1/2}\ $$\leftrightarrow$$\ ^2{D}_{5/2}$ clock transition, the $^2{D}_{3/2} \ $$\leftrightarrow$$\ ^2{P}_{3/2}$ electric dipole transition, and the $^2{D}_{5/2} \ $$\leftrightarrow$$\ ^2{P}_{3/2}$ cleanout transition. From these measurements we calculate the frequencies of the $^2{D}_{3/2}\ $$\leftrightarrow$$\ ^2{P}_{1/2}$ repump transition, the $^2{S}_{1/2} \ $$\leftrightarrow$$\ ^2{D}_{3/2}$ electric quadrupole transition, and the $^2{S}_{1/2} \ $$\leftrightarrow$$\ ^2{P}_{3/2}$ electric dipole transition., Comment: 5 pages, 8 figures

Radium-225 (nuclear spin $I=1/2$) ions possess electronic hyperfine transitions that are first-order insensitive to magnetic field noise, which is advantageous for optical clocks and quantum information science. We report on laser cooling and trapping of radium-225 ions and hyperfine splitting measurements of the ion's $7s$ $^2S_{1/2}$, $7p$ $^2P_{1/2}$, and $6d$ $^2D_{3/2}$ states. We measured the ground state hyperfine constant, $A(^2S_{1/2}) = -27.684511056(9)\ \mathrm{GHz}$, and the quadratic Zeeman coefficient, $C_2 = 142.3(10)\ \mathrm{Hz\ G}^{-2}$, of the $^2S_{1/2} (F=0, m_F = 0) \leftrightarrow~^2S_{1/2} (F=1, m_{F} = 0)$ transition. We also measured the hyperfine constants of the $^2P_{1/2}$ state, $A(^2P_{1/2}) = -5.447(4)\ \mathrm{GHz}$, and the $^2D_{3/2}$ state, $A(^2D_{3/2}) = -619.7(11)\ \mathrm{MHz}$., Comment: 5 pages, 4 figures

We report laser cooling and trapping of $^{224}$Ra$^+$ ions. This was realized via two-step photoionization loading of radium into an ion trap. A robust source for $^{224}$Ra atoms, which have a 3.6-day half-life, was realized with an effusive oven containing $^{228}$Th, which has a 1.9-yr half-life, which continuously generates $^{224}$Ra via its $\alpha$-decay. We characterized the efficacy of this source and found that after depleting built-up radium the thorium decay provides a continuous source of radium atoms suitable for ion trapping. The vacuum system has been sealed for more than 6 months and continues to trap ions on demand. We also report a measurement of the $^{224}$Ra $7s^2\ ^1$S$_0 \rightarrow 7s7p\ ^1$P$_1$ transition frequency: 621 043 830(60) MHz, which is helpful for efficient photoionization. With this measurement and previous isotope shift measurements we find that the frequency of the same transition in $^{226}$Ra is 621 037 830(60) MHz, which disagrees with the most precise measurement, 621 038 489(15) MHz, which is used for the recommended value in the National Institute of Standards and Technology Atomic Spectra Database., Comment: 6 pages, 6 figures

Molecules containing short-lived, radioactive nuclei are uniquely positioned to enable a wide range of scientific discoveries in the areas of fundamental symmetries, astrophysics, nuclear structure, and chemistry. Recent advances in the ability to create, cool, and control complex molecules down to the quantum level, along with recent and upcoming advances in radioactive species production at several facilities around the world, create a compelling opportunity to coordinate and combine these efforts to bring precision measurement and control to molecules containing extreme nuclei. In this manuscript, we review the scientific case for studying radioactive molecules, discuss recent atomic, molecular, nuclear, astrophysical, and chemical advances which provide the foundation for their study, describe the facilities where these species are and will be produced, and provide an outlook for the future of this nascent field.

The Ra EDM experiment uses a pair of high voltage electrodes to search for the atomic electric dipole moment of $^{225}$Ra. We use identical, plane-parallel electrodes with a primary high gradient surface of 200 mm$^2$ to generate reversible DC electric fields. Our statistical sensitivity is linearly proportional to the electric field strength in the electrode gap. We adapted surface decontamination and processing techniques from accelerator physics literature to chemical polish and clean a suite of newly fabricated large-grain niobium and grade-2 titanium electrodes. Three pairs of niobium electrodes and one pair of titanium electrodes were discharge-conditioned with a custom high voltage test station at electric field strengths as high as $+52.5$ kV/mm and $-51.5$ kV/mm over electrode gap sizes ranging from 0.4 mm to 2.5 mm. One pair of large-grain niobium electrodes was discharge-conditioned and validated to operate at $\pm 20$ kV/mm with steady-state leakage current $\leq 25$ pA ($1\sigma$) and a polarity-averaged $98 \pm 19$ discharges per hour. These electrodes were installed in the Ra EDM experimental apparatus, replacing a copper electrode pair, and were revalidated to $\pm 20$ kV/mm. The niobium electrodes perform at an electric field strength 3.1 times larger than the legacy copper electrodes and are ultimately limited by the maximum output of our 30 kV bipolar power supply., Comment: 16 pages, 11 figures