M. Fan

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 $α$-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.

Optical clocks are the apotheosis of precision measurement, but they require frequent maintenance by scientists. The supporting laser systems are a particularly demanding component of these instruments. To reduce complexity and increase robustness we propose an optical clock with trapped alkali-like ions that use the $S_{1/2}\rightarrow D_{3/2}$ electric quadrupole transition. Compared to traditional group-II ion clocks this reduces the number of laser wavelengths required, and uses hyperfine state preparation and readout techniques enabled by the nuclear spin $I=1/2$. We consider $^{225}$Ra$^{+}$ as a candidate system for a clock with three electronic states, and discuss the potential to help realize a transportable optical clock.

We report the first operation of a Ra$^{+}$ optical clock, a promising high-performance clock candidate. The clock uses a single trapped $^{226}$Ra$^{+}$ ion and operates on the $7s\ ^2S_{1/2}\rightarrow$ $6d\ ^2D_{5/2}$ electric quadrupole transition. By self-referencing three pairs of symmetric Zeeman transitions, we demonstrate a frequency instability of 1.1$\times10^{-13}$/$\sqrtτ$, where $τ$ is the averaging time in seconds. The total systematic uncertainty is evaluated to be ${Δν/ ν= 9 \times 10^{-16}}$. Using the clock, we realize the first measurement of the ratio of the $D_{5/2}$ state to the $S_{1/2}$ state Landé $g$-factors: $g_{D}/g_{S}$ = 0.5988053(11). A Ra$^{+}$ optical clock could improve limits on the time variation of the fine structure constant, $\dot α/ α$, in an optical frequency comparison. The ion also has several features that make it a suitable system for a transportable optical clock.

We present an all-optical mass spectrometry technique to identify trapped ions. The new method uses laser-cooled ions to determine the mass of a cotrapped dark ion with a sub-dalton resolution within a few seconds. We apply the method to identify the first controlled synthesis of cold, trapped $\mathrm{RaOH}^+$ and ${\mathrm{RaOCH}_3}^+$. These molecules are promising for their sensitivity to time and parity violations that could constrain sources of new physics beyond the standard model. The nondestructive nature of the mass spectrometry technique may help identify molecular ions or highly charged ions prior to optical spectroscopy. Unlike previous mass spectrometry techniques for small ion crystals that rely on scanning, the method uses a Fourier transform which is inherently broadband and comparatively fast. The technique's speed provides new opportunities for studying state-resolved chemical reactions in ion traps.

The unstable radium nucleus is appealing for probing new physics due to its high mass, octupole deformation and energy level structure. Ion traps, with long hold times and low particle numbers, are excellent for work with radioactive species, such as radium and radium-based molecular ions, where low activity, and hence low total numbers, is desirable. We address the challenges associated with the lack of stable isotopes in a tabletop experiment with a low-activity ($\sim 10 \ μ\mathrm{Ci}$) source where we laser-cool trapped radium ions. With a laser-cooled radium ion we measured the $7p\ ^2P_{1/2}^o$ state's branching fractions to the ground state, $7s\ ^2S_{1/2}$, and a metastable excited state, $6d\ ^2D_{3/2}$, to be $p=0.9104(7)$ and $0.0896(7)$, respectively. With a nearby tellurium reference line we measured the $7s\ ^2S_{1/2} \rightarrow 7p\ ^2P_{1/2}^o$ transition frequency, 640.09663(6) THz.