Marianna S. Safronova

Engineering large-scale quantum computers which simultaneously provide high-fidelity quantum operations, low memory errors, low crosstalk, and reasonable resource usage remains an outstanding challenge across quantum computing platforms. In trapped ions, progress has largely focused on alkaline-earth and ytterbium ions, whose simple electronic structures facilitate control over their internal state. Here we investigate singly-ionized yttrium ($^{89}\mathrm{Y}^+$), a two-valence-electron ion whose ground-state manifold hosts a nuclear-spin qubit and which also features a variety of low-lying metastable manifolds, for applications in quantum information processing. Because experimental data are limited, we perform high-resolution laser-induced fluorescence spectroscopy to measure the hyperfine structure of several low-lying levels, and carry out comprehensive electronic structure calculations to determine lifetimes, transition matrix elements, and hyperfine coefficients for manifolds addressable with visible, near-visible, or infrared wavelengths. Using these results, we analyze schemes for qubit storage, initialization, readout, leakage mitigation, and single- and two-qubit gates. These results position $^{89}\mathrm{Y}^+$ as a uniquely capable next-generation trapped-ion qubit, combining field-insensitive nuclear-spin or clock-qubit storage with spectrally isolated transitions for operations.

Single ion optical clocks have shown systematic frequency uncertainties below $10^{-18}$, but typically require more than one week of averaging to achieve a corresponding statistical uncertainty. This time can be reduced with longer probe times, but comes at the cost of a higher time-dilation shift due to motional heating of the ions in the trap. We show that sympathetic ground-state cooling using electromagnetically-induced transparency (EIT) of an \Al clock ion via a co-trapped \Ca ion during clock interrogation suppresses the heating of the ions. \Al can be kept close to the motional ground state, independent from the chosen interrogation time, at a relative time dilation shift of $(-1.69\pm0.20)\times10^{-18}$. The \Ca cooling light introduces an additional light shift on the \Al clock transition of $(-9.27\pm 1.03)\times10^{-18}$. We project that the uncertainty of this light shift can be further reduced by nearly an order of magnitude. This sympathetic cooling enables seconds of interrogation time with $10^{-19}$ motional and cooling laser-induced uncertainties for \Al and can be employed in other ion clocks as well.

Optical transitions of highly charged ions can be very sensitive to hypothetical beyond-the-Standard-Model phenomena. Those near the $5s-4f$ level crossing, where the $5s$ and $4f$ are degenerate are especially promising. We present predictions from atomic theory and measurements of Os$^{15,16,17+}$ at an electron beam ion trap for identification of several transitions suitable for searches for a hypothetical fifth force and possible violations of local Lorentz invariance. The electric quadrupole (E2) transitions of Os$^{16+}$ that were found are especially suitable for frequency metrology due to their small linewidth of 44 $μ$Hz. Our calculations show the need for including enough inner-shell excitations to predict transition rates between configurations, which can otherwise be overestimated. Ultimately, the predicted interconfiguration transitions were too weak to be detected.

We measured the $g$-factor of the excited state $^3\text{P}_1$ in $\text{Ca}^{14+}$ ion to be $g = 1.499032(6)$ with a relative uncertainty of $4\times10^{-6}$. The magnetic field magnitude is derived from the Zeeman splitting of a $\text{Be}^+$ ion, co-trapped in the same linear Paul trap as the highly charged $\text{Ca}^{14+}$ ion. Furthermore, we experimentally determined the second-order Zeeman coefficient $C_2$ of the $^3\text{P}_0$ - $^3\text{P}_1$ clock transition. For the $m_J=0\rightarrow m_{J'}=0$ transition, we obtain $C_2 = 0.39\pm0.04\text{HzmT}^{-2}$, which is to our knowledge the smallest reported for any atomic transition to date. This confirms the predicted low sensitivity of highly charged ions to higher-order Zeeman effects, making them ideal candidates for high-precision optical clocks. Comparison of the experimental results with our state-of-the art electronic structure calculations shows good agreement, and demonstrates the significance of the frequency-dependent Breit contribution, negative energy states and QED effects on magnetic moments.

We improve by a factor of 4-20 the energy accuracy of the strongest soft X-ray transitions of Fe XVII ions by resonantly exciting them in an electron beam ion trap with a monochromatic beam at the P04 beamline of the PETRA III synchrotron facility. By simultaneously tracking instantaneous photon-energy fluctuations with a high-resolution photoelectron spectrometer, we minimize systematic uncertainties down to 10-15 meV, or velocity equivalent $\pm\sim$5 km s$^{-1}$ in their rest energies, substantially improving our knowledge of this key astrophysical ion. Our large-scale configuration-interaction computations include more than four million relativistic configurations and agree with the experiment at a level without precedent for a 10-electron system. Thereby, theoretical uncertainties for interelectronic correlations become far smaller than those of quantum electrodynamics (QED) corrections. The present QED benchmark strengthens our trust in future calculations of many other complex atomic ions of interest to astrophysics, plasma physics, and for the development of optical clocks with highly charged ions.

Laser cooling of single atoms in optical tweezers is a prerequisite for neutral atom quantum computing and simulation. Resolved sideband cooling comprises a well-established method for efficient motional ground-state preparation, but typically requires careful cancellation of light shifts in so-called magic traps. Here, we study a novel laser cooling scheme which overcomes such constraints, and applies when the ground-state of a narrow cooling transition is trapped stronger than the excited state. We demonstrate our scheme, which exploits sequential addressing of red sideband transitions via frequency chirping of the cooling light, at the example of $^{88}$Sr atoms, and report ground-state populations compatible with recent experiments in magic tweezers. The scheme also induces light-assisted collisions, which are key to the assembly of large atom arrays. Our work enriches the toolbox for tweezer-based quantum technology, also enabling applications for tweezer-trapped molecules and ions that are incompatible with resolved sideband cooling conditions.

We propose a many-ion optical atomic clock based on three-dimensional Coulomb crystals of order one thousand Sn$^{2+}$ ions confined in a linear RF Paul trap. Sn$^{2+}$ has a unique combination of features that is not available in previously considered ions: a $^1$S$_0$ $\leftrightarrow$ $^3$P$_0$ clock transition between two states with zero electronic and nuclear angular momentum (I = J = F = 0) making it immune to nonscalar perturbations, a negative differential polarizability making it possible to operate the trap in a manner such that the two dominant shifts for three-dimensional ion crystals cancel each other, and a laser-accessible transition suitable for direct laser cooling and state readout. We present calculations of the differential polarizability, other relevant atomic properties, and the motion of ions in large Coulomb crystals, in order to estimate the achievable accuracy and precision of Sn$^{2+}$ Coulomb-crystal clocks.

A wide range of quantum sensing technologies are rapidly being integrated into the experimental portfolio of the high energy physics community. Here we focus on sensing with atomic interferometers; mechanical devices read out with optical or microwave fields; precision spectroscopic methods with atomic, nuclear, and molecular systems; and trapped atoms and ions. We give a variety of detection targets relevant to particle physics for which these systems are uniquely poised to contribute. This includes experiments at the precision frontier like measurements of the electron dipole moment and electromagnetic fine structure constant and searches for fifth forces and modifications of Newton's law of gravity at micron-to-millimeter scales. It also includes experiments relevant to the cosmic frontier, especially searches for gravitional waves and a wide variety of dark matter candidates spanning heavy, WIMP-scale, light, and ultra-light mass ranges. We emphasize here the need for more developments both in sensor technology and integration into the broader particle physics community.

We report a precise determination of the lifetime of the (4p)$^2$P$_{3/2}$ state of $^{40}$Ca$^+$, $τ_{\textrm{P}_{3/2}}=6.639(42)$ ns, using a combination of measurements of the induced light shift and scattering rate on a single trapped ion. Good agreement with the result of a recent high-level theoretical calculation, $6.69(6)$ ns [Safronova et al., PRA 83, 012503 (2011)], but a 6-$σ$ discrepancy with the most precise previous experimental value, $6.924(19)$ ns [Jin et al., PRL 70, 3213 (1993)] is found. To corroborate the consistency and accuracy of the new measurements, relativistically corrected ratios of reduced-dipole-matrix elements are used to directly compare our result with a recent result for the P$_{1/2}$ state, yielding a good agreement. The application of the present method to precise determinations of radiative quantities of molecular systems is discussed.

Questioning the presumably most basic assumptions about the structure of space and time has revolutionized our understanding of Nature. State-of-the-art atomic clocks make it possible to precisely test fundamental symmetry properties of spacetime, and search for physics beyond the standard model at low energy scales of just a few electron volts. Here, we experimentally demonstrate for the first time agreement of two single-ion clocks at the $10^{-18}$ level and directly confirm the validity of their uncertainty budgets over a half-year long comparison period. The two clock ions are confined in separate ion traps with quantization axes aligned along nonparallel directions. Hypothetical Lorentz symmetry violations would lead to sidereal modulations of the frequency offset. From the absence of such modulations at the $10^{-19}$ level we deduce stringent limits on Lorentz symmetry violation parameters for electrons in the range of $10^{-21}$, improving previous limits by two orders of magnitude.

We present visible spectra of Ag-like ($4d^{10}4f$) and Cd-like ($4d^{10}4f^2$) ions of Ho (atomic number $Z=67$), Er (68), and Tm (69) observed with a compact electron beam ion trap. For Ag-like ions, prominent emission corresponding to the M1 transitions between the ground state fine structure splitting $4f_{5/2}$--$4f_{7/2}$ is identified. For Cd-like ions, several M1 transitions in the ground state configuration are identified. The transition wavelength and the transition probability are calculated with the relativistic many-body perturbation theory and the relativistic CI + all-order approach. Comparisons between the experiments and the calculations show good agreement.

In many applications a source of the black-body radiation (BBR) can be highly anisotropic. This leads to the BBR shift that depends on tensor polarizability and on the projection of the total angular momentum of ions and atoms in a trap. We derived formula for the anisotropic BBR shift and performed numerical calculations of this effect for Ca$^+$ and Yb$^+$ transitions of experimental interest. These ions used for a design of high-precision atomic clocks, fundamental physics tests such as search for the Lorentz invariance violation and space-time variation of the fundamental constants, and quantum information. Anisotropic BBR shift may be one of the major systematic effect in these experiments.