David B. Hume

Scaling trapped-ion quantum sensors from single ions to large ensembles is a key challenge for next-generation precision measurements. At the same time, many ion species of interest for optical clocks and tests of fundamental physics lack closed cycling transitions required for direct laser cooling and state detection. Collective quantum logic spectroscopy addresses both limitations by coupling an ensemble of sensor, or spectroscopy, ions to one or more logic ions that provide sympathetic cooling and state readout. Here, we establish the fundamental performance limits and operating regimes of this protocol, identifying how the interaction strength, interrogation time, and logic-ensemble size govern sensitivity, dynamic range, and robustness to experimental imperfections. We show that quantum-limited sensitivity can be retained even with a single logic ion, while increasing the number of logic ions substantially improves readout efficiency and robustness. Beyond precision metrology, the same collective interface enables many-body measurements relevant to quantum information processing, including parity measurements and stabilizer-like syndrome extraction. Our results establish collective quantum logic spectroscopy as a scalable framework for optical clocks, quantum-enhanced sensing, and trapped-ion quantum information processing.

Optical atomic clocks have been rapidly developing in recent decades, resulting in major improvements in both precision and accuracy. As a result, they have become instrumental in multiple areas of applied and fundamental research. Despite all atomic frequency references having more than two energy-levels, the commonly used model for evaluating their ultimate limits assumes a two-level atom. This leads to frequency interrogation protocols and theoretical stability bounds that are suboptimal for a true multi-level atom. The most fundamental stability bound assumes two noise sources - quantum projection noise and spontaneous decay from the excited state. In this work, we analyze a model that includes these noise types and is generalized beyond the two-level assumption, where spontaneous decay can branch to more than a single ground state. This model allows for detection and exclusion of atomic frequency interrogations in which the atom decayed, leading to a frequency stability improvement of up to $\approx 4.5 \text{ dB}$ compared with the two-level model. Furthermore, we identify an even greater stability enhancement of $\approx 5.4 \text{ dB}$ for frequency comparisons between atoms in an odd parity Bell state. These enhancements are particularly relevant for the numerous trapped-ion optical clock species that operate close to lifetime-limited stability. We calculate new stability limits for those cases and provide a detailed experimental protocol for frequency interrogation with an $^{27}\text{Al}^{+}$ optical ion clock.

We report a single-ion optical atomic clock with fractional frequency uncertainty of $5.5\times10^{-19}$ and fractional frequency stability of $3.5 \times10^{-16}/\sqrt{τ/\mathrm{s}}$, based on quantum logic spectroscopy of a single $^{27}$Al$^+$ ion. A co-trapped $^{25}$Mg$^+$ ion provides sympathetic cooling and quantum logic readout of the $^{27}$Al$^+$ $^1$S$_0\leftrightarrow^3$P$_0$ clock transition. A Rabi probe duration of 1 s, enabled by laser stability transfer from a remote cryogenic silicon cavity across a 3.6 km fiber link, results in a threefold reduction in instability compared to previous $^{27}$Al$^+$ clocks. Systematic uncertainties are lower due to an improved ion trap electrical design, which reduces excess micromotion, and a new vacuum system, which reduces collisional shifts. We also perform a direction-sensitive measurement of the ac magnetic field due to the RF ion trap, eliminating systematic uncertainty due to field orientation.

In quantum logic spectroscopy (QLS), one species of trapped ion is used as a sensor to detect the state of an otherwise inaccessible ion species. This extends precision measurements to a broader class of atomic and molecular systems for applications like atomic clocks and tests of fundamental physics. Here, we develop a new technique based on a Schrödinger cat interferometer to address the problem of scaling QLS to larger ion numbers. We demonstrate the basic features of this method using various combinations of $^{25}\text{Mg}^+$ logic ions and $^{27}\text{Al}^+$ spectroscopy ions. We observe higher detection efficiency by increasing the number of $^{25}\text{Mg}^+$ ions. Applied to multiple $^{27}\text{Al}^+$, this method will improve the stability of high-accuracy optical clocks and could enable Heisenberg-limited QLS.

Laser cooling and trapping of atoms and atomic ions has led to numerous advances including the observation of exotic phases of matter, development of exquisite sensors and state-of-the-art atomic clocks. The same level of control in molecules could also lead to profound developments such as controlled chemical reactions and sensitive probes of fundamental theories, but the vibrational and rotational degrees of freedom in molecules pose a formidable challenge for controlling their quantum mechanical states. Here, we use quantum-logic spectroscopy (QLS) for preparation and nondestructive detection of quantum mechanical states in molecular ions. We develop a general technique to enable optical pumping and preparation of the molecule into a pure initial state. This allows for the observation of high-resolution spectra in a single ion (here CaH+) and coherent phenomena such as Rabi flopping and Ramsey fringes. The protocol requires a single, far-off resonant laser, which is not specific to the molecule, so that many other molecular ions, including polyatomic species, could be treated with the same methods in the same apparatus by changing the molecular source. Combined with long interrogation times afforded by ion traps, a broad range of molecular ions could be studied with unprecedented control and precision, representing a critical step towards proposed applications, such as precision molecular spectroscopy, stringent tests of fundamental physics, quantum computing, and precision control of molecular dynamics.