Christian Schneider

Dipole-phonon quantum logic (DPQL) leverages the interaction between polar molecular ions and the motional modes of a trapped-ion Coulomb crystal to provide a potentially scalable route to quantum information science. Here, we study a class of candidate molecular ions for DPQL, the cationic alkaline-earth monoxides and monosulfides, which possess suitable structure for DPQL and can be produced in existing atomic ion experiments with little additional complexity. We present calculations of DPQL operations for one of these molecules, CaO$^+$, and discuss progress towards experimental realization. We also further develop the theory of DPQL to include state preparation and measurement and entanglement of multiple molecular ions.

We study an excited atom-polar molecular ion chemical reaction (Ca$^*$ + BaCl$^+$) at low temperature by utilizing a hybrid atom-ion trapping system. The reaction rate and product branching fractions are measured and compared to model calculations as a function of both atomic quantum state and collision energy. At the lowest collision energy we find that the chemical dynamics dramatically differ from capture theory predictions and are primarily dictated by the radiative lifetime of the atomic quantum state instead of the underlying excited-state interaction potential. We provide a simple rule for calculating at what temperature this regime, where the collision complex lifetime is longer than the radiative lifetime of the quantum state, is reached. This effect, which greatly suppresses the reactivity of short-lived excited states, provides a means for directly probing reaction range. It also naturally suppresses unwanted chemical reactions in hybrid trapping experiments, allowing longer molecular ion coherence and interrogation times.

$^{229}$Th is the only nucleus currently under investigation for the development of a nuclear optical clock (NOC) of ultra-high accuracy. The insufficient knowledge of the first nuclear excitation energy of $^{229}$Th has so far hindered direct nuclear laser spectroscopy of thorium ions and thus the development of a NOC. Here, a nuclear laser excitation scheme is detailed, which makes use of thorium atoms instead of ions. This concept, besides potentially leading to the first nuclear laser spectroscopy, would determine the isomeric energy to 40 $μ$eV resolution, corresponding to 10 GHz, which is a $10^4$ times improvement compared to the current best energy constraint. This would determine the nuclear isomeric energy to a sufficient accuracy to allow for nuclear laser spectroscopy of individual thorium ions in a Paul trap and thus the development of a single-ion nuclear optical clock.

We demonstrate an ion shuttling technique for high-resolution control of atom-ion collision energy by translating an ion held within a radio-frequency trap through a magneto-optical atom trap. The technique is demonstrated both experimentally and through numerical simulations, with the experimental results indicating control of ion kinetic energies from $0.05-1$ K with a fractional resolution of $\sim10$ and the simulations demonstrating that kinetic energy control up to $120$ K with a maximum predicted resolution of $\sim100$ is possible, offering order-of-magnitude improvements over most alternative techniques. Lastly, we perform a proof-of-principle chemistry experiment using this technique and outline how the method may be refined in the future and applied to the study of molecular ion chemistry.

Hypermetallic alkaline earth (M) oxides of formula MOM have been studied under plasma conditions that preclude insight into their formation mechanism. We present here the application of emerging techniques in ultracold physics to the synthesis of a mixed hypermetallic oxide, BaOCa$^+$. These methods, augmented by high-level electronic structure calculations, permit detailed investigation of the bonding and structure, as well as the mechanism of its formation via the barrierless reaction of Ca $(^3P_J)$ with BaOCH$_{3}^+$. Further investigations of the reaction kinetics as a function of collision energy over the range 0.005 K to 30 K and of individual Ca fine-structure levels compare favorably with calculations based on long-range capture theory.

Sympathetic cooling of trapped ions through collisions with neutral buffer gases is critical to a variety of modern scientific fields, including fundamental chemistry, mass spectrometry, nuclear and particle physics, and atomic and molecular physics. Despite its widespread use over four decades, there remain open questions regarding its fundamental limitations. To probe these limits, here we examine the steady-state evolution of up to ten barium ions immersed in a gas of three-million laser-cooled calcium atoms. We observe and explain the emergence of nonequilibrium behavior as evidenced by bifurcations in the ion steady-state temperature, parameterized by ion number. We show that this behavior leads to limitations in creating and maintaining translationally cold samples of trapped ions using neutral-gas sympathetic cooling. These results may provide a route to studying nonequilibrium thermodynamics.

Recently, we reported an ion trap experiment with an integrated time-of-flight mass spectrometer (TOFMS) [Phys. Rev. Appl. 2, 034013 (2014)] focussing on the improvement of mass resolution and detection limit due to sample preparation at millikelvin temperatures. The system utilizes a radio-frequency (RF) ion trap with asymmetric drive for storing and manipulating laser-cooled ions and features radial extraction into a compact $275$ mm long TOF drift tube. The mass resolution exceeds $m / Δm = 500$, which provides isotopic resolution over the whole mass range of interest in current experiments and constitutes an improvement of almost an order of magnitude over other implementations. In this manuscript, we discuss the experimental implementation in detail, which is comprised of newly developed drive electronics for generating the required voltages to operate RF trap and TOFMS, as well as control electronics for regulating RF outputs and synchronizing the TOFMS extraction.

Mass spectrometry is used in a wide range of scientific disciplines including proteomics, pharmaceutics, forensics, and fundamental physics and chemistry. Given this ubiquity, there is a worldwide effort to improve the efficiency and resolution of mass spectrometers. However, the performance of all techniques is ultimately limited by the initial phase-space distribution of the molecules being analyzed. Here, we dramatically reduce the width of this initial phase-space distribution by sympathetically cooling the input molecules with laser-cooled, co-trapped atomic ions, improving both the mass resolution and detection efficiency of a time-of-flight mass spectrometer by over an order of magnitude. Detailed molecular dynamics simulations verify the technique and aid with evaluating its effectiveness. Our technique appears to be applicable to other types of mass spectrometers.

Single photon sources based on semiconductor quantum dots offer distinct advantages for quantum information, including a scalable solid-state platform, ultrabrightness, and interconnectivity with matter qubits. A key prerequisite for their use in optical quantum computing and solid-state networks is a high level of efficiency and indistinguishability. Pulsed resonance fluorescence (RF) has been anticipated as the optimum condition for the deterministic generation of high-quality photons with vanishing effects of dephasing. Here, we generate pulsed RF single photons on demand from a single, microcavity-embedded quantum dot under s-shell excitation with 3-ps laser pulses. The pi-pulse excited RF photons have less than 0.3% background contributions and a vanishing two-photon emission probability. Non-postselective Hong-Ou-Mandel interference between two successively emitted photons is observed with a visibility of 0.97(2), comparable to trapped atoms and ions. Two single photons are further used to implement a high-fidelity quantum controlled-NOT gate.

We report on three-dimensional optical trapping of single ions in an optical lattice formed by two counter-propagating laser beams. We characterize the trapping parameters of the standing wave using the ion as a sensor stored in a hybrid trap consisting of a radio-frequency (rf), a dc, and the optical potential. When loading ions directly from the rf into the standing-wave trap, we observe a dominant heating rate. Monte Carlo simulations confirm rf-induced parametric excitations within the deep optical lattice as the main source. We demonstrate a way around this effect by an alternative transfer protocol which involves an intermediate step of optical confinement in a single-beam trap avoiding the temporal overlap of the standing wave and the rf field. Implications arise for hybrid (rf/optical) and pure optical traps as platforms for ultra-cold chemistry experiments exploring atom--ion collisions or quantum simulation experiments with ions, or combinations of ions and atoms.

We recently reported on a proof-of-principle experiment demonstrating optical trapping of an ion in a single-beam dipole trap superimposed by a static electric potential [Nat. Photonics 4, 772--775 (2010)]. Here, we first discuss the experimental procedures focussing on the influence and consequences of the static electric potential. These potentials can easily prevent successful optical trapping, if their configuration is not chosen carefully. Afterwards, we analyse the dipole trap experiments with different analytic models, in which different approximations are applied. According to these models the experimental results agree with recoil heating as the relevant heating effect. In addition, a Monte-Carlo simulation has been developed to refine the analysis. It reveals a large impact of the static electric potential on the dipole trap experiments in general. While it supports the results of the analytic models for the parameters used in the experiments, the analytic models cease their validity for significantly different parameters. Finally, we propose technical improvements for future realizations of experiments with optically trapped ions.

We examine the prospects of discrete quantum walks (QWs) with trapped ions. In particular, we analyze in detail the limitations of the protocol of Travaglione and Milburn (PRA 2002) that has been implemented by several experimental groups in recent years. Based on the first realization in our group (PRL 2009), we investigate the consequences of leaving the scope of the approximations originally made, such as the Lamb--Dicke approximation. We explain the consequential deviations from the idealized QW for different experimental realizations and an increasing number of steps by taking into account higher-order terms of the quantum evolution. It turns out that these become dominant after a few steps already, which is confirmed by experimental results and is currently limiting the scalability of this approach. Finally, we propose a new scheme using short laser pulses, derived from a protocol from the field of quantum computation. We show that the new scheme is not subject to the above-mentioned restrictions, and analytically and numerically evaluate its limitations, based on a realistic implementation with our specific setup. Implementing the protocol with state-of-the-art techniques should allow for substantially increasing the number of steps to 100 and beyond and should be extendable to higher-dimensional QWs.

Direct experimental access to some of the most intriguing quantum phenomena is not granted due to the lack of precise control of the relevant parameters in their naturally intricate environment. Their simulation on conventional computers is impossible, since quantum behaviour arising with superposition states or entanglement is not efficiently translatable into the classical language. However, one could gain deeper insight into complex quantum dynamics by experimentally simulating the quantum behaviour of interest in another quantum system, where the relevant parameters and interactions can be controlled and robust effects detected sufficiently well. We report on the progress in experimentally simulating quantum many-body physics with trapped ions.