Eliminating Qubit-Type Cross-Talk in the omg Protocol.

The omg protocol is a promising paradigm that uses multiple, application-specific, qubit subspaces within the Hilbert space of each single atom during quantum information processing. A key assumption for omg operation is that a subspace can be accessed independently without deleterious effects on information stored in other subspaces. We find that intensity noise during laser-based quantum gates in one subspace can cause decoherence in other subspaces, potentially complicating omg operation. We show, however, that a magnetic-field-induced vector light shift can be used to eliminate this source of decoherence. As this technique simply requires choosing a specific, magnetic field-dependent polarization for the gate lasers, it is straightforward to implement and potentially helpful for omg-based quantum technology.

Raman Scattering Errors in Stimulated-Raman-Induced Logic Gates in

^{133}Ba^{+} is illuminated by a laser that is far detuned from optical transitions, and the resulting spontaneous Raman scattering rate is measured. The observed scattering rate is lower than previous theoretical estimates. The majority of the discrepancy is explained by a more accurate treatment of the scattered photon density of states. This work establishes that, contrary to previous models, there is no fundamental atomic physics limit to laser-driven quantum gates from laser-induced spontaneous Raman scattering.

Franck-Condon Tuning of Optical Cycling Centers by Organic Functionalization.

Laser induced electronic excitations that spontaneously emit photons and decay directly to the initial ground state ("optical cycling transitions") are used in quantum information and precision measurement for state initialization and readout. To extend this primarily atomic technique to large, organic compounds, we theoretically investigate optical cycling of alkaline earth phenoxides and their functionalized derivatives. We find that optical cycle leakage due to wave function mismatch is low in these species, and can be further suppressed by using chemical substitution to boost the electron-withdrawing strength of the aromatic molecular ligand through resonance and induction effects. This provides a straightforward way to use chemical functional groups to construct optical cycling moieties for laser cooling, state preparation, and quantum measurement.

Surface chemical trapping of optical cycling centers.

Quantum information processors based on trapped atoms utilize laser-induced optical cycling transitions for state preparation and measurement. These transitions consist of an electronic excitation from the ground to an excited state and a decay back to the initial ground state, associated with a photon emission. While this technique has been used primarily with atoms, it has also recently been shown to work for some divalent metal hydroxides (e.g. SrOH) and alkoxides (e.g. SrOCH3). This extension to molecules is possible because these molecules feature nearly isolated, atomic-like ground and first-excited electronic states centered on the radical metal atom. We theoretically investigate the extension of this idea to a larger scale by growing the alkyl group, R, beyond the initial methyl group, CH3, while preserving the isolated and highly vertical character of the electronic excitation on the radical metal atom, M. Theory suggests that in the limit as the size of the ligand carbon chain increases, it can be considered a functionalized diamond (or cubic boron nitride) surface. Several requirements must be observed for the cycling centers to function when bound to the surface. First, the surface must have a significant band gap that fully encapsulates both the ground and excited states of the cycling center. Second, while the surface lattice imposes strict limits on the achievable spacing between the SrO- groups, at high coverage, SrO- centers can interact, and show geometric changes and/or electronic state mixing. We show that the coverage of the diamond surface with SrO- cycling centers needs to be significantly sub-monolayer for the functionality of the cycling center to be preserved. Having the lattice-imposed spatial control of SrO- placements will allow nanometer-scale proximity between qubits and will eliminate the need for atom traps for localized cycling emitters. Our results also imply that a functionalization could be done on a scanning microscope tip for local quantum sensing or on photonic structures for optically-mediated quantum information processing.

Dipole-Phonon Quantum Logic with Trapped Polar Molecular Ions.

The interaction between the electric dipole moment of a trapped molecular ion and the phonon modes of the confined Coulomb crystal couples the orientation of the molecule to its motion. We consider the practical feasibility of harnessing this interaction to initialize, process, and read out quantum information encoded in molecular ion qubits without ever optically illuminating the molecules. We present two schemes wherein a molecular ion can be entangled with a cotrapped atomic ion qubit, providing, among other things, a means for molecular state preparation and measurement. We also show that virtual phonon exchange can significantly boost the range of the intermolecular dipole-dipole interaction, allowing strong coupling between widely separated molecular ion qubits.

Dipole-phonon quantum logic with alkaline-earth monoxide and monosulfide cations.

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.

Suppressed Spontaneous Emission for Coherent Momentum Transfer.

Strong optical forces with minimal spontaneous emission are desired for molecular deceleration and atom interferometry applications. We report experimental benchmarking of such a stimulated optical force driven by ultrafast laser pulses. We apply this technique to accelerate atoms, demonstrating up to an average of 19ℏk momentum transfers per spontaneous emission event. This represents more than an order of magnitude improvement in suppression of spontaneous emission compared to radiative scattering forces. For molecular beam slowing, this technique is capable of delivering a many-fold increase in the achievable time-averaged force to significantly reduce both the slowing distance and detrimental losses to dark vibrational states.

Isotope-selective chemistry in the Be+(2S1/2) + HOD → BeOD+/BeOH+ + H/D reaction.

Low temperature reactions between laser-cooled Be+(2S1/2) ions and partially deuterated water (HOD) molecules have been investigated using an ion trap and interpreted with zero-point corrected quasi-classical trajectory calculations on a highly accurate global potential energy surface for the ground electronic state. Both product channels have been observed for the first time, and the branching to BeOD+ + H is found to be 0.58 ± 0.14. The experimental observation is reproduced by both quasi-classical trajectory and statistical calculations. Theoretical analyses reveal that the branching to the two product channels is largely due to the availability of open states in each channel.

Phonon Lasing from Optical Frequency Comb Illumination of Trapped Ions.

We demonstrate the use of a frequency-doubled optical frequency comb to load, cool, and crystallize trapped atomic ions as an alternative to ultraviolet (UV) or even deep UV continuous-wave lasers. We find that the Doppler shift from the atom's oscillation in the trap, driven by the blue-detuned comb teeth, introduces additional cooling and amplification which gives rise to steady-state phonon lasing of the ion's harmonic motion in the trap. The phonon laser's gain saturation keeps the optical frequency comb from continually adding energy without bound. This protection allows us to demonstrate loading and crystallization of hot ions directly with the comb, eliminating the need for a continuous-wave cooling laser, a technique that is extendable to the deep UV.

Spectroscopy of a Synthetic Trapped Ion Qubit.

^{133}Ba^{+} has been identified as an attractive ion for quantum information processing due to the unique combination of its spin-1/2 nucleus and visible wavelength electronic transitions. Using a microgram source of radioactive material, we trap and laser cool the synthetic A=133 radioisotope of barium II in a radio-frequency ion trap. Using the same, single trapped atom, we measure the isotope shifts and hyperfine structure of the 6^{2}P_{1/2}↔6^{2}S_{1/2} and 6^{2}P_{1/2}↔5^{2}D_{3/2} electronic transitions that are needed for laser cooling, state preparation, and state detection of the clock-state hyperfine and optical qubits. We also report the 6^{2}P_{1/2}↔5^{2}D_{3/2} electronic transition isotope shift for the rare A=130 and 132 barium nuclides, completing the spectroscopic characterization necessary for laser cooling all long-lived barium II isotopes.

Laser-type cooling with unfiltered sunlight.

Cooling of systems to sub-Kelvin temperatures is usually done using either a cold bath of particles or spontaneous photon scattering from a laser field; in either case, cooling is driven by interaction with a well-ordered cold (i.e., low-entropy) system. However, there have recently been several schemes proposed for "cooling by heating," in which raising the temperature of some mode drives the cooling of the desired system faster. We discuss how to cool a trapped ion to its motional ground state using unfiltered sunlight at 5800K to drive the cooling. We show how to treat the statistics of thermal light in a single-mode fiber for delivery to the ion and show experimentally how the blackbody spectrum is strongly modified by being embedded in quasi-one-dimension. Quantitative estimates for the achievable cooling rate with our measured fiber-coupled low-dimensional sunlight show promise for demonstrating this implementation of cooling by heating.

Extending the Large Molecule Limit: The Role of Fermi Resonance in Developing a Quantum Functional Group.

Polyatomic molecules equipped with optical cycling centers (OCCs), enabling continuous photon scattering during optical excitation, are exciting candidates for advancing quantum information science. However, as these molecules grow in size and complexity, the interplay of complex vibronic couplings on optical cycling becomes a critical but relatively unexplored consideration. Here, we present an extensive exploration of Fermi resonances in large-scale OCC-containing molecules using high-resolution dispersed laser-induced fluorescence and excitation spectroscopy. These resonances manifest as vibrational coupling leading to intensity borrowing by combination bands near optically active harmonic bands, which require additional repumping lasers for effective optical cycling. To mitigate these effects, we explore altering the vibrational energy level spacing through substitutions on the phenyl ring or changes in the OCC itself. While the complete elimination of vibrational coupling in complex molecules remains challenging, our findings highlight significant mitigation possibilities, opening new avenues for optimizing optical cycling in large polyatomic molecules.

Toward liquid cell quantum sensing: Ytterbium complexes with ultranarrow absorption.

The energetic disorder induced by fluctuating liquid environments acts in opposition to the precise control required for coherence-based sensing. Overcoming fluctuations requires a protected quantum subspace that only weakly interacts with the local environment. We report a ytterbium complex that exhibited an ultranarrow absorption linewidth in solution at room temperature with a full width at half maximum of 0.625 milli-electron volts. Using spectral hole burning, we measured an even narrower linewidth of 410 pico-electron volts at 77 kelvin. Narrow linewidths allowed low-field magnetic circular dichroism at room temperature, used to sense Earth-scale magnetic fields. These results demonstrated that ligand protection in lanthanide complexes could substantially diminish electronic state fluctuations. We have termed this system an "atomlike molecular sensor" (ALMS) and proposed approaches to improve its performance.

Laser Spectroscopy of Aromatic Molecules with Optical Cycling Centers: Strontium(I) Phenoxides.

We report the production and spectroscopic characterization of strontium(I) phenoxide (SrOC6H5 or SrOPh) and variants featuring electron-withdrawing groups designed to suppress vibrational excitation during spontaneous emission from the electronically excited state. Optical cycling closure of these species, which is the decoupling of the vibrational state changes from spontaneous optical decay, is found by dispersed laser-induced fluorescence spectroscopy to be high, in accordance with theoretical predictions. A high-resolution, rotationally resolved laser excitation spectrum is recorded for SrOPh, allowing the estimation of spectroscopic constants and identification of candidate optical cycling transitions for future work. The results confirm the promise of strontium phenoxides for laser cooling and quantum state detection at the single-molecule level.

Pathway toward Optical Cycling and Laser Cooling of Functionalized Arenes.

Rapid and repeated photon cycling has enabled precision metrology and the development of quantum information systems using atoms and simple molecules. Extending optical cycling to structurally complex molecules would provide new capabilities in these areas, as well as in ultracold chemistry. Increased molecular complexity, however, makes realizing closed optical transitions more difficult. Building on already established strong optical cycling of diatomic, linear triatomic, and symmetric top molecules, recent work has pointed the way to cycling of larger molecules, including phenoxides. The paradigm for these systems is an optical cycling center bonded to a molecular ligand. Theory has suggested that cycling may be extended to even larger ligands, like naphthalene, pyrene, and coronene. Herein, we study optical excitation and fluorescent vibrational branching of CaO-[Formula: see text], SrO-[Formula: see text], and CaO-[Formula: see text] and find only weak decay to excited vibrational states, indicating a promising path to full quantum control and laser cooling of large arene-based molecules.

Functionalizing aromatic compounds with optical cycling centres.

Molecular design principles provide guidelines for augmenting a molecule with a smaller group of atoms to realize a desired property or function. We demonstrate that these concepts can be used to create an optical cycling centre, the Ca(I)-O unit, that can be attached to a number of aromatic ligands, enabling the scattering of many photons from the resulting molecules without changing the molecular vibrational state. Such capability plays a central role in quantum state preparation and measurement, as well as laser cooling and trapping, and is therefore a prerequisite for many quantum science and technology applications. We provide further molecular design principles that indicate the ability to optimize and expand this work to an even broader class of molecules. This represents a great step towards a quantum functional group, which may serve as a generic qubit moiety that can be attached to a wide range of molecular structures and surfaces.

Cold N+NH collisions in a magnetic trap.

We present an experimental and theoretical study of atom-molecule collisions in a mixture of cold, trapped N atoms and NH molecules at a temperature of ∼600 mK. We measure a small N+NH trap loss rate coefficient of k(loss)(N+NH)=9(5)(3)×10(-13) cm(3) s(-1). Accurate quantum scattering calculations based on ab initio interaction potentials are in agreement with experiment and indicate the magnetic dipole interaction to be the dominant loss mechanism. Our theory further indicates the ratio of N+NH elastic-to-inelastic collisions remains large (>100) into the mK regime.

Optical Cycling Functionalization of Arenes.

Closed, laser-induced optical transitions ("optical cycling transitions") of molecules can be used for state preparation and measurement in quantum information science and quantum sensing. Increasingly complex molecular species supporting optical cycling can provide new capabilities for quantum science, and it is not clear if there is a limit on their size or complexity. We explore Ca-O-L molecular constructs to support the optical cycling center, Ca, with ligands, L, being arenes. We find that L can be as large as coronene (i.e., CaOC24H11) without losing the diagonality of the Franck-Condon factor (FCF). Furthermore, L can be substituted with electron-withdrawing groups to improve the FCF. Larger L, beyond ∼7 rings, can disrupt the diagonality of the FCF by closing the HOMO-LUMO ligand electronic state gap and reordering with the local states on the cycling center. Overall, we find that optical cycling can be retained for arenes, and we offer a principle for their design.

Isomer-specific kinetics of the C+ + H2O reaction at the temperature of interstellar clouds.

The reaction C+ + H2O → HCO+/HOC+ + H is one of the most important astrophysical sources of HOC+ ions, considered a marker for interstellar molecular clouds exposed to intense ultraviolet or x-ray radiation. Despite much study, there is no consensus on rate constants for formation of the formyl ion isomers in this reaction. This is largely due to difficulties in laboratory study of ion-molecule reactions under relevant conditions. Here, we use a novel experimental platform combining a cryogenic buffer-gas beam with an integrated, laser-cooled ion trap and high-resolution time-of-flight mass spectrometer to probe this reaction at the temperature of cold interstellar clouds. We report a reaction rate constant of k = 7.7(6) × 10-9 cm3 s-1 and a branching ratio of formation η = HOC+/HCO+ = 2.1(4). Theoretical calculations suggest that this branching ratio is due to the predominant formation of HOC+ followed by isomerization of products with internal energy over the isomerization barrier.

Application of a self-injection locked cyan laser for Barium ion cooling and spectroscopy.

Compact, high power lasers with narrow linewidth are important tools for the manipulation of quantum systems. We demonstrate a compact, self-injection locked, Fabry-Perot semiconductor laser diode with high output power at 493 nm. A high quality factor magnesium fluoride whispering gallery mode resonator enables both high passive stability and 1 kHz instantaneous linewidth. We use this laser for laser-cooling, in-situ isotope purifcation, and probing barium atomic ions confined in a radio-frequency ion trap. The results here demonstrate the suitability of these lasers in trapped ion quantum information processing and for probing weak coherent optical transitions.