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At least 73 records · Page 4

Large Momentum Transfer Clock Atom Interferometry on the 689 nm Intercombination Line of Strontium

We report the first realization of large momentum transfer (LMT) clock atom interferometry. Using single-photon interactions on the strontium $^1S_{0^–}^3P_1$ transition, we demonstrate Mach-Zehnder interferometers with state-of-the-art momentum separation of up to 141 $\textit{ℏk}$ and gradiometers of up to 81 $\textit{ℏk}$. Furthermore, we circumvent excited state decay limitations and extend the gradiometer duration to 50 times the excited state lifetime. Because of the broad velocity acceptance of the interferometry pulses, all experiments are performed with laser-cooled atoms at a temperature of 3 μK. This work has applications in high-precision inertial sensing and paves the way for LMT-enhanced clock atom interferometry on even narrower transitions, a key ingredient in proposals for gravitational wave detection and dark matter searches.

74 ATOMIC AND MOLECULAR PHYSICS↗

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.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Symmetry Protected Two-Photon Coherence Time

We report the observation of symmetry protected two-photon coherence time of biphotons generated from backward spontaneous four-wave mixing in laser-cooled 87 Rb atoms. When biphotons are nondegenerate, nonsymmetric photonic absorption loss results in exponential decay of the temporal waveform of the two-photon joint probability amplitude, leading to shortened coherence time. In contrast, in the case of degenerate biphotons, when both paired photons propagate with the same group velocity and absorption coefficient, the two-photon coherence time, protected by space-time symmetry, remains unaffected by medium absorptive losses. Furthermore, our experimental results validate these theoretical predictions. This outcome highlights the pivotal role of symmetry in manipulating and controlling photonic quantum states.

74 ATOMIC AND MOLECULAR PHYSICS↗

High-resolution spectroscopy of barium monofluoride: Odd isotopologues, hyperfine structure, and isotope shifts

Barium monofluoride (BaF) is a promising molecular species for precision tests of fundamental symmetries and interactions. We present a combined theoretical and experimental study of BaF spectra and isotope shifts, focusing in particular on the poorly understood odd isotopologues 137 BaF and 135 BaF. By comparing state-of-the-art ab initio calculations with high-resolution fluorescence and absorption spectroscopy data, we provide a benchmark for electronic structure theory and disentangle the hyperfine and rovibrational spectra of the five most abundant isotopologues, from 138 BaF to 134 BaF. The comprehensive knowledge gained enables a King plot analysis of the isotope shifts that reveals the odd-even staggering of the barium nuclear charge radii. It also paths the way for improved laser cooling of rare BaF isotopologues and crucially supports future measurements of nuclear anapole and Schiff moments.

Kogel, Felix [Univ. of Stuttgart (Germany)] (ORCID↗

A passively pumped vacuum package sustaining cold atoms for more than 200 days

Compact cold-atom sensors depend on vacuum technology. One of the major limitations to miniaturizing these sensors is the active pumps—typically ion pumps—that are required to sustain the low pressure needed for laser cooling. Although passively pumped chambers have been proposed as a solution to this problem, technical challenges have prevented successful operation at the levels needed for cold-atom experiments. The authors present the first demonstration of a vacuum package successfully independent of ion pumps for more than a week; their vacuum package is capable of sustaining a cloud of cold atoms in a magneto-optical trap (MOT) for greater than 200 days using only non-evaporable getters and a rubidium dispenser. Measurements of the MOT lifetime indicate that the package maintains a pressure of better than 2×10−7 Torr. This result will significantly enable the development of compact atomic sensors, including those sensitive to magnetic fields, where the absence of an ion pump will be advantageous.

Little, Bethany J. (ORCID:0000000332892798)↗

Optical nanofiber testbeds for benchmarking membrane-waveguide photonic integrated circuit platforms toward on-chip quantum inertial sensing

Recent advances in cold atom interferometry with optical and magnetic atom guides have set the stage for quantum inertial sensors capable of operating in dynamic environments. In this work, we present three key innovations—evanescent-field (EF) atom guides, optical nanofiber testbeds, and membrane-waveguide photonic integrated circuit (PIC) platforms—to advance EF-guided atom interferometry. First, we demonstrate EF atom guides on optical nanofiber testbeds, which serve as performance benchmarks for our membrane-waveguide PIC platforms. Second, we achieve low-power (⁠ ~ 5 mW) guiding of freely moving, laser-cooled 133 Cs atoms in two-color, traveling-wave EF optical dipole traps at the novel, heat-efficient magic wavelengths of 793 and 937 nm (i.e., “793/937-nm EF atom guides”). Concurrently, we design and fabricate membrane-waveguide PIC platforms for these EF atom guides; in our prior work, we showed that these structures safely accommodate 4–6 times the required optical trap power under vacuum and enable dense cold atom generation via magneto-optical trapping in the vicinity of the optical wavguide for efficient loading. Third, we verify preserved atomic coherence via microwave fields and EF-coupled Doppler-free Raman beams; to our knowledge, this is the first report of coherence fringes driven by co-propagating EF-coupled Raman beams with only 150 nW of total optical power. By providing a direct comparison between optical nanofiber testbeds and membrane-waveguide PIC platforms, our results lay critical groundwork for the on-chip realization of EF-guided atom interferometry and the development of fully integrated, compact, lightweight, and low-power quantum accelerometers and gyroscopes.

Orozco, Adrian [Sandia National Laboratories (SNL-↗

Momentum-exchange interactions in a Bragg atom interferometer suppress Doppler dephasing

Large ensembles of laser-cooled atoms interacting through infinite-range photon-mediated interactions are powerful platforms for quantum simulation and sensing. Here we realize momentum-exchange interactions in which pairs of atoms exchange their momentum states by collective emission and absorption of photons from a common cavity mode, a process equivalent to a spin-exchange or XX collective Heisenberg interaction. The momentum-exchange interaction leads to an observed all-to-all Ising-like interaction in a matter-wave interferometer. A many-body energy gap also emerges, effectively binding interferometer matter-wave packets together to suppress Doppler dephasing in analogy to Mössbauer spectroscopy. The tunable momentum-exchange interaction expands the capabilities of quantum interaction–enhanced matter-wave interferometry and may enable the realization of exotic behaviors, including simulations of superconductors and dynamical gauge fields.

Science & Technology - Other Topics↗

Realization of three- and four-body interactions between momentum states in a cavity

Spin Hamiltonians in condensed matter and quantum sensing typically utilize pairwise or two-body interactions between constituents in the material or ensemble. However, there is growing interest in exploring more general n-body interactions for n > 2. In this study, we realized an effective n = 3-body Hamiltonian interaction using an ensemble of laser-cooled atoms in a high-finesse optical cavity with the pseudospin 1/2 encoded by two atomic momentum states. We applied two dressing tones that induce the atoms to exchange photons via the cavity to realize a virtual six-photon process; lower-order interactions destructively interfered. We also observed signatures of a n = 4-body interaction mediated by a virtual eight-photon process. Our approach may be extensible to three-body interactions in multilevel systems or to even higher-order interactions.

Luo, Chengyi [University of Colorado, Boulder, CO ↗

Characterization of suspended membrane waveguides towards a photonic atom trap integrated platform

We demonstrate an optical waveguide device, capable of supporting the high, in-vacuum, optical power necessary for trapping a single atom or a cold atom ensemble with evanescent fields. Our photonic integrated platform, with suspended membrane waveguides, successfully manages optical powers of 6 mW (500 μ m span) to nearly 30 mW (125 μ m span) over an un-tethered waveguide span. This platform is compatible with laser cooling and magneto-optical traps (MOTs) in the vicinity of the suspended waveguide, called the membrane MOT and the needle MOT, a key ingredient for efficient trap loading. We evaluate two novel designs that explore critical thermal management features that enable this large power handling. This work represents a significant step toward an integrated platform for coupling neutral atom quantum systems to photonic and electronic integrated circuits on silicon.

36 MATERIALS SCIENCE↗

Physics Division Strategic Plan Fiscal Years 2020-2024

The vision of the Physics Division (PHY) at Argonne National Laboratory is to continue enhancing its role as a world-leading institution in basic nuclear physics research and its applications. Key to this vision is for PHY to continue to safely and effectively operate and evolve the capabilities of the Argonne Tandem Linac Accelerator System (ATLAS) facility to best serve its users. ATLAS is the Department of Energy (DOE) accelerator facility for low-energy nuclear physics research. The research carried out by PHY covers many themes in contemporary science but can be distilled into five areas of focus. These themes are interconnected, with continuously evolving synergies between the various groups and facilities in PHY and the broader Laboratory. This five-year strategic plan serves to illustrate our current capabilities and new directions related to these five areas of focus (ATLAS also develops an independent strategic plan): Accelerator research and design. The goal of this theme is to design, fabricate, test, and implement novel accelerator systems, with a focus on high-intensity ion and electron systems. These R&D activities have led to enhancements in the ATLAS accelerator system. Among others, the division’s accelerator systems are in use or planned for use at Fermilab, the Advanced Photon Source, and in a broad variety of applications at the Facility for Rare Isotope Beams (FRIB). Atom trapping and fundamental symmetries. The goal of this theme is to explore and exploit the uses of advanced laser cooling and trapping techniques to manipulate atoms. There are three main areas of focus. First is in the application of the atom trap trace analysis (ATTA) technique for age determination of groundwater and ice by using radio-krypton dating. The next two trapping-based programs involve tests of fundamental symmetries in nature: the cooling and trapping of radium-225 with the aim of determining limits on an observation of its electric dipole moment and precision measurements of the beta decay properties of helium-6 to set limits on the tensor coupling constant. This is complemented by measurements of similar properties in lithium-8 and boron-8. Nuclear astrophysics. The goal of this theme is to enhance our understanding of how elements are created in the universe via explosive nucleosynthesis and how stars evolve. To meet the challenges of this theme, many of the capabilities of ATLAS are being enhanced, including the development of new beams through a new in-flight separator (RAISOR) and the anticipated neutron-generator upgrade of the Californium Rare Isotope Breeder Upgrade facility (nuCARIBU). These are coupled to state-of-the-art instruments such as the Canadian Penning Trap, Helical Orbit Spectrometer, Gammasphere, GRETINA, Multi-Sampling Ionization Chamber, the Fragment Mass Analyzer, and Argonne Gas-filled Fragment Analyzer, and a new low-background experimental area for decay studies. Nuclear structure. The goal of this theme is to understand the structure of nuclei, both stable and radioactive, in terms of single-particle properties, their shapes, and the dynamics governing reactions between them. These include questions such as what are the limits of nuclear stability and what are the properties of super heavy nuclei. As with the nuclear astrophysics theme, the capabilities of ATLAS, guided by the ATLAS user community, are continuously being enhanced to this end. The Division has strategic initiatives to play a leading role in the development of instrumentation and research programs at the FRIB. Quantum chromodynamics (QCD) and hadron physics. The goal of this theme is to lead major research programs focused on revealing the quark and gluon structure of protons, neutrons, nuclei, and short-lived mesons and baryons. These involve major programs at Jefferson Lab, Fermilab, and smaller facilities. They are complemented by theoretical endeavors centered on the question of how hadrons and their properties emerge from QCD. Out of these activities arise strategic initiatives to play a major role in the forthcoming Electron-Ion Collider (EIC).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Molecules Functionalized with Cycling Centers for Quantum Information Science

The ability for a single molecule to produce enough laser-induced fluorescence to control and detect its quantum state is known as optical cycling. This property has been used to great effect in atoms, where the relatively small number of states promotes their ability to repeatedly fluoresce, for applications such as laser cooling, precision measurement, atomic clocks, and quantum information processing. The extension of this capability to molecular species, however, has been difficult, primarily due to their propensity to become vibrationally excited during illumination. This project brought together experts from atomic physics, physical chemistry, and computational quantum chemistry to develop means to create molecules capable of optical cycling. In particular, this program sought to produce an optical cycling center (OCC), a quantum functional group capable of chemical attachment to a wide variety of molecular hosts while retaining (and thereby furnishing to its host) the ability to optically cycle. Following our team’s theoretical identification of promising species, including alkaline-earth phenoxides, we then created these species and in many cases confirmed their optical cycle closure. We now not only know of the existence of a handful of large, molecular species that can be deployed for applications in quantum technologies and measurement, but have improved our knowledge of the molecular mechanisms leading to this discovery, which will enable generalization in the future. The extension of these ideas for informed chemical design of cycling molecules with bespoke properties is now being pursued by multiple groups.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ab initio study and assignment of electronic states in molecular RaCl

Radium compounds have attracted recently considerable attention due to both development of experimental techniques for high-precision laser spectroscopy of molecules with short-lived nuclei and amenability of certain radium compounds for direct cooling with lasers. Currently, radium monofluoride (RaF) is one of the most studied molecules among the radium compounds, both theoretically and recently also experimentally. Complementary studies of further diatomic radium derivatives are highly desired to assess the influence of chemical substitution on diverse molecular parameters, especially on those connected with laser cooling, such as vibronic transition probabilities, and those related to violations of fundamental symmetries. Here in this article high-precision ab initio studies of electronic and vibronic levels of diatomic radium monochloride (RaCl) are presented. Recently developed approaches for treating electronic correlation with Fock-space coupled cluster methods are applied for this purpose. Theoretical results are compared to an early experimental investigation by Lagerqvist and used to partially reassign the experimentally observed transitions and molecular electronic levels of RaCl. Effective constants of $\mathscr{P}$-odd hyperfine interaction W a and $\mathscr{P, T}$-odd scalar-pseudoscalar nucleus-electron interaction Ws in the ground electronic state of RaCl are estimated within the framework of a quasirelativistic Zeroth-Order Regular Approximation approach and compared to parameters in RaF and RaOH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Systems and methods for laser diode array having integrated microchannel cooling

The present disclosure relates to a laser diode system. The system may have at least one laser diode emitter having a substrate, at least one laser diode supported on the substrate, and a facet which a laser beam generated by the laser diode is emitted. A cooling subsystem is included which is disposed in contact with the substrate of the laser diode emitter. The cooling subsystem includes a plurality of cooling fins forming a plurality of elongated channels for circulating a cooling fluid therethrough to cool the laser diode emitter. The cooling fluid also flows over the facet of the laser diode emitter.

Kotovsky, Jack↗

High-resolution infrared spectroscopy of jet cooled CH 2 Br radicals: The symmetric CH stretch manifold and absence of nuclear spin cooling

Direct laser absorption of a slit supersonic discharge expansion provides the first high-resolution spectroscopic results on the symmetric CH stretch excitation (ν 1 ) of the bromomethyl (CH 2 Br) radical in the ground electronic state. Narrowband (<1 MHz) mid-infrared radiation is produced by difference-frequency generation of two visible laser beams, with the open shell halohydrocarbon radical generated by electron dissociative attachment of CH 2 Br 2 in a discharge and rapidly cooled to T rot = 18 ± 1 K in the subsequent slit-jet supersonic expansion. A rovibrational structure in the radical spectrum is fully resolved, as well as additional splittings due to spin-rotation effects and 79 Br/ 81 Br isotopologues in natural abundance. Spectroscopic constants and band origins are determined by fitting the transition frequencies to a non-rigid Watson Hamiltonian, yielding results consistent with a vibrationally averaged planar radical and an unpaired electron in the out-of-plane p π orbital. Additionally, extensive satellite band structure from a vibrational hot band is observed and analyzed. The hot band data is compared to CFOUR/VPT2 (CCSD(T)cc-pVQZ) ab initio anharmonic predictions of the vibration rotation alpha matrix, which permits unambiguous assignment to CH 2 symmetric-stretch excitation built on the singly excited CH 2 out-of-plane bending mode (ν 1 + ν 4 ← ν 4 ). Longitudinal cooling of the Doppler width in the slit-jet expansion geometry also reveals partially resolved hyperfine structure on transitions out of the lowest angular momentum states in excellent agreement with predictions based on microwave studies. High level ab initio MOLPRO calculations [CCSD(T)-f12b/VnZ-f12 (n = 3, 4, CBS)] are also performed with explicitly correlated f12 electron methods for the out-of-plane CH 2 bending mode over the halogen series CH 2 X (X = F, Cl, Br, I), which clearly reveals a non-planar geometry for X = F (with a ΔE ≈ 0.3 kcal/mol barrier) and yet planar equilibrium geometries for X = Cl, Br, and I. Finally, a detailed Boltzmann analysis of the transition intensities provides support for negligible collisional equilibration of the entangled H atom nuclear spin states on the few hundred microsecond time scale and high collision densities of a slit supersonic expansion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Analytic gradients for relativistic exact-two-component equation-of-motion coupled-cluster singles and doubles method

A first implementation of analytic gradients for spinor-based relativistic equation-of-motion coupled-cluster singles and doubles method using an exact two-component Hamiltonian augmented with atomic mean-field spin–orbit integrals is reported. To demonstrate its applicability, we present calculations of equilibrium structures and harmonic vibrational frequencies for the electronic ground and excited states of the radium mono-amide molecule (RaNH 2 ) and the radium mono-methoxide molecule (RaOCH 3 ). Spin–orbit coupling is shown to quench Jahn–Teller effects in the first excited state of RaOCH 3 , resulting in a C 3v equilibrium structure. Furthermore, the calculations also show that the radium atoms in these molecules serve as efficient optical cycling centers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗