We experimentally study the dynamics of quantum knots in a uniform magnetic field in spin-1 Bose-Einstein condensates. The knot is created in the polar magnetic phase, which rapidly undergoes a transition toward the ferromagnetic phase in the presence of the knot. The magnetic order becomes scrambled as the system evolves, and the knot disappears. Strikingly, over long evolution times, the knot decays into a polar-core spin vortex, which is a member of a class of singular SO(3) vortices. The polar-core spin vortex is stable with an observed lifetime comparable to that of the condensate itself. The structure is similar to that predicted to appear in the evolution of an isolated monopole defect, suggesting a possible universality in the observed topological transition.

We report on the experimental observation of a strong-field dressing of an autoionizing two-electron state in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetric Fano line shape of this transition is spectrally resolved, and we observe modifications of the resonance asymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of Microjoules. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, evidences strong-field-induced energy and phase shifts of the doubly excited state, which are extracted from the Fano line-shape asymmetry. The experimental results obtained at the Free-Electron Laser in Hamburg (FLASH) thus correspond to transient energy shifts on the order of a few meV, induced by strong XUV fields. These results open up a new way of performing nonperturbative XUV nonlinear optics for the light-matter interaction of resonant electronic transitions in atoms at short wavelengths.

Phase distortions, or aberrations, can negatively influence the performance of an optical imaging system. Through the use of position-momentum entangled photons, we nonlocally correct for aberrations in one photon’s optical path by intentionally introducing the complementary aberrations in the optical path of the other photon. In particular, we demonstrate the simultaneous nonlocal cancellation of aberrations that are of both even and odd order in the photons’ transverse degrees of freedom. We also demonstrate a potential application of this technique by nonlocally canceling the effect of defocus in a quantum imaging experiment and thereby recover the original spatial resolution.

Thorough control of the optical mode of a single photon is essential for quantum information applications. We present a comprehensive experimental and theoretical study of a light-matter interface based on cavity quantum electrodynamics. We identify key parameters like the phases of the involved light fields and demonstrate absolute, flexible, and accurate control of the time-dependent complex-valued wave function of a single photon over several orders of magnitude. This capability will be an important tool for the development of distributed quantum systems with multiple components that interact via photons.

We experimentally study the excitation modes of bright matter-wave solitons in a quasi-one-dimensional geometry. The solitons are created by quenching the interactions of a Bose-Einstein condensate of cesium atoms from repulsive to attractive in combination with a rapid reduction of the longitudinal confinement. A deliberate mismatch of quench parameters allows for the excitation of breathing modes of the emerging soliton and for the determination of its breathing frequency as a function of atom number and confinement. In addition, we observe signatures of higher-order solitons and the splitting of the wave packet after the quench. Our experimental results are compared to analytical predictions and to numerical simulations of the one-dimensional Gross-Pitaevskii equation.

Pulsed optomechanical measurements enable squeezing, nonclassical state creation, and backaction-free sensing. We demonstrate pulsed measurement of a cryogenic nanomechanical resonator with record precision close to the quantum regime. We use these to prepare thermally squeezed and purified conditional mechanical states, and to perform full state tomography. These demonstrations exploit large vacuum optomechanical coupling in a nanophotonic cavity to reach a single-pulse imprecision of 9 times the mechanical zero-point amplitude $x_{\mathrm{zpf}}$. We study the effect of other mechanical modes that limit the conditional state width to $58x_{\mathrm{zpf}}$, and show how decoherence causes the state to grow in time.

We report the first cooling of atomic anions by laser radiation. ${\mathrm{O}}^{-}$ ions confined in a linear Paul trap were cooled by selectively photodetaching the hottest particles. For this purpose, anions with the highest total energy were illuminated with a 532 nm laser at their maximal radial excursion. Using laser-particle interaction, we realized a both colder and denser ion cloud, achieving a more than threefold temperature reduction from 1.15 to 0.33 eV. Compared with the interaction with a dilute buffer gas, the energy-selective addressing and removal of anions resulted in lower final temperatures, yet acted 10 times faster and preserved twice as large a fraction of ions in the final state. An ensemble of cold negative ions affords the ability to sympathetically cool any other negative ion species, enabling or facilitating a broad range of fundamental studies from interstellar chemistry to antimatter gravity. The technique can be extended to any negative ion species that can be neutralized via photodetachment.

We propose and explore an all-optical technique for ultrafast characterization of electronic ring currents in atoms and molecules, based on high-harmonic generation (HHG). In our approach, a medium is irradiated by an intense reflection-symmetric laser pulse that leads to HHG, where the polarization of the emitted harmonics is strictly linear if the medium is reflection invariant (e.g., randomly oriented atomic or molecular media). The presence of a ring current in the medium breaks this symmetry, causing the emission of elliptically polarized harmonics, where the harmonics’ polarization directly maps the ring current, and the signal is background-free. Scanning the delay between the current excitation and the HHG driving pulse provides an attosecond time-resolved signal for the multielectron dynamics in the excited current (including electron-electron interactions). We analyze the responsible physical mechanism and derive the analytic dependence of the HHG emission on the ring current. The method is numerically demonstrated using quantum models for neon and benzene, as well as through ab initio calculations.

We demonstrate Ramsey-Bordé (RB) atom interferometry for high performance laser stabilization with fractional frequency instability $<2\times {10}^{-16}$ for timescales between 10 and 1000s. The RB spectroscopy laser interrogates two counterpropagating ${}^{40}\mathrm{Ca}$ beams on the ${{}^{1}S}_0-{}^3{P}_1$ transition at 657 nm, yielding 1.6 kHz linewidth interference fringes. Fluorescence detection of the excited state population is performed on the ($4s4p$) ${}^3{P}_1-(4p^2)$ ${}^3{P}_0$ transition at 431 nm. Minimal thermal shielding and no vibration isolation are used. These stability results surpass performance from other thermal atomic or molecular systems by 1 to 2 orders of magnitude, and further improvements look feasible.

To accurately attribute sources and sinks of molecules like ${\mathrm{CO}}_2$, remote sensing missions require line intensities ($S$) with relative uncertainties $u_r(S)<0.1\%$. However, discrepancies in $S$ of $\approx 1\%$ are common when comparing different experiments, thus limiting their potential impact. Here we report a cavity ring-down spectroscopy multi-instrument comparison which revealed that the hardware used to digitize analog ring-down signals caused variability in spectral integrals which yield $S$. Our refined approach improved measurement accuracy 25-fold, resulting in $u_r(S)=0.06\%$.

We experimentally realize a photonic analogue of the anomalous quantum Hall insulator using a two-dimensional (2D) array of coupled ring resonators. Similar to the Haldane model, our 2D array is translation invariant, has a zero net gauge flux threading the lattice, and exploits next-nearest neighbor couplings to achieve a topologically nontrivial band gap. Using direct imaging and on-chip transmission measurements, we show that the band gap hosts topologically robust edge states. We demonstrate a topological phase transition to a conventional insulator by frequency detuning the ring resonators and thereby breaking the inversion symmetry of the lattice. Furthermore, the clockwise or the counterclockwise circulation of photons in the ring resonators constitutes a pseudospin degree of freedom. The two pseudospins acquire opposite hopping phases, and their respective edge states propagate in opposite directions. These results are promising for the development of robust reconfigurable integrated nanophotonic devices for applications in classical and quantum information processing.

We describe an optical atomic clock based on quantum-logic spectroscopy of the ${}^1{S}_0\leftrightarrow {{}^{3}P}_0$ transition in ${}^{27}{\mathrm{Al}}^{+}$ with a systematic uncertainty of $9.4\times {10}^{-19}$ and a frequency stability of $1.2\times {10}^{-15}/\sqrt{\tau }$. A ${}^{25}{\mathrm{Mg}}^{+}$ ion is simultaneously trapped with the ${}^{27}{\mathrm{Al}}^{+}$ ion and used for sympathetic cooling and state readout. Improvements in a new trap have led to reduced secular motion heating, compared to previous ${}^{27}{\mathrm{Al}}^{+}$ clocks, enabling clock operation with ion secular motion near the three-dimensional ground state. Operating the clock with a lower trap drive frequency has reduced excess micromotion compared to previous ${}^{27}{\mathrm{Al}}^{+}$ clocks. Both of these improvements have led to a reduced time-dilation shift uncertainty. Other systematic uncertainties including those due to blackbody radiation and the second-order Zeeman effect have also been reduced.

Stimulated Raman adiabatic passage (stirap) allows efficiently transferring the populations between two discrete quantum states and has been used to prepare molecules in their rovibrational ground state. In realistic molecules, a well-resolved intermediate state is usually selected to implement the resonant stirap. Because of the complex molecular level structures, the detuned stirap always coexists with the resonant stirap and may cause unexpected interference phenomenon. However, it is generally accepted that the detuned stirap can be neglected if compared with the resonant stirap. Here we report on the first observation of interference between the resonant and detuned stirap in the adiabatic creation of ${}^{23}\mathrm{Na}{}^{40}\mathrm{K}$ ground-state molecules. The interference is identified by observing that the number of Feshbach molecules after a round-trip stirap oscillates as a function of the hold time, with a visibility of about 90%. This occurs even if the intermediate excited states are well resolved, and the single-photon detuning of the detuned stirap is about 1 order of magnitude larger than the linewidth of the excited state and the Rabi frequencies of the stirap lasers. Moreover, the observed interference indicates that if more than one hyperfine level of the ground state is populated, the stirap prepares a coherent superposition state among them, but not an incoherent mixed state. Further, the purity of the hyperfine levels of the created ground state can be quantitatively determined by the visibility of the oscillation.

We report on the first experimental demonstration of enantioselective rotational control of chiral molecules with a laser field. In our experiments, two enantiomers of propylene oxide are brought to accelerated unidirectional rotation by means of an optical centrifuge. Using Coulomb explosion imaging, we show that the centrifuged molecules acquire preferential orientation perpendicular to the plane of rotation, and that the direction of this orientation depends on the relative handedness of the enantiomer and the rotating centrifuge field. The observed effect is in agreement with theoretical predictions and is reproduced in numerical simulations of the centrifuge excitation followed by Coulomb explosion of the centrifuged molecules. The demonstrated technique opens new avenues in optical enantioselective control of chiral molecules with a plethora of potential applications in differentiation, separation, and purification of chiral mixtures.

We present a method for producing three-dimensional Bose-Einstein condensates using only laser cooling. The phase transition to condensation is crossed with $2.5\times {10}^4$ ${}^{87}\mathrm{Rb}$ atoms at a temperature of $T_c=0.6\mu \mathrm{K}$ after 1.4 s of cooling. Atoms are trapped in a crossed optical dipole trap and cooled using Raman cooling with far-off-resonant optical pumping light to reduce atom loss and heating. The achieved temperatures are well below the effective recoil temperature. We find that during the final cooling stage at atomic densities above ${10}^{14}{\mathrm{cm}}^{-3}$, careful tuning of trap depth and optical-pumping rate is necessary to evade heating and loss mechanisms. The method may enable the fast production of quantum degenerate gases in a variety of systems including fermions.

We present an experimental study of the high-energy excitation spectra of unitary Fermi gases. Using focused beam Bragg spectroscopy, we locally probe atoms in the central region of a harmonically trapped cloud where the density is nearly uniform, enabling measurements of the dynamic structure factor for a range of temperatures both below and above the superfluid transition. Applying sum rules to the measured Bragg spectra, we resolve the characteristic behavior of the universal contact parameter, $\mathcal{C}$, across the superfluid transition. We also employ a recent theoretical result for the kinetic (second-moment) sum rule to obtain the internal energy of gases at unitarity.

We measure radio frequency (rf) spectra of the homogeneous unitary Fermi gas at temperatures ranging from the Boltzmann regime through quantum degeneracy and across the superfluid transition. For all temperatures, a single spectral peak is observed. Its position smoothly evolves from the bare atomic resonance in the Boltzmann regime to a frequency corresponding to nearly one Fermi energy at the lowest temperatures. At high temperatures, the peak width reflects the scattering rate of the atoms, while at low temperatures, the width is set by the size of fermion pairs. Above the superfluid transition, and approaching the quantum critical regime, the width increases linearly with temperature, indicating non-Fermi-liquid behavior. From the wings of the rf spectra, we obtain the contact, quantifying the strength of short-range pair correlations. We find that the contact rapidly increases as the gas is cooled below the superfluid transition.

We demonstrate the defect-free assembly of versatile target patterns of up 111 neutral atoms, building on a 361-site subset of a micro-optical architecture that readily provides thousands of sites for single-atom quantum systems. By performing multiple assembly cycles in rapid succession, we drastically increase achievable structure sizes and success probabilities. We implement repeated target pattern reconstruction after atom loss and deterministic transport of partial atom clusters necessary for distributing entanglement in large-scale systems. This technique will propel assembled-atom architectures beyond the threshold of quantum advantage and into a regime with abundant applications in quantum sensing and metrology, Rydberg-state mediated quantum simulation, and error-corrected quantum computation.

We experimentally investigate the two-dimensional photoelectron momentum spectra of aligned diatomic molecules in an intense laser field. Our results reveal a novel prominent valley structure in the molecular alignment dependence of the high-energy photoelectron spectra along the laser polarization. Resorting to the molecular strong-field approximation and a simple semiclassical analysis, we show that this valley structure stems from the destructive two-center interference of the laser-driven rescattered electrons in diatomic molecules. Based on this two-center interference with aligned diatomic molecules, we demonstrate for the first time a tomographic method to extract the molecular internuclear separation, providing a more straightforward approach of molecular imaging, in comparison with, e.g., laser-induced electron diffraction and fixed-angle broadband laser-driven electron scattering.

Sign-changing interactions constitute a crucial ingredient in the creation of frustrated many-body systems such as spin glasses. We present here the demonstration of a photon-mediated sign-changing interaction between Bose-Einstein-condensed atoms in a confocal cavity. The interaction between two atoms is of an unusual, nonlocal form proportional to the cosine of the inner product of the atoms’ position vectors. This interaction arises from the differing Gouy phase shifts of the cavity’s degenerate modes. The interaction drives a nonequilibrium Dicke-type phase transition in the system leading to atomic checkerboard density-wave order. Because of the Gouy phase anomalies, the checkerboard pattern can assume either a sinelike or cosinelike character. This state is detected via the holographic imaging of the cavity’s superradiant emission. Together with a companion paper [Y. Guo, V. D. Vaidya, R. M. Kroeze, R. A. Lunney, B. L. Lev, and J. Keeling, Emergent and broken symmetries of atomic self-organization arising from Gouy phases in multimode cavity QED, Phys. Rev. A 99, 053818 (2019)], we explore this interaction’s influence on superradiant phase transitions in multimode cavities. Employing this interaction in cavity QED spin systems may enable the creation of artificial spin glasses and quantum neural networks.