Collective phenomena emerging from nonlinear interactions between multiple oscillators, such as synchronization and frequency locking, find applications in a wide variety of fields. Optomechanical resonators, which are intrinsically nonlinear, combine the scientific assets of mechanical devices with the possibility of long distance controlled interactions enabled by traveling light. Here we demonstrate light-mediated frequency locking of three distant nano-optomechanical oscillators positioned in a cascaded configuration. The oscillators, integrated on a chip along a common coupling waveguide, are optically driven with a single laser and oscillate at gigahertz frequency. Despite an initial mechanical frequency disorder of hundreds of kilohertz, the guided light locks them all with a clear transition in the optical output. The experimental results are described by Langevin equations, paving the way to scalable cascaded optomechanical configurations.

We crystallize up to 15 ${{}^{40}\mathrm{Ca}}^{+}$ ions in a ring with a microfabricated silicon surface Paul trap. Delocalization of the Doppler laser-cooled ions shows that the translational symmetry of the ion ring is preserved at millikelvin temperatures. By characterizing the collective motion of the ion crystals, we identify homogeneous electric fields as the dominant symmetry-breaking mechanism at this energy scale. With increasing ion numbers, such detrimental effects are reduced. We predict that, with only a ten-ion ring, uncompensated homogeneous fields will not break the translational symmetry of the rotational ground state. This experiment opens a door towards studying quantum many-body physics with translational symmetry at the single-particle level.

We report on Raman sideband cooling of ${{}^{25}\mathrm{Mg}}^{+}$ to sympathetically cool the secular modes of motion in a ${{}^{25}\mathrm{Mg}}^{+}\text{−}{{}^{27}\mathrm{Al}}^{+}$ two-ion pair to near the three-dimensional (3D) ground state. The evolution of the Fock-state distribution during the cooling process is studied using a rate-equation simulation, and various heating sources that limit the efficiency of 3D sideband cooling in our system are discussed. We characterize the residual energy and heating rates of all of the secular modes of motion and estimate a secular motion time-dilation shift of $-(1.9\pm 0.1)\times {10}^{-18}$ for an ${{}^{27}\mathrm{Al}}^{+}$ clock at a typical clock probe duration of 150 ms. This is a 50-fold reduction in the secular motion time-dilation shift uncertainty in comparison with previous ${{}^{27}\mathrm{Al}}^{+}$ clocks.

Optical force, coming from momentum exchange during light-matter interactions, has been widely utilized to manipulate microscopic objects, though mostly in vacuum or in liquids. By contrast, due to the light-induced thermal effect, photophoretic force provides an alternative and effective way to transport light-absorbing particles in ambient gases. However, in most cases these forces work independently. Here, by employing the synergy of optical force and photophoretic force, we propose and experimentally demonstrate a configuration which can drive a micron-size metallic plate moving back and forth on a tapered fiber with supercontinuum light in ambient air. Optical pulling and oscillation of the metallic plate are experimentally realized. The results might open exhilarating possibilities in applications of optical driving and energy conversion.

The first ionization potential (IP) and electron affinity (EA) of the gold atom have been determined to an unprecedented accuracy using relativistic coupled cluster calculations up to the pentuple excitation level including the Breit and QED contributions. We reach meV accuracy (with respect to the experimental values) by carefully accounting for all individual contributions beyond the standard relativistic coupled cluster approach. Thus, we are able to resolve the long-standing discrepancy between experimental and theoretical IP and EA of gold.

Excitation and ionization in strong laser fields lies at the heart of such diverse research directions as high-harmonic generation and spectroscopy, laser-induced diffraction imaging, emission of femtosecond electron bunches from nanotips, self-guiding, filamentation and mirrorless lasing during propagation of light in atmospheres. While extensive quantum mechanical and semiclassical calculations on strong-field ionization are well backed by sophisticated experiments, the existing scattered theoretical work aiming at a full quantitative understanding of strong-field excitation lacks experimental confirmation. Here we present experiments on strong-field excitation in both the tunneling and multiphoton regimes and their rigorous interpretation by time dependent Schrödinger equation calculations, which finally consolidates the seemingly opposing strong-field regimes with their complementary pictures. Most strikingly, we observe an unprecedented enhancement of excitation yields, which opens new possibilities in ultrafast strong-field control of Rydberg wave packet excitation and laser intensity characterization.

We experimentally squeeze the thermal motional state of an optically levitated nanosphere by fast switching between two trapping frequencies. The measured phase-space distribution of the center of mass of our particle shows the typical shape of a squeezed thermal state, from which we infer up to 2.7 dB of squeezing along one motional direction. In these experiments the average thermal occupancy is high and, even after squeezing, the motional state remains in the remit of classical statistical mechanics. Nevertheless, we argue that the manipulation scheme described here could be used to achieve squeezing in the quantum regime if preceded by cooling of the levitated mechanical oscillator. Additionally, a higher degree of squeezing could, in principle, be achieved by repeating the frequency-switching protocol multiple times.

We report the first experimental observation of negatively charged hydrogen and deuterium cluster ions, ${\mathrm{H}}_n^{-}$ and ${\mathrm{D}}_n^{-}$, where $n\ge 5$. These anions are formed by an electron addition to liquid helium nanodroplets doped with molecular hydrogen or deuterium. The ions are stable for at least the lifetime of the experiment, which is several tens of microseconds. Only anions with odd values of $n$ are detected, and some specific ions show anomalously high abundances. The sizes of these “magic number” ions suggest an icosahedral framework of ${\mathrm{H}}_2$ (${\mathrm{D}}_2$) molecules in solvent shells around a central ${\mathrm{H}}^{-}$ (${\mathrm{D}}^{-}$) ion. The first three shells, which contain a total of 44 ${\mathrm{H}}_2$ or ${\mathrm{D}}_2$ molecules, appear to be solidlike, but thereafter a more liquidlike arrangement of the ${\mathrm{H}}_2$ (${\mathrm{D}}_2$) molecules is adopted.

The resolution of any spectroscopic or interferometric experiment is ultimately limited by the total time a particle is interrogated. Here we demonstrate the first molecular fountain, a development which permits hitherto unattainably long interrogation times with molecules. In our experiments, ammonia molecules are decelerated and cooled using electric fields, launched upwards with a velocity between 1.4 and 1.9 m/s and observed as they fall back under gravity. A combination of quadrupole lenses and bunching elements is used to shape the beam such that it has a large position spread and a small velocity spread (corresponding to a transverse temperature of $<10\mu \mathrm{K}$ and a longitudinal temperature of $<1\mu \mathrm{K}$) when the molecules are in free fall, while being strongly focused at the detection region. The molecules are in free fall for up to 266 ms, making it possible, in principle, to perform sub-Hz measurements in molecular systems and paving the way for stringent tests of fundamental physics theories.

Ultracold atom-ion mixtures are gaining increasing interest due to their potential applications in ultracold and state-controlled chemistry, quantum computing, and many-body physics. Here, we studied the dynamics of a single ground-state cooled ion during few, to many, Langevin (spiraling) collisions with ultracold atoms. We measured the ion’s energy distribution and observed a clear deviation from the Maxwell-Boltzmann distribution, characterized by an exponential tail, to a power-law distribution best described by a Tsallis function. Unlike previous experiments, the energy scale of atom-ion interactions is not determined by either the atomic cloud temperature or the ion’s trap residual excess-micromotion energy. Instead, it is determined by the force the atom exerts on the ion during a collision which is then amplified by the trap dynamics. This effect is intrinsic to ion Paul traps and sets the lower bound of atom-ion steady-state interaction energy in these systems. Despite the fact that our system is eventually driven out of the ultracold regime, we are capable of studying quantum effects by limiting the interaction to the first collision when the ion is initialized in the ground state of the trap.

A new mechanism of nuclear excitation via two-photon electron transitions (NETP) is proposed and studied theoretically. As a generic example, detailed calculations are performed for the $E1E1$ $1s2s{}^1{S}_0\to 1s^2{}^1{S}_0$ two-photon decay of a He-like ${}^{225}{\mathrm{Ac}}^{87+}$ ion with a resonant excitation of the $3/2+$ nuclear state with an energy of 40.09(5) keV. The probability for such a two-photon decay via the nuclear excitation is found to be $P_{\mathrm{NETP}}=3.5\times {10}^{-9}$ and, thus, is comparable with other mechanisms, such as nuclear excitation by electron transition and by electron capture. The possibility for the experimental observation of the proposed mechanism is thoroughly discussed.

Interferometry using discrete energy levels of nuclear, atomic, or molecular systems is the foundation for a wide range of physical phenomena and enables powerful techniques such as nuclear magnetic resonance, electron spin resonance, Ramsey-based spectroscopy, and laser or maser technology. It also plays a unique role in quantum information processing as qubits may be implemented as energy superposition states of simple quantum systems. Here, we demonstrate quantum interference involving energy states of single quanta of light. In full analogy to the energy levels of atoms or nuclear spins, we implement a Ramsey interferometer with single photons. We experimentally generate energy superposition states of a single photon and manipulate them with unitary transformations to realize arbitrary projective measurements. Our approach opens the path for frequency-encoded photonic qubits in quantum information processing and quantum communication.

We report on the realization of a free-space single-photon absorber, which deterministically absorbs exactly one photon from an input pulse. Our scheme is based on the saturation of an optically thick medium by a single photon due to Rydberg blockade. By converting one absorbed input photon into a stationary Rydberg excitation, decoupled from the light field through fast engineered dephasing, we blockade the full atomic cloud and change our optical medium from opaque to transparent. We show that this results in the subtraction of one photon from the input pulse over a wide range of input photon numbers. We investigate the change of the pulse shape and temporal photon statistics of the transmitted light pulses for different input photon numbers and compare the results to simulations. Based on the experimental results, we discuss the applicability of our single-photon absorber for number resolved photon detection schemes or quantum gate operations.

We observe a dramatic difference in optical line shapes of a ${}^4\mathrm{He}$ Bose-Einstein condensate and a ${}^3\mathrm{He}$ degenerate Fermi gas by measuring the 1557-nm $2{}^{3}S-2{}^{1}S$ magnetic dipole transition (8 Hz natural linewidth) in an optical dipole trap. The 15 kHz FWHM condensate line shape is only broadened by mean field interactions, whereas the degenerate Fermi gas line shape is broadened to 75 kHz FWHM due to the effect of Pauli exclusion on the spatial and momentum distributions. The asymmetric optical line shapes are observed in excellent agreement with line shape models for the quantum degenerate gases. For ${}^4\mathrm{He}$ a triplet-singlet $s$-wave scattering length $a=+50(10{)}_{\mathrm{stat}}(43{)}_{\mathrm{syst}}{a}_0$ is extracted. The high spectral resolution reveals a doublet in the absorption spectrum of the BEC, and this effect is understood by the presence of a weak optical lattice in which a degeneracy of the lattice recoil and the spectroscopy photon recoil leads to Bragg-like scattering.

We demonstrate a quantum gravimeter by combining the advantages of an atom chip for the generation, delta-kick collimation, and coherent manipulation of freely falling Bose-Einstein condensates (BECs) with an innovative launch mechanism based on Bloch oscillations and double Bragg diffraction. Our high-contrast BEC interferometer realizes tens of milliseconds of free fall in a volume as little as a one centimeter cube and paves the way for measurements with sub-$\mu \mathrm{Gal}$ accuracies in miniaturized, robust devices.

Conventional photocells suffer a fundamental efficiency threshold imposed by the principle of detailed balance, reflecting the fact that good absorbers must necessarily also be fast emitters. This limitation can be overcome by “parking” the energy of an absorbed photon in a dark state which neither absorbs nor emits light. Here we argue that suitable dark states occur naturally as a consequence of the dipole-dipole interaction between two proximal optical dipoles for a wide range of realistic molecular dimers. We develop an intuitive model of a photocell comprising two light-absorbing molecules coupled to an idealized reaction center, showing asymmetric dimers are capable of providing a significant enhancement of light-to-current conversion under ambient conditions. We conclude by describing a road map for identifying suitable molecular dimers for demonstrating this effect by screening a very large set of possible candidate molecules.

We demonstrate an efficient cross-phase modulation (XPM) based on a closed-loop double-$\mathrm{\Lambda }$ system. The property of the double-$\mathrm{\Lambda }$ medium can be controlled by changing the phases of the applied optical fields. This phase-dependent XPM scheme can achieve large phase modulations at low-light intensities without requiring cavities or tightly focusing laser beams. With this scheme, we observe a $\pi$-level phase shift with two pulses, both consisting of eight photons in cold rubidium atoms. Such a novel scheme provides a simple route to generate strong interactions between photons and may have potential applications in all-optical quantum signal processing.

Optomechanical systems explore and exploit the coupling between light and the mechanical motion of macroscopic matter. A nonlinear coupling offers rich new physics, in both quantum and classical regimes. We investigate a dynamic, as opposed to the usually studied static, nonlinear optomechanical system, comprising a nanosphere levitated in a hybrid electro-optical trap. The cavity offers readout of both linear-in-position and quadratic-in-position (nonlinear) light-matter coupling, while simultaneously cooling the nanosphere, for indefinite periods of time and in high vacuum. We observe the cooling dynamics via both linear and nonlinear coupling. As the background gas pressure was lowered, we observed a greater than 1000-fold reduction in temperature before temperatures fell below readout sensitivity in the present setup. This Letter opens the way to strongly coupled quantum dynamics between a cavity and a nanoparticle largely decoupled from its environment.

Hydrogen bonding interactions between biological chromophores and their surrounding protein and solvent environment significantly affect the photochemical pathways of the chromophore and its biological function. A common first step in the dynamics of these systems is excited state proton transfer between the noncovalently bound molecules, which stabilizes the system against dissociation and principally alters relaxation pathways. Despite such fundamental importance, studying excited state proton transfer across a hydrogen bond has proven difficult, leaving uncertainties about the mechanism. Through time-resolved photoelectron imaging measurements, we demonstrate how the addition of a single hydrogen bond and the opening of an excited state proton transfer channel dramatically changes the outcome of a photochemical reaction, from rapid dissociation in the isolated chromophore to efficient stabilization and ground state recovery in the hydrogen bonded case, and uncover the mechanism of excited state proton transfer at a hydrogen bond, which follows sequential hydrogen and charge transfer processes.

In optomechanics, electromagnetic fields are harnessed to control a single mode of a mechanically compliant system, while other mechanical degrees of freedom remain unaffected due to the modes’ mutual orthogonality and high quality factor. Extension of the optical control beyond the directly addressed mode would require a controlled coupling between mechanical modes. Here, we introduce an optically controlled coupling between two oscillation modes of an optically levitated nanoparticle. We sympathetically cool one oscillation mode by coupling it coherently to the second mode, which is feedback cooled. Furthermore, we demonstrate coherent energy transfer between mechanical modes and discuss its application for ground-state cooling.