The electric dipole moments of ${({\mathrm{H}}_2\mathrm{O})}_n\mathrm{DCl}$ ($n=3–9$) clusters have been measured by the beam-deflection method. Reflecting the (dynamical) charge distribution within the system, the dipole moment contributes information about the microscopic structure of nanoscale solvation. The addition of a DCl molecule to a water cluster results in a strongly enhanced susceptibility. There is evidence for a noticeable rise in the dipole moment occurring at $n\approx 5–6$. This size is consistent with predictions for the onset of ionic dissociation. Additionally, a molecular-dynamics model suggests that even with a nominally bound impurity an enhanced dipole moment can arise due to the thermal and zero-point motion of the proton and the water molecules. The experimental measurements and the calculations draw attention to the importance of fluctuations in defining the polarity of water-based nanoclusters and generally to the essential role played by motional effects in determining the response of fluxional nanoscale systems under realistic conditions.

This Letter reports the demonstration of laser cooling without spontaneous emission, and thereby addresses a significant controversy. It works by restricting the atom-light interaction to a time short compared to a cycle of absorption followed by natural decay. It is achieved by using the bichromatic force on an atomic transition with a relatively long excited state lifetime and a relatively short cooling time so that spontaneous emission effects are minimized. The observed width of the one-dimensional velocity distribution is reduced by $\times 2$ thereby reducing the “temperature” by $\times 4$. Moreover, our results comprise a compression in phase space because the spatial expansion of the atomic sample is limited. This accomplishment is of interest to direct laser cooling of molecules or in experiments where working space or time is limited.

Optomechanical coupling between a light field and the motion of a cavity mirror via radiation pressure plays an important role for the exploration of macroscopic quantum physics and for the detection of gravitational waves (GWs). It has been used to cool mechanical oscillators into their quantum ground states and has been considered to boost the sensitivity of GW detectors, e.g., via the optical spring effect. Here, we present the experimental characterization of generalized, that is, dispersive and dissipative, optomechanical coupling, with a macroscopic $(1.5\mathrm{mm}{)}^2$-size silicon nitride membrane in a cavity-enhanced Michelson-type interferometer. We report for the first time strong optomechanical cooling based on dissipative coupling, even on cavity resonance, in excellent agreement with theory. Our result will allow for new experimental regimes in macroscopic quantum physics and GW detection.

For atoms or molecules in optical lattices, conventional thermometry methods are often unsuitable due to low particle numbers or a lack of cycling transitions. However, a differential spectroscopic light shift can map temperature onto the line shape with a low sensitivity to trap anharmonicity. We study narrow molecular transitions to demonstrate precise frequency-based lattice thermometry, as well as carrier cooling. This approach should be applicable down to nanokelvin temperatures. We also discuss how the thermal light shift can affect the accuracy of optical lattice clocks.

We report on the observation of cooperative radiation of exactly two neutral atoms strongly coupled to the single mode field of an optical cavity, which is close to the lossless-cavity limit. Monitoring the cavity output power, we observe constructive and destructive interference of collective Rayleigh scattering for certain relative distances between the two atoms. Because of cavity backaction onto the atoms, the cavity output power for the constructive two-atom case ($N=2$) is almost equal to the single-emitter case ($N=1$), which is in contrast to free-space where one would expect an $N^2$ scaling of the power. These effects are quantitatively explained by a classical model as well as by a quantum mechanical model based on Dicke states. We extract information on the relative phases of the light fields at the atom positions and employ advanced cooling to reduce the jump rate between the constructive and destructive atom configurations. Thereby we improve the control over the system to a level where the implementation of two-atom entanglement schemes involving optical cavities becomes realistic.

We prepare a maximally entangled state of two ions and couple both ions to the mode of an optical cavity. The phase of the entangled state determines the collective interaction of the ions with the cavity mode, that is, whether the emission of a single photon into the cavity is suppressed or enhanced. By adjusting this phase, we tune the ion-cavity system from sub- to superradiance. We then encode a single qubit in the two-ion superradiant state and show that this encoding enhances the transfer of quantum information onto a photon.

Single, double, and triple ionization of ${\mathrm{C}}^{1+}$ ions by single photons is investigated in the energy range of 286–326 eV, i.e., in the range from the lowest-energy $K$-vacancy resonances to well beyond the $K$-shell ionization threshold. Clear signatures of ${\mathrm{C}}^{1+}(1s2s^{2}2p^2{}^{2}D,{}^{2}P)$ resonances are found in the triple-ionization channel. The only possible mechanism producing ${\mathrm{C}}^{4+}(1s^2)$ via these resonances is direct triple-Auger decay, i.e., a four-electron process with simultaneous emission of three electrons.

We present the first direct measurement of the gravity-field curvature based on three conjugated atom interferometers. Three atomic clouds launched in the vertical direction are simultaneously interrogated by the same atom interferometry sequence and used to probe the gravity field at three equally spaced positions. The vertical component of the gravity-field curvature generated by nearby source masses is measured from the difference between adjacent gravity gradient values. Curvature measurements are of interest in geodesy studies and for the validation of gravitational models of the surrounding environment. The possibility of using such a scheme for a new determination of the Newtonian constant of gravity is also discussed.

We demonstrate preparation and detection of an atom number distribution in a one-dimensional atomic lattice with the variance $-14\mathrm{dB}$ below the Poissonian noise level. A mesoscopic ensemble containing a few thousand atoms is trapped in the evanescent field of a nanofiber. The atom number is measured through dual-color homodyne interferometry with a pW-power shot noise limited probe. Strong coupling of the evanescent probe guided by the nanofiber allows for a real-time measurement with a precision of $\pm 8\mathrm{atoms}$ on an ensemble of some $10^3\mathrm{atoms}$ in a one-dimensional trap. The method is very well suited for generating collective atomic entangled or spin-squeezed states via a quantum nondemolition measurement as well as for tomography of exotic atomic states in a one-dimensional lattice.

Spin impurities in diamond can be versatile tools for a wide range of solid-state-based quantum technologies, but finding spin impurities that offer sufficient quality in both photonic and spin properties remains a challenge for this pursuit. The silicon-vacancy center has recently attracted much interest because of its spin-accessible optical transitions and the quality of its optical spectrum. Complementing these properties, spin coherence is essential for the suitability of this center as a spin-photon quantum interface. Here, we report all-optical generation of coherent superpositions of spin states in the ground state of a negatively charged silicon-vacancy center using coherent population trapping. Our measurements reveal a characteristic spin coherence time, $T_2^{*}$, exceeding 45 nanoseconds at 4 K. We further investigate the role of phonon-mediated coupling between orbital states as a source of irreversible decoherence. Our results indicate the feasibility of all-optical coherent control of silicon-vacancy spins using ultrafast laser pulses.

The silicon-vacancy (${\mathrm{SiV}}^{-}$) color center in diamond has attracted attention because of its unique optical properties. It exhibits spectral stability and indistinguishability that facilitate efficient generation of photons capable of demonstrating quantum interference. Here we show optical initialization and readout of electronic spin in a single ${\mathrm{SiV}}^{-}$ center with a spin relaxation time of $T_1=2.4\pm 0.2\mathrm{ms}$. Coherent population trapping (CPT) is used to demonstrate coherent preparation of dark superposition states with a spin coherence time of $T_2^{\star }=35\pm 3\mathrm{ns}$. This is fundamentally limited by orbital relaxation, and an understanding of this process opens the way to extend coherence by engineering interactions with phonons. Hyperfine structure is observed in CPT measurements with the ${}^{29}\mathrm{Si}$ isotope which allows access to nuclear spin. These results establish the ${\mathrm{SiV}}^{-}$ center as a solid-state spin-photon interface.

We present a novel method for probing the alignment of the molecular axis of an ultracold, nonpolar dimer. These results are obtained using diatomic ${}^{87}{\mathrm{Rb}}_2$ molecules in the vibrational ground state of the lowest triplet potential $a^3{\mathrm{\Sigma }}_u^{+}$ trapped in a 3D optical lattice. We measure the molecular polarizabilities, which are directly linked to the alignment, along each of the $x$, $y$, and $z$ directions of the lab coordinate system. By preparing the molecules in various, precisely defined rotational quantum states we can control the degree of alignment of the molecular axis with high precision over a large range. Furthermore, we derive the dynamical polarizabilities for a laser wavelength of 1064.5 nm parallel and orthogonal to the molecular axis of the dimer, ${\alpha }_{\parallel }=(8.9\pm 0.9)\times 10^3\mathrm{a}.\mathrm{u}.$ and ${\alpha }_{\perp }=(0.9\pm 0.4)\times 10^3\mathrm{a}.\mathrm{u}.$, respectively. Our findings highlight that the depth of an optical lattice strongly depends on the rotational state of the molecule, which has to be considered in collision experiments. The present work paves the way for reaction studies between aligned molecules in the ultracold temperature regime.

Extending the range of quantum interferometry to a wider class of composite nanoparticles requires new tools to diffract matter waves. Recently, pulsed photoionization light gratings have demonstrated their suitability for high mass matter-wave physics. Here, we extend quantum interference experiments to a new class of particles by introducing photofragmentation beam splitters into time-domain matter-wave interferometry. We present data that demonstrate this coherent beam splitting mechanism with clusters of hexafluorobenzene and we show single-photon depletion gratings based both on fragmentation and ionization for clusters of vanillin. We propose that photofragmentation gratings can act on a large set of van der Waals clusters and biomolecules which are thermally unstable and often resilient to single-photon ionization.

An intense phase-controlled orthogonally polarized two-color ultrashort laser pulse is used to singly ionize and dissociate ${\mathrm{H}}_2$ into a neutral hydrogen atom and a proton. Emission-direction and kinetic-energy dependent asymmetric dissociation of ${\mathrm{H}}_2$ is observed as a function of the relative phase of the orthogonally polarized two-color pulse. Significant asymmetric proton emission is measured in the direction between two polarization axes. Our numerical simulations of the time-dependent Schrödinger equation reproduce many of the observed features. The asymmetry is attributed to the coherent superposition of two-dimensional nuclear wave packets with opposite parities, which have the same energies and overlap in the same emission directions.

According to quantum electrodynamics, the exchange of virtual photons in a system of identical quantum emitters causes a shift of its energy levels. Such shifts, known as cooperative Lamb shifts, have been studied mostly in the near-field regime. However, the resonant electromagnetic interaction persists also at large distances, providing coherent coupling between distant atoms. Here, we report a direct spectroscopic observation of the cooperative Lamb shift of an optical electric-dipole transition in an array of ${\mathrm{Sr}}^{+}$ ions suspended in a Paul trap at inter-ion separations much larger than the resonance wavelength. By controlling the precise positions of the ions, we studied the far-field resonant coupling in chains of up to eight ions, extending to a length of $40\mu \mathrm{m}$. This method provides a novel tool for experimental exploration of cooperative emission phenomena in extended mesoscopic atomic arrays.

Harnessing nonlinearities strong enough to allow single photons to interact with one another is not only a fascinating challenge but also central to numerous advanced applications in quantum information science. Here we report the nonlinear interaction between two single photons. Each photon is generated in independent parametric down-conversion sources. They are subsequently combined in a nonlinear waveguide where they are converted into a single photon of higher energy by the process of sum-frequency generation. Our approach results in the direct generation of photon triplets. More generally, it highlights the potential for quantum nonlinear optics with integrated devices and, as the photons are at telecom wavelengths, it opens the way towards novel applications in quantum communication such as device-independent quantum key distribution.

Atomic comagnetometers are widely used in precision measurements searching for spin interactions beyond the standard model. We describe a new ${}^3\mathrm{He}\text{−}{}^{129}\mathrm{Xe}$ comagnetometer probed by Rb atoms and use it to identify two general classes of systematic effects in gas comagnetometers, one associated with diffusion in second-order magnetic-field gradients and another due to temperature gradients. We also develop and confirm experimentally a general and practical approach for calculating spin relaxation and frequency shifts due to arbitrary magnetic-field gradients.

We demonstrate a way to prepare single photons with a temporal envelope that resembles the time reversal of photons from the spontaneous decay process. We use the photon pairs generated from a time-ordered cascade decay: the detection of the first photon of the cascade is used as a herald for the ground-state transition resonant second photon. We show how the interaction of the heralding photon with an asymmetric Fabry-Perot cavity reverses the temporal shape of its twin photon from a decaying to a rising exponential envelope. This single photon is expected to be ideal for interacting with two-level systems.

Line intensities and oscillator strengths for the controversial $3C$ and $3D$ astrophysically relevant lines in neonlike ${\mathrm{Fe}}^{16+}$ ions are calculated. A large-scale configuration-interaction calculation of oscillator strengths is performed with the inclusion of higher-order electron-correlation effects, suggesting that these contributions cannot explain existing discrepancies between theory and experiment. Then, we investigate nonlinear dynamical effects, showing that, for strong x-ray sources, the modeling of the spectral lines by a peak with an area proportional to the oscillator strength is not sufficient. The dynamical effects give a possible resolution of discrepancies of theory and experiment found by recent measurements, which motivates the use of light-matter interaction models also valid for strong light fields in the analysis and interpretation of astrophysical and laboratory spectra.

We demonstrate cavity QED conditions in the Purcell regime for single quantum emitters on the surface of an optical nanofiber. The cavity is formed by combining an optical nanofiber and a nanofabricated grating to create a composite photonic crystal cavity. By using this technique, significant enhancement of the spontaneous emission rate into the nanofiber guided modes is observed for single quantum dots. Our results pave the way for enhanced on-fiber light-matter interfaces with clear applications to quantum networks.