We studied the nanoplasma formation and explosion dynamics of single large xenon clusters in ultrashort, intense x-ray free-electron laser pulses via ion spectroscopy. The simultaneous measurement of single-shot diffraction images enabled a single-cluster analysis that is free from any averaging over the cluster size and laser intensity distributions. The measured charge state-resolved ion energy spectra show narrow distributions with peak positions that scale linearly with final ion charge state. These two distinct signatures are attributed to highly efficient recombination that eventually leads to the dominant formation of neutral atoms in the cluster. The measured mean ion energies exceed the value expected without recombination by more than an order of magnitude, indicating that the energy release resulting from electron-ion recombination constitutes a previously unnoticed nanoplasma heating process. This conclusion is supported by results from semiclassical molecular dynamics simulations.

Observing the motion of the nuclear wave packets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wave packet in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07 Å and temporal resolution of 230 fs full width at half maximum. The method is not only sensitive to the position but also the shape of the nuclear wave packet.

Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine are used to create a movie of intramolecular motion with a temporal and spatial resolution of 30 fs and 0.3 Å. This high fidelity is due to interference between the nonstationary excitation and the stationary initial charge distribution. The initial state is used as the local oscillator for heterodyne amplification of the excited charge distribution to retrieve real-space movies of atomic motion on ångstrom and femtosecond scales. This x-ray interference has not been employed to image internal motion in molecules before. Coherent vibrational motion and dispersion, dissociation, and rotational dephasing are all clearly visible in the data, thereby demonstrating the stunning sensitivity of heterodyne methods.

A power series approximation for the correlation kernel of time-dependent density-functional theory is presented. Using this approximation in the adiabatic-connection fluctuation-dissipation (ACFD) theorem leads to a new family of Kohn-Sham methods. The new methods yield reaction energies and barriers of unprecedented accuracy and enable a treatment of static (strong) correlation with an accuracy of high-level multireference configuration interaction methods but are single-reference methods allowing for a black-box-like handling of static correlation. The new methods exhibit a better scaling of the computational effort with the system size than rivaling wave-function-based electronic structure methods. Moreover, the new methods do not suffer from the problem of singularities in response functions plaguing previous ACFD methods and therefore are applicable to any type of electronic system.

We report experimental observations of a large Bragg reflection from arrays of cold atoms trapped near a one-dimensional nanoscale waveguide. By using an optical lattice in the evanescent field surrounding a nanofiber with a period nearly commensurate with the resonant wavelength, we observe a reflectance of up to 75% for the guided mode. Each atom behaves as a partially reflecting mirror and an ordered chain of about 2000 atoms is sufficient to realize an efficient Bragg mirror. Measurements of the reflection spectra as a function of the lattice period and the probe polarization are reported. The latter shows the effect of the chiral character of nanoscale waveguides on this reflection. The ability to control photon transport in 1D waveguides coupled to spin systems would enable novel quantum network capabilities and the study of many-body effects emerging from long-range interactions.

We present the first experimental realization of coherent Bragg scattering off a one-dimensional system—two strings of atoms strongly coupled to a single photonic mode—realized by trapping atoms in the evanescent field of a tapered optical fiber, which also guides the probe light. We report nearly 12% power reflection from strings containing only about 1000 cesium atoms, an enhancement of 2 orders of magnitude compared to reflection from randomly positioned atoms. This result paves the road towards collective strong coupling in 1D atom-photon systems. Our approach also allows for a straightforward fiber connection between several distant 1D atomic crystals.

Quantum jumps of a qubit are usually observed between its energy eigenstates, also known as its longitudinal pseudospin component. Is it possible, instead, to observe quantum jumps between the transverse superpositions of these eigenstates? We answer positively by presenting the first continuous quantum nondemolition measurement of the transverse component of an individual qubit. In a circuit QED system irradiated by two pump tones, we engineer an effective Hamiltonian whose eigenstates are the transverse qubit states, and a dispersive measurement of the corresponding operator. Such transverse component measurements are a useful tool in the driven-dissipative operation engineering toolbox, which is central to quantum simulation and quantum error correction.

An optically levitated nanoparticle in vacuum is a paradigm optomechanical system for sensing and studying macroscopic quantum mechanics. While its center-of-mass motion has been investigated intensively, its torsional vibration has only been studied theoretically in limited cases. Here we report the first experimental observation of the torsional vibration of an optically levitated nonspherical nanoparticle in vacuum. We achieve this by utilizing the coupling between the spin angular momentum of photons and the torsional vibration of a nonspherical nanoparticle whose polarizability is a tensor. The torsional vibration frequency can be 1 order of magnitude higher than its center-of-mass motion frequency, which is promising for ground state cooling. We propose a simple yet novel scheme to achieve ground state cooling of its torsional vibration with a linearly polarized Gaussian cavity mode. A levitated nonspherical nanoparticle in vacuum will also be an ultrasensitive nanoscale torsion balance with a torque detection sensitivity on the order of ${10}^{-29}\mathrm{N}\mathrm{m}/\sqrt{\mathrm{Hz}}$ under realistic conditions.

After the ionization of a valence electron, the created hole can migrate ultrafast from one end of the molecule to another. Because of the advent of attosecond pulse techniques, the measuring and understanding of charge migration has become a central topic in attosecond science. Here, we pose the hitherto unconsidered question whether ionizing a core electron will also lead to charge migration. It is found that the created hole in the core stays put, but in response to this hole interesting electron dynamics takes place which can lead to intense charge migration in the valence shell. This migration is typically faster than that after the ionization of a valence electron and transpires on a shorter time scale than the natural decay of the core hole by the Auger process, making the subject very challenging to attosecond science.

We report measurements of energy-dependent photoionization delays between the two outermost valence shells of ${\mathrm{N}}_2\mathrm{O}$ and ${\mathrm{H}}_2\mathrm{O}$. The combination of single-shot signal referencing with the use of different metal foils to filter the attosecond pulse train enables us to extract delays from congested spectra. Remarkably large delays up to 160 as are observed in ${\mathrm{N}}_2\mathrm{O}$, whereas the delays in ${\mathrm{H}}_2\mathrm{O}$ are all smaller than 50 as in the photon-energy range of 20–40 eV. These results are interpreted by developing a theory of molecular photoionization delays. The long delays measured in ${\mathrm{N}}_2\mathrm{O}$ are shown to reflect the population of molecular shape resonances that trap the photoelectron for a duration of up to $\sim 110$ as. The unstructured continua of ${\mathrm{H}}_2\mathrm{O}$ result in much smaller delays at the same photon energies. Our experimental and theoretical methods make the study of molecular attosecond photoionization dynamics accessible.

Long-range metastable molecules consisting of two cesium atoms in high Rydberg states have been observed in an ultracold gas. A sequential three-photon two-color photoassociation scheme is employed to form these molecules in states, which correlate to $np(n+1)s$ dissociation asymptotes. Spectral signatures of bound molecular states are clearly resolved at the positions of avoided crossings between long-range van der Waals potential curves. The experimental results are in agreement with simulations based on a detailed model of the long-range multipole-multipole interactions of Rydberg-atom pair states. We show that a full model is required to accurately predict the occurrence of bound Rydberg macrodimers. The macrodimers are distinguished from repulsive molecular states by their behavior with respect to spontaneous ionization and possible decay channels are discussed.

We prepare number stabilized ultracold atom clouds through the real-time analysis of nondestructive images and the application of feedback. In our experiments, the atom number $N\sim 10^6$ is determined by high precision Faraday imaging with uncertainty $\mathrm{\Delta }N$ below the shot noise level, i.e., $\mathrm{\Delta }N<\sqrt{N}$. Based on this measurement, feedback is applied to reduce the atom number to a user-defined target, whereupon a second imaging series probes the number stabilized cloud. By this method, we show that the atom number in ultracold clouds can be prepared below the shot noise level.

We consider two separate atoms interacting with a single-mode optical or microwave resonator. When the frequency of the resonator field is twice the atomic transition frequency, we show that there exists a resonant coupling between one photon and two atoms, via intermediate virtual states connected by counterrotating processes. If the resonator is prepared in its one-photon state, the photon can be jointly absorbed by the two atoms in their ground state which will both reach their excited state with a probability close to one. Like ordinary quantum Rabi oscillations, this process is coherent and reversible, so that two atoms in their excited state will undergo a downward transition jointly emitting a single cavity photon. This joint absorption and emission process can also occur with three atoms. The parameters used to investigate this process correspond to experimentally demonstrated values in circuit quantum electrodynamics systems.

We realize a single particle microscope by using deterministically extracted laser-cooled ${}^{40}{\mathrm{Ca}}^{+}$ ions from a Paul trap as probe particles for transmission imaging. We demonstrate focusing of the ions to a spot size of $5.8\pm 1.0\mathrm{nm}$ and a minimum two-sample deviation of the beam position of 1.5 nm in the focal plane. The deterministic source, even when used in combination with an imperfect detector, gives rise to a fivefold increase in the signal-to-noise ratio as compared with conventional Poissonian sources. Gating of the detector signal by the extraction event suppresses dark counts by 6 orders of magnitude. We implement a Bayes experimental design approach to microscopy in order to maximize the gain in spatial information. We demonstrate this method by determining the position of a $1\mu \mathrm{m}$ circular hole structure to a precision of 2.7 nm using only 579 probe particles.

We report a test of the universality of free fall by comparing the gravity acceleration of the ${}^{87}\mathrm{Rb}$ atoms in $m_F=+1$ versus those in $m_F=-1$, of which the corresponding spin orientations are opposite. A Mach-Zehnder-type atom interferometer is exploited to alternately measure the free fall acceleration of the atoms in these two magnetic sublevels, and the resultant Eötvös ratio is ${\eta }_S=(0.2\pm 1.2)\times {10}^{-7}$. This also gives an upper limit of $5.4\times {10}^{-6}{\mathrm{m}}^{-2}$ for a possible gradient field of the spacetime torsion. The interferometer using atoms in $m_F=\pm 1$ is highly sensitive to the magnetic field inhomogeneity. A double differential measurement method is developed to alleviate the inhomogeneity influence, of which the effectiveness is validated by a magnetic field modulating experiment.

We experimentally demonstrate a nonlinear detection scheme exploiting time-reversal dynamics that disentangles continuous variable entangled states for feasible readout. Spin-exchange dynamics of Bose-Einstein condensates is used as the nonlinear mechanism which not only generates entangled states but can also be time reversed by controlled phase imprinting. For demonstration of a quantum-enhanced measurement we construct an active atom SU(1,1) interferometer, where entangled state preparation and nonlinear readout both consist of parametric amplification. This scheme is capable of exhausting the quantum resource by detecting solely mean atom numbers. Controlled nonlinear transformations widen the spectrum of useful entangled states for applied quantum technologies.

The surface temperature dependence of the ortho-to-para conversion of ${\mathrm{H}}_2$ on amorphous solid water is first reported. A combination of photostimulated desorption and resonance-enhanced multiphoton ionization techniques allowed us to sensitively probe the conversion on the surface of amorphous solid water at temperatures of 9.2–16 K. Within a narrow temperature window of 8 K, the conversion time steeply varied from $\sim 4.1\times {10}^3$ to $\sim 6.4\times {10}^2\mathrm{s}$. The observed temperature dependence is discussed in the context of previously suggested models and the energy dissipation process. The two-phonon process most likely dominates the conversion rate at low temperatures.

We develop an approach to generate finite-range atomic interactions via optical Rydberg-state excitation and study the underlying excitation dynamics in theory and experiment. In contrast to previous work, the proposed scheme is based on resonant optical driving and the establishment of a dark state under conditions of electromagnetically induced transparency (EIT). Analyzing the driven dissipative dynamics of the atomic gas, we show that the interplay between coherent light coupling, radiative decay, and strong Rydberg-Rydberg atom interactions leads to the emergence of sizable effective interactions while providing remarkably long coherence times. The latter are studied experimentally in a cold gas of strontium atoms for which the proposed scheme is most efficient. Our measured atom loss is in agreement with the theoretical prediction based on binary effective interactions between the driven atoms.

The momentum transfer between a photon and an object defines a fundamental limit for the precision with which the object can be measured. If the object oscillates at a frequency ${\mathrm{\Omega }}_0$, this measurement backaction adds quanta $\hslash {\mathrm{\Omega }}_0$ to the oscillator’s energy at a rate ${\mathrm{\Gamma }}_{\text{recoil}}$, a process called photon recoil heating, and sets bounds to coherence times in cavity optomechanical systems. Here, we use an optically levitated nanoparticle in ultrahigh vacuum to directly measure ${\mathrm{\Gamma }}_{\text{recoil}}$. By means of a phase-sensitive feedback scheme, we cool the harmonic motion of the nanoparticle from ambient to microkelvin temperatures and measure its reheating rate under the influence of the radiation field. The recoil heating rate is measured for different particle sizes and for different excitation powers, without the need for cavity optics or cryogenic environments. The measurements are in quantitative agreement with theoretical predictions and provide valuable guidance for the realization of quantum ground-state cooling protocols and the measurement of ultrasmall forces.

We measure the coherent scattering of light by a cloud of laser-cooled atoms with a size comparable to the wavelength of light. By interfering a laser beam tuned near an atomic resonance with the field scattered by the atoms, we observe a resonance with a redshift, a broadening, and a saturation of the extinction for increasing atom numbers. We attribute these features to enhanced light-induced dipole-dipole interactions in a cold, dense atomic ensemble that result in a failure of standard predictions such as the “cooperative Lamb shift”. The description of the atomic cloud by a mean-field model based on the Lorentz-Lorenz formula that ignores scattering events where light is scattered recurrently by the same atom and by a microscopic discrete dipole model that incorporates these effects lead to progressively closer agreement with the observations, despite remaining differences.