Tuning hard x-ray excitation energy along Cl $1s\to {\sigma }^{*}$ resonance in gaseous HCl allows manipulating molecular fragmentation in the course of the induced multistep ultrafast dissociation. The observations are supported by theoretical modeling, which shows a strong interplay between the topology of the potential energy curves, involved in the Auger cascades, and the so-called core-hole clock, which determines the time spent by the system in the very first step. The asymmetric profile of the fragmentation ratios reflects different dynamics of nuclear wave packets dependent on the photon energy.

We demonstrate cavity cooling of all motional degrees of freedom of an atomic ensemble using light that is far detuned from the atomic transitions by several gigahertz. The cooling is achieved by cavity-induced frequency-dependent asymmetric enhancement of the atomic emission spectrum, thereby extracting thermal kinetic energy from the atomic system. Within 100 ms, the atomic temperature is reduced from 200 to $10\mu \mathrm{K}$, where the final temperature is mainly limited by the linewidth of the cavity. In principle, the technique can be applied to molecules and atoms with complex internal energy structure.

Spacetime curvature induces tidal forces on the wave function of a single quantum system. Using a dual light-pulse atom interferometer, we measure a phase shift associated with such tidal forces. The macroscopic spatial superposition state in each interferometer (extending over 16 cm) acts as a nonlocal probe of the spacetime manifold. Additionally, we utilize the dual atom interferometer as a gradiometer for precise gravitational measurements.

We perform magnetically assisted Sisyphus laser cooling of the triatomic free radical strontium monohydroxide (SrOH). This is achieved with principal optical cycling in the rotationally closed $P(N^{\prime \prime }=1)$ branch of either the ${\tilde{X}}^2{\mathrm{\Sigma }}^{+}(000)\leftrightarrow {\tilde{A}}^2{\mathrm{\Pi }}_{1/2}(000)$ or the ${\tilde{X}}^2{\mathrm{\Sigma }}^{+}(000)\leftrightarrow {\tilde{B}}^2{\mathrm{\Sigma }}^{+}(000)$ vibronic transitions. Molecules lost into the excited vibrational states during the cooling process are repumped back through the $\tilde{B}(000)$ state for both the (100) level of the Sr-O stretching mode and the $(02^{0}0)$ level of the bending mode. The transverse temperature of a SrOH molecular beam is reduced in one dimension by 2 orders of magnitude to $\sim 750\mu \mathrm{K}$. This approach opens a path towards creating a variety of ultracold polyatomic molecules by means of direct laser cooling.

We introduce a method for the verification of nonclassical light which is independent of the complex interaction between the generated light and the material of the detectors. This is accomplished by means of a multiplexing arrangement. Its theoretical description yields that the coincidence statistics of this measurement layout is a mixture of multinomial distributions for any classical light field and any type of detector. This allows us to formulate bounds on the statistical properties of classical states. We apply our directly accessible method to heralded multiphoton states which are detected with a single multiplexing step only and two detectors, which are in our work superconducting transition-edge sensors. The nonclassicality of the generated light is verified and characterized through the violation of the classical bounds without the need for characterizing the used detectors.

We present an exact single-electron picture that describes the correlated electron dynamics in strong laser fields. Our approach is based on the factorization of the electronic wave function as a product of a marginal and a conditional amplitude. The marginal amplitude, which depends only on one electronic coordinate and yields the exact one-electron density and current density, obeys a time-dependent Schrödinger equation with an effective time-dependent potential. The exact equations are used to derive an approximation that is a step towards general and feasible ab initio single-electron calculations for molecules. The derivation also sheds new light on the usual interpretation of the single-active electron approximation. From the study of model systems, we find that the exact and approximate single-electron potentials for processes with negligible two-electron ionization lead to qualitatively similar dynamics, but that the ionization barrier in the exact single-electron potential may be explicitly time dependent.

We demonstrate matter-wave interference in a warm vapor of rubidium atoms. Established approaches to light-pulse atom interferometry rely on laser cooling to concentrate a large ensemble of atoms into a velocity class resonant with the atom optical light pulse. In our experiment, we show that clear interference signals may be obtained without laser cooling. This effect relies on the Doppler selectivity of the atom interferometer resonance. This interferometer may be configured to measure accelerations, and we demonstrate that multiple interferometers may be operated simultaneously by addressing multiple velocity classes.

Multiparticle quantum interference is critical for our understanding and exploitation of quantum information, and for fundamental tests of quantum mechanics. A remarkable example of multi-partite correlations is exhibited by the Greenberger-Horne-Zeilinger (GHZ) state. In a GHZ state, three particles are correlated while no pairwise correlation is found. The manifestation of these strong correlations in an interferometric setting has been studied theoretically since 1990 but no three-photon GHZ interferometer has been realized experimentally. Here we demonstrate three-photon interference that does not originate from two-photon or single photon interference. We observe phase-dependent variation of three-photon coincidences with $(92.7\pm 4.6)\%$ visibility in a generalized Franson interferometer using energy-time entangled photon triplets. The demonstration of these strong correlations in an interferometric setting provides new avenues for multiphoton interferometry, fundamental tests of quantum mechanics, and quantum information applications in higher dimensions.

Quantum interference of two independent particles in pure quantum states is fully described by the particles’ distinguishability: the closer the particles are to being identical, the higher the degree of quantum interference. When more than two particles are involved, the situation becomes more complex and interference capability extends beyond pairwise distinguishability, taking on a surprisingly rich character. Here, we study many-particle interference using three photons. We show that the distinguishability between pairs of photons is not sufficient to fully describe the photons’ behavior in a scattering process, but that a collective phase, the triad phase, plays a role. We are able to explore the full parameter space of three-photon interference by generating heralded single photons and interfering them in a fiber tritter. Using multiple degrees of freedom—temporal delays and polarization—we isolate three-photon interference from two-photon interference. Our experiment disproves the view that pairwise two-photon distinguishability uniquely determines the degree of nonclassical many-particle interference.

The shot-noise limited peak sensitivity of cavity-enhanced interferometric measurement devices, such as gravitational-wave detectors, can be improved by increasing the cavity finesse, even when comparing fixed intracavity light powers. For a fixed light power inside the detector, this comes at the price of a proportional reduction in the detection bandwidth. High sensitivity over a large span of signal frequencies, however, is essential for astronomical observations. It is possible to overcome this standard sensitivity-bandwidth limit using nonclassical correlations in the light field. Here, we investigate the internal squeezing approach, where the parametric amplification process creates a nonclassical correlation directly inside the interferometer cavity. We theoretically analyze the limits of the approach and measure 36% increase in the sensitivity-bandwidth product compared to the classical case. To our knowledge, this is the first experimental demonstration of an improvement in the sensitivity-bandwidth product using internal squeezing, opening the way for a new class of optomechanical force sensing devices.

Photon blockade is a dynamical quantum-nonlinear effect in driven systems with an anharmonic energy ladder. For a single atom strongly coupled to an optical cavity, we show that atom driving gives a decisively larger optical nonlinearity than cavity driving. This enhances single-photon blockade and allows for the implementation of two-photon blockade where the absorption of two photons suppresses the absorption of further photons. As a signature, we report on three-photon antibunching with simultaneous two-photon bunching observed in the light emitted from the cavity. Our experiment constitutes a significant step towards multiphoton quantum-nonlinear optics.

We describe a quantum state transfer protocol, where a quantum state of photons stored in a first cavity can be faithfully transferred to a second distant cavity via an infinite 1D waveguide, while being immune to arbitrary noise (e.g., thermal noise) injected into the waveguide. We extend the model and protocol to a cavity QED setup, where atomic ensembles, or single atoms representing quantum memory, are coupled to a cavity mode. We present a detailed study of sensitivity to imperfections, and apply a quantum error correction protocol to account for random losses (or additions) of photons in the waveguide. Our numerical analysis is enabled by matrix product state techniques to simulate the complete quantum circuit, which we generalize to include thermal input fields. Our discussion applies both to photonic and phononic quantum networks.

We report on the creation of homogeneous Fermi gases of ultracold atoms in a uniform potential. In the momentum distribution of a spin-polarized gas, we observe the emergence of the Fermi surface and the saturated occupation of one particle per momentum state: the striking consequence of Pauli blocking in momentum space for a degenerate gas. Cooling a spin-balanced Fermi gas at unitarity, we create homogeneous superfluids and observe spatially uniform pair condensates. For thermodynamic measurements, we introduce a hybrid potential that is harmonic in one dimension and uniform in the other two. The spatially resolved compressibility reveals the superfluid transition in a spin-balanced Fermi gas, saturation in a fully polarized Fermi gas, and strong attraction in the polaronic regime of a partially polarized Fermi gas.

Analytic results for (Q)ED processes in external fields are limited to a few special cases, such as plane waves. However, the strong focusing of intense laser fields implies a need to go beyond the plane wave model. By exploiting Poincaré symmetry and superintegrability we show how to construct, and solve without approximation, new models of laser-matter interactions. We illustrate the method with a model of a radially polarized (TM) laser beam, for which we exactly determine the classical orbits and quantum wave functions. Including in this way the effects of transverse field structure should improve predictions and analyses for experiments at intense laser facilities.

We report on experiments which show that ${\mathrm{C}}_{60}$ can ionize in an indirect, quasithermal boiloff process after absorption of a single photon. The process involves a large number of incoherently excited valence electrons and yields electron spectra with a Boltzmann distribution with temperatures exceeding ${10}^4\mathrm{K}$. It is expected to be present for other molecules and clusters with a comparatively large number of valence electrons. The astrophysical consequences are briefly discussed.

The electronic stopping cross sections (SCS) of Ta and Gd for slow protons have been investigated experimentally. The data are compared to the results for Pt and Au to learn how electronic stopping in transition and rare earth metals correlates with features of the electronic band structures. The extraordinarily high SCS observed for protons in Ta and Gd cannot be understood in terms of a free electron gas model, but are related to the high densities of both occupied and unoccupied electronic states in these metals.

We have demonstrated that a supersonic beam of methyl radicals (${\mathrm{CH}}_3$) in the ground rotational state of both para and ortho species has been slowed down to standstill with a magnetic molecular decelerator, and successfully captured spatially in an anti-Helmholtz magnetic trap for $>1\mathrm{s}$. The trapped ${\mathrm{CH}}_3$ radicals have a mean translational temperature of about 200 mK with an estimated density of $>5.0\times 10^7{\mathrm{cm}}^{-3}$. The methyl radical is an ideal system for the study of cold molecules not only because of its high reactivities at low temperatures, but also because further cooling below 1 mK is plausible via sympathetic cooling with ultracold atoms. The demonstrated trapping capability of methyl radicals opens up various possibilities for realizing ultracold ensembles of molecules towards Bose-Einstein condensation of polyatomic molecules and investigations of reactions governed by quantum statistics.

We show that a laser pulse can always be found that induces a desired optical response from an arbitrary dynamical system. As illustrations, driving fields are computed to induce the same optical response from a variety of distinct systems (open and closed, quantum and classical). As a result, the observed induced dipolar spectra without detailed information on the driving field are not sufficient to characterize atomic and molecular systems. The formulation may also be applied to design materials with specified optical characteristics. These findings reveal unexplored flexibilities of nonlinear optics.

We employ radio-frequency spectroscopy to investigate a polarized spin mixture of ultracold ${}^6\mathrm{Li}$ atoms close to a broad Feshbach scattering resonance. Focusing on the regime of strong repulsive interactions, we observe well-defined coherent quasiparticles even for unitarity-limited interactions. We characterize the many-body system by extracting the key properties of repulsive Fermi polarons: the energy $E_{+}$, the effective mass $m^{*}$, the residue $Z$, and the decay rate $\mathrm{\Gamma }$. Above a critical interaction, $E_{+}$ is found to exceed the Fermi energy of the bath, while $m^{*}$ diverges and even turns negative, thereby indicating that the repulsive Fermi liquid state becomes energetically and thermodynamically unstable.

We present a transportable optical clock (TOC) with ${}^{87}\mathrm{Sr}$. Its complete characterization against a stationary lattice clock resulted in a systematic uncertainty of $7.4\times {10}^{-17}$, which is currently limited by the statistics of the determination of the residual lattice light shift, and an instability of $1.3\times {10}^{-15}/\sqrt{\tau }$ with an averaging time $\tau$ in seconds. Measurements confirm that the systematic uncertainty can be reduced to below the design goal of $1\times {10}^{-17}$. To our knowledge, these are the best uncertainties and instabilities reported for any transportable clock to date. For autonomous operation, the TOC has been installed in an air-conditioned car trailer. It is suitable for chronometric leveling with submeter resolution as well as for intercontinental cross-linking of optical clocks, which is essential for a redefinition of the International System of Units (SI) second. In addition, the TOC will be used for high precision experiments for fundamental science that are commonly tied to precise frequency measurements and its development is an important step to space-borne optical clocks.