Describing the dynamics of nuclei in molecules requires a potential energy surface, which is traditionally provided by the Born-Oppenheimer or adiabatic approximation. However, we also need to assign masses to the nuclei. There, the Born-Oppenheimer picture does not account for the inertia of the electrons, and only bare nuclear masses are considered. Nowadays, experimental accuracy challenges the theoretical predictions of rotational and vibrational spectra and requires the participation of electrons in the internal motion of the molecule. More than 80 years after the original work of Born and Oppenheimer, this issue has still not been solved, in general. Here, we present a theoretical and numerical framework to address this problem in a general and rigorous way. Starting from the exact factorization of the electron-nuclear wave function, we include electronic effects beyond the Born-Oppenheimer regime in a perturbative way via position-dependent corrections to the bare nuclear masses. This maintains an adiabaticlike point of view: The nuclear degrees of freedom feel the presence of the electrons via a single potential energy surface, whereas the inertia of electrons is accounted for and the total mass of the system is recovered. This constitutes a general framework for describing the mass acquired by slow degrees of freedom due to the inertia of light, bounded particles; thus, it is applicable not only in electron-nuclear systems but in light-heavy nuclei or ions as well. We illustrate this idea with a model of proton transfer, where the light particle is the proton and the heavy particles are the oxygen atoms to which the proton is bounded. Inclusion of the light-particle inertia allows us to gain orders of magnitude in accuracy. The electron-nuclear perspective is adopted, instead, to calculate position-dependent mass corrections using density functional theory for a few polyatomic molecules at their equilibrium geometry. These data can serve as input for the computation of high-precision molecular spectra.

We introduce the time-dependent variational Monte Carlo method for continuous-space Bose gases. Our approach is based on the systematic expansion of the many-body wave function in terms of multibody correlations and is essentially exact up to adaptive truncation. The method is benchmarked by comparison to an exact Bethe ansatz or existing numerical results for the integrable Lieb-Liniger model. We first show that the many-body wave function achieves high precision for ground-state properties, including energy and first-order as well as second-order correlation functions. Then, we study the out-of-equilibrium, unitary dynamics induced by a quantum quench in the interaction strength. Our time-dependent variational Monte Carlo results are benchmarked by comparison to exact Bethe ansatz results available for a small number of particles, and are also compared to quench action results available for noninteracting initial states. Moreover, our approach allows us to study large particle numbers and general quench protocols, previously inaccessible beyond the mean-field level. Our results suggest that it is possible to find correlated initial states for which the long-term dynamics of local density fluctuations is close to the predictions of a simple Boltzmann ensemble.

We measure entropy and short-range correlations of ultracold fermionic atoms in an optical lattice for a range of interaction strengths, temperatures, and fillings. In particular, we extract the mutual information between a single lattice site and the rest of the system from a comparison between the reduced density matrix of a single lattice site and the thermodynamic entropy. Moreover, we determine the single-particle density matrix between nearest neighbors from thermodynamic observables and show that even in a strongly interacting Mott insulator fermions are significantly delocalized over short distances in the lattice.

A central goal within quantum optics is to realize efficient, controlled interactions between photons and atomic media. A fundamental limit in nearly all applications based on such systems arises from spontaneous emission, in which photons are absorbed by atoms and then rescattered into undesired channels. In typical theoretical treatments of atomic ensembles, it is assumed that this rescattering occurs independently, and at a rate given by a single isolated atom, which in turn gives rise to standard limits of fidelity in applications such as quantum memories for light or photonic quantum gates. However, this assumption can in fact be dramatically violated. In particular, it has long been known that spontaneous emission of a collective atomic excitation can be significantly suppressed through strong interference in emission between atoms. While this concept of “subradiance” is not new, thus far the techniques to exploit the effect have not been well understood. In this work, we provide a comprehensive treatment of this problem. First, we show that in ordered atomic arrays in free space, subradiant states acquire an elegant interpretation in terms of optical modes that are guided by the array, which only emit due to scattering from the ends of the finite system. We also go beyond the typically studied regime of a single atomic excitation and elucidate the properties of subradiant states in the many-excitation limit. Finally, we introduce the new concept of “selective radiance.” Whereas subradiant states experience a reduced coupling to all optical modes, selectively radiant states are tailored to simultaneously radiate efficiently into a desired channel while scattering into undesired channels is suppressed, thus enabling an enhanced atom-light interface. We show that these states naturally appear in chains of atoms coupled to nanophotonic structures, and we analyze the performance of photon storage exploiting such states. We find numerically that selectively radiant states allow for a photon storage error that scales exponentially better with the number of atoms than previously known bounds.

Coupling photons to Rydberg excitations in a cold atomic gas yields unprecedentedly large optical nonlinearities at the level of individual light quanta. Here, the basic mechanism exploits the strong interactions between Rydberg atoms to block the formation of nearby dark-state polaritons. However, the dissipation associated with this mechanism ultimately limits the performance of many practical applications. In this work, we propose a new approach to strong photon interactions via a largely coherent mechanism at drastically suppressed photon losses. Rather than a polariton blockade, it is based on an interaction-induced conversion between distinct types of dark-state polaritons with different propagation characteristics. We outline a specific implementation of this approach and show that it permits us to turn a single photon into an effective mirror with a robust and continuously tunable reflection phase. We describe potential applications, including a detailed discussion of achievable operational fidelities.

Laser guide stars employed at astronomical observatories provide artificial wavefront reference sources to help correct (in part) the impact of atmospheric turbulence on astrophysical observations. Following the recent commissioning of the 4 Laser Guide Star Facility (4LGSF) on Unit Telescope 4 (UT4) of the Very Large Telescope (VLT), we characterize the spectral signature of the uplink beams from the 22-W lasers to assess the impact of laser scattering from the 4LGSF on science observations. We use the Multi-Unit Spectroscopic Explorer (MUSE) optical integral field spectrograph mounted on the Nasmyth B focus of UT4 to acquire spectra at a resolution of $R\cong 3000$ of the uplink laser beams over the wavelength range of 4750 Å–9350 Å. We report the first detection of laser-induced Raman scattering by ${\mathrm{N}}_2$, ${\mathrm{O}}_2$, ${\mathrm{CO}}_2$, ${\mathrm{H}}_2\mathrm{O}$, and (tentatively) ${\mathrm{CH}}_4$ molecules in the atmosphere above the astronomical observatory of Cerro Paranal. In particular, our observations reveal the characteristic spectral signature of laser photons—but 480 Å to 2210 Å redder than the original laser wavelength of 5889.959 Å—landing on the 8.2-m primary mirror of UT4 after being Raman-scattered on their way up to the sodium layer. Laser-induced Raman scattering, a phenomenon not usually discussed in the astronomical context, is not unique to the observatory of Cerro Paranal, but it is common to any astronomical telescope employing a laser guide star (LGS) system. It is thus essential for any optical spectrograph coupled to a LGS system to thoroughly handle the possibility of a Raman spectral contamination via a proper baffling of the instrument and suitable calibrations procedures. These considerations are particularly applicable for the HARMONI optical spectrograph on the upcoming Extremely Large Telescope (ELT). At sites hosting multiple telescopes, laser-collision-prediction tools should also account for the presence of Raman emission from the uplink laser beam(s) to avoid the unintentional contamination of observations acquired with telescopes in the vicinity of a LGS system.

The pulse duration, and, more generally, the temporal intensity profile of free-electron laser (FEL) pulses, is of utmost importance for exploring the new perspectives offered by FELs; it is a nontrivial experimental parameter that needs to be characterized. We measured the pulse shape of an extreme ultraviolet externally seeded FEL operating in high-gain harmonic generation mode. Two different methods based on the cross-correlation of the FEL pulses with an external optical laser were used. The two methods, one capable of single-shot performance, may both be implemented as online diagnostics in FEL facilities. The measurements were carried out at the seeded FEL facility FERMI. The FEL temporal pulse characteristics were measured and studied in a range of FEL wavelengths and machine settings, and they were compared to the predictions of a theoretical model. The measurements allowed a direct observation of the pulse lengthening and splitting at saturation, in agreement with the proposed theory.

Virtually all interactions that are relevant for atomic and condensed matter physics are mediated by quantum fluctuations of the electromagnetic field vacuum. Consequently, controlling the vacuum fluctuations can be used to engineer the strength and the range of interactions. Recent experiments have used this premise to demonstrate novel quantum phases or entangling gates by embedding electric dipoles in photonic cavities or wave guides, which modify the electromagnetic fluctuations. Here, we show theoretically that the enhanced fluctuations in the antisqueezed quadrature of a squeezed vacuum state allow for engineering interactions between electric dipoles without the need for a photonic structure. Thus, the strength and range of the interactions can be engineered in a time-dependent way by changing the spatial profile of the squeezed vacuum in a traveling-wave geometry, which also allows the implementation of chiral dissipative interactions. Using experimentally realized squeezing parameters and including realistic losses, we predict single-atom cooperativities $C$ of up to 10 for the squeezed-vacuum-enhanced interactions.

Trapped Rydberg ions are a promising new system for quantum information processing. They have the potential to join the precise quantum operations of trapped ions and the strong, long-range interactions between Rydberg atoms. Combining the two systems is not at all straightforward. Rydberg atoms are severely affected by electric fields which may cause Stark shifts and field ionization, while electric fields are used to trap ions. Thus, a thorough understanding of the physical properties of Rydberg ions due to the trapping electric fields is essential for future applications. Here, we report the observation of two fundamental trap effects. First, we investigate the interaction of the Rydberg electron with the trapping electric quadrupole fields which leads to Floquet sidebands in the excitation spectra. Second, we report on the modified trapping potential in the Rydberg state compared to the ground state that results from the strong polarizability of the Rydberg ion. By controlling both effects we observe resonance lines close to their natural linewidth demonstrating an unprecedented level of control of this novel quantum platform.

The combination of interactions and static gauge fields plays a pivotal role in our understanding of strongly correlated quantum matter. Cold atomic gases endowed with a synthetic dimension are emerging as an ideal platform to experimentally address this interplay in quasi-one-dimensional systems. A fundamental question is whether these setups can give access to pristine two-dimensional phenomena, such as the fractional quantum Hall effect, and how. We show that unambiguous signatures of bosonic and fermionic Laughlin-like states can be observed and characterized in synthetic ladders. We theoretically diagnose these Laughlin-like states focusing on the chiral current flowing in the ladder, on the central charge of the low-energy theory, and on the properties of the entanglement entropy. Remarkably, Laughlin-like states are separated from conventional liquids by Lifschitz-type transitions, characterized by sharp discontinuities in the current profiles, which we address using extensive simulations based on matrix-product states. Our work provides a qualitative and quantitative guideline towards the observability and understanding of strongly correlated states of matter in synthetic ladders. In particular, we unveil how state-of-the-art experimental settings constitute an ideal starting point to progressively tackle two-dimensional strongly interacting systems from a ladder viewpoint, opening a new perspective for the observation of non-Abelian states of matter.

Reconnections and interactions of filamentary coherent structures play a fundamental role in the dynamics of fluids, redistributing energy and helicity among the length scales and inducing fine-scale turbulent mixing. Unlike ordinary fluids, where vorticity is a continuous field, in quantum fluids vorticity is concentrated into discrete (quantized) vortex lines turning vortex reconnections into isolated events, making it conceptually easier to study. Here, we report experimental and numerical observations of three-dimensional quantum vortex interactions in a cigar-shaped atomic Bose-Einstein condensate. In addition to standard reconnections, already numerically and experimentally observed in homogeneous systems away from boundaries, we show that double reconnections, rebounds, and ejections can also occur as a consequence of the nonhomogeneous, confined nature of the system.

We experimentally observe the decay dynamics of deterministically created isolated monopoles in spin-1 Bose-Einstein condensates. As the condensate undergoes a change between magnetic phases, the isolated monopole gradually evolves into a spin configuration hosting a Dirac monopole in its synthetic magnetic field. We characterize in detail the Dirac monopole by measuring the particle densities of the spin states projected along different quantization axes. Importantly, we observe the spontaneous emergence of nodal lines in the condensate density that accompany the Dirac monopole. We also demonstrate that the monopole decay accelerates in weaker magnetic field gradients.

We investigate the possibility of a bistable phase in an open many-body system. To this end, we discuss the microscopic dynamics of a continuously off-resonantly driven Rydberg lattice gas in the regime of strong decoherence. Our experimental results reveal a prolongation of the temporal correlations exceeding the lifetime of a single Rydberg excitation and show strong evidence for the formation of finite-sized Rydberg excitation clusters in the steady state. We simulate the dynamics of the system using a simplified and a full many-body rate-equation model. The results are compatible with the formation of metastable states associated with a bimodal counting distribution as well as dynamic hysteresis. However, a scaling analysis reveals that the correlation times remain finite for all relevant system parameters, which suggests the formation of many small Rydberg clusters and finite correlation lengths of Rydberg excitations. These results constitute strong evidence against the presence of a global bistable phase previously suggested to exist in this system.

In this work, we analyze the dynamical properties of periodically driven band models. Focusing on the case of Bose-Einstein condensates, and using a mean-field approach to treat interparticle collisions, we identify the origin of dynamical instabilities arising from the interplay between the external drive and interactions. We present a widely applicable generic numerical method to extract instability rates and link parametric instabilities to uncontrolled energy absorption at short times. Based on the existence of parametric resonances, we then develop an analytical approach within Bogoliubov theory, which quantitatively captures the instability rates of the system and provides an intuitive picture of the relevant physical processes, including an understanding of how transverse modes affect the formation of parametric instabilities. Importantly, our calculations demonstrate an agreement between the instability rates determined from numerical simulations and those predicted by theory. To determine the validity regime of the mean-field analysis, we compare the latter to the weakly coupled conserving approximation. The tools developed and the results obtained in this work are directly relevant to present-day ultracold-atom experiments based on shaken optical lattices and are expected to provide an insightful guidance in the quest for Floquet engineering.

Organic dye molecules have been used in a great number of scientific and technological applications, but their wider use in quantum optics has been hampered by transitions to short-lived vibrational levels, which limit their coherence properties. To remedy this, one can take advantage of optical resonators. Here, we present the first results on coherent molecule-resonator coupling, where a single polycyclic aromatic hydrocarbon molecule extinguishes 38% of the light entering a microcavity at liquid helium temperature. We also demonstrate fourfold improvement of single-molecule stimulated emission compared to free-space focusing and take first steps for coherent mechanical manipulation of the molecular transition. Our approach of coupling molecules to an open and tunable microcavity with a very low mode volume and moderately low quality factors of the order of $10^3$ paves the way for the realization of nonlinear and collective quantum optical effects.

In the presence of disorder, an interacting closed quantum system can undergo many-body localization (MBL) and fail to thermalize. However, over long times, even weak couplings to any thermal environment will necessarily thermalize the system and erase all signatures of MBL. This presents a challenge for experimental investigations of MBL since no realistic system can ever be fully closed. In this work, we experimentally explore the thermalization dynamics of a localized system in the presence of controlled dissipation. Specifically, we find that photon scattering results in a stretched exponential decay of an initial density pattern with a rate that depends linearly on the scattering rate. We find that the resulting susceptibility increases significantly close to the phase transition point. In this regime, which is inaccessible to current numerical studies, we also find a strong dependence on interactions. Our work provides a basis for systematic studies of MBL in open systems and opens a route towards extrapolation of closed-system properties from experiments.

We discuss Bragg scattering on both Bose and Fermi gases with strong short-range interactions in the deep inelastic regime of large wave vector transfer $q$, where the dynamic structure factor is dominated by a resonance near the free-particle energy $\hslash \omega ={ϵ}_{\mathbf{q}}={\hslash }^2{q}^2/2m$. Using a systematic short-distance expansion, the structure factor at high momentum is shown to exhibit a nontrivial dependence on frequency characterized by two separate scaling regimes. First, for frequencies that differ from the single-particle energy by terms of order $\mathcal{O}(q)$ (i.e., small deviations compared to the single-particle energy), the dynamic structure factor is described by the impulse approximation of Hohenberg and Platzman. Second, deviations of order $\mathcal{O}(q^2)$ (i.e., of the same order or larger than the single-particle energy) are described by the operator product expansion, with a universal crossover connecting both regimes. The scaling is consistent with the leading asymptotics for a number of sum rules in the large momentum limit. Furthermore, we derive an exact expression for the shift and width of the single-particle peak at large momentum due to interactions, thus extending a result by Beliaev [J. Exp. Theor. Phys. 7, 299 (1958)] for the low-density Bose gas to arbitrary values of the scattering length $a$. The shift exhibits a maximum around $qa\simeq 1$, which is connected with a maximum in the static structure factor due to strong short-range correlations. For Bose gases with moderate interaction strengths, the theoretically predicted shift is consistent with the value observed by Papp et al. [Phys. Rev. Lett. 101, 135301 (2008)]. Finally, we develop a diagrammatic theory for the dynamic structure factor which accounts for the correlations beyond Bogoliubov theory. It covers the full range of momenta and frequencies and provides an explicit example for the emergence of asymptotic scaling at large momentum.

We investigate many-body dynamics in a one-dimensional interacting periodically driven system, based on a partially filled version of Thouless’s topologically quantized adiabatic pump. The corresponding single-particle Floquet bands are chiral, with the Floquet spectrum realizing nontrivial cycles around the quasienergy Brillouin zone. For generic filling, with either bosons or fermions, the system is gapless and is expected to rapidly absorb energy from the driving field. We identify parameter regimes where scattering between Floquet bands of opposite chirality is exponentially suppressed, opening a long time window in which the system prethermalizes to an infinite-temperature state restricted to a single Floquet band. In this quasi-steady state, the time-averaged current takes a universal value determined solely by the density of particles and the topological winding number of the populated Floquet band. This remarkable behavior may be readily studied experimentally in recently developed cold atom systems.

In optics, the interaction of atoms with the magnetic field of light is almost always ignored since its strength is many orders of magnitude weaker compared to the interaction with the electric field. In this article, by using a magnetic-dipole transition within the $4f$ shell of europium ions, we show a strong interaction between a green laser and an ensemble of atomic ions. The electrons move coherently between the ground and excited ionic levels (Rabi flopping) by interacting with the magnetic field of the laser. By measuring the Rabi flopping frequency as the laser intensity is varied, we report the first direct measurement of a magnetic-dipole matrix element in the optical region of the spectrum. Using density-matrix simulations of the ensemble, we infer the generation of coherent magnetization with magnitude $5.5\times {10}^{-3}\mathrm{A}/\mathrm{m}$, which is capable of generating left-handed electromagnetic waves of intensity $1\mathrm{nW}/{\mathrm{cm}}^2$. These results open up the prospect of constructing left-handed materials using sharp transitions of atoms.

We construct and classify chiral topological phases in driven (Floquet) systems of strongly interacting bosons, with finite-dimensional site Hilbert spaces, in two spatial dimensions. The construction proceeds by introducing exactly soluble models with chiral edges, which in the presence of many-body localization (MBL) in the bulk are argued to lead to stable chiral phases. These chiral phases do not require any symmetry and in fact owe their existence to the absence of energy conservation in driven systems. Surprisingly, we show that they are classified by a quantized many-body index, which is well defined for any MBL Floquet system. The value of this index, which is always the logarithm of a positive rational number, can be interpreted as the entropy per Floquet cycle pumped along the edge, formalizing the notion of quantum-information flow. We explicitly compute this index for specific models and show that the nontrivial topology leads to edge thermalization, which provides an interesting link between bulk topology and chaos at the edge. We also discuss chiral Floquet phases in interacting fermionic systems and their relation to chiral bosonic phases.