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Atoms with a highly excited electron, called Rydberg atoms, can form unusual types of molecular bonds

Vibrational dynamics in conventional molecules usually takes place on a timescale of picoseconds or shorter. A striking exception are ultralong-range Rydberg molecules, for which dynamics is dramatically slowed down as a consequence of the huge bond length of up to several micrometers. Here, we report on the direct observation of vibrational dynamics of a recently observed Rydberg-atom-ion molecule. By applying a weak external electric field of a few mV/cm, we are able to control the orientation of the photoassociated ultralong-range Rydberg molecules and induce vibrational dynamics by quenching the electric field. A high resolution ion microscope allows us to detect the molecule's orientation and its temporal vibrational dynamics in real space. Our study opens the door to the control of molecular dynamics in Rydberg molecules., 7 pages, 4 figures

The combination of topology and quantum criticality can give rise to an exotic mix of counterintuitive effects. Here, we show that unexpected topological properties take place in a paradigmatic strongly-correlated Hamiltonian: the 1D extended Bose-Hubbard model. In particular, we reveal the presence of two distinct topological quantum critical points with localized edge states and gapless bulk excitations. Our results show that the topological critical points separate two phases, one topologically protected and the other topologically trivial, both characterized by a long-range ordered string correlation function. The long-range order persists also at the topological critical points and it reflects the presence of localized edge states protected by a finite charge gap. Finally, we introduce a super-resolution quantum gas microscopy scheme for dipolar dysprosium atoms, which provides a reliable route towards the experimental study of topological quantum critical points., 7 pages, 3 figures + 3 pages, 2 figures

Since the achievement of quantum degeneracy in gases of chromium atoms in 2004, the experimental investigation of ultracold gases made of highly magnetic atoms has blossomed. The field has yielded the observation of many unprecedented phenomena, in particular those in which long-range and anisotropic dipole–dipole interactions (DDIs) play a crucial role. In this review, we aim to present the aspects of the magnetic quantum-gas platform that make it unique for exploring ultracold and quantum physics as well as to give a thorough overview of experimental achievements. Highly magnetic atoms distinguish themselves by the fact that their electronic ground-state configuration possesses a large electronic total angular momentum. This results in a large magnetic moment and a rich electronic transition spectrum. Such transitions are useful for cooling, trapping, and manipulating these atoms. The complex atomic structure and large dipolar moments of these atoms also lead to a dense spectrum of resonances in their two-body scattering behaviour. These resonances can be used to control the interatomic interactions and, in particular, the relative importance of contact over dipolar interactions. These features provide exquisite control knobs for exploring the few- and many-body physics of dipolar quantum gases. The study of dipolar effects in magnetic quantum gases has covered various few-body phenomena that are based on elastic and inelastic anisotropic scattering. Various many-body effects have also been demonstrated. These affect both the shape, stability, dynamics, and excitations of fully polarised repulsive Bose or Fermi gases. Beyond the mean-field instability, strong dipolar interactions competing with slightly weaker contact interactions between magnetic bosons yield new quantum-stabilised states, among which are self-bound droplets, droplet assemblies, and supersolids. Dipolar interactions also deeply affect the physics of atomic gases with an internal degree of freedom as these interactions intrinsically couple spin and atomic motion. Finally, long-range dipolar interactions can stabilise strongly correlated excited states of 1D gases and also impact the physics of lattice-confined systems, both at the spin-polarised level (Hubbard models with off-site interactions) and at the spinful level (XYZ models). In the present manuscript, we aim to provide an extensive overview of the various related experimental achievements up to the present.

We theoretically investigate the ground states and the spectrum of elementary excitations across the superfluid to droplet crystallization transition of an oblate dipolar Bose-Einstein condensate. We systematically identify regimes where spontaneous rotational symmetry breaking leads to the emergence of a supersolid phase with characteristic collective excitations, such as the Higgs amplitude mode. Furthermore, we study the dynamics across the transition and show how these supersolids can be realized with standard protocols in state-of-the-art experiments., 10 pages, 2+1 figures

Phase transitions share the universal feature of enhanced fluctuations near the transition point. Here we show that density fluctuations reveal how a Bose-Einstein condensate of dipolar atoms spontaneously breaks its translation symmetry and enters the supersolid state of matter -- a phase that combines superfluidity with crystalline order. We report on the first direct in situ measurement of density fluctuations across the superfluid-supersolid phase transition. This allows us to introduce a general and straightforward way to extract the static structure factor, estimate the spectrum of elementary excitations and image the dominant fluctuation patterns. We observe a strong response in the static structure factor and infer a distinct roton minimum in the dispersion relation. Furthermore, we show that the characteristic fluctuations correspond to elementary excitations such as the roton modes, which have been theoretically predicted to be dominant at the quantum critical point, and that the supersolid state supports both superfluid as well as crystal phonons., 11 pages, 5 + 3 figures

The advent of the quantum gas microscope allowed for the in situ probing of ultracold gaseous matter on an unprecedented level of spatial resolution. The study of phenomena on ever smaller length scales as well as the probing of three-dimensional systems is, however, fundamentally limited by the wavelength of the imaging light, for all techniques based on linear optics. Here we report on a high-resolution ion microscope as a versatile and powerful experimental tool to investigate quantum gases. The instrument clearly resolves atoms in an optical lattice with a spacing of $532\,\text{nm}$ over a field of view of 50 sites and offers an extremely large depth of field on the order of at least $70\,\mu\text{m}$. With a simple model, we extract an upper limit for the achievable resolution of approximately $200\,\text{nm}$ from our data. We demonstrate a pulsed operation mode which in the future will enable 3D imaging and allow for the study of ionic impurities and Rydberg physics.

We observe signatures of radial and angular roton excitations around a droplet crystallization transition in dipolar Bose-Einstein condensates. In situ measurements are used to characterize the density fluctuations near this transition. The static structure factor is extracted and used to identify the radial and angular roton excitations by their characteristic symmetries. These fluctuations peak as a function of interaction strength indicating the crystallization transition of the system. We compare our observations to a theoretically calculated excitation spectrum allowing us to connect the crystallization mechanism with the softening of the angular roton modes., Comment: 10 pages, 4 + 4 figures

Parametric single-photon generation is a key technology for quantum-optical applications. Here we report on the development and commissioning of a highly specialized 1010 nm fiber amplifier for such a novel parametric single-photon source.

We exploit the effect of light-induced atomic desorption to produce high atomic densities ($n\gg k^3$) in a rubidium vapor cell. An intense off-resonant laser is pulsed for roughly one nanosecond on a micrometer-sized sapphire-coated cell, which results in the desorption of atomic clouds from both internal surfaces. We probe the transient atomic density evolution by time-resolved absorption spectroscopy.With a temporal resolution of $\approx1\,\mathrm{ns}$, we measure the broadening and line shift of the atomic resonances. Both broadening and line shift are attributed to dipole-dipole interactions. This fast switching of the atomic density and dipolar interactions could be the basis for future quantum devices based on the excitation blockade., Comment: 13 pages, 4+6 figures

We report three-photon continuous-wave laser excitation of nitric oxide to high lying electronic Rydberg states and its conversion into a detectable current in the nA regime using our optogalvanic trace-gas sensor prototype.

We demonstrate an atomic Faraday dichroic beam splitter suitable to spatially separate signal and idler fields from pump degenerate four-wave mixing in an atomic source. By rotating the plane of polarization of one mode $90^{\circ}$ with respect to the other, a subsequent polarizing beam splitter separates the two frequencies, which differ by only 13.6 GHz, and achieves a suppression of $(-26.3\pm0.1)$ and $(-21.2\pm0.1)$ dB in the two outputs, with a corresponding transmission of 97 and 99 %. This technique avoids the need to use spatial separation of four-wave mixing modes and thus opens the door for the process efficiency to be enhanced in waveguide experiments. As a proof-of-principle we generate light via four-wave mixing in $^{87}$Rb loaded into a hollow-core photonic crystal fiber and interface it with the atomic Faraday dichroic beam splitter., 8 pages, 7 figures

In this article, we theoretically investigate the first- and second-order quantum dissipative phase transitions of a three-mode cavity with a Hubbard interaction. In both types, there is a mean-field (MF) limit cycle phase where the local U(1) symmetry and the time-translational symmetry of the Liouvillian superoperator are spontaneously broken. In MF, this spontaneous symmetry breaking manifests itself through the appearance of an unconditionally and fully squeezed state at the cavity output, connected to the well-known Goldstone mode. By employing the Wigner function formalism, hence, properly including the quantum noise, we show that away from the thermodynamic limit and within the quantum regime, fluctuations notably limit the coherence time of the Goldstone mode due to the phase diffusion. Our theoretical predictions suggest that interacting multimode photonic systems are rich, versatile test beds for investigating the crossovers between the mean-field picture and quantum phase transitions, a problem that can be investigated in various platforms including superconducting circuits, semiconductor microcavities, atomic Rydberg polaritons, and cuprite excitons.

Quantum fluctuations can stabilize Bose–Einstein condensates (BEC) against the mean-field collapse. Stabilization of the condensate has been observed in quantum degenerate Bose–Bose mixtures and dipolar BECs. The fine-tuning of the interatomic interactions can lead to the emergence of two new states of matter: liquid-like self-bound quantum droplets and supersolid crystals formed from these droplets. We review the properties of these exotic states of matter and summarize the experimental progress made using dipolar quantum gases and Bose–Bose mixtures. We conclude with an outline of important open questions that could be addressed in the future.

We investigate transport dynamics of a single low-energy ionic impurity in a Bose-Einstein condensate. The impurity is implanted into the condensate starting from a single Rydberg excitation, which is ionized by a sequence of fast electric field pulses aiming to minimize the ion's initial kinetic energy. Using a small electric bias field, we study the subsequent collisional dynamics of the impurity subject to an external force. The fast ion-atom collision rate, stemming from the dense degenerate host gas and the large ion-atom scattering cross section, allows us to study a regime of frequent collisions of the impurity within only tens of microseconds. Comparison of our measurements with stochastic trajectory simulations based on sequential Langevin collisions indicate diffusive transport properties of the impurity and allows us to measure its mobility. Furthermore, working with a free and untrapped ion provides unique means to distinguish single realizations, where the impurity is subject to inelastic molecular-ion formation via three-body recombination. We study the cold chemistry of these events and find evidence for subsequent rovibrational quenching collisions of the produced molecule. Our results open a novel path to study dynamics of charged quantum impurities in ultracold matter., Comment: 10 pages, 9 figures

The paradigm of cavity QED is a two-level emitter interacting with a high-quality factor single-mode optical resonator. The hybridization of the emitter and photon wave functions mandates large vacuum Rabi frequencies and long coherence times; features that so far have been successfully realized with trapped cold atoms and ions, and localized solid-state quantum emitters such as superconducting circuits, quantum dots, and color centers Reiserer and Rempe (Rev Modern Phys 87:1379, 2015), Faraon et al. (Phys Rev 81:033838, 2010). Thermal atoms, on the other hand, provide us with a dense emitter ensemble and in comparison to the cold systems are more compatible with integration, hence enabling large-scale quantum systems. However, their thermal motion and large transit-time broadening is a major bottleneck that has to be circumvented. A promising remedy could benefit from the highly controllable and tunable electromagnetic fields of a nano-photonic cavity with strong local electric-field enhancements. Utilizing this feature, here we investigate the interaction between fast moving thermal atoms and a nano-beam photonic crystal cavity (PCC) with large quality factor and small mode volume. Through fully quantum mechanical calculations, including Casimir-Polder potential (i.e. the effect of the surface on radiation properties of an atom), we show, when designed properly, the achievable coupling between the flying atom and the cavity photon would be strong enough to lead to quantum interference effects in spite of short interaction times. In addition, the time-resolved detection of different trajectories can be used to identify single and multiple atom counts. This probabilistic approach will find applications in cavity QED studies in dense atomic media and paves the way towards realizing large-scale, room-temperature macroscopic quantum systems aimed at out of the lab quantum devices., Projekt DEAL

We investigate inelastic collision dynamics of a single cold ion in a Bose-Einstein condensate. We observe rapid ion-atom-atom three-body recombination leading to formation of weakly bound molecular ions followed by secondary two-body molecule-atom collisions quenching the rovibrational states towards deeper binding energies. In contrast to previous studies exploiting hybrid ion traps, we work in an effectively field-free environment and generate a free low-energy ionic impurity directly from the atomic ensemble via Rydberg excitation and ionization. This allows us to implement an energy-resolved field-dissociation technique to trace the relaxation dynamics of the recombination products. Our observations are in good agreement with numerical simulations based on Langevin capture dynamics and provide complementary means to study stability and reaction dynamics of ionic impurities in ultracold quantum gases., Comment: 5 pages, 3 figures. arXiv admin note: substantial text overlap with arXiv:2007.00309

Dipolar quantum droplets are exotic quantum objects that are self-bound due to the subtle balance of attraction, repulsion, and quantum correlations. Here we present a systematic study of the critical atom number of these self-bound droplets, comparing the experimental results with extended mean-field Gross-Pitaevskii equation and quantum Monte Carlo simulations of the dilute system. The respective theoretical predictions differ, questioning the validity of the current theoretical state-of-the-art description of quantum droplets within the extended Gross-Pitaevskii equation framework and indicating that correlations in the system are significant. Furthermore, we show that our system can serve as a sensitive testing ground for many-body theories in the near future.

We theoretically investigate the spectrum of elementary excitations of a trapped dipolar quantum gas across the BEC-supersolid phase transition. Our calculations reveal the existence of distinct Higgs amplitude and Nambu-Goldstone modes that emerge from the softening roton modes of the dipolar BEC at the phase transition point. On the supersolid side of the transition, the energy of the Higgs amplitude mode increases rapidly, leading to a strong coupling to higher-lying modes. Our Letter highlights how the symmetry-breaking nature of the supersolid state translates to finite-size systems.

A supersolid is a counter-intuitive state of matter that combines the frictionless flow of a superfluid with the crystal-like periodic density modulation of a solid. Since the first prediction in the 1950s, experimental efforts to realize this state have focussed mainly on Helium, where supersolidity remains elusive. Recently, supersolidity has also been studied intensively in ultracold quantum gases, and some of its defining properties have been induced in spin-orbit coupled Bose-Einstein condensates (BECs) and BECs coupled to two crossed optical cavities. However, the periodicity of the crystals in both systems is fixed to the wavelength of the applied periodic optical potentials. Recently, hallmark properties of a supersolid -- the periodic density modulation and simultaneous global phase coherence -- have been observed in arrays of dipolar quantum droplets, where the crystallization happens in a self-organized manner due to intrinsic interactions. In this letter, we prove the genuine supersolid nature of these droplet arrays by directly observing the low-energy Goldstone mode. The dynamics of this mode is reminiscent of the effect of second sound in other superfluid systems and features an out-ofphase oscillation of the crystal array and the superfluid density. This mode exists only due to the phase rigidity of the experimentally realized state, and therefore confirms the genuine superfluidity of the supersolid.

The level structure of negative-ions near the electron detachment limit dictates the low-energy scattering of an electron with the parent neutral atom. We demonstrate that a single ultracold atom bound inside a Rydberg orbit forming an ultralong-range Rydberg molecule provides an atomic-scale system which is highly sensitive to electron-neutral scattering and thus allows for detailed insights into the underlying near-threshold anion states. Our measurements reveal the so far unobserved fine structure of the $^3P_J$ triplet of Rb$^-$ and allow us to extract parameters of the associated $p$-wave scattering resonances which deviate from previous theoretical estimates. Moreover, we observe a novel alignment mechanism for Rydberg molecules mediated by spin-orbit coupling in the negative ion., 11 pages, 6 figures

We study theoretically and experimentally the emergence of supersolid properties in a dipolar Bose-Einstein condensate. The theory reveals a ground state phase diagram with three distinct regimes - a regular Bose-Einstein condensate, incoherent and coherent arrays of quantum droplets. In the latter the droplets are connected by a finite superfluid density, which leads - in addition to the periodic density modulation - to a robust phase coherence throughout the whole system. We further theoretically demonstrate that we are able to dynamically approach the ground state in our experiment and that its lifetime is only limited by three-body losses. Experimentally we probe and confirm the signatures of the phase diagram by observing the in-situ density modulation as well as the phase coherence using matter wave interference.

We investigate the phenomenon of bistability in a thermal gas of cesium atoms excited to Rydberg states. We present both measurements and a numerical model of the phenomena based on collisions. By directly measuring the plasma frequency, we show that the origin of the bistable behavior lies in the creation of a plasma formed by ionized Rydberg atoms. Recombination of ions and electrons manifests as fluorescence which allows us to characterize the plasma properties and study the transient dynamics of the hysteresis that occurs. We determine scaling parameters for the point of plasma formation, and verify our numerical model by comparing measured and simulated spectra. These measurements yield a detailed microscopic picture of ionization and avalanche processes occurring in thermal Rydberg gases. From this set of measurements, we conclude that plasma formation is a fundamental ingredient in the optical bistability taking place in thermal Rydberg gases and imposes a limit on usable Rydberg densities for many applications., Comment: 13 pages, 10 figures

The development of highly customized technical devices is a decisive feature of technically complex setups, as frequently observed in quantum experiments. This paper describes the development and realization of an Yb-doped all-fiber amplifier system designed for such a special application, more specifically, an on-demand single-photon source based on four-wave mixing with rubidium Rydberg atoms. The laser is capable of generating bandwidth-limited configurable nanosecond pulses up to peak powers of >100 W and with pulse repetition frequencies (PRF) between 50 Hz and 1 MHz at selectable wavelengths (1008–1024 nm). Especially the amplification of the 1010 nm reference seed at the lower edge of the amplification range for Yb-based fibers is challenging and tends to produce amplified spontaneous emission (ASE) at higher wavelengths. To achieve high ASE suppression, particularly at low pulse repetition frequencies, two acousto-optical modulators (AOM) are utilized both for pulse picking and for temporal filtering. The synchronization between pulse repetition frequency and AOM driver signal allows pulse amplitude fluctuations to be kept below 1%, while ASE is suppressed by at least 85 dB (PRF = 1 MHz) and 65 dB (PRF = 1 kHz).

We investigate the properties of a trace-gas sensing scheme based on Rydberg excitations at the example of an idealized model system. Rydberg states in thermal rubidium (Rb) are created using a 2-photon cw excitation. These Rydberg-excited atoms ionize via collisions with a background gas of nitrogen (N2). The emerging charges are then measured as an electric current, which is on the order of several picoampere. Due to the 2-photon excitation, this sensing method has a large intrinsic selectivity combined with a promising sensitivity of 10 ppb at an absolute concentration of 1 ppm. The determination of the detection limit is limited by the optical reference measurement but is at least 500 ppb.

We study the long-range interaction of a single ion with a highly excited ultracold Rydberg atom and report on the direct observation of ion-induced Rydberg excitation blockade mediated over tens of micrometer distances. Our hybrid ion-atom system is directly produced from an ultracold atomic ensemble via near-threshold photo-ionization of a single Rydberg excitation, employing a two-photon scheme which is specifically suited for generating a very low-energy ion. The ion's motion is precisely controlled by small electric fields, which allows us to analyze the blockade mechanism for a range of principal quantum numbers. Finally, we explore the capability of the ion as a high-sensitivity single-atom-based electric field sensor. The observed ion - Rydberg-atom interaction is of current interest for entanglement generation or studies of ultracold chemistry in hybrid ion-atom systems., 7 pages, 7 figures

This paper describes some of the recent trends in the use of integrated circuit (IC) technology for the design of smart quantum sensors. To this end, after a brief introduction into the topic of quantum sensing including its intrinsic advantages and associated challenges, a number of emerging applications including the fields of IC-based inductive electron and nuclear spin detection as well as Rydberg gas sensing and NV center based sensing are used to highlight the great potential of the IC-based quantum sensing approach.

Over the last 10 years the supported data rates of high performance coherent ASICs have increased by more than 10 x. We review the evolution and main building blocks of those ASICs and compare different options to optimize performance.

Rydberg atoms in room temperature vapor cells are promising candidates for realizing new kinds of quantum devices and sensors. However, the alkali vapor, which is most commonly used, introduces new technological challenges. We demonstrate the applicability of anodic bonding as a sealing method for vapor cells, which preserves vacuum levels down to 10-7 mbar for several years, while being compatible with thin-film electronics on glass. We furthermore prove, that the implementation of such thin-film electronics inside a highly reactive atmosphere of alkali vapor is possible. We also propose a new kind of gas sensor based on Rydberg excitations as a competitive and promising application of our Rydberg detection scheme.

Tailored quantum states of light can be created via a transfer of collective quantum states of matter to light modes. Such collective quantum states emerge in interacting many-body systems if thermal fluctuations are overcome by sufficient interaction strengths. Therefore, typically ultracold temperatures or strong confinement are required. We show that the exaggerated interactions between giant Rydberg atoms allow for collective quantum states even above room temperature. The emerging Rydberg blockade allows then only for a single Rydberg excitation. We experimentally implement a four-wave mixing scheme to demonstrate an on-demand single-photon source. The combination of glass cell technology, identical atoms, and operation around room temperature promises scalability and integrability. This approach has the potential for various applications in quantum information processing and communication., Comment: 12 pages, 5 figures total, supplementary information

We present transport measurements on a dipolar superfluid using a Bose-Einstein condensate of $^{162}\mathrm{Dy}$ with strong magnetic dipole-dipole interactions. By moving an attractive laser beam through the condensate we observe an anisotropy in superfluid flow. This observation is compatible with an anisotropic critical velocity for the breakdown of dissipationless flow, which, in the spirit of the Landau criterion, can directly be connected to the anisotropy of the underlying dipolar excitation spectrum. In addition, the heating rate above this critical velocity reflects the same anisotropy. Our observations are in excellent agreement with simulations based on the Gross-Pitaevskii equation and highlight the effect of dipolar interactions on macroscopic transport properties, rendering dissipation anisotropic.

We demonstrate real-time transmission of 16 Tb/s (80x200Gb/s) over 1020km TeraWave ULL fiber with 170km span length using the world's first 200Gb/s CFP2-DCO module with a record low power consumption less than 0.1W/Gbps.