Sympathetic Cooling and Slowing of Molecules with Rydberg Atoms.

We propose to sympathetically slow and cool polar molecules in a cold, low-density beam using laser-cooled Rydberg atoms. The elastic collision cross sections between molecules and Rydberg atoms are large enough to efficiently thermalize the molecules even in a low-density environment. Molecules traveling at 100 m/s can be stopped in under 30 collisions with little inelastic loss. Our method does not require photon scattering from the molecules and can be generically applied to complex species for applications in precision measurement, quantum information science, and controlled chemistry.

Observation of Rydberg Blockade Due to the Charge-Dipole Interaction between an Atom and a Polar Molecule.

We demonstrate Rydberg blockade due to the charge-dipole interaction between a single Rb atom and a single RbCs molecule confined in optical tweezers. The molecule is formed by magnetoassociation of a Rb+Cs atom pair and subsequently transferred to the rovibrational ground state with an efficiency of 91(1)%. Species-specific tweezers are used to control the separation between the atom and molecule. The charge-dipole interaction causes blockade of the transition to the Rb(52s) Rydberg state, when the atom-molecule separation is set to 310(40) nm. The observed excitation dynamics are in good agreement with simulations using calculated interaction potentials. Our results open up the prospect of a hybrid platform where quantum information is transferred between individually trapped molecules using Rydberg atoms.

Model of charge transfer collisions between C60 and slow ions.

A semiclassical model describing the charge transfer collisions of C60 fullerene with different slow ions has been developed to analyze available observations. These data reveal multiple Breit-Wigner-like peaks in the cross sections, with subsequent peaks of reactive cross sections decreasing in magnitude. Calculations of charge transfer probabilities, quasi-resonant cross sections, and cross sections for reactive collisions have been performed using semiempirical interaction potentials between fullerenes and ion projectiles. All computations have been carried out with realistic wave functions for C60's valence electrons derived from the simplified jellium model. The quality of these electron wave functions has been successfully verified by comparing theoretical calculations and experimental data on the small angle cross sections of resonant C60+C60 + collisions. Using the semiempirical potentials to describe resonant scattering phenomena in C60 collisions with ions and Landau-Zener charge transfer theory, we calculated theoretical cross sections for various C60 charge transfer and fragmentation reactions which agree with experiments.

Ultralong-Range Rydberg Bimolecules.

We predict that ultralong-range Rydberg bimolecules form in collisions between polar molecules in cold and ultracold settings. The interaction of Λ-doublet nitric oxide (NO) with long-lived Rydberg NO(nf, ng) molecules forms ultralong-range Rydberg bimolecules with GHz energies and kilo-Debye permanent electric dipole moments. The Hamiltonian includes both the anisotropic charge-molecular dipole interaction and the electron-NO scattering. The rotational constant for the Rydberg bimolecules is in the MHz range, allowing for microwave spectroscopy of rotational transitions in Rydberg bimolecules. Considerable orientation of NO dipole can be achieved. The Rydberg molecules described here hold promise for studies of a special class of long-range bimolecular interactions.

Quantum Rydberg Central Spin Model.

We consider dynamics of a Rydberg impurity in a cloud of ultracold bosonic atoms in which the Rydberg electron undergoes spin-changing collisions with surrounding atoms. This system realizes a new type of quantum impurity problems that compounds essential features of the Kondo model, the Bose polaron, and the central spin model. To capture the interplay of the Rydberg-electron spin dynamics and the orbital motion of atoms, we employ a new variational method that combines an impurity-decoupling transformation with a Gaussian ansatz for the bath particles. We find several unexpected features of this model that are not present in traditional impurity problems, including interaction-induced renormalization of the absorption spectrum that eludes simple explanations from molecular bound states, and long-lasting oscillations of the Rydberg-electron spin. We discuss generalizations of our analysis to other systems in atomic physics and quantum chemistry, where an electron excitation of high orbital quantum number interacts with a spinful quantum bath.

Effective Three-Body Interactions in Cs(6s)-Cs(nd) Rydberg Trimers.

Ultralong-range Rydberg trimer molecules are spectroscopically observed in an ultracold gas of Cs(nd_{3/2}) atoms. The anisotropy of the atomic Rydberg state allows for the formation of angular trimers, whose energies may not be obtained from integer multiples of dimer energies. These nonadditive trimers coexist with Rydberg dimers. The existence of such effective three-body interactions is confirmed with the observation of asymmetric line profiles and interpreted by a theoretical approach that includes relativistic spin interactions. Simulations of the observed spectra with and without angular trimer lines lend convincing support to the existence of effective three-body interactions.

Creation of Rydberg Polarons in a Bose Gas.

We report spectroscopic observation of Rydberg polarons in an atomic Bose gas. Polarons are created by excitation of Rydberg atoms as impurities in a strontium Bose-Einstein condensate. They are distinguished from previously studied polarons by macroscopic occupation of bound molecular states that arise from scattering of the weakly bound Rydberg electron from ground-state atoms. The absence of a p-wave resonance in the low-energy electron-atom scattering in Sr introduces a universal behavior in the Rydberg spectral line shape and in scaling of the spectral width (narrowing) with the Rydberg principal quantum number, n. Spectral features are described with a functional determinant approach (FDA) that solves an extended Fröhlich Hamiltonian for a mobile impurity in a Bose gas. Excited states of polyatomic Rydberg molecules (trimers, tetrameters, and pentamers) are experimentally resolved and accurately reproduced with a FDA.

Mesoscopic Rydberg Impurity in an Atomic Quantum Gas.

Giant impurity excitations are powerful probes for exploring new regimes of far out of equilibrium dynamics in few- and many-body quantum systems, and in situ observations of correlations. Motivated by recent experimental progress in spectroscopic studies of Rydberg excitations in ultracold atoms, we develop a new theoretical approach for describing multiscale dynamics of Rydberg excitations in quantum Bose gases. We find that the crossover from few- to many-body dynamics manifests in a dramatic change in spectral profile from resolved molecular lines to broad Gaussian distributions representing a superpolaronic state in which many atoms bind to the Rydberg impurity. We discuss signatures of this crossover in the temperature and density dependence of the spectra.

Electric Field Cancellation on Quartz by Rb Adsorbate-Induced Negative Electron Affinity.

We investigate the (0001) surface of single crystal quartz with a submonolayer of Rb adsorbates. Using Rydberg atom electromagnetically induced transparency, we investigate the electric fields resulting from Rb adsorbed on the quartz surface, and measure the activation energy of the Rb adsorbates. We show that the adsorbed Rb induces negative electron affinity (NEA) on the quartz surface. The NEA surface allows low energy electrons to bind to the surface and cancel the electric field from the Rb adsorbates. Our results will be important for integrating Rydberg atoms into hybrid quantum systems, as fundamental probes of atom-surface interactions, and for studies of 2D electron gases bound to surfaces.

Theory of Ultralong-Range Rydberg Molecule Formation Incorporating Spin-Dependent Relativistic Effects: Cs(6s)-Cs(np) as Case Study.

We calculate vibrational spectra of ultralong-range Cs(32p) Rydberg molecules that form in an ultracold gas of Cs atoms. We account for the partial-wave scattering of the Rydberg electrons from the Cs perturber atoms by including the full set of spin-resolved 1,3 SJ and 1,3 PJ scattering phase shifts, and allow for the mixing of singlet (S=0) and triplet (S=1) spin states through Rydberg electron spin-orbit and ground state electron hyperfine interactions. Excellent agreement with observed data in Saßmannshausen et al. [Phys. Rev. Lett. 2015, 113, 133201] in line positions and profiles is obtained. We also determine the spin-dependent permanent electric dipole moments for these molecules. This is the first such calculation of ultralong-range Rydberg molecules for which all of the relativistic contributions are accounted.

Control of multiple excited image states around segmented carbon nanotubes.

Electronic image states around segmented carbon nanotubes can be confined and shaped along the nanotube axis by engineering the image potential. We show how several such image states can be prepared simultaneously along the same nanotube. The inter-electronic distance can be controlled a priori by engineering tubes of specific geometries. High sensitivity to external electric and magnetic fields can be exploited to manipulate these states and their mutual long-range interactions. These building blocks provide access to a new kind of tailored interacting quantum systems.

Quantum synchronization of quantum van der Pol oscillators with trapped ions.

The van der Pol oscillator is the prototypical self-sustained oscillator and has been used to model nonlinear behavior in biological and other classical processes. We investigate how quantum fluctuations affect phase locking of one or many van der Pol oscillators. We find that phase locking is much more robust in the quantum model than in the equivalent classical model. Trapped-ion experiments are ideally suited to simulate van der Pol oscillators in the quantum regime via sideband heating and cooling of motional modes. We provide realistic experimental parameters for 171Yb+ achievable with current technology.

Potential energy curves for the interaction of Ag(5s) and Ag(5p) with noble gas atoms.

We investigate the interaction of ground and excited states of a silver atom with noble gases (NG), including helium. Born-Oppenheimer potential energy curves are calculated with quantum chemistry methods and spin-orbit effects in the excited states are included by assuming a spin-orbit splitting independent of the internuclear distance. We compare our results with experimentally available spectroscopic data, as well as with previous calculations. Because of strong spin-orbit interactions, excited Ag-NG potential energy curves cannot be fitted to Morse-like potentials. We find that the labeling of the observed vibrational levels has to be shifted by one unit.

Long-range interactions of excited He atoms with the alkaline earth atoms Mg, Ca, and Sr.

Dispersion coefficients for the long-range interactions of the first four excited states of He, i.e., He(2 (1, 3)S) and He(2 (1, 3)P), with the low-lying states of the alkaline earth atoms Mg, Ca, and Sr are calculated by summing over the reduced matrix elements of multipole transition operators.

Observation of blueshifted ultralong-range Cs2 Rydberg molecules.

We observe ultralong-range blueshifted Cs(2) molecular states near ns(1/2) Rydberg states in an optical dipole trap, where 31≤n≤34. The accidental near degeneracy of (n-4)l and ns Rydberg states for l>2 in Cs, due to the small fractional ns quantum defect, leads to nonadiabatic coupling among these states, producing potential wells above the ns thresholds. Two important consequences of admixing high angular momentum states with ns states are the formation of large permanent dipole moments, ~15-100 Debye, and accessibility of these states via two-photon association. The observed states are in excellent agreement with theory.

Anisotropic hyperfine interactions limit the efficiency of spin-exchange optical pumping of ³He nuclei.

We use accurate ab initio and quantum scattering calculations to demonstrate that the maximum ³He spin polarization that can be achieved in spin-exchange collisions with potassium (³9K) and silver (¹°7Ag) atoms is limited by the anisotropic hyperfine interaction. We find that spin exchange in Ag-He collisions occurs much faster than in K-He collisions over a wide range of temperatures (10-600 K). Our analysis indicates that measurements of trap loss rates of ²S atoms in the presence of cold ³He gas may be used to probe anisotropic spin-dependent interactions in atom-He collisions.

Rydberg atom mediated polar molecule interactions: a tool for molecular-state conditional quantum gates and individual addressability.

We study the possibility to use interaction between a polar molecule in the ground electronic and vibrational state and a Rydberg atom to construct two-qubit gates between molecular qubits and to coherently control molecular states. A polar molecule within the electron orbit in a Rydberg atom can either shift the Rydberg state, or form a Rydberg molecule. Both the atomic shift and the Rydberg molecule states depend on the initial internal state of the polar molecule, resulting in molecular state dependent van der Waals or dipole-dipole interaction between Rydberg atoms. Rydberg atoms mediated interaction between polar molecules can be enhanced up to 10(3) times. We describe how the coupling between a polar molecule and a Rydberg atom can be applied to coherently control molecular states, and specifically, to individually address molecules in an optical lattice, and to non-destructively readout molecular qubits.

Formation and dynamics of van der Waals molecules in buffer-gas traps.

We show that weakly bound He-containing van der Waals molecules can be produced and magnetically trapped in buffer-gas cooling experiments, and provide a general model for the formation and dynamics of these molecules. Our analysis shows that, at typical experimental parameters, thermodynamics favors the formation of van der Waals complexes composed of a helium atom bound to most open-shell atoms and molecules, and that complex formation occurs quickly enough to ensure chemical equilibrium. For molecular pairs composed of a He atom and an S-state atom, the molecular spin is stable during formation, dissociation, and collisions, and thus these molecules can be magnetically trapped. Collisional spin relaxation is too slow to affect trap lifetimes. However, (3)He-containing complexes can change spin due to adiabatic crossings between trapped and untrapped Zeeman states, mediated by the anisotropic hyperfine interaction, causing trap loss. We provide a detailed model for Ag(3)He molecules, using ab initio calculation of Ag-He interaction potentials and spin interactions, quantum scattering theory, and direct Monte Carlo simulations to describe formation and spin relaxation in this system. The calculated rate of spin-change agrees quantitatively with experimental observations, providing indirect evidence for molecular formation in buffer-gas-cooled magnetic traps. Finally, we discuss the possibilities for spectroscopic detection of these complexes, including a calculation of expected spectra for Ag(3)He, and report on our spectroscopic search for Ag(3)He, which produced a null result.

Ultracold giant polyatomic Rydberg molecules: coherent control of molecular orientation.

We predict the existence of a class of ultracold giant molecules formed from trapped ultracold Rydberg atoms and polar molecules. The interaction which leads to the formation of such molecules is the anisotropic, long-range charge-dipole interaction. We show that prominent candidate molecules such as deuterated hydroxyl (OD) and KRb should bind to Rydberg rubidium atoms, with energies E(b)≃5-25 GHz at distances R≃0.1-1 µm. These molecules form in double wells, mimicking chiral molecules, with each well containing a particular dipole orientation. We prepare a set of correlated dressed electron-dipole eigenstates which are used in an on-resonance Raman scheme to coherently control the molecular dipole orientation.

Formation of van der Waals molecules in buffer-gas-cooled magnetic traps [corrected].

We predict that a large class of helium-containing cold polar molecules form readily in a cryogenic buffer gas, achieving densities as high as 10(12) cm(-3). We explore the spin relaxation of these molecules in buffer-gas-loaded magnetic traps and identify a loss mechanism based on Landau-Zener transitions arising from the anisotropic hyperfine interaction. Our results show that the recently observed strong T(-6) thermal dependence of the spin-change rate of silver (Ag) trapped in dense (3)He is accounted for by the formation and spin change of Ag(3)He van der Waals molecules, thus providing indirect evidence for molecular formation in a buffer-gas trap.