Quantum state-dependent anion-neutral detachment processes.

The detachment loss dynamics between rubidium atoms (Rb) and oxygen anions (O-) are studied in a hybrid atom-ion trap. The amount of excited rubidium present in the atomic ensemble is actively controlled, providing a tool to tune the electronic quantum state of the system and, thus, the anion-neutral interaction dynamics. For a ground state Rb interacting with O-, the detachment induced loss rate is consistent with zero, while the excited state Rb yields a significantly higher loss rate. The results are interpreted via ab initio potential energy curves and compared to the previously studied Rb-OH- system, where an associative electronic detachment reactive loss process hinders the sympathetic cooling of the anion. This implies that with the loss channels closed for ground-state Rb and O- anion, this system provides a platform to observe sympathetic cooling of an anion with an ultracold heavy buffer gas.

Buffer-Gas Cooling of a Single Ion in a Multipole Radio Frequency Trap Beyond the Critical Mass Ratio.

We theoretically investigate the dynamics of a trapped ion immersed in a spatially localized buffer gas. For a homogeneous buffer gas, the ion's energy distribution reaches a stable equilibrium only if the mass of the buffer gas atoms is below a critical value. This limitation can be overcome by using multipole traps in combination with a spatially confined buffer gas. Using a generalized model for elastic collisions of the ion with the buffer-gas atoms, the ion's energy distribution is numerically determined for arbitrary buffer-gas distributions and trap parameters. Three regimes characterized by the respective analytic form of the ion's equilibrium energy distribution are found. Final ion temperatures down to the millikelvin regime can be achieved by adiabatically decreasing the spatial extension of the buffer gas and the effective ion trap depth (forced sympathetic cooling).

Heteronuclear Efimov Scenario with Positive Intraspecies Scattering Length.

We investigate theoretically and experimentally the heteronuclear Efimov scenario for a three-body system that consists of two bosons and one distinguishable particle with positive intraspecies scattering lengths. The three-body parameter at the three-body scattering threshold and the scaling factor between consecutive Efimov resonances are found to be controlled by the scattering length between the two bosons, approximately independent of short-range physics. We observe two excited-state Efimov resonances in the three-body recombination spectra of an ultracold mixture of fermionic ^{6}Li and bosonic ^{133}Cs atoms close to a Li-Cs Feshbach resonance, where the Cs-Cs interaction is positive. Deviation of the obtained scaling factor of 4.0(3) from the universal prediction of 4.9 and the absence of the ground state Efimov resonance shed new light on the interpretation of the universality and the discrete scaling behavior of heteronuclear Efimov physics.

Indirect dynamics in a highly exoergic substitution reaction.

The highly exoergic nucleophilic substitution reaction F(-) + CH3I shows reaction dynamics strikingly different from that of substitution reactions of larger halogen anions. Over a wide range of collision energies, a large fraction of indirect scattering via a long-lived hydrogen-bonded complex is found both in crossed-beam imaging experiments and in direct chemical dynamics simulations. Our measured differential scattering cross sections show large-angle scattering and low product velocities for all collision energies, resulting from efficient transfer of the collision energy to internal energy of the CH3F reaction product. Both findings are in strong contrast to the previously studied substitution reaction of Cl(-) + CH3I [Science 2008, 319, 183-186] at all but the lowest collision energies, a discrepancy that was not captured in a subsequent study at only a low collision energy [J. Phys. Chem. Lett. 2010, 1, 2747-2752]. Our direct chemical dynamics simulations at the DFT/B97-1 level of theory show that the reaction is dominated by three atomic-level mechanisms, an indirect reaction proceeding via an F(-)-HCH2I hydrogen-bonded complex, a direct rebound, and a direct stripping reaction. The indirect mechanism is found to contribute about one-half of the overall substitution reaction rate at both low and high collision energies. This large fraction of indirect scattering at high collision energy is particularly surprising, because the barrier for the F(-)-HCH2I complex to form products is only 0.10 eV. Overall, experiment and simulation agree very favorably in both the scattering angle and the product internal energy distributions.

Associative detachment in anion-atom reactions involving a dipole-bound electron.

Associative electronic detachment (AED) between anions and neutral atoms leads to the detachment of the anion's electron resulting in the formation of a neutral molecule. It plays a key role in chemical reaction networks, like the interstellar medium, the Earth's ionosphere and biochemical processes. Here, a class of AED involving a closed-shell anion (OH-) and alkali atoms (rubidium) is investigated by precisely controlling the fraction of electronically excited rubidium. Reaction with the ground state atom gives rise to a stable intermediate complex with an electron solely bound via dipolar forces. The stability of the complex is governed by the subtle interplay of diabatic and adiabatic couplings into the autodetachment manifold. The measured rate coefficients are in good agreement with ab initio calculations, revealing pronounced steric effects. For excited state rubidium, however, a lower reaction rate is observed, indicating dynamical stabilization processes suppressing the coupling into the autodetachment region. Our work provides a stringent test of ab initio calculations on anion-neutral collisions and constitutes a generic, conceptual framework for understanding electronic state dependent dynamics in AEDs.

Inelastic collisions of ultracold polar LiCs molecules with caesium atoms in an optical dipole trap.

We investigate collisions of ultracold polar LiCs molecules and ultracold caesium atoms. LiCs molecules are formed in an optical dipole trap by photoassociation of caesium and lithium atoms via the B(1)Π excited state followed by spontaneous emission to the X(1)Σ(+) ground state and the lowest triplet state a(3)Σ(+). The molecules are then stored together with caesium atoms in the same optical trap. Rate coefficients for the loss of molecules induced by collisions with surrounding Cs atoms are measured for molecular ensembles produced via different photoassociation resonances. The results are analyzed in terms of the unitarity limit for the inelastic rates and predictions from the universal model of Idziaszek and Julienne (Phys. Rev. Lett., 2010, 104, 113202).

Floquet Hamiltonian engineering of an isolated many-body spin system.

Controlling interactions is the key element for the quantum engineering of many-body systems. Using time-periodic driving, a naturally given many-body Hamiltonian of a closed quantum system can be transformed into an effective target Hamiltonian that exhibits vastly different dynamics. We demonstrate such Floquet engineering with a system of spins represented by Rydberg states in an ultracold atomic gas. By applying a sequence of spin manipulations, we change the symmetry properties of the effective Heisenberg XYZ Hamiltonian. As a consequence, the relaxation behavior of the total spin is drastically modified. The observed dynamics can be qualitatively captured by a semiclassical simulation. Engineering a wide range of Hamiltonians opens vast opportunities for implementing quantum simulation of nonequilibrium dynamics in a single experimental setting.

Evidence of antiblockade in an ultracold Rydberg gas.

We present the experimental observation of the antiblockade in an ultracold Rydberg gas recently proposed by Ates et al. [Phys. Rev. Lett. 98, 023002 (2007)]. Our approach allows the control of the pair distribution in the gas and is based on a strong coupling of one transition in an atomic three-level system, while introducing specific detunings of the other transition. When the coupling energy matches the interaction energy of the Rydberg long-range interactions, the otherwise blocked excitation of close pairs becomes possible. A time-resolved spectroscopic measurement of the Penning ionization signal is used to identify slight variations in the Rydberg pair distribution of a random arrangement of atoms. A model based on a pair interaction Hamiltonian is presented which well reproduces our experimental observations and allows one to deduce the distribution of nearest-neighbor distances.

Calculations of static dipole polarizabilities of alkali dimers: prospects for alignment of ultracold molecules.

The rapid development of experimental techniques to produce ultracold alkali molecules opens the ways to manipulate them and to control their dynamics using external electric fields. A prerequisite quantity for such studies is the knowledge of their static dipole polarizability. In this paper, we computed the variations with internuclear distance and with vibrational index of the static dipole polarizability components of all homonuclear alkali dimers including Fr(2), and of all heteronuclear alkali dimers involving Li to Cs, in their electronic ground state and in their lowest triplet state. We use the same quantum chemistry approach as in our work on dipole moments [Aymar and Dulieu, J. Chem. Phys. 122, 204302 (2005)], based on pseudopotentials for atomic core representation, Gaussian basis sets, and effective potentials for core polarization. Polarizabilities are extracted from electronic energies using the finite-field method. For the heaviest species Rb(2), Cs(2), and Fr(2) and for all heteronuclear alkali dimers, such results are presented for the first time. The accuracy of our results on atomic and molecular static dipole polarizabilities is discussed by comparing our values with the few available experimental data and elaborate calculations. We found that for all alkali pairs, the parallel and perpendicular components of the ground state polarizabilities at the equilibrium distance R(e) scale as (R(e))(3), which can be related to a simple electrostatic model of an ellipsoidal charge distribution. Prospects for possible alignment and orientation effects with these molecules in forthcoming experiments are discussed.

Laser frequency stabilization using a commercial wavelength meter.

We present the characterization of a laser frequency stabilization scheme using a state-of-the-art wavelength meter based on solid Fizeau interferometers. For a frequency-doubled Ti-sapphire laser operated at 461 nm, an absolute Allan deviation below 10-9 with a standard deviation of 1 MHz over 10 h is achieved. Using this laser for cooling and trapping of strontium atoms, the wavemeter scheme provides excellent stability in single-channel operation. Multi-channel operation with a multimode fiber switch results in fluctuations of the atomic fluorescence correlated to residual frequency excursions of the laser. The wavemeter-based frequency stabilization scheme can be applied to a wide range of atoms and molecules for laser spectroscopy, cooling, and trapping.

Direct observation of ultrafast many-body electron dynamics in an ultracold Rydberg gas.

Many-body correlations govern a variety of important quantum phenomena such as the emergence of superconductivity and magnetism. Understanding quantum many-body systems is thus one of the central goals of modern sciences. Here we demonstrate an experimental approach towards this goal by utilizing an ultracold Rydberg gas generated with a broadband picosecond laser pulse. We follow the ultrafast evolution of its electronic coherence by time-domain Ramsey interferometry with attosecond precision. The observed electronic coherence shows an ultrafast oscillation with a period of 1 femtosecond, whose phase shift on the attosecond timescale is consistent with many-body correlations among Rydberg atoms beyond mean-field approximations. This coherent and ultrafast many-body dynamics is actively controlled by tuning the orbital size and population of the Rydberg state, as well as the mean atomic distance. Our approach will offer a versatile platform to observe and manipulate non-equilibrium dynamics of quantum many-body systems on the ultrafast timescale.

Photoionization of optically trapped ultracold atoms with a high-power light-emitting diode.

Photoionization of laser-cooled atoms using short pulses of a high-power light-emitting diode (LED) is demonstrated. Light pulses as short as 30 ns have been realized with the simple LED driver circuit. We measure the ionization cross section of (85)Rb atoms in the first excited state, and show how this technique can be used for calibrating efficiencies of ion detector assemblies.

Versatile cold atom target apparatus.

We report on a compact and transportable apparatus that consists of a cold atomic target at the center of a high resolution recoil ion momentum spectrometer. Cold rubidium atoms serve as a target which can be operated in three different modes: in continuous mode, consisting of a cold atom beam generated by a two-dimensional magneto-optical trap, in normal mode in which the atoms from the beam are trapped in a three-dimensional magneto-optical trap (3D MOT), and in high density mode in which the 3D MOT is operated in dark spontaneous optical trap configuration. The targets are characterized using photoionization.

High-precision semiconductor wavelength sensor based on a double-layer photo diode.

We present a wavelength sensor setup for monochromatic visible light, based on the double-layer photo diode WS-7.56. Employing high-precision electronics and automatic compensation of different error sources, we achieve a measurement accuracy of ±0.025 nm with a resolution below 0.01 nm. The described apparatus is particularly suited for the determination of small laser frequency deviations in atomic physics experiments. Various design issues as well as error sources and diode characteristics are discussed.

Survival probabilities in coherent exciton transfer with trapping.

In the quest for signatures of coherent transport we consider exciton trapping in the continuous-time quantum walk framework. The survival probability displays different decay domains, related to distinct regions of the spectrum of the Hamiltonian. For linear systems and at intermediate times the decay obeys a power law, in contrast with the corresponding exponential decay found in incoherent continuous-time random walk situations. To differentiate between the coherent and incoherent mechanisms, we present an experimental protocol based on a frozen Rydberg gas structured by optical dipole traps.

Experimental investigation of ultracold atom-molecule collisions.

Ultracold collisions between Cs atoms and Cs2 dimers in the electronic ground state are observed in an optically trapped gas of atoms and molecules. The Cs2 molecules are formed in the triplet ground state by cw photoassociation through the outer well of the 0-(g) (P3/2) excited electronic state. Inelastic atom-molecule collisions converting internal excitation into kinetic energy lead to a loss of Cs2 molecules from the dipole trap. Rate coefficients are determined for collisions involving Cs atoms in either the F=3 or F=4 hyperfine ground state, and Cs2 molecules in either highly vibrationally excited states (nu'=32-47) or in low vibrational states (nu'=4-6) of the a3 summation(u)+ triplet ground state. The rate coefficients beta approximately 10(-10) cm3/s are found to be largely independent of the vibrational and rotational excitation indicating unitary limited cross sections.

Optical dipole trap inside a laser resonator.

We report the first realization, to our knowledge, of an optical dipole trap inside the active resonator of a laser. The concept, which is demonstrated with a CO2 laser (lambda = 10.6 microm), combines the advantages of optical power enhancement (up to 1.3-kW peak power) with the intrinsic stability of laser intensity as a result of the feedback of the active laser medium. Two kinds of trapping geometries are presented: a Gaussian trap in a transverse TEM00 mode and a boxlike transverse confinement in a superposition of transverse modes. In addition, longitudinal superlattices are created by two-frequency operation of the laser. Transfer efficiencies of up to 50% from a cesium magneto-optical trap are achieved. Storage times (7 = 0.3 s) are mainly limited by the background gas pressure. Possible sources of additional loss of atoms are discussed.