Picosecond-Scale Ultrafast Many-Body Dynamics in an Ultracold Rydberg-Excited Atomic Mott Insulator.

We report the observation and control of ultrafast many-body dynamics of electrons in ultracold Rydberg-excited atoms, spatially ordered in a three-dimensional Mott insulator (MI) with unity filling in an optical lattice. By mapping out the time-domain Ramsey interferometry in the picosecond timescale, we can deduce entanglement growth indicating the emergence of many-body correlations via dipolar forces. We analyze our observations with different theoretical approaches and find that the semiclassical model breaks down, thus indicating that quantum fluctuations play a decisive role in the observed dynamics. Combining picosecond Rydberg excitation with MI lattice thus provides a platform for simulating nonequilibrium dynamics of strongly correlated systems in synthetic ultracold atomic crystals, such as in a metal-like quantum gas regime.

Ultrafast Creation of Overlapping Rydberg Electrons in an Atomic BEC and Mott-Insulator Lattice.

We study an array of ultracold atoms in an optical lattice (Mott insulator) excited with a coherent ultrashort laser pulse to a state where single-electron wave functions spatially overlap. Beyond a threshold principal quantum number where Rydberg orbitals of neighboring lattice sites overlap with each other, the atoms efficiently undergo spontaneous Penning ionization resulting in a drastic change of ion-counting statistics, sharp increase of avalanche ionization, and the formation of an ultracold plasma. These observations signal the actual creation of electronic states with overlapping wave functions, which is further confirmed by a significant difference in ionization dynamics between a Bose-Einstein condensate and a Mott insulator. This system is a promising platform for simulating electronic many-body phenomena dominated by Coulomb interactions in the condensed phase.

Diffusive to Nonergodic Dipolar Transport in a Dissipative Atomic Medium.

We investigate the dipole-mediated transport of Rydberg impurities through an ultracold gas of atoms prepared in an auxiliary Rydberg state. In one experiment, we continuously probe the system by coupling the auxiliary Rydberg state to a rapidly decaying state that realizes a dissipative medium. In situ imaging of the impurities reveals diffusive spreading controlled by the intensity of the probe laser. By preparing the same density of hopping partners, but then switching off the dressing fields, the spreading is effectively frozen. This is consistent with numerical simulations, which indicate the coherently evolving system enters a nonergodic extended phase. This opens the way to study transport and localization phenomena in systems with long-range hopping and controllable dissipation.

Relaxation of an Isolated Dipolar-Interacting Rydberg Quantum Spin System.

How do isolated quantum systems approach an equilibrium state? We experimentally and theoretically address this question for a prototypical spin system formed by ultracold atoms prepared in two Rydberg states with different orbital angular momenta. By coupling these states with a resonant microwave driving, we realize a dipolar XY spin-1/2 model in an external field. Starting from a spin-polarized state, we suddenly switch on the external field and monitor the subsequent many-body dynamics. Our key observation is density dependent relaxation of the total magnetization much faster than typical decoherence rates. To determine the processes governing this relaxation, we employ different theoretical approaches that treat quantum effects on initial conditions and dynamical laws separately. This allows us to identify an intrinsically quantum component to the relaxation attributed to primordial quantum fluctuations.

Correlated Exciton Transport in Rydberg-Dressed-Atom Spin Chains.

We investigate the transport of excitations through a chain of atoms with nonlocal dissipation introduced through coupling to additional short-lived states. The system is described by an effective spin-1/2 model where the ratio of the exchange interaction strength to the reservoir coupling strength determines the type of transport, including coherent exciton motion, incoherent hopping, and a regime in which an emergent length scale leads to a preferred hopping distance far beyond nearest neighbors. For multiple impurities, the dissipation gives rise to strong nearest-neighbor correlations and entanglement. These results highlight the importance of nontrivial dissipation, correlations, and many-body effects in recent experiments on the dipole-mediated transport of Rydberg excitations.

Observation of Efimov resonances in a mixture with extreme mass imbalance.

We observe two consecutive heteronuclear Efimov resonances in an ultracold Li-Cs mixture by measuring three-body loss coefficients as a function of magnetic field near a Feshbach resonance. The first resonance is detected at a scattering length of a_((0))=-320(10)a_((0)), corresponding to ∼7(∼3) times the Li-Cs (Cs-Cs) van der Waals range. The second resonance appears at 5.8(1.0)a_((0)), close to the unitarity-limited regime at the sample temperature of 450 nK. Indication of a third resonance is found in the atom loss spectra. The scaling of the resonance positions is close to the predicted universal scaling value of 4.9 for zero temperature. Deviations from universality might be caused by finite-range and temperature effects, as well as magnetic field-dependent Cs-Cs interactions.

Full counting statistics of laser excited Rydberg aggregates in a one-dimensional geometry.

We experimentally study the full counting statistics of few-body Rydberg aggregates excited from a quasi-one-dimensional atomic gas. We measure asymmetric excitation spectra and increased second and third order statistical moments of the Rydberg number distribution, from which we determine the average aggregate size. Estimating rates for different excitation processes we conclude that the aggregates grow sequentially around an initial grain. Direct comparison with numerical simulations confirms this conclusion and reveals the presence of liquidlike spatial correlations. Our findings demonstrate the importance of dephasing in strongly correlated Rydberg gases and introduce a way to study spatial correlations in interacting many-body quantum systems without imaging.

Observing the dynamics of dipole-mediated energy transport by interaction-enhanced imaging.

Electronically highly excited (Rydberg) atoms experience quantum state-changing interactions similar to Förster processes found in complex molecules, offering a model system to study the nature of dipole-mediated energy transport under the influence of a controlled environment. We demonstrate a nondestructive imaging method to monitor the migration of electronic excitations with high time and spatial resolution, using electromagnetically induced transparency on a background gas acting as an amplifier. The continuous spatial projection of the electronic quantum state under observation determines the many-body dynamics of the energy transport.

Spontaneous avalanche ionization of a strongly blockaded Rydberg gas.

We report the sudden and spontaneous evolution of an initially correlated gas of repulsively interacting Rydberg atoms to an ultracold plasma. Under continuous laser coupling we create a Rydberg ensemble in the strong blockade regime, which at longer times undergoes an ionization avalanche. By combining optical imaging and ion detection, we access the full information on the dynamical evolution of the system, including the rapid increase in the number of ions and a sudden depletion of the Rydberg and ground state densities. Rydberg-Rydberg interactions are observed to strongly affect the dynamics of plasma formation. Using a coupled rate-equation model to describe our data, we extract the average energy of electrons trapped in the plasma, and an effective cross section for ionizing collisions between Rydberg atoms and atoms in low-lying states. Our results suggest that the initial correlations of the Rydberg ensemble should persist through the avalanche. This would provide the means to overcome disorder-induced heating, and offer a route to enter new strongly coupled regimes.

Sub-Poissonian statistics of Rydberg-interacting dark-state polaritons.

We observe individual dark-state polaritons as they propagate through an ultracold atomic gas involving Rydberg states coupled via an electromagnetically induced transparency resonance. Strong long-range interactions between Rydberg excitations give rise to a blockade between polaritons, resulting in large optical nonlinearities and modified polariton number statistics. By combining optical imaging and high-fidelity detection of the Rydberg polaritons we investigate both aspects of this coupled atom-light system. We map out the full nonlinear optical response as a function of atomic density and follow the temporal evolution of polaritons through the atomic cloud. In the blockade regime, the statistical fluctuations of the polariton number drop well below the quantum noise limit. The low level of fluctuations indicates that photon correlations modified by the strong interactions have a significant backaction on the Rydberg atom statistics.

Interaction enhanced imaging of individual Rydberg atoms in dense gases.

We propose a new all-optical method to image individual Rydberg atoms embedded within dense gases of ground state atoms. The scheme exploits interaction-induced shifts on highly polarizable excited states of probe atoms, which can be spatially resolved via an electromagnetically induced transparency resonance. Using a realistic model, we show that it is possible to image individual Rydberg atoms with enhanced sensitivity and high resolution despite photon-shot noise and atomic density fluctuations. This new imaging scheme could be extended to other impurities such as ions, and is ideally suited to equilibrium and dynamical studies of complex many-body phenomena involving strongly interacting particles. As an example we study blockade effects and correlations in the distribution of Rydberg atoms optically excited from a dense gas.

Formation and relaxation of RbHe exciplexes on He nanodroplets studied by femtosecond pump and picosecond probe spectroscopy.

Vibrationally resolved photoionization spectra of RbHe exciplexes forming on He nanodroplets are recorded using femtosecond pump-probe spectroscopy with amplitude-shaped probe pulses. The time-evolution of the spectra reveals an exciplex formation time ~10 ps followed by vibrational relaxation extending up to ≳ 1 ns. This points to an indirect, time-delayed desorption process of RbHe off the He surface.

Nanosecond photofragment imaging of adiabatic molecular alignment.

Adiabatic alignment of CH(3)I, induced by the anisotropic interaction of this symmetric top molecule with the intense field of a nonresonant infrared laser pulse, has been studied using velocity map imaging. We are using photodissociation imaging with pulsed nanosecond lasers to probe the distribution of the molecular axis in the laboratory space. In contrast to the commonly used probing with femtosecond laser pulses, this technique directly yields the degree of alignment over an extended space-time volume. This will be relevant for future reactive scattering experiments with laser-aligned molecules. The obtained degree of alignment, (cos (2)θ), measured as a function of the infrared laser intensity, agrees well with a quantum calculation for rotationally cold methyl iodide. The strong infrared laser is also found to modify the photofragmentation dynamics and open up pathways to CH(3)I(+) formation and subsequent fragmentation.

Coherent population trapping with controlled interparticle interactions.

We investigate coherent population trapping in a strongly interacting ultracold Rydberg gas. Despite the strong van der Waals interactions and interparticle correlations, we observe the persistence of a resonance with subnatural linewidth at the single-particle resonance frequency as we tune the interaction strength. This narrow resonance cannot be understood within a mean-field description of the strong Rydberg-Rydberg interactions. Instead, a many-body density matrix approach, accounting for the dynamics of interparticle correlations, is shown to reproduce the observed spectral features.

Photoassociation spectroscopy of the B 1Pi state of LiCs.

We present an accurate potential energy curve of the B (1)Pi state in the LiCs molecule for which vibrational levels between v(') = 0 and v(') = 35 (bound by 11.4 GHz) were measured by photoassociation spectroscopy in an ultracold ensemble of (7)Li and (133)Cs atoms. By the combination of conventional spectroscopic data of the B-X system and the new photoassociation measurements a very precise value of the dissociation energy of the ground state X (1)Sigma(+) of LiCs was determined to be D(0) = 5783.495(5) cm(-1).

Absolute photodetachment cross section measurements of the O(-) and OH(-) anion.

Absolute total photodetachment cross sections of O(-) and OH(-) anions stored in a multipole radio frequency trap have been measured using a novel laser depletion tomography method. For OH(-) the total cross sections of 8.5(1)(stat)(3)(syst) and 8.1(1)(stat)(7)(syst)x10(-18) cm(2), measured at 662 and 632 nm, respectively, were found constant in the temperature range of 8-300 K. The O(-) cross sections 5.9(1)(stat)(2)(syst) and 6.3(1)(stat)(2)(syst)x10(-18) cm(2) measured at 170 K at 662 and 532 nm, respectively, agree within error estimations with preceding experiments and increase the accuracy of the widely used calibration standard for relative photodetachment measurements of diverse atomic and molecular species.

Formation of ultracold dipolar molecules in the lowest vibrational levels by photoassociation.

We recently reported the formation of ultracold LiCs molecules in the rovibrational ground state X1sigma+, v" = 0,J" = 0 (J. Deiglmayr et al., Phys. Rev. Lett., 2008, 101, 133004). Here we discuss details of the experimental setup and present a thorough analysis of the photoassociation step including the photoassociation line shape. We predict the distribution of produced ground state molecules using accurate potential energy curves combined with an ab initio dipole transition moment and compare this prediction with experimental ionization spectra. Additionally we improve the value of the dissociation energy for the X1sigma+ state by high resolution spectroscopy of the vibrational ground state.

Formation of ultracold polar molecules in the rovibrational ground state.

Ultracold LiCs molecules in the absolute ground state X1Sigma+, v'' = 0, J'' = 0 are formed via a single photoassociation step starting from laser-cooled atoms. The selective production of v'' = 0, J'' = 2 molecules with a 50-fold higher rate is also demonstrated. The rotational and vibrational state of the ground state molecules is determined in a setup combining depletion spectroscopy with resonant-enhanced multiphoton ionization time-of-flight spectroscopy. Using the determined production rate of up to 5 x 10(3) molecules/s, we describe a simple scheme which can provide large samples of externally and internally cold dipolar molecules.

Inverse temperature dependent lifetimes of transient S(N)2 ion-dipole complexes.

The association and collisional stabilization of the S(N)2 entrance channel complex [Cl(-)...CH3Cl]* is studied in a low-temperature radiofrequency ion trap. The temperature dependence of the ternary rate coefficient is measured and a much stronger inverse temperature dependence than expected from a simple statistical calculation is found. From these data the lifetime of the transient S(N)2 complex has been derived as a function of temperature. It is suggested that the inverse temperature dependent rates of nonsymmetric S(N)2 reactions are related to the observed inverse temperature dependence of the transient ion-dipole complexes.

Nonstandard behavior of a negative ion reaction at very low temperatures.

We have studied the negative ion reaction NH2-+H_{2}-->NH_{3}+H- in the temperature range from 300 to 8 K. We observe a strongly suppressed probability for proton transfer at room temperature. With decreasing temperature, this probability increases, in accordance with a longer lifetime of an intermediate anion-neutral complex. At low temperatures, a maximum in the reaction rate coefficient is observed that suggests the presence of a very small barrier at long range or a quantum mechanical resonance feature.