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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.

Anion-molecule nucleophilic substitution (S(N)2) reactions are known for their rich reaction dynamics, caused by a complex potential energy surface with a submerged barrier and by weak coupling of the relevant rotational-vibrational quantum states. The dynamics of the S(N)2 reaction of Cl- + CH3I were uncovered in detail by using crossed molecular beam imaging. As a function of the collision energy, the transition from a complex-mediated reaction mechanism to direct backward scattering of the I- product was observed experimentally. Chemical dynamics calculations were performed that explain the observed energy transfer and reveal an indirect roundabout reaction mechanism involving CH3 rotation.

We report on the observation of ultralong range interactions in a gas of cold Rubidium Rydberg atoms. The van-der-Waals interaction between a pair of Rydberg atoms separated as far as 100,000 Bohr radii features two important effects: Spectral broadening of the resonance lines and suppression of excitation with increasing density. The density dependence of these effects is investigated in detail for the S-and P-Rydberg states with main quantum numbers n ∼ 60 and n ∼ 80 excited by narrow-band continuous-wave laser light. The density-dependent suppression of excitation can be interpreted as the onset of an interaction-induced local blockade.PACS numbers: 32.80. Rm,32.80.Pj,34.20.Cf,03.67.Lx With the advances in laser cooling and trapping, new perspectives for the investigation of Rydberg atoms [1] have been opening. When cooled to very low temperatures, the core motion can be neglected for the timescales of excitation ("frozen Rydberg gas"). Unexpected effects have been discovered, such as the many-body diffusion of excitation [2,3], the population of high-angularmomentum states through free charges [4], or the spontaneous formation and recombination of ultracold plasmas [5,6]. Other fascinating features of cold, interacting Rydberg atoms have been proposed but not been observed so far, e.g. the creation of ultralong range molecules [7,8], whereas molecular crossover resonances have already been found experimentally [9]. One outstanding property of Rydberg atoms is their high polarizability, caused by the large distance between the outer electron and the core. This leads to strong electric field sensitivity and strong long-range dipole-dipole and vander-Waals (vdW) interactions are expected. First indications of interaction effects between Rydberg gases at high densities have been found in an atomic beam experiment [10] and, more recently, collisional evidence for ultralong range interactions in a cold Rydberg gas has been reported [11]. In a frozen gas these interactions make Rydberg atoms possible candidates for quantum information processing [12,13]. One promising approach is based on the concept of a dipole blockade [13], i.e. the inhibition of multiple Rydberg excitations in a confined volume due to interaction-induced energy shifts.In this Letter we report on experimental evidence for ultralong range interactions in a frozen Rydberg gas and we present high-resolution spectroscopic signatures of these interactions. citation from a cold gas [14]. Different to these findings, our experiment makes use of a tunable narrow-bandwidth continuous-wave (cw) laser for Rydberg excitation and thus allows for high-resolution spectroscopy of the resonance lines. By varying the density of Rydberg atoms in a controlled way, the influence of interactions on the strength and the shape of these lines is investigated in detail. Signatures of ultralong range interactions appear as spectral broadening of the excitation lines and saturation of the resonance peak height, the latter being an indication of the dipole blockade.To re...

We have calculated the long-range interaction potential curves of highly excited Rydberg atom pairs for the combinations Li–Li, Na–Na, K–K, Rb–Rb and Cs–Cs in a perturbative approach. The dispersion C-coefficients are determined for all symmetries of molecular states that correlate to the ns–ns, np–np and nd–nd asymptotes. Fitted parameters are given for the scaling of the C-coefficients as a function of the principal quantum number n for all homonuclear pairs of alkali metal atoms.

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.

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) a0 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.The control of interactions in ultracold atomic systems via magnetically tunable Feshbach resonances opens up new pathways for the investigation of few-and manybody physics [1]. One intriguing example is the access to the universal regime, which is characterized by a magnitude of the scattering length a exceeding all other length scales of the system. In the limit of at least two resonant pairwise interactions, an infinite series of three-body bound-states, the so called Efimov states, exists [2][3][4]. Counterintuitively, these trimers persist even for a < 0, where the two body potential does not support a boundstate. The ratio between two subsequent trimer energies follows a discrete scale invariance with a universal scaling factor of exp(−2π/s 0 ). Here, s 0 only depends on the quantum statistics of the constituent atoms, their mass ratio, and the number of resonant interactions [3, 5]. This scale invariance is also reflected in those values of a where the energy of the bound-states coincides with the threshold of three free atoms for a < 0, resulting in enhanced three-body loss. When the position of the first resonance is given by a − only depends on the characteristic range r 0 of the interatomic van der Waals potential [6][7][8][9][10][11]. The universal scaling factor acquires a value of 22.7 for equal mass constituents and features a drastic reduction in heteronuclear massimbalanced systems of two heavy and one light particle [3, 5], resulting e.g. in a factor of 4.9 for a 6 Li-133 Cs mixture.In ultracold atom experiments, Efimov resonances become evident in the three-body loss coefficient L 3 in the rate equation for atom lossṅ = −L 3 n 3 . Here, n denotes the number density of atoms, and L 3 ∝ C(a)a 4 . The Efimov physics are contained in the dimensionless, logperiodic function C(a). Thus far, Efimov resonances have been studied in several equal mass systems [6,7,[12][13][14][15][16][17][18], where the scaling between different resonances is predicted to follow C(a) = C(22.7a). This large scaling factor demands a level of temperature and magnetic field control which makes the observation of an excited Efimov states highly involved. There had been indication of such an excited state in a three-component Fermi gas of 6 Li atoms ...

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.