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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...