Upper limits to the reaction rate coefficients of C(n)(-) and C(n)H(-) (n = 2, 4, 6) with molecular hydrogen.

In the interstellar medium (ISM) ion­molecule reactions play a key role in forming complex molecules. Since 2006, after the radioastronomical discovery of the first of by now six interstellar anions, interest has grown in understanding the formation and destruction pathways of negative ions in the ISM. Experiments have focused on reactions and photodetachment of the identified negatively charged ions. Hints were found that the reactions of CnH(­) with H2 may proceed with a low (<10(­13) cm(3) s(­1)), but finite rate [Eichelberger, B.; et al. Astrophys. J. 2007, 667, 1283]. Because of the high abundance of molecular hydrogen in the ISM, a precise knowledge of the reaction rate is needed for a better understanding of the low-temperature chemistry in the ISM. A suitable tool to analyze rare reactions is the 22-pole radiofrequency ion trap. Here, we report on reaction rates for Cn(­) and CnH(­) (n = 2, 4, 6) with buffer gas temperatures of H2 at 12 and 300 K. Our experiments show the absence of these reactions with an upper limit to the rate coefficients between 4 × 10(­16) and 5 × 10(­15) cm(3) s(­1), except for the case of C2(­), which does react with a finite rate with H2 at low temperatures. For the cases of C2H(­) and C4H(­), the experimental results were confirmed with quantum chemical calculations. In addition, the possible influence of a residual reactivity on the abundance of C4H(­) and C6H(­) in the ISM were estimated on the basis of a gas-phase chemical model based on the KIDA database. We found that the simulated ion abundances are already unaffected if reaction rate coefficients with H2 were below 10(­14) cm(3) s(­1).

High resolution spatial map imaging of a gaseous target.

Electrostatic ion imaging with the velocity map imaging mode is a widely used method in atomic and molecular physics and physical chemistry. In contrast, the spatial map imaging (SMI) mode has received very little attention, despite the fact that it has been proposed earlier [A. T. J. B. Eppink and D. H. Parker, Rev. Sci. Instrum. 68, 3477 (1997)]. Here, we present a detailed parametric characterization of SMI both by simulation and experiment. One-, two- and three-dimensional imaging modes are described. The influence of different parameters on the imaging process is described by means of a Taylor expansion. To experimentally quantify elements of the Taylor expansion and to infer the spatial resolution of our spectrometer, photoionization of toluene with a focused laser beam has been carried out. A spatial resolution of better than 4 µm out of a focal volume of several mm in diameter has been achieved. Our results will be useful for applications of SMI to the characterization of laser beams, the overlap control of multiple particle or light beams, and the determination of absolute collision cross sections.

Internal state thermometry of cold trapped molecular anions.

Photodetachment spectroscopy of OH(-) and H(3)O(2)(-) anions has been performed in a cryogenic 22-pole radiofrequency multipole trap. Measurements of the detachment cross section as a function of laser frequency near threshold have been analysed. Using this bound-free spectroscopy approach we could demonstrate rotational and vibrational cooling of the trapped anions by the buffer gas in the multipole trap. Below 50 K the OH(-) rotational temperature shows deviations from the buffer gas temperature, and possible causes for this are discussed. For H(3)O(2)(-) vibrational cooling of the lowest vibrational quantum states into the vibrational ground state is observed. Its photodetachment cross section near threshold is modelled with a Franck-Condon model, with a detachment threshold that is lower, but still in agreement with the expected threshold for this system.

Coherent interaction of a single fermion with a small bosonic field.

We have experimentally studied few-body impurity systems consisting of a single fermionic atom and a small bosonic field on the sites of an optical lattice. Quantum phase revival spectroscopy has allowed us to accurately measure the absolute strength of Bose-Fermi interactions as a function of the interspecies scattering length. Furthermore, we observe the modification of Bose-Bose interactions that is induced by the interacting fermion. Because of an interference between Bose-Bose and Bose-Fermi phase dynamics, we can infer the mean fermionic filling of the mixture and quantify its increase (decrease) when the lattice is loaded with attractive (repulsive) interspecies interactions.

Time-resolved observation of coherent multi-body interactions in quantum phase revivals.

Interactions lie at the heart of correlated many-body quantum phases. Typically, the interactions between microscopic particles are described as two-body interactions. However, it has been shown that higher-order multi-body interactions could give rise to novel quantum phases with intriguing properties. So far, multi-body interactions have been observed as inelastic loss resonances in three- and four-body recombinations of atom-atom and atom-molecule collisions. Here we demonstrate the presence of effective multi-body interactions in a system of ultracold bosonic atoms in a three-dimensional optical lattice, emerging through virtual transitions of particles from the lowest energy band to higher energy bands. We observe such interactions up to the six-body case in time-resolved traces of quantum phase revivals, using an atom interferometric technique that allows us to precisely measure the absolute energies of atom number states at a lattice site. In addition, we show that the spectral content of these time traces can reveal the atom number statistics at a lattice site, similar to foundational experiments in cavity quantum electrodynamics that yield the statistics of a cavity photon field. Our precision measurement of multi-body interaction energies provides crucial input for the comparison of optical-lattice quantum simulators with many-body quantum theory.

Anomalous expansion of attractively interacting fermionic atoms in an optical lattice.

The interplay of thermodynamics and quantum correlations can give rise to counterintuitive phenomena in many-body systems. We report on an isentropic effect in a spin mixture of attractively interacting fermionic atoms in an optical lattice. As we adiabatically increase the attraction between the atoms, we observe that the gas expands instead of contracting. This unexpected behavior demonstrates the crucial role of the lattice potential in the thermodynamics of the fermionic Hubbard model.

State selective production of molecules in optical lattices.

We demonstrate quantum control over both internal and external quantum degrees of freedom in a high number of identical "chemical reactions," carried out in an array of microtraps in a 3D optical lattice. Starting from a Mott insulating phase of an ultracold atomic quantum gas, we use two-photon Raman transitions to create molecules on lattice sites occupied by two atoms. In the atom-molecule conversion process, we can control both the internal rovibronic and external center of mass quantum state of the molecules. The lattice isolates the microscopic chemical reactions from each other, thereby allowing photoassociation spectra without collisional broadening even at high densities of up to 2 x 10(15) cm(-3).