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arXiv:1211.2436 · Physical Review A

Reactive collisions of trapped anions with ultracold atoms

Johannes Deiglmayr, A. Göritz, Th. Best, Matthias Weidemüller, Roland Wester

Published Oct 31, 2012• 58 citations
arXivHTMLPDF

Abstract

We present a scheme to embed molecular anions in a gas of ultracold rubidium atoms as a route towards the preparation of cold molecular ions by collisional cooling with ultracold atoms. Associative detachment as an important loss process in collisions between OH${}^{\ensuremath{-}}$ molecules and rubidium atoms is studied. The density distribution of trapped negative ions in the multipole radio frequency trap is measured by photodetachment tomography, which allows us to derive absolute rate coefficients for the process. We define a regime where translational and internal cooling of molecular ions embedded into the ultracold atomic cloud can be achieved.

DOI
10.1103/physreva.86.043438

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We present a scheme to embed molecular anions in a gas of ultracold rubidium atoms as a route towards the preparation of cold molecular ions by collisional cooling with ultracold atoms. Associative detachment as an important loss process in collisions between OH\ensuremath−{}^{\ensuremath{-}}\ensuremath− molecules and rubidium atoms is studied. The density distribution of trapped negative ions in the multipole radio frequency trap is measured by photodetachment tomography, which allows us to derive absolute rate coefficients for the process. We define a regime where translational and internal cooling of molecular ions embedded into the ultracold atomic cloud can be achieved.
The absolute photodetachment cross section of OH- anions at a rotational and translational temperature of 170 K is determined by measuring the detachment-induced decay rate of the anions in a multipole radio-frequency ion trap. In comparison with previous results, the obtained cross section shows the importance of the initial rotational-state distribution. Using a tomography scan of the photodetachment laser through the trapped ion cloud, the derived cross section is model-independent and thus features a small systematic uncertainty. The tomography also yields the column density of the OH- anions in the 22-pole ion trap in good agreement with the expected trapping potential of a large field free region bound by steep potential walls.
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.
This dissertation reports sympathetic cooling of the molecular hydroxyl anion (OH– ) via collisions with ultra cold rubidium (Rb) atoms. The anion’s translational and rotational degrees of freedom were cooled simultaneously. A new generation hybrid atom-ion trap (HAITrap) has been set up, combining an octupole radio frequency (rf) trap for ion storage and a dark-spontaneous force optical trap (darkSPOT) for Rb atoms. While the octupole rf-trap provides a large rf-field-free region decreasing rf-induced collisional heating, the darkSPOT reinforces this effect by locating the atom cloud in the center of the ion trap. The darkSPOT also enables to generate large dark state fractions, suppressing associative detachment and thus ion losses. Evidence on translational sympathetic cooling in the HAITrap was provided using two methods of kinetic thermometry: photodetachment tomography (PD) and measurements of the time of flight (ToF) distribution. The ToF analysis has shown to be more conclusive and numerical simulations validated the experimental findings qualitatively. Based on a one dimensional ToF-temperature mapping, the narrowest measured energy spread would correspond to a temperature of 35 ± 5K. Deviations from thermal distributions were observed, as predicted from a theoretical model developed by our group. Rotational sympathetic cooling was observed via state selective photodetachment (SSPD). This was performed by pre-cooling the atoms with helium buffer gas at 295K and further cooling the ions with Rb at 300 μK. SSPD thermometry yielded a 70% decrease of the anions rotational temperature after interaction with Rb. These experimental findings could have direct applications in cold collision studies, quantum control of chemical reactions or sympathetic cooling of anti-protons.
Ultracold cold molecular ions promise new directions in various studies of fundamental physics, such as precision measurements, ultracold chemistry and quantum information sciences. All these exciting applications require the molecular ion to be prepared at ground state of motional and internal degrees of freedom. It has been proposed that this stringent goal could be achieved through sympa-thetic cooling via collisions with laser-cooled neutral atoms. Three fundamentalissues of this method are addressed in this thesis.First, an analytical model is established to accurately describe collision-induced heating of a single ion in contact with cold neutral atoms. This model reveals that micromotion interruption is the cause of heating, and gives results about steady-state temperature and sympathetic cooling rate verified by Monte-Carlo simulations. It also provides insight into the power-law tails observed in theenergy distribution of the trapped ion.Next, we consider the case of multiple ions, whose inter-particle Coulomb repulsion causes ions in the Coulomb crystal state to spontaneously melt into a gas phase ion cloud, due to the same micromotion interruption mechanism. The analysis of this problem with a plasma model leads to the experimental determination of a quantity central to plasma physics, Coulomb Logarithm, in anion trap.Finally, we demonstrate a molecular ion spectroscopy technique through the example of trap-depletion photodissociation of BaCl + . Although not sensitive to rotational structure, this method already reveals much about the fundamental quantum physics in the photodissociation process. The measured cross-section results paves the road toward state-selective spectroscopy currently going on in our lab.
Abstract We present a theoretical investigation of reactive and non-reactive collisions of Li and Rb atoms with C 2 − molecular anions at low temperatures in the context of sympathetic cooling in hybrid trap experiments. Based on accurate potential energy surfaces for the singlet and triplet states of the Li– C 2 − and Rb– C 2 − systems, we show that the associative electronic detachment reaction is inefficient but that it occurs with a large rate for collisions involving excited states of either Li/Rb or C 2 − . We also investigate rotationally inelastic collisions in order to explore the cooling of the translational and rotational degrees of freedom of C 2 − in hybrid ion-atom traps. The effect of micromotion is taken into account by considering Tsallis distributions of collision energies. We show that the translational cooling occurs much more rapidly than rotational cooling and that the presence of excited atoms leads to losses of anions on a timescale comparable to that of rotational cooling.
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.