cold molecules; laser cooling; cold chemistry; ion traps; chemical reaction dynamics; ion-molecule chemistry; Coulomb crystals
Roesch Daniel, Willitsch Stefan, Chang Yuan-Pin, Kuepper Jochen (2014), Chemical reactions of conformationally selected 3-aminophenol molecules in a beam with Coulomb-crystallized Ca plus ions, in JOURNAL OF CHEMICAL PHYSICS
, 140(12), 124202.
Hall Felix H. J., Eberle Pascal, Hegi Gregor, Raoult Maurice, Aymar Mireille, Dulieu Olivier, Willitsch Stefan (2013), Ion-neutral chemistry at ultralow energies: dynamics of reactive collisions between laser-cooled Ca+ ions and Rb atoms in an ion-atom hybrid trap, in MOLECULAR PHYSICS
, 111(14-15), 2020-2032.
Hall Felix H. J., Aymar Mireille, Raoult Maurice, Dulieu Olivier, Willitsch Stefan (2013), Light-assisted cold chemical reactions of barium ions with rubidium atoms, in MOLECULAR PHYSICS
, 111(12-13), 1683-1690.
Willitsch Stefan (2013), MOLECULAR PHYSICS Ultracold menage a trois, in NATURE PHYSICS
, 9(8), 461-462.
Chang Yuan-Pin, Dlugolecki Karol, Küpper Jochen, Rösch Daniel, Wild Dieter, Willitsch Stefan (2013), Specific Chemical Reactivities of Spatially Separated 3-Aminophenol Conformers with Cold Ca+ Ions, in Science
, 342(6254), 98.
Willitsch Stefan (2013), Ultracold ménage a trois, in Nature Physics
, 9, 461.
Hall Felix H. J., Willitsch Stefan (2012), Millikelvin Reactive Collisions between Sympathetically Cooled Molecular Ions and Laser-Cooled Atoms in an Ion-Atom Hybrid Trap, in PHYSICAL REVIEW LETTERS
, 109(23), 233202.
Recent advances in the preparation of "cold" molecules and ions at very low translational energies (E_trans/k_B<1 K) in the gas phase have opened up perspectives to study chemical reactions in a new physical regime. In conjunction with recently established techniques for the simultaneous preparation of the internal, i.e., rotational-vibrational, quantum state of the cold molecules, it has become possible not only to investigate, but also to control chemical processes at a level of accuracy which has not been possible before. The present project aims at investigating chemical reactions of atomic and molecular ions with neutral atoms at collision energies E_coll/k_B>1 mK (the "cold regime"). By simultaneously preparing the reaction partners in a well-defined internal quantum state, ion-neutral chemical processes will be studied with full quantum-state resolution over a collision energy range spanning up to six orders magnitude. These objectives will be reached by extending a recently developed "hybrid trap" for the simultaneous trapping and cooling of atomic ions and neutral atoms with a threshold-photoionisation setup for the state-selected generation of molecular ions. Subsequent sympathetic cooling of their translational motion will enable the study of reactive processes with ultracold Rb atoms down to mK energies. Besides taking ion-neutral reaction studies into a new physical domain, the experimental tools established in the present project will also enable unprecedented levels of control over reactive processes with molecular ions by precisely determining their quantum state and position in space as well as accurately controlling the collision energy with the neutrals. In a first step, we will study the dynamics of reactive collisions of simple systems, i.e., atomic ions and ultracold atoms. Using the model reactions Ca^+ + Rb and Ba^+ + Rb, we will characterise general features of cold ionic collisions. These include light-assisted processes such as radiative charge exchange and molecule formation. Our experiments will also serve to test ion-neutral scattering models in the cold regime. Subsequently, we will enhance the scope of our studies to molecular collision partners and investigate reactive processes between state-selected molecular ions such as N_2^+ and Br_2^+ and ultracold Rb atoms. The aim is to to elucidate molecular phenomena in cold ionic collisions, in particular electron transfer and radiation-driven processes. Finally, we will take the first steps to extend our studies to reactions of polyatomic ions such as H_2O^+, CO_2^+ and NH_3^+.