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. Evide...