Preparation and detection of states with simultaneous spin alignment and selectable molecular orientation in PbO

We are pursuing an experiment to measure the electric dipole moment of the electron using the molecule PbO. This measurement requires the ability to prepare quantum states with selectable orientation of the molecular axis and, simultaneously, alignment of the electron spin perpendicular to this axis. It also requires efficient detection of the evolution of the spin-alignment direction within such a state. We describe a series of experiments that have achieved these goals, and the features and limitations of the techniques. Our results include observation of and explanation for a small electric-field dependence of the magnetic g factor in the oriented states. We also discuss possible approaches for improved efficiency in this and similar systems.