Abstract: Techniques for achieving complete quantum control over atoms have been developed and perfected over the past four decades with great success. This work has led to multiple Nobel prizes and has been the catalyst for rapid advances in a broad array of research fields. A natural progression forward is to develop control over molecules. Compared with atoms, molecules have an increased complexity in their internal structure due to their additional degrees of freedom of rotations and vibrations. Control over these additional degrees of freedom would allow for the study of chemistry with unprecedented detail, the study of new many-body effects, and more precise tests of fundamental physics.

In this talk, I will discuss recent results demonstrating rotational cooling of the silicon monoxide cation (SiO⁺) via optical pumping with a spectrally pulse-shaped broadband laser. Cooling is achieved on a <100-ms time scale and attains a ground state population of 94(3)% (T=0.53(6) K). I also describe a new approach to pulse shaping for steady state preparation of arbitrary rovibrational states including highly excited rotational states known as ​“super rotors.” The technique, available to a class of molecules exhibiting nearly diagonal Franck-Condon factors, is demonstrated on SiO⁺ through the steady-state preparation of a narrow rotational population distribution (∆N=3) centered around arbitrary targeted rotational states between N=0 and N=65.