Collision-Induced C60 Rovibrational Relaxation Probed by State-Resolved Nonlinear Spectroscopy

Quantum state-resolved spectroscopy was recently achieved for C60 molecules when cooled by buffer gas collisions and probed with a midinfrared frequency comb. This rovibrational quantum state resolution for the largest molecule on record is facilitated by the remarkable symmetry and rigidity of C60, which also present new opportunities and challenges to explore energy transfer between quantum states in this many-atom system. Here we combine state-specific optical pumping, buffer gas collisions, and ultrasensitive intracavity nonlinear spectroscopy to initiate and probe the rotation-vibration energy transfer and relaxation. This approach provides the first detailed characterization of C60 collisional energy transfer for a variety of collision partners, and determines the rotational and vibrational inelastic collision cross sections. These results compare well with our theoretical modeling of the collisions, and establish a route towards quantum state control of a new class of unprecedentedly large molecules.