Collision-Induced <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline" overflow="scroll"><mml:msub><mml:mrow><mml:mi mathvariant="normal">C</mml:mi></mml:mrow><mml:mn>60</mml:mn></mml:msub></mml:math> Rovibrational Relaxation Probed by State-Resolved Nonlinear Spectroscopy
Lee R. Liu, P. Bryan Changala, Marissa L. Weichman, Qizhong Liang, Jutta Toscano, Jacek Kłos, Svetlana Kotochigova, David J. Nesbitt, Jun Ye
Abstract
Quantum state-resolved spectroscopy was recently achieved for C 60 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 C 60 , 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 C 60 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.