Abstract

Laser cooling, trapping, and coherent control of ultracold atoms and molecules has afforded the possibility of assembling pristine and highly tunable quantum many body systems. This relies on excellent experimental control over ultracold atoms or molecules and their interactions. Another paradigm we are exploring is to treat single polyatomic molecules as inherently quantum many body systems due to their strongly interacting constituent nuclei and electrons. In addition, a diverse array of intramolecular coupling mechanisms arise "for free" in polyatomic molecules, such as rovibronic coupling, hyperfine-rotation coupling, covalent bonds between atoms, and nuclear and electron exchange statistics. The key to unlock these phenomena in the lab is quantum-state resolved spectroscopy, which relaxes the requirements for experimental control. However, in general, molecular complexity comes at the price of spectral broadening and congestion. C₆₀, with its rigid molecular cage structure and high degree of symmetry, is a notable exception, enabling quantum state resolved spectroscopy in an unusually large polyatomic molecule. We present an experimental rovibrational spectrum of gas phase C₆₀ fullerene, obtained by QCL (Quantum Cascade Laser) cavity enhanced absorption spectroscopy.

© 2023 The Author(s)