Zwitterions Functionalized by Optical Cycling Centers: Toward Laser-Coolable Polyatomic Molecular Cations

Extending the Large Molecule Limit: The Role of Fermi Resonance in Developing a Quantum Functional Group

“…Functionalizing large molecules with optical cycling centers (OCCs) is being explored as a means for extending the exquisite control available in quantum information science to the chemical domain. − Success requires that these OCCs absorb and emit many photons without changing their vibrational states. To accomplish this task, molecular design rules are being developed, aided and validated by experiments, to guide the creation of the ideal quantum functional groups. − For example, prior work has demonstrated that alkaline earth alkoxides provide a general and versatile chemical moiety for optical cycling applications, as the alkaline earth radical electron can be excited without perturbing the vibrational structure of the molecule. ,,− Similarly, traditional physical organic principles, such as electron-withdrawing, have been shown to improve OCCs performance. , Further, experimental and theoretical extensions to more complex acenes, , diamondoids, and even surfaces suggest an exciting path forward for creating increasingly complex and functional quantum systems.…”