4.8 Article

Franck-Condon Tuning of Optical Cycling Centers by Organic Functionalization

Journal

PHYSICAL REVIEW LETTERS
Volume 126, Issue 12, Pages -

Publisher

AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.126.123002

Keywords

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Funding

  1. U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0019245]

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The study investigates the possibility of using chemical functional groups to construct optical cycling units, finding that optical cycle leakage can be effectively reduced through chemical substitution to enhance the electron-withdrawing strength of the aromatic molecular ligand. This offers a new approach for implementing optical cycling technology in large organic compounds.
Laser induced electronic excitations that spontaneously emit photons and decay directly to the initial ground state (optical cycling transitions) are used in quantum information and precision measurement for state initialization and readout. To extend this primarily atomic technique to large, organic compounds, we theoretically investigate optical cycling of alkaline earth phenoxides and their functionalized derivatives. We find that optical cycle leakage due to wave function mismatch is low in these species, and can be further suppressed by using chemical substitution to boost the electron-withdrawing strength of the aromatic molecular ligand through resonance and induction effects. This provides a straightforward way to use chemical functional groups to construct optical cycling moieties for laser cooling, state preparation, and quantum measurement.

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