Franck-Condon tuning of optical cycling centers by organic functionalization

Abstract

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 organic compounds, we theoretically investigate optical cycling of alkaline earth phenoxides and their functionalized derivatives. We find that optical cycle leakage due to wavefunction 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.

6 pages, 3 figures

References in corpus (5)

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• Direct Laser Cooling of a Symmetric Top Molecule
• High accuracy theoretical investigations of CaF, SrF, and BaF and implications for laser-cooling
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Cited by in corpus (16)

• Magneto-Optical Trapping and Sub-Doppler Cooling of a Polyatomic Molecule
• Laser cooled molecules
• Functionalizing Aromatic Compounds with Optical Cycling Centers
• Accurate prediction and measurement of vibronic branching ratios for laser cooling linear polyatomic molecules
• Establishing a nearly closed cycling transition in a polyatomic molecule
• Complete Controllability Despite Degeneracy: Quantum Control of Enantiomer-Specific State Transfer in Chiral Molecules
• Observation and laser spectroscopy of ytterbium monomethoxide, YbOCH${}_3$
• Optical Trapping of a Polyatomic Molecule in an $\ell$-Type Parity Doublet State
• Blackbody thermalization and vibrational lifetimes of trapped polyatomic molecules
• Laser spectroscopy of aromatic molecules with optical cycling centers: strontium (I) phenoxides
• Fully saturated hydrocarbons as hosts of optical cycling centers
• Multivalent optical cycling centers in polyatomic molecules
• Clock-line-mediated Sisyphus Cooling
• Decoherence dynamics in molecular qubits: Exponential, Gaussian and beyond
• Optical cycling in charged complexes with Ra-N bonds
• Vibronic coupling limits the use of high-lying electronic states in complex molecules for laser cooling