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Pathway toward Optical Cycling and Laser Cooling of Functionalized Arenes

  • Debayan Mitra*
    Debayan Mitra
    Department of Physics, Harvard University, Cambridge, Massachusetts 02138, United States
    Harvard-MIT Center for Ultracold Atoms, Cambridge, Massachusetts 02138, United States
    *[email protected]
  • Zack D. Lasner
    Zack D. Lasner
    Department of Physics, Harvard University, Cambridge, Massachusetts 02138, United States
    Harvard-MIT Center for Ultracold Atoms, Cambridge, Massachusetts 02138, United States
  • Guo-Zhu Zhu
    Guo-Zhu Zhu
    Department of Physics and Astronomy, University of California, Los Angeles, California 90095, United States
    Center for Quantum Science and Engineering, University of California, Los Angeles, California 90095, United States
    Challenge Institute for Quantum Computation, University of California, Los Angeles, California 90095, United States
    More by Guo-Zhu Zhu
  • Claire E. Dickerson
    Claire E. Dickerson
    Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, United States
  • Benjamin L. Augenbraun
    Benjamin L. Augenbraun
    Department of Physics, Harvard University, Cambridge, Massachusetts 02138, United States
    Harvard-MIT Center for Ultracold Atoms, Cambridge, Massachusetts 02138, United States
  • Austin D. Bailey
    Austin D. Bailey
    Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, United States
  • Anastassia N. Alexandrova
    Anastassia N. Alexandrova
    Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, United States
    Center for Quantum Science and Engineering, University of California, Los Angeles, California 90095, United States
  • Wesley C. Campbell
    Wesley C. Campbell
    Department of Physics and Astronomy, University of California, Los Angeles, California 90095, United States
    Center for Quantum Science and Engineering, University of California, Los Angeles, California 90095, United States
    Challenge Institute for Quantum Computation, University of California, Los Angeles, California 90095, United States
  • Justin R. Caram
    Justin R. Caram
    Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, United States
    Center for Quantum Science and Engineering, University of California, Los Angeles, California 90095, United States
  • Eric R. Hudson
    Eric R. Hudson
    Department of Physics and Astronomy, University of California, Los Angeles, California 90095, United States
    Center for Quantum Science and Engineering, University of California, Los Angeles, California 90095, United States
    Challenge Institute for Quantum Computation, University of California, Los Angeles, California 90095, United States
  • , and 
  • John M. Doyle
    John M. Doyle
    Department of Physics, Harvard University, Cambridge, Massachusetts 02138, United States
    Harvard-MIT Center for Ultracold Atoms, Cambridge, Massachusetts 02138, United States
Cite this: J. Phys. Chem. Lett. 2022, 13, 30, 7029–7035
Publication Date (Web):July 28, 2022
https://doi.org/10.1021/acs.jpclett.2c01430
Copyright © 2022 American Chemical Society

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    Abstract

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    Rapid and repeated photon cycling has enabled precision metrology and the development of quantum information systems using atoms and simple molecules. Extending optical cycling to structurally complex molecules would provide new capabilities in these areas, as well as in ultracold chemistry. Increased molecular complexity, however, makes realizing closed optical transitions more difficult. Building on already established strong optical cycling of diatomic, linear triatomic, and symmetric top molecules, recent work has pointed the way to cycling of larger molecules, including phenoxides. The paradigm for these systems is an optical cycling center bonded to a molecular ligand. Theory has suggested that cycling may be extended to even larger ligands, like naphthalene, pyrene, and coronene. Herein, we study optical excitation and fluorescent vibrational branching of CaO-, SrO-, and CaO- and find only weak decay to excited vibrational states, indicating a promising path to full quantum control and laser cooling of large arene-based molecules.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.2c01430.

    • Technical details of the experimental setup, data acquisition, and fitting procedure; additional information on estimation of uncertainty and theoretical calculations along with Table S1 with all measured values (PDF)

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    Cited By

    This article is cited by 6 publications.

    1. Guo-Zhu Zhu, Guanming Lao, Claire E. Dickerson, Justin R. Caram, Wesley C. Campbell, Anastassia N. Alexandrova, Eric R. Hudson. Extending the Large Molecule Limit: The Role of Fermi Resonance in Developing a Quantum Functional Group. The Journal of Physical Chemistry Letters 2024, 15 (2) , 590-597. https://doi.org/10.1021/acs.jpclett.3c03177
    2. Hryhory Sinenka, Yurii Bruyakin, Andrei Zaitsevskii, Timur Isaev, Anastasia V. Bochenkova. Zwitterions Functionalized by Optical Cycling Centers: Toward Laser-Coolable Polyatomic Molecular Cations. The Journal of Physical Chemistry Letters 2023, 14 (25) , 5784-5790. https://doi.org/10.1021/acs.jpclett.3c00904
    3. Claire E. Dickerson, Cecilia Chang, Han Guo, Anastassia N. Alexandrova. Fully Saturated Hydrocarbons as Hosts of Optical Cycling Centers. The Journal of Physical Chemistry A 2022, 126 (51) , 9644-9650. https://doi.org/10.1021/acs.jpca.2c06647
    4. Guanming Lao, Guo-Zhu Zhu, Claire E. Dickerson, Benjamin L. Augenbraun, Anastassia N. Alexandrova, Justin R. Caram, Eric R. Hudson, Wesley C. Campbell. Laser Spectroscopy of Aromatic Molecules with Optical Cycling Centers: Strontium(I) Phenoxides. The Journal of Physical Chemistry Letters 2022, 13 (47) , 11029-11035. https://doi.org/10.1021/acs.jpclett.2c03040
    5. Leonid Shirkov, Michał Tomza. Long-range interactions of aromatic molecules with alkali-metal and alkaline-earth-metal atoms. The Journal of Chemical Physics 2023, 158 (9) , 094109. https://doi.org/10.1063/5.0135929
    6. Phelan Yu, Adrian Lopez, William A. Goddard, Nicholas R. Hutzler. Multivalent optical cycling centers: towards control of polyatomics with multi-electron degrees of freedom. Physical Chemistry Chemical Physics 2022, 25 (1) , 154-170. https://doi.org/10.1039/D2CP03545F

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