| Autor: |
Zhu GZ; Department of Physics and Astronomy, University of California, Los Angeles, California 90095, United States., Lao G; Department of Physics and Astronomy, University of California, Los Angeles, California 90095, United States., Dickerson CE; Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, United States., Caram JR; 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., Campbell WC; 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., Alexandrova AN; 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., Hudson ER; 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. |
| Abstrakt: |
Polyatomic molecules equipped with optical cycling centers (OCCs), enabling continuous photon scattering during optical excitation, are exciting candidates for advancing quantum information science. However, as these molecules grow in size and complexity, the interplay of complex vibronic couplings on optical cycling becomes a critical but relatively unexplored consideration. Here, we present an extensive exploration of Fermi resonances in large-scale OCC-containing molecules using high-resolution dispersed laser-induced fluorescence and excitation spectroscopy. These resonances manifest as vibrational coupling leading to intensity borrowing by combination bands near optically active harmonic bands, which require additional repumping lasers for effective optical cycling. To mitigate these effects, we explore altering the vibrational energy level spacing through substitutions on the phenyl ring or changes in the OCC itself. While the complete elimination of vibrational coupling in complex molecules remains challenging, our findings highlight significant mitigation possibilities, opening new avenues for optimizing optical cycling in large polyatomic molecules. |
