Optical cycling in polyatomic molecules with complex hyperfine structure

Abstract

We have developed and demonstrated a scheme to achieve rotationally-closed photon cycling in polyatomic molecules with complex hyperfine structure and sensitivity to hadronic symmetry violation, specifically ${}^{171}$YbOH and ${}^{173}$YbOH. We calculate rotational branching ratios for spontaneous decay and identify repumping schemes which use electro-optical modulators (EOMs) to address the hyperfine structure. We demonstrate our scheme by cycling photons in a molecular beam and verify that we have achieved rotationally-closed cycling by measuring optical pumping into unaddressed vibrational states. Our work makes progress along the path toward utilizing photon cycling for state preparation, readout, and laser cooling in precision measurements of polyatomic molecules with complex hyperfine structure.

10 pages, 7 figures

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• Laser cooled 137BaF molecules for measuring nuclear-spin-dependent parity violation
• Molecular laser cooling using serrodynes: Implementation, characterization and prospects
• High-resolution spectroscopy of barium monofluoride: Odd isotopologues, hyperfine structure and isotope shifts
• Magnetic hyperfine structure constants of ${}^{137}$BaF in the ${}^2{\Pi }_{1/2}$ and ${}^2{\Pi }_{3/2}$ excited states
• Molecular Quantum Control Algorithm Design by Reinforcement Learning