Establishing a nearly closed cycling transition in a polyatomic molecule

Abstract

We study optical cycling in the polar free radical calcium monohydroxide (CaOH) and establish an experimental path towards scattering $\sim$$10^4$ photons. We report rovibronic branching ratio measurements with precision at the $\sim 10^{-4}$ level and observe weak symmetry-forbidden decays to bending modes with non-zero vibrational angular momentum. Calculations are in excellent agreement with these measurements and predict additional decay pathways. Additionally, we perform high-resolution spectroscopy of the $\tilde{\text{X}}{}^2{\Sigma }^{+}(12^{0}0)$ and $\tilde{\text{X}}{}^2{\Sigma }^{+}(12^{2}0)$ hybrid vibrational states of CaOH. These advances establish a path towards radiative slowing, 3D magneto-optical trapping, and sub-Doppler cooling of CaOH.

References in corpus (13)

• Many-Body Physics with Ultracold Gases
• Probing many-body dynamics on a 51-atom quantum simulator
• Cold molecules: Progress in Quantum Engineering of Chemistry and Quantum Matter
• Precision Measurement of Time-Reversal Symmetry Violation with Laser-Cooled Polyatomic Molecules
• Direct Laser Cooling of a Symmetric Top Molecule
• Laser-Cooled Polyatomic Molecules for Improved Electron Electric Dipole Moment Searches
• 1D Magneto-Optical Trap of Polyatomic Molecules
• Molecular Asymmetry and Optical Cycling: Laser Cooling Asymmetric Top Molecules
• Realizing unconventional quantum magnetism with symmetric top molecules
• Determination of CaOH and CaOCH${}_3$ vibrational branching ratios for direct laser cooling and trapping
• Prospects for laser cooling of polyatomic molecules with increasing complexity
• Franck-Condon tuning of optical cycling centers by organic functionalization
• Observation and laser spectroscopy of ytterbium monomethoxide, YbOCH${}_3$

Cited by in corpus (19)

• Magneto-Optical Trapping and Sub-Doppler Cooling of a Polyatomic Molecule
• Polyatomic Molecules as Quantum Sensors for Fundamental Physics
• Functionalizing Aromatic Compounds with Optical Cycling Centers
• Accurate prediction and measurement of vibronic branching ratios for laser cooling linear polyatomic molecules
• Optical Trapping of a Polyatomic Molecule in an $\ell$-Type Parity Doublet State
• Characterizing the Fundamental Bending Vibration of a Linear Polyatomic Molecule for Symmetry Violation Searches
• Molecular Laser-Cooling in a Dynamically Tunable Repulsive Optical Trap
• Vibronic branching ratios for nearly-closed rapid photon cycling of SrOH
• Magneto-optical trapping of a heavy polyatomic molecule for precision measurement
• Large molasses-like cooling forces for molecules using polychromatic optical fields: A theoretical description
• Bichromatic Imaging of Single Molecules in an Optical Tweezer Array
• Blackbody thermalization and vibrational lifetimes of trapped polyatomic molecules
• Intensity-borrowing mechanisms pertinent to laser cooling of linear polyatomic molecules
• ExoMol line lists -- XLVII. Rovibronic molecular line list of the calcium monohydroxide radical (CaOH)
• Multivalent optical cycling centers in polyatomic molecules
• Theoretical rovibronic spectroscopy of the calcium monohydroxide radical (CaOH)
• Vibrational Branching Ratios for Laser-Cooling of Nonlinear Strontium-Containing Molecules
• Low-$J$ transitions in ${\tilde{A}}^2\Pi (0,0,0)-{\tilde{X}}^2{\Sigma }^{+}(0,0,0)$ band of buffer-gas-cooled CaOH
• Cold CH radicals for laser cooling and trapping