Optical cycling on thorium monoxide for an improved test of fundamental symmetries
Optical cycling refers to repeated excitation and spontaneous emission on an electronic transition in an atom or molecule. Optical cycling in molecules can enable a wide range of quantum control and readout techniques, but unfortunately it has only been demonstrated on a small class of alkalilike or alkaline-earth-like molecules. Thorium monoxide (ThO), a molecule used in one of the most precise permanent electron electric dipole moment (eEDM) searches (ACME†) [Andreev et al., Nature (London) 562, 355 (2018)], does not fall into this category. In this work, we demonstrate the first optical cycling on this nonconventional class over a range of experimental parameter space, including laser intensity, polarization switching rate, and interaction time. We show that both the 𝐽 = 1 and 𝐽 = 2 rotational levels of ThO molecule are capable of cycling an average of 11(2) photons with a single laser, at scattering rates of 1.9(6) × 10 6 and 2.3(7) × 10 6 s −1 , respectively, before population is lost to other vibronic levels. We outline a scheme to apply this demonstrated optical cycling in an ACME-style eEDM measurement, improving the detection efficiency by over fourfold compared to noncycling fluorescence detection. This would lead to over a twofold enhancement in the statistical sensitivity of the eEDM search. This optical-cycling scheme can be further extended to scatter ∼100 photons, which would enable a wider range of quantum control and sensing using ThO molecules.