Alexander Frenett

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 , ], 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.

Design and Applications of a Zeeman-Sisyphus Decelerator |

Zeeman-Sisyphus Deceleration of Polyatomic Molecules |

We present a robust, continuous molecular decelerator that employs high magnetic fields and few optical pumping steps. CaOH molecules are slowed, accumulating at low velocities in a range sufficient for loading both magnetic and magneto-optical traps. During the slowing, the molecules scatter only 7 photons, removing around 8 K of energy. Because large energies can be removed with only a few spontaneous radiative decays, this method can be applied to nearly any paramagnetic atomic or molecular species, opening a general path to trapping of complex molecules.

We present a robust, continuous molecular decelerator that employs high magnetic fields and few optical pumping steps. CaOH molecules are slowed, accumulating at low velocities in a range sufficient for loading both magnetic and magneto-optical traps. During the slowing, the molecules scatter only seven photons, removing around 8 K of energy. Because large energies can be removed with only a few spontaneous radiative decays, this method can in principle be applied to nearly any paramagnetic atomic or molecular species, opening a general path to trapping of complex molecules.

Vibrational overtones in deeply bound molecules are sensitive probes for variation of the proton-to-electron mass ratio μ. In nonpolar molecules, these overtones may be driven as two-photon transitions. Here, we present procedures for experiments with O2+, including state-preparation through photoionization, a two-photon probe, and detection. We calculate transition dipole moments between all X2Пg vibrational levels and those of the A2Пu excited electronic state. Using these dipole moments, we calculate two-photon transition rates and AC-Stark-shift systematics for the overtones. We estimate other systematic effects and statistical precision. Two-photon vibrational transitions in O2+ provide multiple routes to improved searches for μ variation.