Abstract Doppler and Sisyphus cooling of 174YbOH are achieved and studied. This polyatomic molecule has high sensitivity to physics beyond the Standard Model and represents a new class of species for future high-precision probes of new T-violating physics. The transverse temperature of the YbOH beam is reduced by nearly two orders of magnitude to < 600 μK and the phase-space density is increased by a factor of > 6 via Sisyphus cooling. We develop a full numerical model of the laser cooling of YbOH and find excellent agreement with the data. We project that laser cooling and magneto-optical trapping of long-lived samples of YbOH molecules are within reach and these will allow a high sensitivity probe of the electric dipole moment of the electron. The approach demonstrated here is easily generalized to other isotopologues of YbOH that have enhanced sensitivity to other symmetry-violating electromagnetic moments.
Abstract Doppler and Sisyphus cooling of 174YbOH are achieved and studied. This polyatomic molecule has high sensitivity to physics beyond the Standard Model and represents a new class of species for future high-precision probes of new T-violating physics. The transverse temperature of the YbOH beam is reduced by nearly two orders of magnitude to < 600 μK and the phase-space density is increased by a factor of > 6 via Sisyphus cooling. We develop a full numerical model of the laser cooling of YbOH and find excellent agreement with the data. We project that laser cooling and magneto-optical trapping of long-lived samples of YbOH molecules are within reach and these will allow a high sensitivity probe of the electric dipole moment of the electron. The approach demonstrated here is easily generalized to other isotopologues of YbOH that have enhanced sensitivity to other symmetry-violating electromagnetic moments.
Ultracold polyatomic molecules containing heavy nuclei, such as SrOH and YbOH, are sensitive to T- symmetry violating and P-symmetry violating physics beyond the Standard Model through the electron’s electric dipole moment. Furthermore, SrOH is sensitive to ultralight Dark Matter through measuring time variations of fundamental constants. However, in order to make full use of these molecules, they need to be cooled to ultracold temperatures and held in optical traps. We have realized a magneto-optical trap (MOT) of SrOH and used this as the essential element to achieve optical trap- ping in the microKelvin temperature regime. We observed MOT lifetimes approaching 200 ms with temperatures ∼ 1 mK and observed damped oscillations in the MOT. We further cooled the SrOH molecules to ∼ 40 μ K using Λ-enhanced gray molasses, and compressed the cloud to about 100 μm size using the conveyor belt MOT technique. Using this ultracold dense cloud of SrOH, we loaded an optical dipole trap (ODT), with a molecular lifetime of 1.2(1) seconds. In separate experiments with YbOH, which is heavier than SrOH, we demonstrated a novel deceleration method (Zeeman- Sisyphus deceleration) that can slow YbOH to under 20 m/s with only a few photons scattered utilizing high magnetic fields up to 2.5 T. By driving spin-flip transitions at the maxima and minima of the magnetic fields, slowing was achieved, which is a critical first step toward loading of a MOT for this species. We addressed the challenges associated with driving spin-flip transitions in molecules that have molecular perturbations among the electronic excited states and developed an understanding of the physics of such systems that is applicable to a wide range of molecules.
Molecules controlled at the single-quantum-state level offer wide-ranging applications spanning many of the frontiers of modern physics. Within the past decade, simple diatomic molecules have been brought under full quantum control both via assembly from pre-cooled atoms and by direct laser cooling. Polyatomic molecules\footnote{Molecules that contain three or more atoms.} have attracted focus as novel quantum resources providing distinct advantages (and challenges) compared to both atoms and diatomic molecules. For example, nearly all polyatomic molecules have long-lived states that can be fully polarized at low applied electric fields. These and other features generic to polyatomic molecules can be applied to quantum simulation, quantum chemistry, and tests of fundamental physics beyond the Standard Model. While these structural features of polyatomic molecules are highly promising for applications, they complicate the process of bringing molecules under full quantum control. In this thesis, we describe a series of experimental and theoretical advances toward the production of ultracold complex polyatomic molecules. We demonstrate the first laser cooling of the polyatomic radical ytterbium monohydroxide (YbOH), a promising candidate to search for particles and interactions beyond the Standard Model of particle physics. We develop a novel deceleration technique (``Zeeman-Sisyphus deceleration") capable of slowing molecular beams to trappable velocities while scattering fewer than 10 optical photons. This deceleration method is demonstrated using CaOH molecules, a lighter analog of YbOH. In order to determine a viable pathway to full three-dimensional cooling and trapping of YbOH, we develop a spectroscopic technique to measure vibrational branching ratios with relative intensity sensitivity around 1 part in 105, approximately two orders of magnitude beyond the previous state of the art. We also perform the first spectroscopic observations and characterizations of the related molecule ytterbium monomethoxide, YbOCH3, a promising species to probe beyond-the-Standard-Model physics. In addition, we show theoretically that an entire class of asymmetric top molecules can be laser cooled using essentially the same techniques used for much simpler species. Measurements of the vibrational branching ratios for a few prototypical asymmetric to molecules (CaSH and CaNH2) are presented to confirm these predictions.
That the universe contains a disproportionate amount of matter compared to antimatter cannot be explained by the standard model of particle physics; this is because it contains too little charge-parity (CP) symmetry violation. Low energy experiments with atoms and molecules can be extremely sensitive probes for many types of new physics. An active area of research is the search for electric dipole moments (EDMs) of fundamental particles or nuclei; a nonzero EDM would be evidence for new sources of CP violation. Ytterbium monofluoride (YbF) molecules in a supersonic beam are currently being used to measure the electric dipole moment of the electron (eEDM). This thesis presents progress towards a new, more sensitive eEDM experiment that will use a slower YbF beam source and transverse laser cooling to collimate this beam. We have demonstrated laser cooling of YbF in one transverse dimension to less than 100 μK, which is below the Doppler cooling limit. This was done using a Sisyphus-type mechanism called magnetic field induced laser cooling. We also demonstrate polarisation gradient cooling of YbF. After rebuilding and upgrading much of the experiment, we cooled the beam in both transverse dimensions. By scanning experimental parameters, we have gained insight into the cooling mechanisms, and the optimum conditions for laser cooling. We placed an upper limit of a few mK on the transverse temperature of the molecules, although I argue that the true temperature must be very much lower. The number of ultracold molecules was carefully quantified and found to be 2.0(4)x10^5 per pulse. These experiments lay the foundations for an eEDM sensitivity improvement by up to a factor of 100.
Cold molecules are attractive for a wide range of scientific applications, including quantum computation, the study of chemical reactions, and tests of fundamental physics. Laser cooling has proved to be an invaluable technique in the cooling of atoms. This technique was once thought to be infeasible for molecules, because it is difficult to find a closed cycling transition due to their vibrational structure. Recently, laser cooling of several diatomic species has been demonstrated. These molecules possess electronic transitions with highly diagonal Franck-Condon matrices, which make it possible to drive a quasi-closed cycling transition. Ytterbium fluoride (YbF) molecules are amenable to laser cooling and are especially interesting because they are used to measure the electron's electric dipole moment (eEDM). Measurements of the eEDM test the prediction of theories that extend the Standard Model of particle physics. The sensitivity of an eEDM experiment could be greatly increased by using ultracold molecules produced by direct laser cooling. This thesis presents work done towards producing a laser-cooled beam of YbF for an eEDM experiment. This work includes the construction of the cooling experiment, a novel method for efficiently combining laser beams of very similar frequencies, results of spectroscopic measurements to find the required transitions for laser cooling, the results of initial optical cycling experiments, and the first laser cooling results of YbF. Using a one-dimensional optical molasses, a beam of molecules is Doppler cooled in one transverse direction to a temperature of approximately 70 mK. Preliminary evidence of cooling to lower temperatures through a Sisyphus mechanism is also presented. Finally, paths towards improving the laser cooling are suggested. The work opens the door to improved measurements of the eEDM using ultracold YbF molecules.
Polyatomic molecules are promising platforms for conducting precision measurements to probe the Standard Model, owing to their unique degrees of freedom including vibrations and rotations. In particular, ultracold SrOH has sensitivity to the variation of the proton to electron mass ratio μ and subsequently to scalar ultralight dark matter (UDM) fields. We discuss the laser slowing, sub-Doppler cooling, and trapping of SrOH and present an order of magnitude improved trap number through the use of transverse cooling of the molecular beam resulting in ∼104 optically trapped molecules. This would allow for a two order of magnitude improvement on the current best sensitivities to UDM over four decades of mass. Probing μ-variation is not only important for UDM studies, but has more general implications for a variety of fundamental physics searches. Additionally, this increase in trapped molecule number makes SrOH a viable candidate in the search for the electron's electric dipole moment (eEDM) for fundamental symmetry violations. These techniques are broadly applicable, and make cooling and trapping heavier and more complex molecules with greater sensitivity to fundamental physics more viable.
Abstract We use narrow-band laser excitation of Yb atoms to substantially enhance the brightness of a cold beam of YbOH, a polyatomic molecule with high sensitivity to physics beyond the standard model (BSM). By exciting atomic Yb to the metastable 3P1 state in a cryogenic environment, we significantly increase the chemical reaction cross-section for collisions of Yb with reactants. We characterize the dependence of the enhancement on the properties of the laser light, and study the final state distribution of the YbOH products. The resulting bright, cold YbOH beam can be used to increase the statistical sensitivity in searches for new physics utilizing YbOH, such as electron electric dipole moment and nuclear magnetic quadrupole moment experiments. We also perform new quantum chemical calculations that confirm the enhanced reactivity observed in our experiment and compare reaction pathways of Yb(3P) with the reactants H2O and H2O2. More generally, our work presents a broad approach for improving experiments that use cryogenic molecular beams for laser cooling and precision measurement searches of BSM physics.