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arXiv:2002.00056 · Physical Review X

Sub-Doppler Cooling and Compressed Trapping of YO Molecules at μK Temperatures

Shiqian Ding, Yewei Wu, Ian A. Finneran, Justin J. Burau, Jun Ye

Published Jun 3, 2020• 109 citations
arXivHTMLPDF

Abstract

Complex molecular structure demands customized solutions to laser cooling by extending its general set of principles and practices.Compared with other laser-cooled molecules, yttrium monoxide (YO) exhibits a large electron-nucleus interaction, resulting in a dominant hyperfine interaction over the electron spinrotation coupling.The YO ground state is thus comprised of two manifolds of closely spaced states, with one of them possessing a negligible Landé g factor.This unique energy level structure favors dual-frequency dc magneto-optical trapping (MOT) and gray molasses cooling (GMC).We report exceptionally robust cooling of YO at 4 μK over a wide range of laser intensity, detunings (one-and two-photon), and magnetic field.The magnetic insensitivity enables the spatial compression of the molecular cloud by alternating GMC and MOT under the continuous operation of the quadrupole magnetic field.A combination of these techniques produces a laser-cooled molecular sample with the highest phase space density in free space.

DOI
10.1103/physrevx.10.021049

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Complex molecular structure demands customized solutions to laser cooling by extending its general set of principles and practices.Compared with other laser-cooled molecules, yttrium monoxide (YO) exhibits a large electron-nucleus interaction, resulting in a dominant hyperfine interaction over the electron spinrotation coupling.The YO ground state is thus comprised of two manifolds of closely spaced states, with one of them possessing a negligible Landé g factor.This unique energy level structure favors dual-frequency dc magneto-optical trapping (MOT) and gray molasses cooling (GMC).We report exceptionally robust cooling of YO at 4 μK over a wide range of laser intensity, detunings (one-and two-photon), and magnetic field.The magnetic insensitivity enables the spatial compression of the molecular cloud by alternating GMC and MOT under the continuous operation of the quadrupole magnetic field.A combination of these techniques produces a laser-cooled molecular sample with the highest phase space density in free space.
We report laser cooling and trapping of yttrium monoxide molecules in an optical lattice. We show that gray molasses cooling remains exceptionally efficient for yttrium monoxide molecules inside the lattice with a molecule temperature as low as 6.1(6) μK. This approach has produced a trapped sample of 1200 molecules, with a peak spatial density of ∼1.2×10^{10} cm^{-3}, and a peak phase-space density of ∼3.1×10^{-6}. By ramping down the lattice depth, we cool the molecules further to 1.0(2) μK, 20 times colder than previously reported for laser-cooled molecules in a trap.
Direct laser cooling of molecules has reached a phase-space density exceeding 10^{-6} in optical traps but with rather small molecular numbers. To progress toward quantum degeneracy, a mechanism that combines sub-Doppler cooling and magneto-optical trapping would facilitate near unity transfer of ultracold molecules from the magneto-optical trap (MOT) to a conservative optical trap. Using the unique energy level structure of YO molecules, we demonstrate the first blue-detuned MOT for molecules that is optimized for both gray-molasses sub-Doppler cooling and relatively strong trapping forces. This first sub-Doppler molecular MOT provides an increase of phase-space density by 2 orders of magnitude over any previously reported molecular MOT.
Laser cooling and magneto-optical trapping of neutral atoms has been a driving force in physics over the last few decades by providing an efficient method to produce cold and dense samples of cold atoms. Polar molecules which can have strong, long-range dipolar interactions and possess more rich internal structure promise a wide range of new physics and chemistry studies if they can be controlled efficiently. Until recently, the only way to achieve sub-milliKelvin level temperatures in molecules was to associate two precooled atomic species, which while very effective, has a firm bound on the chemical diversity accessible. While laser cooling of molecules relies on fortuitous molecular properties, it will significantly increase the choices of species available for molecular cooling.In this thesis I present the improved optical deceleration of the molecule yttrium monoxide (YO) and the loading of molecules into a 3-D magneto-optical trap (MOT). By making an improved choice of repumping scheme from our groups’ previous work, our photon scattering rate has been increased. By also improving our buffer gas cell source, we produce a much larger flux (2000 times higher) of slowed molecules at 5 m/s to reach the trapping region. I have designed and implemented 3-D MOT field coils operating at 5 MHz, and demonstrated a successful operation of a 3-D MOT. This is the first 3-D laser trapping of an oxide and the first of a molecule with an electronic state intermediate to the main cycling transition states.I have also performed a study of the transition from the ground state to the intermediate electronic state, which has a narrower linewidth of 150 kHz, in contrast to the main cycling transition’s linewidth of 5 MHz. This transition is well suited to second-stage narrow line cooling after loading molecules with the main MOT transition, which will allow direct laser cooling of a molecule to the 10 uK regime.
The electronic energy level structure of yttrium monoxide (YO) provides a long-lived, low-lying 2 Δ state ideal for high-precision molecular spectroscopy, narrowline laser cooling at the single photon-recoil limit, and studying dipolar physics with unprecedented interaction strength. High-resolution laser spectroscopy of ultracold laser-cooled YO molecules is used to study the Stark effect in the A ′ 2 Δ 3 / 2 J = 3 / 2 state. An immediate onset of the linear Stark effect is observed in the presence of weak applied electric fields due to the near-degenerate Λ doublet and the large electric dipole moment. By applying a small electric field the Stark-insensitive state is spectroscopically isolated and the absolute transition frequency to the X 2 Σ + electronic ground state is determined with a fractional frequency uncertainty of 9 × 10 − 12 . This electric field control is necessary to implement a quasi-closed photon-cycling scheme that preserves parity. With this scheme the first narrowline laser cooling of a molecule is demonstrated, reducing the temperature of sub-Doppler cooled YO in two dimensions.
In red-detuned magneto-optical traps (MOTs) of molecules, sub-Doppler heating competes with Doppler cooling, resulting in high temperature and low density. A solution is offered by the blue-detuned MOT where sub- Doppler cooling dominates and the cloud is compressed. Several blue-detuned molecular MOTs have been implemented. A recent implementation relies on a pair of orthogonally polarized components whose frequency separation is smaller than the transition linewidth. We identify the trapping force in these MOTs. At a certain magnetic field, there is a state that is dark to the laser propagating in one direction, but not to the counterpropagating one. This Zeeman-induced dark state (ZIDS) sets up an imbalance in the photon scattering rate, leading to a restoring force. We also study the role of the moving lattices generated by the closely spaced frequency components of the light. We show that there is a velocity-dependent force that drives the molecules toward the speeds of these moving lattices, and that over a relevant range of magnetic fields this combines with the ZIDS force to transport molecules toward the center of the MOT. Here, gray molasses cooling, assisted by nonadiabatic transitions driven by the time-varying polarization of the light field, cools the molecules toward zero velocity. We study these mechanisms for model systems with simple level structures and then extend them to molecules with ground-state hyperfine structure.
We report three-dimensional trapping of an oxide molecule (YO), using a radio-frequency magneto-optical trap (MOT). The total number of molecules trapped is ∼1.5×10^{4}, with a temperature of 4.1(5) mK. This diversifies the frontier of molecules that are laser coolable and paves the way for the second-stage narrow-line cooling in this molecule to the microkelvin regime. Futhermore, the new challenges of creating a 3D MOT of YO resolved here indicate that MOTs of more complex nonlinear molecules should be feasible as well.