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arXiv:2212.07472 · Physical Review Letters

Blue-Detuned Magneto-optical Trap of Molecules

Justin J. Burau, Parul Aggarwal, Kameron Mehling, Jun Ye

Published May 10, 2023• 44 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevlett.130.193401

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We report the realization of a blue-detuned magneto-optical trap (BDM) of BaF molecules. The (1 + 1) type BDM and (1 + 2) type conveyor-belt MOT are explored. While the (1+1) BDM provides only weak trapping force, the conveyor-belt MOT significantly compresses the molecular cloud, achieving a radius of 320(20) μm, a temperature of 240(60) μK, and a peak density of 1.3{\times}10^7 cm^{-3}, representing a significant improvement over the red MOT. Interestingly, the conveyor-belt MOT of BaF exhibits a large capture velocity, and the loading efficiency from red MOT reaches near unity even without gray molasses. We confirm this by directly loading slowed molecules into the conveyor-belt MOT.

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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.
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.
Direct laser cooling and trapping of molecules to temperature below the Doppler limit and density exceeding 108{10}^{8}108 are challenging due to the sub-Doppler heating effects of a molecular magneto-optical trap (MOT). In our previous paper [S. Xu et al., Phys. Rev. Res. 4, L042036 (2022)], we presented a general approach to engineering the sub-Doppler force by tuning the AC Stark shift with the addition of a blue-detuned laser. Here, by employing the Bayesian optimization method to optical Bloch equations, we have identified multiple blue-detuned MOT schemes for the CaF molecule. From the three-dimensional Monte Carlo simulation, we obtained a MOT temperature and density of 14 $\textmu{}\mathrm{K}$ and $4.5\ifmmode\times\else\texttimes\fi{}{10}^{8} {\mathrm{cm}}^{\ensuremath{-}3}$, respectively. Our findings present a potential avenue for directly loading molecular MOTs into conservative traps, which can capitalize on the high density and low temperature of the MOTs.
It has been more than 30 years since the first demonstration of a magneto-optical trap (MOT) using sodium atoms. Since then the MOT has revolutionised the field of atomic physics by facilitating the emergence of a broad range of productive avenues of research using atoms prepared at low temperatures and high densities. This thesis describes the development of a novel kind of magneto-optical trap: the blue-detuned MOT. Unlike in all previous MOTs the light is blue detuned from atomic resonances and drives "type-II" transitions that have dark ground-state sub-levels. A discussion of the position-dependent and velocity-dependent forces experienced by an atom or molecule in a MOT is first used to consolidate recent theoretical work and, in particular, to introduce the concept of a blue-detuned MOT. The design and construction of an experiment that has been built to demonstrate a blue-detuned MOT using \Rb{87} is described. A thorough characterisation of this novel MOT has been performed. At high magnetic field gradients, radiation-pressure-limited densities exceeding 101110^{11}1011~cm−3^{-3}−3 have been reached whilst temperatures are cooled below 30~\si{\micro K} by the efficient and robust sub-Doppler cooling mechanisms. The maximum phase-space density measured is 6×10−66\times10^{-6}6×10−6, which is higher than in most normal atomic MOTs, comparable to the best dark SPOTs, and a million times higher than that reported for red-detuned type-II MOTs. This makes the blue-detuned MOT particularly attractive for molecules where laser cooling and trapping always uses type-II transitions. For the first time, a study of trap loss due to ultra-cold collisions between atoms occurring in the presence of near-resonant blue-detuned light is undertaken. Finally, the experiment is used to demonstrate many new and unreported configurations of MOT for \Rb{87}, showing that a comprehensive understanding of complicated MOTs is now possible, and presenting a clear direction for further research.
A key method to produce trapped and laser-cooled molecules is the magneto-optical trap (MOT), which is conventionally created using light red detuned from an optical transition. In this work, we report a MOT for CaF molecules created using blue-detuned light. The blue-detuned MOT (BDM) achieves temperatures well below the Doppler limit and provides the highest densities and phase-space densities reported to date in CaF MOTs. Our results suggest that BDMs are likely achievable in many relatively light molecules including polyatomic ones, but our measurements suggest that BDMs will be challenging to realize in substantially heavier molecules due to sub-mK trap depths. In addition to record temperatures and densities, we find that the BDM substantially simplifies and enhances the loading of molecules into optical tweezer arrays, which are a promising platform for quantum simulation and quantum information processing. Notably, the BDM reduces molecular number requirements ninefold compared to a conventional red-detuned MOT, while not requiring additional hardware. Our work therefore substantially simplifies preparing large-scale molecular tweezer arrays, which are a novel platform for simulation of quantum many-body dynamics and quantum information processing with molecular qubits.
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 the realization of a blue-detuned magneto-optical trap (BDM) of BaF molecules. The (1 + 1) type BDM and (1 + 2) type conveyor-belt MOT are explored. While the (1+1) BDM provides only weak trapping force, the conveyor-belt MOT significantly compresses the molecular cloud, achieving a radius of 320(20) μm, a temperature of 240(60) μK, and a peak density of 1.3{\times}10^7 cm^{-3}, representing a significant improvement over the red MOT. Interestingly, the conveyor-belt MOT of BaF exhibits a large capture velocity, and the loading efficiency from red MOT reaches near unity even without gray molasses. We confirm this by directly loading slowed molecules into the conveyor-belt MOT.