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arXiv:2201.04750 · Physical Review A

Doppler cooling of buffer-gas-cooled barium monofluoride molecules

Yuhe Zhang, Zixuan Zeng, Qian Liang, Wenhao Bu, Bo Yan

Published Mar 14, 2022• 28 citations
arXivHTMLPDF

Abstract

We demonstrate one-dimensional Doppler cooling of a beam of buffer-gas-cooled barium monofluoride (BaF) molecules. This represents a key step towards further cooling and trapping of BaF molecules. The dependencies of the cooling efficiency on the detuning of laser, the intensity of the laser, and the bias field are systematically studied. Furthermore, the numerical simulations with a Monte Carlo method agree quite well with our data.

DOI
10.1103/physreva.105.033307

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We demonstrate one-dimensional Doppler cooling of a beam of buffer-gas-cooled barium monofluoride (BaF) molecules. This represents a key step towards further cooling and trapping of BaF molecules. The dependencies of the cooling efficiency on the detuning of laser, the intensity of the laser, and the bias field are systematically studied. Furthermore, the numerical simulations with a Monte Carlo method agree quite well with our data.
We reported a detailed experimental study of the cold collision of barium monofluoride (BaF) with buffer gas and the high-resolution spectroscopy relevant with direct laser cooling. BaF molecules are efficiently produced with laser ablation and buffer-gas cooled in a cryogenic apparatus. The laser cooling relevant transition $|X\phantom{\rule{0.16em}{0ex}}^{2}\mathrm{\ensuremath{\Sigma}},v=0,N=1\ensuremath{\rangle}$ to $|A\phantom{\rule{0.16em}{0ex}}^{2}\mathrm{\ensuremath{\Pi}},{v}^{\ensuremath{'}}=0,{J}^{\ensuremath{'}}=1/2\ensuremath{\rangle}$ is identified. The collision cross section with buffer gas is measured to be $1.4(7)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}\phantom{\rule{4.pt}{0ex}}{\text{cm}}^{\ensuremath{-}2}$, which is very suitable for buffer-gas cooling. Both rotational and vibrational temperatures are effectively cooled, and a large amount of molecules are quenched into the desired states. Our study provides an important benchmark for further laser cooling of the BaF molecule.
We report an experimental investigation on the Doppler-free saturated absorption spectroscopy of buffer-gas-cooled Barium monofluoride (BaF) molecules in a 4 K cryogenic cell. The obtained spectra with a resolution of 19 MHz, much smaller than previously observed in absorption spectroscopy, clearly resolve the hyperfine transitions. Moreover, we use these high-resolution spectra to fit the hyperfine splittings of excited A ( v = 0) state and find the hyperfine splitting of the laser-cooling-relevant A 2 Π 1/2 ( v = 0, J = 1/2,+) state is about 18 MHz, much higher than the previous theoretically predicted value. This provides important missing information for laser cooling of BaF molecules.
We demonstrate buffer-gas cooling, high-resolution spectroscopy, and cycling fluorescence of cold barium monofluoride (BaF) molecules. Our source produces an intense and internally cold molecular beam containing the different BaF isotopologues with a mean forward velocity of 190m/s190\phantom{\rule{0.16em}{0ex}}\mathrm{m}/\mathrm{s}190m/s. For a well-collimated beam of 138Ba19F^{138}\mathrm{Ba}\phantom{\rule{0.16em}{0ex}}^{19}\mathrm{F}138Ba19F we observe a flux of >1010>{10}^{10}>1010 molecules ${\mathrm{sr}}^{\ensuremath{-}1}\phantom{\rule{0.16em}{0ex}}{\mathrm{pulse}}^{\ensuremath{-}1}$ in the $X{\phantom{\rule{0.16em}{0ex}}}^{2}\mathrm{\ensuremath{\Sigma}}$, N=1N=1N=1 state in our downstream detection region. Studying the absorption line strength of the intermediate ${A}^{\ensuremath{'}}\mathrm{\ensuremath{\Delta}}$ state we infer a lifetime of ${\ensuremath{\tau}}_{\mathrm{\ensuremath{\Delta}}}=790\ifmmode\pm\else\textpm\fi{}346\phantom{\rule{0.16em}{0ex}}\mathrm{ns}$, significantly longer than previously estimated. Finally, highly diagonal Franck-Condon factors and magnetic remixing of dark states allow us to realize a quasicycling transition in 138Ba19F^{138}\mathrm{Ba}\phantom{\rule{0.16em}{0ex}}^{19}\mathrm{F}138Ba19F that is suitable for future laser cooling of this heavy diatomic molecule.
A full density-matrix simulation is performed for optical deflection of a barium monofluoride (138Ba19F^{138}\mathrm{Ba}^{19}\mathrm{F}138Ba19F) beam using the bichromatic force, which employs pairs of counterpropagating laser beams that are offset in frequency. We show that the force is sufficient to separate BaF molecules from the other products generated in a helium-buffer-gas-cooled ablation source. For our simulations, the density-matrix and force equations are numerically integrated during the entire time that the molecules pass through a laser beam to ensure that effects of the evolution of the Doppler shift and of the optical intensity and phase at the position of the molecule are properly included. The results of this paper are compared to those of a deflection scheme [A. Marsman, D. Heinrich, M. Horbatsch, and E. A. Hessels, Phys. Rev. A 107, 032811 (2023)] which uses $\ensuremath{\pi}$ pulses to drive frequency-resolved transitions. This paper is part of an effort by the EDM3{\mathrm{EDM}}^{3}EDM3 collaboration to measure the electric dipole moment of the electron using BaF molecules embedded in a cryogenic argon solid. Separation of BaF molecules will aid in producing a sufficiently pure solid.
Laser cooling of molecules is a powerful technique for producing cold, slow beams for precision measurements and quantum control, yet its implementation remains challenging due to molecular complexity. Here, we combine a cryogenic buffer gas beam, an electrostatic hexapole lens, and 2D transverse Doppler laser cooling to produce a bright beam of barium monofluoride (138Ba19F) molecules. We study both numerically and experimentally the laser cooling effect as a function of laser detuning, laser power, laser alignment, and interaction time. We find a scattering rate of 6.1(1.4) × 105 s−1 on the laser cooling transition (14% of the expected maximum) and identify suboptimal dark Zeeman state remixing, suboptimal laser sideband powers and detunings, and a lack of vibrational repump laser intensity as possible causes of such a low rate. Using 3 tuneable lasers with appropriate sidebands and detuning, each molecule scatters approximately 400 photons during 2D laser cooling, limited by the interaction time and scattering rate. Leaks to dark states are less than 10%. Finally, we use the experimental results to benchmark the trajectory simulations to predict the achievable flux 3.5 m downstream for a planned eEDM experiment. Laser cooling is a powerful technique that enables precision measurements and quantum control, yet its implementation in molecules remains challenging due to their complex structures. Here, the authors apply 2D transverse laser cooling to a focused beam of cold barium monofluoride (138Ba19F) molecules to significantly increase beam brightness.
We demonstrate laser cooling of barium monofluoride ( BaF 138 ) molecules. We use serrodynes to synthesize time-sequenced optical spectra that can be precisely tailored to the hyperfine structure of this heaviest nonradioactive alkaline earth monofluoride. By optimizing these optical spectra, we realize strong Sisyphus cooling forces that efficiently collimate a molecular beam. Our technique is an important step toward using intense beams of barium monofluoride for precision measurement applications, and will be useful for cooling other molecular species with complex level structure. Published by the American Physical Society 2024