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arXiv:2004.09570 · New Journal of Physics

Optical cycling, radiative deflection and laser cooling of barium monohydride (138Ba1H)

Rees L. McNally, Ivan Kozyryev, Sebastian Vazquez-Carson, Konrad Wenz, Tianli Wang, Tanya Zelevinsky

Published Jul 8, 2020• 51 citations
arXivHTMLPDF

Abstract

We present the first experimental demonstration of radiation pressure force deflection and direct laser cooling for barium monohydride (BaH) molecules resulting from multiple photon scattering. Despite a small recoil velocity (2.7 mm s −1 ) and a long excited state lifetime (137 ns), we use 1060 nm laser light exciting the X → A electronic transition of BaH to deflect a cryogenic buffer-gas beam and reduce its transverse velocity spread. Multiple experimental methods are employed to characterize the optical cycling dynamics and benchmark theoretical estimates based on rate equation models as well as solutions of the Lindblad master equation for the complete multilevel system. Broader implications for laser cooling and magneto-optical trapping of heavy-metal-containing molecules with narrow transition linewidths are presented. Our results pave the way for producing a new class of ultracold molecules—alkaline earth monohydrides—via direct laser cooling and trapping, opening the door to realizing a new method for delivering ultracold hydrogen atoms (Lane 2015 Phys . Rev . A 92 , 022511).

DOI
10.1088/1367-2630/aba3e9

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Laser cooling and trapping of heavy alkaline-earth element barium have been demonstrated for the first time ever. For any possible cycling transition in barium that could provide strong cooling forces, the excited state has a very large branching probability to metastable states. Additional lasers are thus needed to bring the atoms back in to the cooling cycle. In this work barium atoms were efficiently collected in a magneto-optical trap (MOT) by large optical forces from the strong 6s2 1S0 – 6s6p 1P1 transition. Trapping of barium has been achieved using up to seven lasers simultaneously. The properties of the barium MOT were characterized. The efficiency of capturing an atom from a thermal atomic beam into the MOT is 0.4(1) %. The developed scheme is very efficient for collecting atoms. Loss rate mechanisms from the trap were studied by observing the decay of the trap population. Typical lifetimes of the MOT cloud are on the order of one second and are limited mainly due to insufficient repumping of metastable states. The range of velocities from which barium atoms can be captured into the MOT is about 30 m/s. Different laser transitions were employed for repumping barium atoms from the 6s5d 3D1 and the 6s5d 3D2 states. They lead to similar trap populations and lifetimes. The temperature of the cold atomic barium cloud was determined to about 5 mK. Atomic properties of the 5d2 3F2 state were studied with trapped atoms, in particular it's lifetime was determined as 160(10) s. This work has shown a possible scheme to trap atoms with a leaky cooling cycle. Since atoms with such properties are the majority of the elements in the periodic table, the number of optically trapable elements can be significantly enlarged. Of particular high interest is radium, which is chemical homologue to barium. The interest in radium stems from it's high sensitivity to possible nuclear and electron permanent electric dipole moments (EDM's). An EDM violates parity as well as time reversal and is therefore of fundamental importance. Searches for such EDM's are among the main research goals of the recently commissioned TRImP facility at KVI.

•Jan 1, 2008•4 citations
We present the first experimental demonstration of radiation pressure force deflection and direct laser cooling for barium monohydride (BaH) molecules resulting from multiple photon scattering. Despite a small recoil velocity (2.7 mm s −1 ) and a long excited state lifetime (137 ns), we use 1060 nm laser light exciting the X → A electronic transition of BaH to deflect a cryogenic buffer-gas beam and reduce its transverse velocity spread. Multiple experimental methods are employed to characterize the optical cycling dynamics and benchmark theoretical estimates based on rate equation models as well as solutions of the Lindblad master equation for the complete multilevel system. Broader implications for laser cooling and magneto-optical trapping of heavy-metal-containing molecules with narrow transition linewidths are presented. Our results pave the way for producing a new class of ultracold molecules—alkaline earth monohydrides—via direct laser cooling and trapping, opening the door to realizing a new method for delivering ultracold hydrogen atoms (Lane 2015 Phys . Rev . A 92 , 022511).
Ultracold molecules promise a revolutionary test bed for quantum science with applications ranging from experiments that probe the nature of our universe, to hosting new platforms for quantum computing. Cooling and trapping molecules in the ultracold regime is the first step to unlocking the wide array of proposed applications, and developing these techniques to control molecules is a key but challenging research field. In this thesis, we describe progress towards a new apparatus designed to cool and trap barium monohydride (BaH), a molecule that is amenable to laser cooling and has prospects as a precursor for ultracold atomic hydrogen. The same complexity that makes molecules interesting objects of study creates challenges for optical control. To mitigate some of these challenges, we first cool the molecules using cryogenic techniques and technologies. Our apparatus uses a cryogenic buffer gas to thermalize BaH within a contained cell. The molecules are extracted into a beam with millikelvin transverse temperature, and forward velocities <100 m/s. The BaH beam in this work is the brightest hydride beam to date, with molecule density and kinetic characteristics well suited for laser cooling and trapping.
Abstract We demonstrate optical cycling and laser cooling of a cryogenic buffer-gas beam of calcium monohydride (CaH) molecules. We measure vibrational branching ratios for laser cooling transitions for both excited electronic states A and B. Furthermore, we measure that repeated photon scattering via the A ← X transition is achievable at a rate of ∼ 1.6 × 1 0 6 photons s−1 and demonstrate interaction-time limited scattering of ∼ 200 photons by repumping the largest vibrational decay channel. We also demonstrate a sub-Doppler cooling technique, namely the magnetically assisted Sisyphus effect, and use it to cool the transverse temperature of a molecular beam of CaH. Using a standing wave of light, we lower the transverse temperature from 12.2(1.2) mK to 5.7(1.1) mK. We compare these results to a model that uses optical Bloch equations and Monte Carlo simulations of the molecular beam trajectories. This work establishes a clear pathway for creating a magneto-optical trap (MOT) of CaH molecules. Such a MOT could serve as a starting point for production of ultracold hydrogen gas via dissociation of a trapped CaH cloud.
Barium monohydride (BaH) is an attractive candidate for extending laser cooling and trapping techniques to diatomic hydrides. The apparatus and high-resolution optical spectroscopy presented here demonstrate progress toward this goal. A cryogenic buffer-gas-cooled molecular beam of BaH was constructed and characterized. Pulsed laser ablation into cryogenic helium buffer gas delivers $\ensuremath{\sim}1\ifmmode\times\else\texttimes\fi{}{10}^{10}$ molecules/sr/pulse in the $X^{2}\mathrm{\ensuremath{\Sigma}}^{+}$ (${v}^{\ensuremath{'}\ensuremath{'}}=0,{N}^{\ensuremath{'}\ensuremath{'}}=1$) state of primary interest. More than $1\ifmmode\times\else\texttimes\fi{}{10}^{7}$ of these molecules per pulse enter the downstream science region with forward velocities below 100 m/s and transverse temperature of 0.1 K. This molecular beam enabled high-resolution optical spectra of BaH in quantum states relevant to laser slowing and cooling. The reported measurements include hyperfine structure and magnetic ggg factors in the $X^{2}\mathrm{\ensuremath{\Sigma}}^{+}$, $B^{2}\mathrm{\ensuremath{\Sigma}}^{+}$, and $A^{2}\mathrm{\ensuremath{\Pi}}_{1/2}$ states.
We describe a simple experimental apparatus for laser ablation of barium monohydride (BaH) molecules and the study of their rovibrational spectra relevant to direct laser cooling. BaH is a promising candidate for laser cooling and ultracold fragmentation, both of which are precursors to novel experiments in many-body physics and precision measurement. We present a detailed analysis of the properties of ablation plumes that can improve the understanding of surface ablation and deposition technologies. A range of absorption spectroscopy and collisional thermalization regimes has been studied. We directly measured the Franck-Condon factor of the $B{\phantom{\rule{0.16em}{0ex}}}^{2}{\mathrm{\ensuremath{\Sigma}}}^{+}({v}^{\ensuremath{'}}=0)\ensuremath{\leftarrow}X{\phantom{\rule{0.16em}{0ex}}}^{2}{\mathrm{\ensuremath{\Sigma}}}^{+}({v}^{\ensuremath{'}\ensuremath{'}}=1)$ cycling transition. Prospects for production of a high luminosity cryogenic BaH beam are outlined.
Abstract We demonstrate multiple photon cycling and radiative force deflection on the triatomic free radical strontium monohydroxide (SrOH). Optical cycling is achieved on SrOH in a cryogenic buffer-gas beam by employing the rotationally closed P ( N ″ = 1 ) branch of the vibronic transition X ˜ 2 Σ + ( 000 ) ↔ A ˜ 2 Π 1 / 2 ( 000 ) . A single repumping laser excites the Sr–O stretching vibrational mode, and photon cycling of the molecule deflects the SrOH beam by an angle of 0.2 ° via scattering of ∼100 photons per molecule. This approach can be used for direct laser cooling of SrOH and more complex, isoelectronic species.
Laser cooling and trapping of heavy alkaline-earth element barium have been demonstrated for the first time ever. For any possible cycling transition in barium that could provide strong cooling forces, the excited state has a very large branching probability to metastable states. Additional lasers are thus needed to bring the atoms back in to the cooling cycle. In this work barium atoms were efficiently collected in a magneto-optical trap (MOT) by large optical forces from the strong 6s2 1S0 – 6s6p 1P1 transition. Trapping of barium has been achieved using up to seven lasers simultaneously. The properties of the barium MOT were characterized. The efficiency of capturing an atom from a thermal atomic beam into the MOT is 0.4(1) %. The developed scheme is very efficient for collecting atoms. Loss rate mechanisms from the trap were studied by observing the decay of the trap population. Typical lifetimes of the MOT cloud are on the order of one second and are limited mainly due to insufficient repumping of metastable states. The range of velocities from which barium atoms can be captured into the MOT is about 30 m/s. Different laser transitions were employed for repumping barium atoms from the 6s5d 3D1 and the 6s5d 3D2 states. They lead to similar trap populations and lifetimes. The temperature of the cold atomic barium cloud was determined to about 5 mK. Atomic properties of the 5d2 3F2 state were studied with trapped atoms, in particular it's lifetime was determined as 160(10) s. This work has shown a possible scheme to trap atoms with a leaky cooling cycle. Since atoms with such properties are the majority of the elements in the periodic table, the number of optically trapable elements can be significantly enlarged. Of particular high interest is radium, which is chemical homologue to barium. The interest in radium stems from it's high sensitivity to possible nuclear and electron permanent electric dipole moments (EDM's). An EDM violates parity as well as time reversal and is therefore of fundamental importance. Searches for such EDM's are among the main research goals of the recently commissioned TRImP facility at KVI.