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Molecular Physics

Inelastic collisions of CaH with He at cryogenic temperatures

Vijay Singh, Kyle S. Hardman, Mei-Ju Lu, Aja Ellis, Muir J. Morrison, Jonathan D. Weinstein

Published Jun 13, 2013• 9 citations
Publisher

Abstract

Using helium buffer gas cooling, we have prepared dense samples of ground-state molecular calcium monohydride (CaH X 2Σ) at cryogenic temperatures. We have used optical pumping to polarise the spin state of the CaH molecules and we have measured the inelastic collisions of molecular CaH with atomic helium at temperatures from 2 to 7 K. The measured CaH electronic spin depolarisation rate coefficient increases rapidly with increasing temperature, increasing from 2 × 10−13 cm3 s−1 to over 10−11 cm3 s−1. The strong dependence of rate coefficient on temperature is attributed to the CaH population in the first excited rotational state.

DOI
10.1080/00268976.2013.772668

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Using helium buffer gas cooling, we have prepared dense samples of ground-state molecular calcium monohydride (CaH X 2Σ) at cryogenic temperatures. We have used optical pumping to polarise the spin state of the CaH molecules and we have measured the inelastic collisions of molecular CaH with atomic helium at temperatures from 2 to 7 K. The measured CaH electronic spin depolarisation rate coefficient increases rapidly with increasing temperature, increasing from 2 × 10−13 cm3 s−1 to over 10−11 cm3 s−1. The strong dependence of rate coefficient on temperature is attributed to the CaH population in the first excited rotational state.
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.
An experiment is described in which 108 CaH molecules have been confined in a magnetic trap at a temperature of 400 mK. The elastic scattering cross section of CaH on 3He was measured to be σelequals(1.5±0.6)×10-14cm2. A lower bound of Γrotational⩾10-15cm3s-1 was placed on the rotational elastic collision rate coefficient, and an upper bound of Γν<10-15 cm3s-1 was placed on the vibrational relaxation rate coefficient. The rate coefficient for spin changing collisions was measured to be, within an order magnitude, Γ Zequals10-17 cm3 s-1.
In a recent experiment [Weinstein et al., Nature 395, 148 (1998)] we magnetically trapped 108 ground-state calcium monohydride molecules, CaH(X 2Σ,v″=0, J″=0). The molecules were prepared by laser ablation of a solid sample of CaH2 and loaded via thermalization with a cold (<1 K) He3 buffer gas. The magnetic trap was formed by superconducting coils arranged in the anti-Helmholtz configuration. The detection was done by laser fluorescence spectroscopy excited at 635 nm (in the B 2Σ,v′=0−X 2Σ,v″=0 band) and detected at 692 nm (within the B,v′=0−X,v″=1 band). Both a photomultiplier tube and a CCD camera were used. Due to the thermalization of molecular rotation, only a transition from the lowest rotational state could be detected at zero field, N′=1, J′=3/2←N″=0, J″=1/2. In the magnetic field this rotational transition splits into two features, one shifted towards lower and one towards higher frequencies. The measured shifts are linear in field strength and indicate a small difference (0.02 μB) in the magnetic moments between the ground and excited states. Here we present a theoretical analysis of the observed magnetic shifts. These are identified as arising from a rotational perturbation of the B 2Σ,v′=0 state by a close-lying A 2Π,v′=1 state that lends the B state some of its A character. We find that the Hamiltonian can be well approximated by a 3×3 matrix built out of elements that connect states from within the Σ-doublet and the Π3/22 manifolds. The interaction parameter describing the Σ−Π coupling in the Zeeman Hamiltonian is determined from the observed shifts and the field-free molecular parameters of CaH given by Berg and Klyning [Phys. Scr. 10, 331 (1974)] and by Martin [J. Mol. Spectrosc 108, 66 (1984)].
We present cross sections for rotational, vibrational, and fine-structure transitions in He–CaH(2Σ) collisions at cold and ultracold temperatures calculated using the ab initio potential energy surface reported in the preceding paper. Rotational quenching is fast, vibrational quenching is slow. The spin-rotational interaction, although small and having no influence at temperatures above 10 K, changes significantly the rate coefficients for rotational quenching at lower temperatures. The theoretical rotational, vibrational, and elastic cross sections are compared with the results of a buffer gas cooling experiment carried out at a temperature of about 0.4 K. The theoretical predictions for the vibrational and elastic cross sections are larger than the measured values. The sensitivity to the potential energy surface is explored. A modified surface diminishes but does not remove the differences between theory and experiment.
Collision cross sections between oxygen molecules and helium atoms are computed at translational energies between 0.1 K and 10.0 K, motivated by the recently demonstrated cooling of molecules by a helium buffer gas. Detailed calculations based on a rigid-rotor model demonstrate the differences among various isotopic combinations of oxygen atoms and also serve to illustrate resonant features unique to cold molecules. Comparisons of elastic versus spin-changing inelastic collision rates suggest that buffer-gas cooling is likely to be a widely applicable tool for producing cold molecular samples.