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Physical Review A

Spin-orbit interaction and large inelastic rates in bismuth-helium collisions

Stephen Maxwell, Matthew T. Hummon, Y. H. Wang, Alexei A. Buchachenko, Roman V. Krems, John M. Doyle

Published Oct 17, 2008• 14 citations
Publisher

Abstract

We present a combined experimental and theoretical study of cold collisions between bismuth and helium atoms in strong magnetic fields and demonstrate that the spin-orbit interaction coupling between different nonrelativistic states of Bi leads to rapid Zeeman relaxation. The Zeeman relaxation of Bi in the ground electronic state is found to be very efficient due to the admixture of electronic excited states which show an interaction anisotropy due to their nonzero electronic orbital angular momentum. Our results indicate that dense ensembles of heavy relativistic atoms will generally be unstable in magnetic traps due to significant spin relaxation induced by spin-orbit interactions.

DOI
10.1103/physreva.78.042706

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The Journal of Chemical Physics•Sep 8, 2005•15 citations
We present a combined experimental and theoretical study of cold collisions between bismuth and helium atoms in strong magnetic fields and demonstrate that the spin-orbit interaction coupling between different nonrelativistic states of Bi leads to rapid Zeeman relaxation. The Zeeman relaxation of Bi in the ground electronic state is found to be very efficient due to the admixture of electronic excited states which show an interaction anisotropy due to their nonzero electronic orbital angular momentum. Our results indicate that dense ensembles of heavy relativistic atoms will generally be unstable in magnetic traps due to significant spin relaxation induced by spin-orbit interactions.
We present a combined experimental and theoretical study of cold collisions between bismuth and helium atoms in strong magnetic fields and demonstrate that the spin-orbit interaction coupling between different nonrelativistic states of Bi leads to rapid Zeeman relaxation. The Zeeman relaxation of Bi in the ground electronic state is found to be very efficient due to the admixture of electronic excited states which show an interaction anisotropy due to their nonzero electronic orbital angular momentum. Our results indicate that dense ensembles of heavy relativistic atoms will generally be unstable in magnetic traps due to significant spin relaxation induced by spin-orbit interactions.
We investigate Zeeman relaxation in cold Sb(${}^{4}{S}_{3/2}^{\ensuremath{\circ}}$)--He collisions in a magnetic field. Ensembles of >>>1013{10}^{13}1013 laser-ablated Sb atoms are cooled in cryogenic 4{}^{4}4He buffer gas to 800 mK and inelastic collisions are observed to equilibrate the mJ{m}_{J}mJ​-state distribution to the translational temperature. The ratio $\ensuremath{\gamma}$ of momentum transfer to inelastic collision rates is measured to be $\ensuremath{\leqslant}9.1\ifmmode\times\else\texttimes\fi{}{10}^{2}$. We also perform quantum scattering calculations of Sb--4{}^{4}4He collisions, based on ab initio interaction potentials, that demonstrate significant anisotropy of the ground state induced by the spin-orbit interaction. Agreement is obtained between theory and experiment with a $\ensuremath{\approx}101010%$ increase in the ab initio potential depth. This work suggests that buffer-gas-cooled pnictogen atoms lighter than Sb can be loaded into a magnetic trap.
We present a combined experimental and theoretical study of angular momentum depolarization in cold collisions of 2P^{2}P2P atoms in the presence of an external magnetic field. We show that collision-induced Zeeman relaxation of Ga(2P1/2)\text{Ga}({^{2}P}_{1/2})Ga(2P1/2​) and In(2P1/2)\text{In}({^{2}P}_{1/2})In(2P1/2​) atoms in cold 4He^{4}\text{H}\text{e}4He gas is dramatically suppressed compared to atoms in 2P3/2{^{2}P}_{3/2}2P3/2​ states. Using rigorous quantum-scattering calculations based on ab initio interaction potentials, we demonstrate that Zeeman transitions in collisions of atoms in 2P1/2{^{2}P}_{1/2}2P1/2​ electronic states occur via couplings to the 2P3/2{^{2}P}_{3/2}2P3/2​ state induced by the anisotropy of the interaction potential. Our results suggest the feasibility of sympathetic cooling and magnetic trapping of 2P1/2{^{2}P}_{1/2}2P1/2​-state atoms, such as halogens, thereby opening up exciting areas of research in precision spectroscopy and cold-controlled chemistry.
Inelastic collision processes driven by anistropic interactions are investigated below 1 K. Three distinct experiments are presented. First, for the atomic species antimony (Sb), rapid relaxation is observed in collisions with \\(^4He\\). We identify the relatively large spin-orbit coupling as the primary mechanism which distorts the electrostatic potential to introduce significant anisotropy to the ground \\(^4S_{3/2}\\) state. The collisions are too rapid for the experiment to fix a specific value, but an upper bound is determined, with the elastic-to-inelastic collision ratio \\(\\gamma \\leq 9.1 x 10^2\\). In the second experiment, inelastic \\(\\mathcal{m}_J\\)-changing and \\(J\\)-changing transition rates of aluminum (Al) are measured for collisions with \\(^3He\\). The experiment employs a clean method using a single pump/probe laser to measure the steady-state magnetic sublevel population resulting from the competition of optical pumping and inelastic collisions. The collision ratio \\(\\gamma\\) is measured for both \\(\\mathcal{m}_J\\)- and \\(J\\)-changing processes as a function of magnetic field and found to be in agreement with the theoretically calculated dependence, giving support to the theory of suppressed Zeeman relaxation in spherical \\(^2P_{1/2}\\) states [1]. In the third experiment, very rapid atom-atom relaxation is observed for the trapped lanthanide rare-earth atoms erbium (Er) and thulium (Tm). Both are nominally nonspherical \\((L \\neq 0)\\) atoms that were previously observed to have strongly suppressed electronic interaction anisotropy in collisions with helium \\((\\gamma > 10^4-10^5, [2,3])\\). No suppression is observed in collisions between these atoms \\((\\gamma \\lesssim 10)\\), which likely implies that evaporative cooling them in a magnetic trap will be impossible. Taken together, these studies reveal more of the role of electrostatic anisotropy in cold atomic collisions.
Current research in magnetic trapping of the metal atoms is commented upon from the viewpoint of the theory of interatomic interactions and collision dynamics at sub-kelvin temperatures. Atom–atom interactions that lead to collision-induced transitions between different Zeeman states of complex atoms are discussed using the concept of interaction anisotropy. Theoretical results for Zeeman relaxation dynamics for lanthanides, transition and heavy main group metals are reviewed and compared with recent experimental findings. Possible directions of future research are outlined.
Based on measurements of the Zeeman relaxation in a cold gas of (3)He [C. I. Hancox, S. C. Doret, M. I. Hummon, L. Luo, and J. M. Doyle, Nature (London) 431, 281 (2004)], we show that the electronic interaction anisotropy between rare-earth atoms with nonzero electronic orbital angular momenta and helium is extremely small. The interaction of the rare-earth atoms with He gives rise to several adiabatic potentials with different electronic symmetries. It is demonstrated that the energy splitting between these potentials does not exceed 0.09 cm(-1) at interatomic distances larger than the turning point for collisions at 0.8 K, including the region of the van der Waals interaction minima.