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Physical Review Letters

Detection and Lifetime Measurement of Rb-He Quasibound Molecules

F. A. Franz, C. H. Volk

Published Dec 22, 1975• 10 citations
Publisher

Abstract

Quasibound Rb-He Van der Waals molecules have been observed through their influence on the electron spin relaxation of optically pumped ${\mathrm{Rb}}^{85}$ and ${\mathrm{Rb}}^{87}$. The natural lifetime of the complex has been measured to be 6\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}10}$ sec.

DOI
10.1103/physrevlett.35.1704

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Quasibound Rb-He Van der Waals molecules have been observed through their influence on the electron spin relaxation of optically pumped Rb85{\mathrm{Rb}}^{85}Rb85 and Rb87{\mathrm{Rb}}^{87}Rb87. The natural lifetime of the complex has been measured to be 6\ifmmode\times\else\texttimes\fi{}10\ensuremath−10{10}^{\ensuremath{-}10}10\ensuremath−10 sec.
Spin relaxation of optically pumped Rb85{\mathrm{Rb}}^{85}Rb85 and Rb87{\mathrm{Rb}}^{87}Rb87 atoms colliding with light-noble-gas atoms is shown to be strongly influenced by an anomalous relaxation process which we attribute to the formation and destruction of bound and quasibound Van der Waals molecules. The anomalous relaxation rate has been measured and analyzed in Ne, complementing an earlier study in He. Relative rates of formation of complexes in two- and three-body collisions have been determined. The correlation time for the quasimolecular interaction in Rb-Ne has been found to be 6.7 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}10}$ ${p}^{\ensuremath{-}1}$ sec, where ppp is the Ne pressure in Torr. Nuclear-spin-independent cross sections for the relaxation of 〈Sz〉〈{S}_{z}〉〈Sz​〉 in sudden binary collisions of Rb atoms with noble-gas atoms have been measured to be (units of ${10}^{\ensuremath{-}24}$ cm2{\mathrm{cm}}^{2}cm2: $\ensuremath{\sigma}(\mathrm{Rb}\ensuremath{-}\mathrm{He})=3.1$ $\ensuremath{\sigma}(\mathrm{Rb}\ensuremath{-}\mathrm{Ne})=19$ $\ensuremath{\sigma}(\mathrm{Rb}\ensuremath{-}\mathrm{Ar})=630$ $\ensuremath{\sigma}(\mathrm{Rb}\ensuremath{-}{\mathrm{N}}_{2})=83$. Relaxation in sudden binary collisions is shown to follow the theoretically expected nuclear spin dynamics: two relaxation rates in the ratios 8:1 for Rb87{\mathrm{Rb}}^{87}Rb87 and 18:1 for Rb85{\mathrm{Rb}}^{85}Rb85 have been measured. Diffusion coefficients of Rb in the various buffer gases have been measured to be (units of cm2{\mathrm{cm}}^{2}cm2/ sec, at 305\ifmmode^\circ\else\textdegree\fi{}K): ${D}_{0}(\mathrm{Rb}\ensuremath{-}\mathrm{He})=0.42$, ${D}_{0}(\mathrm{Rb}\ensuremath{-}\mathrm{Ne})=0.235$, ${D}_{0}(\mathrm{Rb}\ensuremath{-}\mathrm{Ar})=0.16$, ${D}_{0}(\mathrm{Rb}\ensuremath{-}{\mathrm{N}}_{2})=0.16$. Nuclear-spin-independent cross sections for the relaxation of 〈Jz〉〈{J}_{z}〉〈Jz​〉 in the 52P125^{2}P_{\frac{1}{2}}52P21​​ state of Rb have been measured to be 3.4 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}16}$ cm2{\mathrm{cm}}^{2}cm2 for Rb-He, and 5.9 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}16}$ cm2{\mathrm{cm}}^{2}cm2 for Rb-Ne. Anomalies, disagreements, and puzzles occurring in earlier measurements of ground-state relaxation in Rb are shown to be largely resolved when considered in the light of the new results.
Relaxation experiments performed on optically polarized Rb atoms in a rare gas have been previously reported; their detailed interpretation is given below. It is shown that the relaxation governed by the spin-orbit interaction is strongly affected by the formation of chemically unstable Rb-Kr molecules bound by van der Waals forces. Two processes of molecule formation are analyzed: binary resonant collisions leading to metastable states and three-body collisions producing actual bound states. A relaxation model valid for any disorientation probability per single Rb-Kr interaction is developed. Aside from clear evidence for the existence of alkali-rare-gas molecules, the success of the theoretical interpretation of the relaxation experiments yields the equilibrium constant $\mathcal{K}=1.7\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}22}$ cm3{\mathrm{cm}}^{3}cm3/molecule for the reaction Rb+Kr \ensuremath{\rightleftharpoons} Rb-Kr at 300\ifmmode^\circ\else\textdegree\fi{}K, the average lifetime of a Rb-Kr molecule in the gas phase, $\ensuremath{\tau}=0.65\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$ sec, at a krypton pressure of one Torr, and the average spin-orbit coupling constant in a Rb-Kr molecule, $\overline{\ensuremath{\gamma}}{h}^{\ensuremath{-}1}=0.63$ MHz. It is also shown that the spin-orbit potential is predominantly short-range.
We have investigated the spin-rotation interaction in the van der Waals molecule RbKr using molecular-beam magnetic-resonance techniques. The bound $^{2}\ensuremath{\Sigma}$ molecules were produced in an expansion-cooled molecular beam and the interaction between the electronic spin angular momentum ($\ensuremath{\hbar}\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$) of the rubidium valence electron and the rotational angular momentum ($\ensuremath{\hbar}\stackrel{\ensuremath{\rightarrow}}{\mathrm{N}}$) of the molecule was probed by magnetic resonance. A value for the strength of the interaction and a model of its dependence upon the internuclear separation were obtained. Results of numerical calculations of all bound and quasibound vibrational-rotational states of the RbKr ground-state potential are presented. These wave functions permit a detailed comparison of the results obtained by this technique and those obtained by M. Bouchiat et al. using optical-pumping techniques in a high-temperature gas cell. Excellent agreement is obtained when all of the relevant molecular states are considered.