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Refereaces and Notes(1) Weiske, T.; Whme, D. K.; HruUk, J.; Krltschmer, W.; Schwarz, H. (2) ROSS, M. M.; Callahan, J. H. J. Phys. Chem. 1991, 95, 5720. (3) Caldwell, K. A.; Giblin, D. E.; Hsu, C. S.; Cox, D.; Gross, M. L. J. (4) Campbell, E. E. 9.; Ulmer, G.; Hertel, I. V. Z . Phys. D 1992, 23, 1. (5) Weiske, T.; H d k , J.; mhme, D. K.; Schwarz, H. Helv. Chim. Acra (6) WanHsu, M. T.; Rincon, M. E.; Kemper, P. R.; Bowers. M. T. Chem. Phys. Let?. 1990,174, 223. (28) Lifshitz, C.; Iraqi, M.; Fischer, J. E.; Pews, T. In?. J. Mars Spectrom. Ion Processes 1991, 107, 565. (29) Sandler, P.; Lifshitz, C.; Klots, C. E. Chem. Phys. Lett, submitted for publication. Chem. 1991, 95, 10564.
157.Atomic muonium (Mu, the light isotope of hydrogen) is easily encapsulated inside fullerene cages and acts as a highly sensitive microscopic probe of both the fullerene's rotational dynamics and the anisotropy in its electronic distribution. Zerolfield muon spin relaxation studies of MU@C!~~ as a function of temperature reveal the appearance of the Mu triplet precession upon orientational ordering of the fullerene at 270 K, signaling the presence of an axially symmetric hyperfine interaction. A small 2pz admixture is found in the ground-state wave function of Mu@C~O; as a result, the electron density reproduces perfectly the internal shape of the fullerene skeleton, including the small "pinching" in the equator.Positive muons (p+) may bind an electron to form a muonium atom (Mu = &), the light isotope of hydrogen (mMu -(1/9)mH),l Mu encapsulated inside fullereneZ cages has been recently observed*-5 by transverse-field muon spin rotation (TF-pSR) techniques. Here we present the results of a muon spin relaxation study of the endohedral Mu@Cm complex in zerofleld (ZF-pSR) between 10 and 310 K. A singlafrequency oscillation at Y -0.70 (2) MHz appears on cooling near 270 K and signals the presence of an axially symmetric hyperfine interaction that lifts the Mu triplet degeneracy. The rapid tumbling of the fullmne molecules drastically shws upon orientational ordering, and the M U @ C ,~ rotational correlation time is estimated to be -30 ( 5 ) ns at 200 K. Below 150 K, there is evidence for a completely asymmetric hyperfine matrix, indicating a further change in molecular motion. The results show that muonium, trapped in thecavityof a fullcrenc, can be used as a higbly sensitive micrawpic probe of both the molecule's rotational dynamics and the anisotropy in its electronic distribution.The CT0 samp!e (-98.5% average purity, -500 mg) was prepared as desmbed previously? Sublimation7 at 650 O C followed by extended annealing at 250 OC (22 days) leads to highly crystalline material with no traces of trapped solvent and a facccentered-cubic structure at room temperature. The sample was characterized by powder X-ray and high-resolution neutron diffraction, "C NMR spectroscopy, and prompt y-ray neutron activation analysis. ZF-pSR experiments (52 pT) w m performed in longitudinal geometry8 between 10 and 310 K usin...