In this work we use magnetic deflection of V, Nb, and Ta atomic clusters to measure their magnetic moments. While only a few of the clusters show weak magnetism, all odd-numbered clusters deflect due to the presence of a single unpaired electron. Surprisingly, for the majority of V and Nb clusters an atomic-like behavior is found, which is a direct indication of the absence of spin-lattice interaction. This is in agreement with Kramers degeneracy theorem for systems with a half-integer spin. This purely quantum phenomenon is surprisingly observed for large systems of more than 20 atoms, and also indicates various quantum relaxation processes, via Raman two-phonon and Orbach high-spin mechanisms. In heavier, Ta clusters, the relaxation is always present, probably due to larger masses and thus lower phonon energies, as well as increased spin-orbit coupling.
From magnetic deflection experiments on isolated Co doped Nb clusters we made the interesting observation of some clusters being magnetic, while others appear to be non-magnetic. There are in principle two explanations for this behavior. Either the local moment at the Co site is completely quenched or it is screened by the delocalized electrons of the cluster, i.e. the Kondo effect. In order to reveal the physical origin, we conducted a combined theoretical and experimental investigation. First, we established the ground state geometry of the clusters by comparing the experimental vibrational spectra with those obtained from a density functional theory study. Then, we performed an analyses based on the Anderson impurity model. It appears that the non-magnetic clusters are due to a complete quenching of the local Co moment and not due to the Kondo effect. In addition, the magnetic behavior of the clusters can be understood from an inspection of their electronic structure.Here magnetism is favored when the effective hybridization around the chemical potential is small, while the absence of magnetism is signalled by a large effective hybridization around the chemical potential.
Here we present the results of experimental study of magnetic properties of samarium clusters doped with a single oxygen atom. In a recent theoretical study it was observed that for pure Sm clusters a transition from fully nonmagnetic to weakly magnetic occurs due to a valence change occurring at a size of eight atoms. Here we found, first, that pure Sm clusters could not be synthesized due to the strong oxidation tendency of Sm and the inability to sufficiently remove oxygen from the setup. Therefore, we studied Sm n O clusters. Since the oxygen contributes to the binding, the valence transition for Sm n O clusters may be expected to occur for a smaller cluster size than for pure Sm clusters. Indeed from our experiments the valence transition is indicated to occur for n = 4 Sm atoms instead of n = 8. Furthermore, the observed magnetic moment as function of cluster size for Sm n O clusters shows a strong dependency of the magnetic moment on the cluster size. A large total magnetic moment is observed for Sm 6 O, Sm 7 O, Sm 13 O and Sm 14 O compared to the smaller moment for Sm 8 O to Sm 12 O and Sm 15 O to Sm 18 O.
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