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Magnetotransport and ferromagnetism in thin films of Co2Si nanoclusters are investigated experimentally and theoretically. The nanoclusters are fabricated by an inert-gas condensation-type cluster-deposition method and have an average size of 11.3 nm. Unlike the bulk Co2Si that exhibits a very weak net magnetic moment only below 10 K, the nanoclusters exhibit room-temperature ferromagnetism with a substantial saturation magnetization. Key features of the system are its closeness to the Stoner transition, magnetic moments induced by spin polarization starting from surface atoms, and nonuniaxial anisotropy associated with the orthorhombic crystal structure of Co2Si. A method is introduced to determine the effective anisotropy using the experimental magnetization data of this complex system and its relationship with the two lowest-order nonuniaxial anisotropy constants. On decreasing temperature from 300 K, the nanoclusters show electron-transport properties unusual for a ferromagnetic metal, including an increase of Hall resistivity and a nonmonotonic change of negative magnetoresistance with a peak at around 100 K. The underlying physics is explained on the basis of the large polarization of surface spins and variation in the degree of their misalignments due to temperature-dependent effective anisotropy.

Neutron powder diffraction (NPD) and x-ray magnetic circular dichroism (XMCD) spectroscopy are employed to investigate the magnetism and spin structure in single-phase B20 Co_1.043Si_0.957. The magnetic contributions to the NPD data measured in zero fields are consistent with the helical order among the allowed spin structures derived from group theory. The magnitude of the magnetic moment is (0.3 ± 0.1) μ_B/Co according to NPD, while the surface magnetization probed by XMCD at 3 kOe is (0.18–0.31) μ_B/Co. Both values are substantially larger than the bulk magnetization of 0.11 μ_B/Co determined from magnetometry at 70 kOe and 2 K. These experimental data indicate the formation of a helical spin phase and the associated conical states in high magnetic fields.