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Register a new userNanoscale Dichotomy of Ti 3d Carriers Mediating the Ferromagnetism in Co:TiO2 Anatase Thin Films
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We study the surface and bulk electronic structure of the room-temperature ferromagnet Co:TiO2 anatase films using soft and hard x-ray photoemission spectroscopy with probe sensitivities of ~1 nm and ~10 nm, respectively. We obtain direct evidence of metallic Ti$^{3+}$ states in the bulk, which get suppressed to give a surface semiconductor, thus indicating a surface-bulk dichotomy. X-ray absorption and high-sensitivity resonant photoemission spectroscopy reveal Ti$^{3+}$ electrons at the Fermi level (E$_F$) and high-spin Co$^{2+}$ electrons occurring away from E$_F$. The results show the importance of the charge neutrality condition: Co$^{2+}$ + V$_{O}$$^{2-}$ + 2Ti$^{4+}$ $leftrightarrow$ Co$^{2+}$ + 2Ti$^{3+}$ (V$_O$ is oxygen vacancy), which gives rise to the elusive Ti 3d carriers mediating ferromagnetism via the Co 3d-O 2p-Ti 3d exchange interaction pathway of the occupied orbitals.
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We revisit the most widely investigated and controversial oxide diluted magnetic semiconductor (DMS), Co:TiO2, with a new high temperature film growth, and show that the corresponding material is not only an intrinsic DMS ferromagnet, but also supports a percolative mechanism of ferromagnetism. We establish the uniformity of dopant distribution across the film cross section by Z-contrast imaging via scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS) at spatial resolution of 0.4 nm and the oxidized 2+ valence state of cobalt by x-ray absorption spectroscopy (XAS). The dependence of magnetic properties on cobalt concentration is consistent with the defect polaron percolation model. The peculiar increase in the transport activation energy above a specific cobalt concentration further emphasizes the polaron contribution to magnetic order.
We present evidence for spin polarized charge carriers in In$_2$O$_3$ films. Both In$_2$O$_3$ and Cr doped In$_2$O$_3$ films exhibit room temperature ferromagnetism after vacuum annealing, with a saturation moment of approximately 0.5 emu/cm$^3$. We used Point Contact Andreev Reflection measurements to directly determine the spin polarization, which was found to be approximately 50$pm$5% for both compositions. These results are consistent with suggestions that the ferromagnetism observed in certain oxide semiconductors may be carrier mediated.
It is shown that dilute niobium doping has significant effect on the ferromagnetism and microstructure of dilutely cobalt-doped anatase TiO2 films. Epitaxial films of anatase TiO2 with 3% Co, without and with 1% niobium doping were grown by pulsed-laser deposition at 875 C at different oxygen pressures. For growth at 10^{-5} Torr niobium doping suppresses the ferromagnetism, while it enhances the same in films grown at 10^{-4} Torr. High-resolution Z-contrast Scanning Transmission Electron Microscopy and Electron Energy Loss Spectroscopy show uniform surface segregation of cobalt-rich Ti_{1-x-y}Co_{x}Nb_{y}O_{2-d} phase, but without cobalt metal clusters.
Pulsed laser deposited films of Co doped anatase TiO2 are examined for Co substitutionality, ferromagnetism, transport, magnetotransport and optical properties. Our results show limited solubility (up to ~ 2 %) of Co in the as-grown films and formation of Co clusters thereafter. For Ti0.93Co0.07O2-d sample, which exhibits a Curie temperature (Tc) over 1180 K, we find the presence of 20-50 nm Co clusters as well as a small concentration of Co incorporated into the remaining matrix. After being subjected to the high temperature anneal during the first magnetization measurement, the very same sample shows a Tc ~ 650 K and almost full matrix incorporation of Co. This Tc is close to that of as-grown Ti0.99Co0.01O2-d sample (~ 700 K). The transport, magnetotransport and optical studies also reveal interesting effects of the matrix incorporation of Co. These results are indicative of an intrinsic Ti1-xCoxO2-d diluted magnetic semiconductor with Tc of about 650-700 K.
We studied the ferroelectric and ferromagnetic properties of compressive strained and unstrained BiMnO3 thin films grown by rf-magnetron sputtering. BiMnO3 samples exhibit a 2D cube-on-cube growth mode and a pseudo-cubic struc-ture up to a thickness of 15 nm and of 25 nm when deposited on (001) SrTiO3 and (110) DyScO3, respectively. Above these thicknesses we observe a switching to a 3D island growth and a simultaneous structural change to a monoclinic structure characterized by a (00l) orientation of the monoclinic unit cell. While ferromagnetism is observed below Tc = 100 K for all samples, signatures of room temperature ferroelectricity were found only in the pseudo-cubic ultra-thin films, indicating a correlation between electronic and structural orders.
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