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Register a new userPercolative Ferromagnetism in Anatase Co:TiO2
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Added by
Satishchandra B. Ogale
Publication date
2005
fields
Physics
and research's language is
English
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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.
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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.
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.
The 1/f noise in pentacene thin film transistors has been measured as a function of device thickness from well above the effective conduction channel thickness to only two conducting layers. Over the entire thickness range, the spectral noise form is 1/f, and the noise parameter varies as (gate voltage)-1, confirming that the noise is due to mobility fluctuations, even in the thinnest films. Hooges parameter varies as an inverse power-law with conductivity for all film thicknesses. The magnitude and transport characteristics of the spectral noise are well explained in terms of percolative effects arising from the grain boundary structure.
Oxygen vacancies created in anatase TiO2 by UV photons (80 - 130 eV) provide an effective electron-doping mechanism and induce a hitherto unobserved dispersive metallic state. Angle resolved photoemission (ARPES) reveals that the quasiparticles are large polarons. These results indicate that anatase can be tuned from an insulator to a polaron gas to a weakly correlated metal as a function of doping and clarify the nature of conductivity in this material.
This paper reports on the structural and optical properties of Co-doped TiO2 thin films grown onto (0001) Al2O3 substrates by non-reactive pulsed laser deposition (PLD) using argon as buffer gas. It is shown that by keeping constant the substrate temperature at as low as 310 C and varying only the background gas pressure between 7 Pa and 70 Pa, it is possible to grow either epitaxial rutile or pure anatase thin films, as well as films with a mixture of both polymorphs. The optical band gaps of the films are red shifted in comparison to the values usually reported for undoped TiO2, which is consistent with n-type doping of the TiO2 matrix. Such band gap red shift brings the absorption edge of the Co-doped TiO2 films into the visible region, which might favour their photocatalytic activity. Furthermore, the band gap red shift depends on the films phase composition, increasing with the increase of the Urbach energy for increasing rutile content.
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