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Register a new userSignature of Carrier-Induced Ferromagnetism in Ti_{1-x}Co_{x}O_{2-delta}: Exchange Interaction Between High-Spin Co 2+ and the Ti 3d Conduction Band
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X-ray photoemission spectroscopy measurements were performed on thin-film samples of rutile Ti_{1-x}Co_{x}O_{2-delta} to reveal the electronic structure. The Co 2p core level spectra indicate that the Co ions take the high-spin Co 2+ configuration, consistent with substitution on the Ti site. The high spin state and the shift due to the exchange splitting of the conduction band suggest strong hybridization between carriers in the Ti 3d t2g band and the t2g states of the high-spin Co 2+. These observations support the argument that room temperature ferromagnetism in Ti_{1-x}Co_{x}O_{2-delta} is intrinsic.
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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.
Neutron diffraction and thermodynamics techniques were used to probe the evolution of the magnetic properties of Tb(Co_{x}Ni_{1-x})_{2}B_{2}C. A succession of magnetic modes was observed as x is varied: the longitudinal modulated k=(0.55,0,0) state at x=0 is transformed into a collinear k=([nicefrac]<LaTeX> icefrac{1}{2}</LaTeX>,0,[nicefrac]<LaTeX> icefrac{1}{2}</LaTeX>) antiferromagnetic state at x= 0.2, 0.4; then into a transverse c-axis modulated k=(0,0,[nicefrac]<LaTeX> icefrac{1}{3}</LaTeX>) mode at x= 0.6, and finally into a simple ferromagnetic structure at x= 0.8 and 1. Concomitantly, the low-temperature orthorhombic distortion of the tetragonal unit cell at x=0 is reduced smoothly such that for x >= 0.4 only a tetragonal unit cell is manifested. Though predicted theoretically earlier, this is the first observation of the k=(0,0,[nicefrac]<LaTeX> icefrac{1}{3}</LaTeX>) mode in borocarbides; our findings of a succession of magnetic modes upon increasing x also find support from a recently proposed theoretical model. The implication of these findings and their interpretation on the magnetic structure of the RM_{2}B_{2}C series are also discussed.
We present the electronic structure of Sr_{1-(x+y)}La_{x+y}Ti_{1-x}Cr_{x}O_{3} investigated by high-resolution photoemission spectroscopy. In the vicinity of Fermi level, it was found that the electronic structure were composed of a Cr 3d local state with the t_{2g}^{3} configuration and a Ti 3d itinerant state. The energy levels of these Cr and Ti 3d states are well interpreted by the difference of the charge-transfer energy of both ions. The spectral weight of the Cr 3d state is completely proportional to the spin concentration x irrespective of the carrier concentration y, indicating that the spin density can be controlled by x as desired. In contrast, the spectral weight of the Ti 3d state is not proportional to y, depending on the amount of Cr doping.
The magnetic properties of polycrystalline Tb(Co_{x}Ni_{1-x})_{2}B_{2}C (x=0.2,0.4,0.6,0.8) samples were probed by magnetization, specific heat, ac susceptibility, and resistivity techniques. For x{ eq}0.4, the obtained curves are consistent with the features expected for the corresponding magnetic modes, namely k_{1}=(0.55,0,0) at x=0; k_{2}=([nicefrac] icefrac{1}{2}</LaTeX>,0,[nicefrac]<LaTeX> icefrac{1}{2}) at x= 0.2; k_{3}=(0,0,[nicefrac] icefrac{1}{3}) at x= 0.6, and k_{4}=(0,0,0) at x= 0.8 and 1. For x=0.4, even though the neutron diffraction indicates a k_{2} mode, but with a reduced magnetic moment, the magnetization, the ac susceptibility, and resistivity indicate two magnetic events; furthermore, deviation from Curie-Weiss behavior is observed below 150 K for this sample. These features, together with the evolution of both magnetic moment and critical temperature, are attributed to an interplay between competing magnetic couplings; for the particular x=0.4 case, additional factors such as crystalline electric field effects may be in operation.
Recent low temperature heat capacity (C$_P$) measurements on polycrystalline samples of the pyrochlore antiferromagnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+delta}$ have shown a strong sensitivity to the precise Tb concentration $x$, with a large anomaly exhibited for $x sim 0.005$ at $T_C sim 0.5$ K and no such anomaly and corresponding phase transition for $x le 0$. We have grown single crystal samples of Tb$_{2+x}$Ti$_{2-x}$O$_{7+delta}$, with approximate composition $x=-0.001, +0.0042$, and $+0.0147$, where the $x=0.0042$ single crystal exhibits a large C$_P$ anomaly at $T_C$=0.45 K, but neither the $x=-0.001$ nor the $x=+0.0147$ single crystals display any such anomaly. We present new time-of-flight neutron scattering measurements on the $x=-0.001$ and the $x=+0.0147$ samples which show strong $left(frac{1}{2},frac{1}{2},frac{1}{2}right)$ quasi-Bragg peaks at low temperatures characteristic of short range antiferromagnetic spin ice (AFSI) order at zero magnetic field but only under field-cooled conditions, as was previously observed in our $x = 0.0042$ single crystal. These results show that the strong $left(frac{1}{2},frac{1}{2},frac{1}{2}right)$ quasi-Bragg peaks and gapped AFSI state at low temperatures under field cooled conditions are robust features of Tb$_2$Ti$_2$O$_7$, and are not correlated with the presence or absence of the C$_P$ anomaly and phase transition at low temperatures. Further, these results show that the ordered state giving rise to the C$_P$ anomaly is confined to $0 leq x leq 0.01$ for Tb$_{2+x}$Ti$_{2-x}$O$_{7+delta}$, and is not obviously connected with conventional order of magnetic dipole degrees of freedom.
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