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Tuning in magnetic modes in Tb(Co_{x}Ni_{1-x})_{2}B_{2}C: from longitudinal spin-density waves to simple ferromagnetism

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 Added by M. ELMassalami
 Publication date 2012
  fields Physics
and research's language is English




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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.



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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.
The ground states of the frustrated pyrochlore oxide Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ have been studied by inelastic neutron scattering experiments. Three single-crystal samples are investigated; one shows no phase transition ($x=-0.007<x_{text{c}}sim -0.0025$), being a putative quantum spin-liquid (QSL), and the other two ($x=0.000, 0.003$) show electric quadrupole ordering (QO) below $T_{text{c}} sim 0.5$ K. The QSL sample shows continuum excitation spectra with an energy scale 0.1 meV as well as energy-resolution limited (nominally) elastic scattering. As $x$ is increased, pseudospin wave of the QO state emerges from this continuum excitation, which agrees with that of powder samples and consequently verifies good $x$ control for the present single crystal samples.
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.
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.
Superconductivity and ferromagnetism are two antagonistic cooperative phenomena, which makes it difficult for them to coexist. Here we demonstrate experimentally that they do coexist in EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ with $0.2leq xleq0.4$, in which superconductivity is associated with Fe-3$d$ electrons and ferromagnetism comes from the long-range ordering of Eu-4$f$ moments via Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions. The coexistence is featured by large saturated ferromagnetic moments, high and comparable superconducting and magnetic transition temperatures, and broad coexistence ranges in temperature and field. We ascribe this unusual phenomenon to the robustness of superconductivity as well as the multi-orbital characters of iron pnictides.
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