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A double-spiral spin ordering in the helimagnet YBaCuFeO$_{5}$
Authors:
Yu-Hui Liang,
Chun-Hao Lai,
Chin-Wei Wang,
Shinichiro Yano,
Daisuke Okuyama,
Taku J. Sato,
Yusuke Nambu,
Shih-Chang Weng,
Yen-Chung Lai,
Wei-Tin Chen,
Kirrily C. Rule,
Chao-Hung Du
Abstract:
Materials with a spiral spin ordering always show a rich phase diagram and can be a playground for studying the exotic physical properties associated with spiral magnetism. Using neutron elastic and resonant x-ray scattering on a high-quality single crystal YBaCuFeO$_{5}$, we demonstrate YBaCuFeO$_{5}$ to be a helimagnet consisting of a double-spiral spin ordering. YBaCuFeO$_{5}$ undergoes a comme…
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Materials with a spiral spin ordering always show a rich phase diagram and can be a playground for studying the exotic physical properties associated with spiral magnetism. Using neutron elastic and resonant x-ray scattering on a high-quality single crystal YBaCuFeO$_{5}$, we demonstrate YBaCuFeO$_{5}$ to be a helimagnet consisting of a double-spiral spin ordering. YBaCuFeO$_{5}$ undergoes a commensurate to incommensurate magnetic phase transition at $T_{N2}$$\sim$ 175 K, and the incommensurate phase consists of two spin-ordered components. Both components have different periodicities but with the same propagating direction along the {\it c}-axis below $T_{N2}$. Using resonant x-ray scattering at the Fe and Cu \textit{K}-edges, we further demonstrate that both spiral spin orderings result from the Fe$^{3+}$ and Cu$^{2+}$, respectively, forming a double-spiral spin ordering structure. This can be understood to be caused by the coupling between both sublattices of Fe$^{3+}$ and Cu$^{2+}$ with the atomic lattice.
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Submitted 27 March, 2025;
originally announced March 2025.
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Detailed dynamics of a moving magnetic skyrmion lattice in MnSi observed using a small-angle neutron scattering under an alternating electric current flow
Authors:
D. Okuyama,
M. Bleuel,
Q. Ye,
J. Krzywon,
N. Nagaosa,
A. Kikkawa,
Y. Taguchi,
Y. Tokura,
J. D. Reim,
Y. Nambu,
T. J. Sato
Abstract:
Lattice formation of swirling textures is ubiquitous in solid-state materials, such as a magnetic skyrmion lattice in chiral magnets. In the magnetic skyrmion lattices, their moving states and dynamics under external perturbations are still unrevealed, although a detailed understanding of the dynamics is crucial to realizing spintronic applications, such as magnetic domain-wall racetrack memory. H…
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Lattice formation of swirling textures is ubiquitous in solid-state materials, such as a magnetic skyrmion lattice in chiral magnets. In the magnetic skyrmion lattices, their moving states and dynamics under external perturbations are still unrevealed, although a detailed understanding of the dynamics is crucial to realizing spintronic applications, such as magnetic domain-wall racetrack memory. Here, we report in detail on the transient state of a moving magnetic skyrmion lattice in bulk single-crystalline MnSi under alternating current (AC) using small-angle neutron scattering. A rotation and concomitant broadening of the spot width in the azimuthal direction of the magnetic skyrmion reflections originating from the plastic deformation of the magnetic skyrmion lattice were found only at low AC frequencies, whereas above the threshold AC frequency (ft ~ 0.12 Hz) the rotation was not observed, and the spot width becomes sharper. The observed complex response of the magnetic skyrmion reflections can be explained by the change in dislocation density in the magnetic skyrmion lattice. At frequencies higher than ft, the magnetic skyrmions oscillate removing the dislocations, indicating that the dislocation density is controlled by the AC frequency.
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Submitted 26 April, 2024;
originally announced April 2024.
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Unraveling the magnetic structure of YbNiSn single crystal via crystal growth and neutron diffraction
Authors:
Hung-Cheng Wu,
Ai Nakamura,
Daisuke Okuyama,
Kazuhiro Nawa,
Dai Aoki,
Taku J Sato
Abstract:
Neutron and x-ray diffraction experiments were performed on the ternary intermetallic compound YbNiSn, formerly categorized as a ferromagnetic Kondo compound. At zero field, an increase in scattering intensity was observed on top of allowed and forbidden nuclear reflections below Tc, breaking the reflection condition of the crystal symmetry Pnma. This indicates that the magnetic structure of YbNiS…
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Neutron and x-ray diffraction experiments were performed on the ternary intermetallic compound YbNiSn, formerly categorized as a ferromagnetic Kondo compound. At zero field, an increase in scattering intensity was observed on top of allowed and forbidden nuclear reflections below Tc, breaking the reflection condition of the crystal symmetry Pnma. This indicates that the magnetic structure of YbNiSn is antiferromagnetic-type, rather than the previously proposed simple collinear ferromagnetic structure. Temperature dependence of the scattering intensity of the 011 reflection confirmed the magnetic ordering at 5.77(2) K. No incommensurate satellite reflection was observed at 2.5 K. By applying external magnetic field of 1 T along the a axis, the magnetic intensity at the nuclear-forbidden 001 position was suppressed, while a slight enhancement at the nuclear-allowed 002 position was observed. This suggests a spin-flip transition under the external magnetic field along the a axis in YbNiSn. The proposed magnetic structures at zero field and 1 T correspond to the magnetic space groups of Pn'm'a and Pnm'a', respectively. The piezomagnetic effect and the switch between the two magnetic space groups by the external stress, which could be detected by the anomalous Hall effect, are proposed.
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Submitted 19 May, 2023;
originally announced May 2023.
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Higher-order modulations in the skyrmion-lattice phase of Cu$_2$OSeO$_3$
Authors:
Johannes D. Reim,
Shinnosuke Matsuzaka,
Koya Makino,
Seno Aji,
Ryo Murasaki,
Daiki Higashi,
Daisuke Okuyama,
Yusuke Nambu,
Elliot P. Gilbert,
Norman Booth,
Shinichiro Seki,
Yoshinori Tokura,
Taku J Sato
Abstract:
Using small angle neutron scattering, we have investigated higher-order peaks in the skyrmion-lattice phase of Cu$_2$OSeO$_3$, in which two different skyrmion lattices, SkX1 and SkX2, are known to form. For each skyrmion-lattice phase, we observed two sets of symmetrically inequivalent peaks at the higher-order-reflection positions with the indices $(110)$ and $(200)$. Under the condition where th…
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Using small angle neutron scattering, we have investigated higher-order peaks in the skyrmion-lattice phase of Cu$_2$OSeO$_3$, in which two different skyrmion lattices, SkX1 and SkX2, are known to form. For each skyrmion-lattice phase, we observed two sets of symmetrically inequivalent peaks at the higher-order-reflection positions with the indices $(110)$ and $(200)$. Under the condition where the SkX1 and SkX2 coexist, we confirmed the absence of the scattering at $\mathbf{Q}$ positions combining reflections from the two phases, indicating a significantly weak double-scattering component. Detailed analysis of the peak profile, as well as the temperature and magnetic-field dependence of the peak intensity, also supports the intrinsic higher-order modulation rather than the parasitic double scattering. The two higher-order modulations show contrasting magnetic-field dependence; the former $(110)$ increases as the field is increased, whereas the latter $(200)$ decreases. This indicates that, in Cu$_2$OSeO$_3$, skyrmions are weakly distorted, and the distortion is field-dependent in a way that the dominant higher-order modulation switches from $(110)$ to $(200)$ under field. Monte Carlo simulations under sweeping external magnetic field qualitatively reproduce the observed magnetic-field dependence, and suggests that the higher-order modulations correspond to the superlattices of weak swirlings appearing in the middle of the original triangular-latticed skyrmions.
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Submitted 18 April, 2022;
originally announced April 2022.
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Structural and magnetic properties of the quasicrystal approximant Au$_{65}$Ga$_{21}$Tb$_{14}$
Authors:
Kazuhiro Nawa,
Maxim Avdeev,
Asuka Ishikawa,
Hiroyuki Takakura,
Chin-Wei Wang,
Daisuke Okuyama,
Ryo Murasaki,
Ryuji Tamura,
Taku J Sato
Abstract:
Magnetic properties of the quasicrystal approximant Au$_{65}$Ga$_{21}$Tb$_{14}$ were investigated by the magnetization and the neutron diffraction experiments. The temperature dependences of the magnetic susceptibility and the magnetization curve indicate dominant ferromagnetic interactions, while the whirling antiferromagnetic order was found from the neutron diffraction experiments. In the antif…
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Magnetic properties of the quasicrystal approximant Au$_{65}$Ga$_{21}$Tb$_{14}$ were investigated by the magnetization and the neutron diffraction experiments. The temperature dependences of the magnetic susceptibility and the magnetization curve indicate dominant ferromagnetic interactions, while the whirling antiferromagnetic order was found from the neutron diffraction experiments. In the antiferromagnetic phase, the magnetic moments are aligned almost perpendicular to a pseudo five-fold symmetry axis, which should correspond to the easy-axis direction of a Tb atom. The magnetic properties similar to those of Au$_{72}$Al$_{14}$Tb$_{14}$ in spite of the difference in the electron-per-atom ratio suggest the robustness of the easy-axis anisotropy against the chemical substitution of the nonmagnetic atoms.
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Submitted 2 April, 2022;
originally announced April 2022.
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Magnetism of Kitaev spin-liquid candidate material RuBr$_3$
Authors:
Yoshinori Imai,
Kazuhiro Nawa,
Yasuhiro Shimizu,
Wakana Yamada,
Hideyuki Fujihara,
Takuya Aoyama,
Ryotaro Takahashi,
Daisuke Okuyama,
Takamasa Ohashi,
Masato Hagihala,
Shuki Torii,
Daisuke Morikawa,
Masami Terauchi,
Takayuki Kawamata,
Masatsune Kato,
Hirotada Gotou,
Masayuki Itoh,
Taku J. Sato,
Kenya Ohgushi
Abstract:
The ruthenium halide $α$-RuCl$_{3}$ is a promising candidate for a Kitaev spin liquid. However, the microscopic model describing $α$-RuCl$_{3}$ is still debated partly because of a lack of analogue materials for $α$-RuCl$_{3}$, which prevents tracking of electronic properties as functions of controlled interaction parameters. Here, we report a successful synthesis of RuBr$_{3}$. The material RuBr…
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The ruthenium halide $α$-RuCl$_{3}$ is a promising candidate for a Kitaev spin liquid. However, the microscopic model describing $α$-RuCl$_{3}$ is still debated partly because of a lack of analogue materials for $α$-RuCl$_{3}$, which prevents tracking of electronic properties as functions of controlled interaction parameters. Here, we report a successful synthesis of RuBr$_{3}$. The material RuBr$_{3}$~possesses BiI$_3$-type structure (space group: $R\overline{3}$) where Ru$^{3+}$ form an ideal honeycomb lattice. Although RuBr$_{3}$ has a negative Weiss temperature, it undergoes a zigzag antiferromagnetic transition at $T_\mathrm{N}=34$ K, as does $α$-RuCl$_{3}$. Our analyses indicate that the Kitaev and non-Kitaev interactions can be modified in ruthenium trihalides by changing the ligand sites, which provides a new platform for exploring Kitaev spin liquids.
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Submitted 31 August, 2021;
originally announced September 2021.
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Antiferromagnetic order of ferromagnetically coupled dimers in the double pyrovanadate CaCoV$_2$O$_7$
Authors:
Ryo Murasaki,
Kazuhiro Nawa,
Daisuke Okuyama,
Maxim Avdeev,
Taku J Sato
Abstract:
Magnetic properties of the pyrovanadate CaCoV$_2$O$_7$ have been studied by means of the bulk magnetization and neutron powder diffraction measurements. Magnetic susceptibility in the paramagnetic phase shows Curie-Weiss behavior with negative Weiss temperature $Θ\simeq -22.5$ K, indicating dominant antiferromagnetic interactions. At $T_{\rm N} = 3.44$ K, CaCoV$_2$O$_7$ shows antiferromagnetic ord…
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Magnetic properties of the pyrovanadate CaCoV$_2$O$_7$ have been studied by means of the bulk magnetization and neutron powder diffraction measurements. Magnetic susceptibility in the paramagnetic phase shows Curie-Weiss behavior with negative Weiss temperature $Θ\simeq -22.5$ K, indicating dominant antiferromagnetic interactions. At $T_{\rm N} = 3.44$ K, CaCoV$_2$O$_7$ shows antiferromagnetic order, accompanied by a weak net ferromagnetic moment of $\sim 0.05$~$μ_{\rm B}/{\rm Co}^{2+}$. Neutron powder diffraction confirms the formation of antiferromagnetic order below $T_{\rm N}$. It was further confirmed from the magnetic structure determination that the two Co$^{2+}$ ions in the adjacent edge-sharing octahedra have almost parallel (ferromagnetic) spin arrangement, indicative of a formation of a ferromagnetic spin dimer. The antiferromagnetic order is, in turn, stabilized by sizable inter-dimer antiferromagnetic interactions.
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Submitted 2 August, 2021;
originally announced August 2021.
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Structural-transition-driven antiferromagnetic to spin-glass transition in Cd-Mg-Tb 1/1 approximants
Authors:
Farid Labib,
Daisuke Okuyama,
Nobuhisa Fujita,
Tsunetomo Yamada,
Satoshi Ohhashi,
Daisuke Morikawa,
Kenji Tsuda,
Taku J. Sato,
An-Pang Tsai
Abstract:
The magnetic susceptibility of the 1/1 approximants to icosahedral quasicrystals in a series of Cd85-xMgxTb15 (x = 5, 10, 15, 20) alloys was investigated in detail. The occurrence of antiferromagnetic to spin-glass-like transition was noticed by increasing Mg. Transmission electron microscopy analysis evidenced a correlation between the magnetic transition and suppression of the monoclinic superla…
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The magnetic susceptibility of the 1/1 approximants to icosahedral quasicrystals in a series of Cd85-xMgxTb15 (x = 5, 10, 15, 20) alloys was investigated in detail. The occurrence of antiferromagnetic to spin-glass-like transition was noticed by increasing Mg. Transmission electron microscopy analysis evidenced a correlation between the magnetic transition and suppression of the monoclinic superlattice ordering with respect to the orientation of the Cd4 tetrahedron at T > 100 K. The possible origins of this phenomenon were discussed in detail. The occurrence of the antiferromagnetic to spin-glass -like magnetic transition is associated with the combination of chemical disorder due to a randomized substitution of Cd with Mg and the orientational disorder of the Cd4 tetrahedra.
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Submitted 28 July, 2020;
originally announced July 2020.
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Magnetic properties of icosahedral quasicrystals and their cubic approximants in the Cd-Mg-RE (RE = Gd, Tb, Dy, Ho, Er, and Tm) systems
Authors:
Farid Labib,
Daisuke Okuyama,
Nobuhisa Fujita,
Tsunetomo Yamada,
Satoshi Ohhashi,
Taku J. Sato,
An-Pang Tsai
Abstract:
A systematic investigation has been performed to elucidate effects of Rare-Earth (RE) type and local atomic configuration on magnetic properties of icosahedral quasicrystal (iQC) and their cubic approximants (2/1 and 1/1 ACs) in the ternary Cd-Mg-RE (RE = Gd, Tb, Dy, Ho, Er, and Tm) systems. At low temperatures, iQC and 2/1 ACs exhibit spin-glass-like freezing for RE = Gd, Tb, Dy, and Ho, while Er…
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A systematic investigation has been performed to elucidate effects of Rare-Earth (RE) type and local atomic configuration on magnetic properties of icosahedral quasicrystal (iQC) and their cubic approximants (2/1 and 1/1 ACs) in the ternary Cd-Mg-RE (RE = Gd, Tb, Dy, Ho, Er, and Tm) systems. At low temperatures, iQC and 2/1 ACs exhibit spin-glass-like freezing for RE = Gd, Tb, Dy, and Ho, while Er and Tm systems do not show freezing behaviour down to the base temperature ~ 2 K. The 1/1 ACs exhibit either spin-glass-like freezing or antiferromagnetic (AFM) ordering depending on their constituent Mg content. The Tf values show increasing trend from iQC to 2/1 and 1/1 ACs. In contrast, the absolute values of Weiss temperature for iQCs are larger than those in 2/1 and 1/1 ACs, indicating that the total AFM interactions between the neighboring spins are larger in aperiodic, rather than periodic systems. Competing spin interactions originating from the long-range Ruderman-Kittel-Kasuya-Yoshida mechanism along with chemical disorder of Cd/Mg ions presumably account for the observed spin-glass-like behavior in Cd-Mg-RE iQCs and ACs.
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Submitted 21 May, 2020;
originally announced May 2020.
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Ferroelectric atomic displacement in multiferroic tetragonal perovskite Sr$_{1/2}$Ba$_{1/2}$MnO$_3$
Authors:
D. Okuyama,
K. Yamauchi,
H. Sakai,
Y. Taguchi,
Y. Tokura,
K. Sugimoto,
T. J. Sato,
T. Oguchi
Abstract:
We investigate the crystal structure in multiferroic tetragonal perovskite Sr$_{1/2}$Ba$_{1/2}$MnO$_3$ with high accuracy of the order of 10$^{-3}$ Angstrom for an atomic displacement. The large atomic displacement for Mn ion from the centerosymmetric position, comparable with the off-centering distortion in the tetragonal ferroelectric BaTiO$_3$, is observed in the ferroelectric phase (…
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We investigate the crystal structure in multiferroic tetragonal perovskite Sr$_{1/2}$Ba$_{1/2}$MnO$_3$ with high accuracy of the order of 10$^{-3}$ Angstrom for an atomic displacement. The large atomic displacement for Mn ion from the centerosymmetric position, comparable with the off-centering distortion in the tetragonal ferroelectric BaTiO$_3$, is observed in the ferroelectric phase ($T_\mathrm{N}$ $\leq$ $T$ $\leq$ $T_\mathrm{C}$). In stark contrast, in the multiferroic phase ($T$ $\leq$ $T_\mathrm{N}$), the atomic displacement for Mn ion is suppressed, but those for O ions are enlarged. The atomic displacements in the polar crystal structures are also analyzed in terms of the ferroelectric modes. In the ferroelectric phase, the atomic displacements are decomposed into dominant positive Slater, negative Last, and small positive Axe modes. The suppression of Slater and Last modes, the sign change of Last mode, and the enlargement of Axe mode are found in the multiferroic phase. The ferroelectric distortion is well reproduced by a first-principles calculation based on Berry phase method, providing an additional information on competing mechanisms to induce the polarization, electronic $p$-$d$ hybridization vs. magnetic exchange-striction.
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Submitted 6 February, 2020;
originally announced February 2020.
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Effect of Ge-substitution on Magnetic Properties in the Itinerant Chiral Magnet MnSi
Authors:
Seno Aji,
Hidesato Ishida,
Daisuke Okuyama,
Kazuhiro Nawa,
Tao Hong,
Taku J Sato
Abstract:
We have investigated the effect of Ge-substitution to the magnetic ordering in the B20 itinerant chiral magnet MnSi prepared by melting and annealing under ambient pressure. From metallurgical survey, the solubility limit of Ge was found to be $x=0.144(5)$ with annealing temperature $T_\mathrm{an} = 1073$ K. Magnetization measurements on MnSi$_{1-x}$Ge$_x$ samples show that the helical ordering te…
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We have investigated the effect of Ge-substitution to the magnetic ordering in the B20 itinerant chiral magnet MnSi prepared by melting and annealing under ambient pressure. From metallurgical survey, the solubility limit of Ge was found to be $x=0.144(5)$ with annealing temperature $T_\mathrm{an} = 1073$ K. Magnetization measurements on MnSi$_{1-x}$Ge$_x$ samples show that the helical ordering temperature $T_{\mathrm{c}}$ increases rapidly in the low-$x$ range, whereas it becomes saturated at higher concentration $x>~0.1$. The Ge substitution also increases both the saturation magnetization $M_\mathrm{s}$ and the critical field to the fully polarized state $H_\mathrm{c2}$. In contrast to the saturation behavior of $T_\mathrm{c}$, those parameters increase linearly up to the highest Ge concentration investigated. In the temperature-magnetic field phase diagram, we found enlargement of the skyrmion phase region for large $x$ samples. We, furthermore, observed the non-linear behavior of helical modulation vector $k$ as a function of Ge concentration, which can be described qualitatively using the mean field approximation.
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Submitted 29 September, 2019;
originally announced September 2019.
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Controlling the stoichiometry of the triangular lattice antiferromagnet Li$_{1+x}$Zn$_{2-y}$Mo$_3$O$_8$
Authors:
K. E. Sandvik,
D. Okuyama,
K. Nawa,
M. Avdeev,
T. J. Sato
Abstract:
The control of the stoichiometry of Li$_{1+x}$Zn$_{2-y}$Mo$_3$O$_8$ was achieved by the solid-state-reaction. We found that the best sample that has the chemical composition Li$_{0.95(4)}$Zn$_{1.92(8)}$Mo$_3$O$_8$ was obtained from the starting nominal composition with Li : Zn : Mo : O = $(1+w)$ : $(2.8-w)$ : $3$ : $8.6$ with $w = -0.1$, indicating that the stoichiometry is greatly improved compar…
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The control of the stoichiometry of Li$_{1+x}$Zn$_{2-y}$Mo$_3$O$_8$ was achieved by the solid-state-reaction. We found that the best sample that has the chemical composition Li$_{0.95(4)}$Zn$_{1.92(8)}$Mo$_3$O$_8$ was obtained from the starting nominal composition with Li : Zn : Mo : O = $(1+w)$ : $(2.8-w)$ : $3$ : $8.6$ with $w = -0.1$, indicating that the stoichiometry is greatly improved compared to those in the earlier reports. For larger $w$ detailed structural analysis indicates that the mixed sites of Li and Zn are preferentially occupied by Li atoms, as well as the fraction of the non-magnetic secondary phase Zn$_2$Mo$_3$O$_8$ decreases. Magnetic susceptibility of the improved stoichiometry powder samples shows a broad hump in the temperature range of 100 $< T <$ 200 K. This suggests that the development of antiferromagnetic correlations at the high temperatures is inherent to the ideal stoichiometric LiZn$_2$Mo$_3$O$_8$.
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Submitted 8 January, 2019;
originally announced January 2019.
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Degenerate ground state in the classical pyrochlore antiferromagnet Na$_3$Mn(CO$_3$)$_2$Cl
Authors:
Kazuhiro Nawa,
Daisuke Okuyama,
Maxim Avdeev,
Hiroyuki Nojiri,
Masahiro Yoshida,
Daichi Ueta,
Hideki Yoshizawa,
Taku J. Sato
Abstract:
In an ideal classical pyrochlore antiferromagnet without perturbations, an infinite degeneracy at a ground state leads to absence of a magnetic order and spin-glass transition. Here we present Na$_3$Mn(CO$_3$)$_2$Cl as a new candidate compound where classical spins are coupled antiferromagnetically on the pyrochlore lattice, and report its structural and magnetic properties.The temperature depende…
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In an ideal classical pyrochlore antiferromagnet without perturbations, an infinite degeneracy at a ground state leads to absence of a magnetic order and spin-glass transition. Here we present Na$_3$Mn(CO$_3$)$_2$Cl as a new candidate compound where classical spins are coupled antiferromagnetically on the pyrochlore lattice, and report its structural and magnetic properties.The temperature dependences of the magnetic susceptibility and heat capacity, and the magnetization curve are consistent with those of an $S$ = 5/2 pyrochlore lattice antiferromagnet with nearest-neighbor interactions of 2 K. Neither an apparent signature of a spin-glass transition nor a magnetic order is detected in magnetization and heat capacity measurements, or powder neutron diffraction experiments. On the other hand, an antiferromagnetic short-range order from the nearest neighbors is evidenced by the $Q$-dependence of the diffuse scattering which develops around 0.85 Å$^{-1}$. A high degeneracy near the ground state in Na$_3$Mn(CO$_3$)$_2$Cl is supported by the magnetic entropy estimated as almost 4 J K$^{-2}$ mol$^{-1}$ at 0.5 K.
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Submitted 11 October, 2018;
originally announced October 2018.
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Deformation of the Magnetic Skyrmion Lattice in MnSi under Electric Current Flow
Authors:
D. Okuyama,
M. Bleuel,
J. S. White,
Q. Ye,
J. Krzywon,
G. Nagy,
Z. Q. Im,
I. Zivkovic,
M. Bartkowiak,
H. M. Ronnow,
S. Hoshino,
J. Iwasaki,
N. Nagaosa,
A. Kikkawa,
Y. Taguchi,
Y. Tokura,
D. Higashi,
J. D. Reim,
Y. Nambu,
T. J. Sato
Abstract:
Using small-angle neutron scattering (SANS), we investigate the deformation of the magnetic skyrmion lattice in bulk single-crystalline MnSi under electric current flow. A significant broadening of the skyrmion-lattice-reflection peaks was observed in the SANS pattern for current densities greater than a threshold value j_t ~ 1 MA/m^2 (10^6 A/m^2). We show this peak broadening to originate from a…
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Using small-angle neutron scattering (SANS), we investigate the deformation of the magnetic skyrmion lattice in bulk single-crystalline MnSi under electric current flow. A significant broadening of the skyrmion-lattice-reflection peaks was observed in the SANS pattern for current densities greater than a threshold value j_t ~ 1 MA/m^2 (10^6 A/m^2). We show this peak broadening to originate from a spatially inhomogeneous rotation of the skyrmion lattice, with an inverse rotation sense observed for opposite sample edges aligned with the direction of current flow. The peak broadening (and the corresponding skyrmion lattice rotations) remain finite even after switching off the electric current. These results indicate that skyrmion lattices under current flow experience significant friction near the sample edges, and plastic deformation due to pinning effects, these being important factors that must be considered for the anticipated skyrmion-based applications in chiral magnets at the nanoscale.
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Submitted 19 July, 2018;
originally announced July 2018.
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Spin Seebeck effect in a polar antiferromagnet $α$-Cu$_{2}$V$_{2}$O$_{7}$
Authors:
Y. Shiomi,
R. Takashima,
D. Okuyama,
G. Gitgeatpong,
P. Piyawongwatthana,
K. Matan,
T. J. Sato,
E. Saitoh
Abstract:
We have studied the longitudinal spin Seebeck effect in a polar antiferromagnet $α$-Cu$_{2}$V$_{2}$O$_{7}$ in contact with a Pt film. Below the antiferromagnetic transition temperature of $α$-Cu$_{2}$V$_{2}$O$_{7}$, spin Seebeck voltages whose magnetic field dependence is similar to that reported in antiferromagnetic MnF$_{2}$$\mid$Pt bilayers are observed. Though a small weak-ferromagnetic moment…
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We have studied the longitudinal spin Seebeck effect in a polar antiferromagnet $α$-Cu$_{2}$V$_{2}$O$_{7}$ in contact with a Pt film. Below the antiferromagnetic transition temperature of $α$-Cu$_{2}$V$_{2}$O$_{7}$, spin Seebeck voltages whose magnetic field dependence is similar to that reported in antiferromagnetic MnF$_{2}$$\mid$Pt bilayers are observed. Though a small weak-ferromagnetic moment appears owing to the Dzyaloshinskii-Moriya interaction in $α$-Cu$_{2}$V$_{2}$O$_{7}$, the magnetic field dependence of spin Seebeck voltages is found to be irrelevant to the weak ferromagnetic moments. The dependences of the spin Seebeck voltages on magnetic fields and temperature are analyzed by a magnon spin current theory. The numerical calculation of spin Seebeck voltages using magnetic parameters of $α$-Cu$_{2}$V$_{2}$O$_{7}$ determined by previous neutron scattering studies reveals that the magnetic-field and temperature dependences of the spin Seebeck voltages for $α$-Cu$_{2}$V$_{2}$O$_{7}$$\mid$Pt are governed by the changes in magnon lifetimes with magnetic fields and temperature.
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Submitted 19 September, 2017;
originally announced September 2017.
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Tiny adiabatic-demagnetization refrigerator for a commercial superconducting quantum interference device magnetometer
Authors:
Taku J Sato,
Daisuke Okuyama,
Hideo Kimura
Abstract:
A tiny adiabatic-demagnetization refrigerator (T-ADR) has been developed for a commercial superconducting quantum interference device magnetometer [Magnetic Property Measurement System (MPMS) from Quantum Design]. The whole T-ADR system is fit in a cylindrical space of the diameter $8.5$ mm and the length $250$ mm, and can be inserted into the narrow sample tube of MPMS. A sorption pump is self-co…
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A tiny adiabatic-demagnetization refrigerator (T-ADR) has been developed for a commercial superconducting quantum interference device magnetometer [Magnetic Property Measurement System (MPMS) from Quantum Design]. The whole T-ADR system is fit in a cylindrical space of the diameter $8.5$ mm and the length $250$ mm, and can be inserted into the narrow sample tube of MPMS. A sorption pump is self-contained in T-ADR, and hence no complex gas handling system is necessary. With the single crystalline Gd$_3$Ga$_5$O$_{12}$ garnet ($\sim 2$ grams) used as a magnetic refrigerant, the routinely achievable lowest temperature is $\sim 0.56$ K. The lower detection limit for a magnetization anomaly is $\sim 1 \times 10^{-7}$ emu, estimated from fluctuation of the measured magnetization. The background level is $\sim 5 \times 10^{-5}$ emu below 2 K at $H = 100$ Oe, which is largely attributable to a contaminating paramagnetic signal from the magnetic refrigerant.
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Submitted 2 December, 2016;
originally announced December 2016.
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Magnon dispersion shift in the induced-ferromagnetic phase of the noncentrosymmetric MnSi
Authors:
Taku J Sato,
Daisuke Okuyama,
Tao Hong,
Akiko Kikkawa,
Yasujiro Taguchi,
Taka-hisa Arima,
Yoshinori Tokura
Abstract:
Small angle neutron inelastic scattering measurement has been performed to study the magnon dispersion relation in the field-induced-ferromagnetic phase of the noncentrosymmetric binary compound MnSi. For the magnons propagating parallel or anti-parallel to the external magnetic field, we experimentally confirmed that the dispersion relation is asymmetrically shifted along the magnetic field direc…
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Small angle neutron inelastic scattering measurement has been performed to study the magnon dispersion relation in the field-induced-ferromagnetic phase of the noncentrosymmetric binary compound MnSi. For the magnons propagating parallel or anti-parallel to the external magnetic field, we experimentally confirmed that the dispersion relation is asymmetrically shifted along the magnetic field direction. This magnon dispersion shift is attributed to the relativistic Dzyaloshinskii-Moriya interaction, which is finite in noncentrosymmetric magnets, such as MnSi. The shift direction is found to be switchable by reversing the external magnetic field direction.
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Submitted 29 September, 2016;
originally announced September 2016.
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Thermal stability and irreversibility of skyrmion-lattice phases in Cu$_2$OSeO$_3$
Authors:
Koya Makino,
Johannes D. Reim,
Daiki Higashi,
Daisuke Okuyama,
Taku J. Sato,
Yusuke Nambu,
Elliot P. Gilbert,
Norman Booth,
Shinichiro Seki,
Yoshinori Tokura
Abstract:
Small angle neutron scattering measurements have been performed to study the thermodynamic stability of skyrmion-lattice phases in Cu$_2$OSeO$_3$. We found that the two distinct skyrmion-lattice phases [SkX(1) and SkX(2) phases] can be stabilized through different thermal histories; by cooling from the paramagnetic phase under finite magnetic field, the SkX(2) phase is selected. On the other hand,…
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Small angle neutron scattering measurements have been performed to study the thermodynamic stability of skyrmion-lattice phases in Cu$_2$OSeO$_3$. We found that the two distinct skyrmion-lattice phases [SkX(1) and SkX(2) phases] can be stabilized through different thermal histories; by cooling from the paramagnetic phase under finite magnetic field, the SkX(2) phase is selected. On the other hand, the 30$^{\circ}$-rotated SkX(1) phase becomes dominant by heating the sample from the ordered conical phase under finite field. This difference in stabilization is surprisingly similar to the irreversibility observed in spin glasses. The zero-field cooling results in the co-existence of the two phases. It is further found that once one of the skyrmion-lattice phases is formed, it is hardly destabilized. This indicates unusual thermal stability of the two skyrmion-lattice phases originating from an unexpectedly large energy barrier between them.
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Submitted 3 February, 2017; v1 submitted 22 August, 2016;
originally announced August 2016.
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Utilization of mechanical alloying method for flux growth of single crystalline BaFe$_2$(As$_{1-x}$P$_x$)$_2$
Authors:
Kosuke Z. Takahashi,
Daisuke Okuyama,
Taku J. Sato
Abstract:
Mechanical alloying method has been employed to prepare the Ba-Fe-As-P precursors, necessary for the Ba-(As,P) flux growth of the single crystalline BaFe$_2$(As$_{1-x}$P$_x$)$_2$. By alloying constituent elementals mechanically, the Ba-(As,P) precursors are successfully formed at the room temperature within one hour, significantly reducing preparation time. Using the mechanically alloyed precursor…
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Mechanical alloying method has been employed to prepare the Ba-Fe-As-P precursors, necessary for the Ba-(As,P) flux growth of the single crystalline BaFe$_2$(As$_{1-x}$P$_x$)$_2$. By alloying constituent elementals mechanically, the Ba-(As,P) precursors are successfully formed at the room temperature within one hour, significantly reducing preparation time. Using the mechanically alloyed precursors, we have grown single crystals of BaFe$_2$(As$_{1-x}$P$_x$)$_2$ with the sizes up to 5~mm $\times$ 5~mm $\times$ 0.1~mm.
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Submitted 28 April, 2016;
originally announced April 2016.
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Incommensurate Magnetic Structure in the Cubic Noncentrosymmetric Ternary Compound Pr5Ru3Al2
Authors:
Koya Makino,
Daisuke Okuyama,
Maxim Avdeev,
Taku J Sato
Abstract:
We performed magnetic susceptibility and neutron powder diffraction experiments on the ternary compound Pr5Ru3Al2. It belongs to the noncentrosymmetric and nonmirrorsymmetric cubic I213 space group. The previously reported ferromagnetic transition at 24 K was not detected in our improved quality samples. Instead, magnetic ordering was observed in the DC magnetic susceptibility at 3.8 K. Neutron po…
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We performed magnetic susceptibility and neutron powder diffraction experiments on the ternary compound Pr5Ru3Al2. It belongs to the noncentrosymmetric and nonmirrorsymmetric cubic I213 space group. The previously reported ferromagnetic transition at 24 K was not detected in our improved quality samples. Instead, magnetic ordering was observed in the DC magnetic susceptibility at 3.8 K. Neutron powder diffraction further indicates that an incommensurate magnetic structure is established below 3.8 K, with the magnetic modulation vector (0.066, 0.066, 0.066) (r.l.u.). Using the magnetic representation analysis, we propose the block helical structure as a candidate for the incommensurate magnetic structure.
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Submitted 5 April, 2016;
originally announced April 2016.
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All-in/all-out magnetic domains: X-ray diffraction imaging and magnetic field control
Authors:
Samuel Tardif,
Soshi Takeshita,
Hiroyuki Ohsumi,
Jun-ichi Yamaura,
Daisuke Okuyama,
Zenji Hiroi,
Masaki Takata,
Taka-hisa Arima
Abstract:
Long-range non-collinear all-in/all-out magnetic order has been directly observed for the first time in real space in the pyrochlore Cd$_2$Os$_2$O$_7$ using resonant magnetic microdiffraction at the Os L$_3$ edge. Two different antiferromagnetic domains related by time-reversal symmetry could be distinguished and have been mapped within the same single crystal. The two types of domains are akin to…
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Long-range non-collinear all-in/all-out magnetic order has been directly observed for the first time in real space in the pyrochlore Cd$_2$Os$_2$O$_7$ using resonant magnetic microdiffraction at the Os L$_3$ edge. Two different antiferromagnetic domains related by time-reversal symmetry could be distinguished and have been mapped within the same single crystal. The two types of domains are akin to magnetic twins and were expected - yet unobserved so far - in the all-in/all-out model. Even though the magnetic domains are antiferromagnetic, we show that their distribution can be controlled using a magnetic field-cooling procedure.
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Submitted 21 July, 2014;
originally announced July 2014.
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Ferrimagnetism and spontaneous ordering of transition-metals in La2CrFeO6 double-perovskite films
Authors:
S. Chakraverty,
A. Ohtomo,
D. Okuyama,
M. Saito,
M. Okude,
R. Kumai,
T. Arima,
Y. Tokura,
S. Tsukimoto,
Y. Ikuhara,
M. Kawasaki
Abstract:
We report on atomic ordering of B-site transition-metals and magnetic properties of epitaxial La2CrFeO6 double-perovskite films grown by pulsed-laser deposition under various conditions. The highest ordered sample exhibited a fraction of antisite-disorder of only 0.05 and a saturation magnetization of ~2μ_{B} per formula unit at 5 K. The result is consistent with the antiferromagnetic ordering of…
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We report on atomic ordering of B-site transition-metals and magnetic properties of epitaxial La2CrFeO6 double-perovskite films grown by pulsed-laser deposition under various conditions. The highest ordered sample exhibited a fraction of antisite-disorder of only 0.05 and a saturation magnetization of ~2μ_{B} per formula unit at 5 K. The result is consistent with the antiferromagnetic ordering of local spin moment (3d^{3}_{\downarrow}3d^{5}_{\uparrow}; S = -3/2+5/2 = 1). Therefore, the magnetic ground state of La2CrFeO6 double-perovskite that has been long debate is unambiguously revealed to be ferrimagnetic. Our results present a wide opportunity to explore novel magnetic properties of binary transition-metal perovskites upon epitaxial stabilization of the ordered phase.
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Submitted 29 July, 2011;
originally announced July 2011.
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Versatile helimagnetic phases under magnetic fields in cubic perovskite SrFeO3
Authors:
S. Ishiwata,
M. Tokunaga,
Y. Kaneko,
D. Okuyama,
Y. Tokunaga,
S. Wakimoto,
K. Kakurai,
T. Arima,
Y. Taguchi,
Y. Tokura
Abstract:
A helical spin texture is of great current interest for a host of novel spin-dependent transport phenomena. We report a rich variety of nontrivial, helimagnetic phases in the simple cubic perovskite SrFeO3 under magnetic fields up to 42 T. Magnetic and resistivity measurements revealed that the proper-screw spin phase proposed for SrFeO3 can be subdivided into at least five kinds of ordered phases…
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A helical spin texture is of great current interest for a host of novel spin-dependent transport phenomena. We report a rich variety of nontrivial, helimagnetic phases in the simple cubic perovskite SrFeO3 under magnetic fields up to 42 T. Magnetic and resistivity measurements revealed that the proper-screw spin phase proposed for SrFeO3 can be subdivided into at least five kinds of ordered phases. Near the multicritical point, an unconventional anomalous Hall effect was found to show up and was interpreted as due to a possible long-period noncoplanar spin texture with scalar spin chirality.
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Submitted 26 July, 2011;
originally announced July 2011.
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Magnetically-Driven Ferroelectric Atomic Displacements in perovskite like YMnO3
Authors:
D. Okuyama,
S. Ishiwata,
Y. Takahashi,
K. Yamauchi,
S. Picozzi,
K. Sugimoto,
H. Sakai,
M. Takata,
R. Shimano,
Y. Taguchi,
T. Arima,
Y. Tokura
Abstract:
Magnetically-driven ferroelectric atomic displacements of the order of 10$^{-3} Angstrom have been observed in orthorhombic (perovskite like) YMnO$_3$ by a single-crystal synchrotron x-ray diffraction. The refined polar structure shows the characteristic bond alternation driven by the exchange striction in staggered Mn-O-Mn arrays with $\uparrow\uparrow\downarrow\downarrow$ type ordering, giving r…
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Magnetically-driven ferroelectric atomic displacements of the order of 10$^{-3} Angstrom have been observed in orthorhombic (perovskite like) YMnO$_3$ by a single-crystal synchrotron x-ray diffraction. The refined polar structure shows the characteristic bond alternation driven by the exchange striction in staggered Mn-O-Mn arrays with $\uparrow\uparrow\downarrow\downarrow$ type ordering, giving rise to a spontaneous polarization along a-axis. First-principles calculations based on the Berry phase method as well as on the experimentally refined crystal structure can reproduce the observed polarization value.
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Submitted 13 July, 2011;
originally announced July 2011.
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Electrons doped in cubic perovskite SrMnO3: isotropic metal versus chainlike ordering of Jahn-Teller polarons
Authors:
H. Sakai,
S. Ishiwata,
D. Okuyama,
A. Nakao,
H. Nakao,
Y. Murakami,
Y. Taguchi,
Y. Tokura
Abstract:
Single crystals of electron-doped SrMnO3 with a cubic perovskite structure have been systematically investigated as the most canonical (orbital-degenerate) double-exchange system, whose ground states have been still theoretically controversial. With only 1-2% electron doping by Ce substitution for Sr, a G-type antiferromagnetic metal with a tiny spin canting in a cubic lattice shows up as the grou…
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Single crystals of electron-doped SrMnO3 with a cubic perovskite structure have been systematically investigated as the most canonical (orbital-degenerate) double-exchange system, whose ground states have been still theoretically controversial. With only 1-2% electron doping by Ce substitution for Sr, a G-type antiferromagnetic metal with a tiny spin canting in a cubic lattice shows up as the ground state, where the Jahn-Teller polarons with heavy mass are likely to form. Further electron doping above 4%, however, replaces this isotropic metal with an insulator with tetragonal lattice distortion, accompanied by a quasi-one-dimensional 3z^2-r^2 orbital ordering with the C-type antiferromagnetism. The self-organization of such dilute polarons may reflect the critical role of the cooperative Jahn-Teller effect that is most effective in the originally cubic system.
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Submitted 16 October, 2010;
originally announced October 2010.
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Epitaxial-strain effect on charge/orbital order in Pr0.5Ca0.5MnO3 films
Authors:
D. Okuyama,
M. Nakamura,
Y. Wakabayashi,
H. Itoh,
R. Kumai,
H. Yamada,
Y. Taguchi,
T. Arima,
M. Kawasaki,
Y. Tokura
Abstract:
Effect of growth orientation on charge- and orbital-ordering (CO-OO) phenomena has been studied for Pr0.5Ca0.5MnO3 epitaxial thin films fabricated on (LaAlO3)0.3-(SrAl0.5Ta0.5O3)0.7 (LSAT) substrates by means of resistivity, synchrotron x-ray diffraction, and polarized optical microscopy measurements. CO-OO transition is observed around 220 K for a film grown on an LSAT (011) substrate ((011)-fi…
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Effect of growth orientation on charge- and orbital-ordering (CO-OO) phenomena has been studied for Pr0.5Ca0.5MnO3 epitaxial thin films fabricated on (LaAlO3)0.3-(SrAl0.5Ta0.5O3)0.7 (LSAT) substrates by means of resistivity, synchrotron x-ray diffraction, and polarized optical microscopy measurements. CO-OO transition is observed around 220 K for a film grown on an LSAT (011) substrate ((011)-film), similarly to a bulk sample, while a film grown on a (001) plane of LSAT ((001)-film) shows much higher transition temperature around 300 K. The domain size of OO is approximately 3 times as large in the (011)-film as in the (001)-film. These results demonstrate that various properties of CO-OO phenomena can be controlled with the growth orientation via the epitaxial strain from the substrate.
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Submitted 31 August, 2009;
originally announced August 2009.
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Lattice-form dependent orbital shape and charge disproportionation in charge- and orbital-ordered manganites
Authors:
D. Okuyama,
Y. Tokunaga,
R. Kumai,
Y. Taguchi,
T. Arima,
Y. Tokura
Abstract:
The orbital shapes and charge disproportionations at nominal Mn$^{3+}$ and Mn$^{4+}$ sites for the charge- and orbital-ordered phases have been studied on half-doped manganites Pr(Sr$_{0.1}$Ca$_{0.9}$)$_2$Mn$_2$O$_7$ and Eu$_{0.5}$Ca$_{1.5}$MnO$_4$ with double-layer and single-layer Mn-O networks, respectively, by means of x-ray structural analyses, in comparison with Pr$_{0.5}$Ca$_{0.5}$MnO…
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The orbital shapes and charge disproportionations at nominal Mn$^{3+}$ and Mn$^{4+}$ sites for the charge- and orbital-ordered phases have been studied on half-doped manganites Pr(Sr$_{0.1}$Ca$_{0.9}$)$_2$Mn$_2$O$_7$ and Eu$_{0.5}$Ca$_{1.5}$MnO$_4$ with double-layer and single-layer Mn-O networks, respectively, by means of x-ray structural analyses, in comparison with Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ with the pseudo cubic network. In a single-layer Eu$_{0.5}$Ca$_{1.5}$MnO$_4$ system, the ($y^2-z^2$)/($z^2-x^2$)-type orbital shape is observed, while the ($3y^2-r^2$)/($3x^2-r^2$)-type orbital shape in a pseudo cubic Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ system. In a double-layer Pr(Sr$_{0.1}$Ca$_{0.9}$)$_2$Mn$_2$O$_7$ system, the orbital shape is found to undergo a large change upon thermally induced rotation of orbital stripe. Furthermore, clear charge disproportionation is observed for the pseudo cubic and double-layer systems, while not in the single-layer system. These results indicate that the orbital shape and charge disproportionation are sensitive to the dimension of Mn-O network.
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Submitted 7 July, 2009;
originally announced July 2009.
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Quadrupolar Order and Structural Phase Transition in DyB4 with Geometrical Frustration
Authors:
Daisuke Okuyama,
Takeshi Matsumura,
Hironori Nakao,
Youichi Murakami
Abstract:
Structural phase transition accompanying with quadrupolar ordering in DyB4 with Shastry-Sutherland type geometrical frustration has been studied by X-ray diffraction. Previous study [D. Okuyama et al.: J. Phys. Soc. Jpn. 74 (2005) 2434.] using resonant X-ray scattering revealed short-range ordering of the Ozx-type quadrupolar moments and the c-plane component of the magnetic moments in addition…
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Structural phase transition accompanying with quadrupolar ordering in DyB4 with Shastry-Sutherland type geometrical frustration has been studied by X-ray diffraction. Previous study [D. Okuyama et al.: J. Phys. Soc. Jpn. 74 (2005) 2434.] using resonant X-ray scattering revealed short-range ordering of the Ozx-type quadrupolar moments and the c-plane component of the magnetic moments in addition to long-range ordering of the c-axis component of the magnetic moments. The present report focuses on the lattice distortion below the quadrupolar ordering temperature at TN2=12.7 K. The (0 0 l=integer) fundamental lattice reflection splits into four peaks along the h and k directions and the (h=even 0 0) reflection becomes broad along the l direction. This indicates that a structural transition from tetragonal to monoclinic takes place below TN2 together with the ordering of the quadrupolar moments.
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Submitted 14 September, 2007;
originally announced September 2007.
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Frustration-driven successive metamagnetic transitions in TbB4
Authors:
T. Inami,
K. Ohwada,
Y. H. Matsuda,
Z. W. Ouyang,
H. Nojiri,
D. Okuyama,
T. Matsumura,
Y. Murakami
Abstract:
Resonant magnetic x-ray diffraction experiments on the Shastry-Sutherland lattice TbB$_4$ were carried out under strong pulsed magnetic fields up to 30 T. TbB$_4$ exhibits a multi-step magnetization process above 16 T when magnetic fields are applied along the c-axis. We examined the intensity of the 010 magnetic reflection as a function of magnetic field and found that the magnetization plateau…
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Resonant magnetic x-ray diffraction experiments on the Shastry-Sutherland lattice TbB$_4$ were carried out under strong pulsed magnetic fields up to 30 T. TbB$_4$ exhibits a multi-step magnetization process above 16 T when magnetic fields are applied along the c-axis. We examined the intensity of the 010 magnetic reflection as a function of magnetic field and found that the magnetization plateau phases are accompanied by large XY components of magnetic moments, in contrast to normal fractional magnetization plateau phases. The magnetization was calculated using a simple spin model deduced from the above result. Finally we propose that frustration is the key to understanding the observed multi-step magnetization.
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Submitted 21 August, 2008; v1 submitted 6 September, 2007;
originally announced September 2007.
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X-ray Anomalous Scattering of Diluted Magnetic Oxide Semiconductors: Possible Evidence of Lattice Deformation for High Temperature Ferromagnetism
Authors:
Takeshi Matsumura,
Daisuke Okuyama,
Shinya Niioka,
Hideaki Ishida,
Tadashi Satoh,
Youichi Murakami,
Hidemi Toyosaki,
Yasuhiro Yamada,
Tomoteru Fukumura,
Masashi Kawasaki
Abstract:
We have examined whether the Co ions crystallographically substitute on the Ti sites in rutile and anatase Ti_{1-x}$Co$_{x}$O$_{2-delta}$ thin films that exhibit room-temperature ferromagnetism. Intensities of the x-ray Bragg reflection from the films were measured around the $K…
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We have examined whether the Co ions crystallographically substitute on the Ti sites in rutile and anatase Ti_{1-x}$Co$_{x}$O$_{2-delta}$ thin films that exhibit room-temperature ferromagnetism. Intensities of the x-ray Bragg reflection from the films were measured around the $K$-absorption-edge of Co. If the Co ions randomly substitute on the Ti sites, the intensity should exhibit an anomaly due to the anomalous dispersion of the atomic scattering factor of Co. However, none of the anatase and rutile samples did exhibit an anomaly, unambiguously showing that the Co ions in Ti$_{1-x}$Co$_{x}$O$_{2-delta}$ are not exactly located at the Ti sites of TiO$_2$. The absence of the anomaly is probably caused by a significant deformation of the local structure around Co due to the oxygen vacancy. We have applied the same method to paramagnetic Zn$_{1-x}$Co$_{x}$O thin films and obtained direct evidence that the Co ions are indeed substituted on the Zn sites.
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Submitted 28 August, 2007;
originally announced August 2007.
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Quadrupolar Frustration in Shastry-Sutherland Lattice of DyB4 Studied by Resonant X-ray Scattering
Authors:
Daisuke Okuyama,
Takeshi Matsumura,
Hironori Nakao,
Youichi Murakami
Abstract:
We have observed geometrical frustration of quadrupolar and magnetic moments in dysprosium tetraboride, DyB4, where the rare-earth sites form a Shastry-Sutherland lattice. Resonant x-ray scattering at the LIII absorption edge of Dy was utilized. Analysis of the energy, polarization, temperature, and azimuthal-angle dependences of the E1 resonance of the (1 0 0) forbidden reflection show that the…
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We have observed geometrical frustration of quadrupolar and magnetic moments in dysprosium tetraboride, DyB4, where the rare-earth sites form a Shastry-Sutherland lattice. Resonant x-ray scattering at the LIII absorption edge of Dy was utilized. Analysis of the energy, polarization, temperature, and azimuthal-angle dependences of the E1 resonance of the (1 0 0) forbidden reflection show that the magnetic and quadrupolar components within the frustrated c plane have a short-range correlation, suggesting that the moments are fluctuating. By contrast, the basic antiferromagnetic component along the c axis has a long-range order.
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Submitted 14 September, 2007; v1 submitted 14 June, 2005;
originally announced June 2005.
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Multipole tensor analysis of the resonant x-ray scattering by quadrupolar and magnetic order in DyB2C2
Authors:
Takeshi Matsumura,
Daisuke Okuyama,
Nobuyuki Oumi,
Kazuma Hirota,
Hironori Nakao,
Youichi Murakami,
Yusuke Wakabayashi
Abstract:
Resonant x-ray scattering (RXS) experiment has been performed for the (3 0 1.5) superlattice reflection in the antiferroquadrupolar and antiferromagnetic phase of DyB2C2. Azimuthal-angle dependence of the resonance enhanced intensities for both dipolar (E1) and quadrupolar (E2) resonant processes has been measured precisely with polarization analysis. Every scattering channel exhibits distinctiv…
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Resonant x-ray scattering (RXS) experiment has been performed for the (3 0 1.5) superlattice reflection in the antiferroquadrupolar and antiferromagnetic phase of DyB2C2. Azimuthal-angle dependence of the resonance enhanced intensities for both dipolar (E1) and quadrupolar (E2) resonant processes has been measured precisely with polarization analysis. Every scattering channel exhibits distinctive azimuthal dependence, differently from the symmetric reflection at (0 0 0.5) which was studied previously. We have analyzed the results using a theory developed by Lovesey et al., which directly connects atomic tensors with the cross-section of RXS. The fitting results indicate that the azimuthal dependences can be explained well by the atomic tensors up to rank 2. Rank 3 and rank 4 tensors are reflected in the data very little. In addition, The coupling scheme among the 4f quadrupolar moment, 5d ortitals, and the lattice has been determined from the interference among the Thomson scattering from the lattice distortion and the resonant scatterings of E1 and E2 processes. It has also been established from the RXS of the (3 0 1.5) reflection that the canting of the 4f quadrupolar moments exists up to T_Q. We also discuss a possible wavefunction of the ground state from the point-charge model calculation.
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Submitted 20 November, 2004;
originally announced November 2004.
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d-f Coulomb and quadrupole-strain interactions in DyB2C2 observed by resonant x-ray scattering
Authors:
T. Matsumura,
D. Okuyama,
N. Oumi,
K. Hirota,
H. Nakao,
Y. Murakami,
Y. Wakabayashi
Abstract:
Experimental evidence of the d-f Coulomb interaction responsible for the resonant x-ray scattering (RXS) from antiferroquadrupolar order in DyB2C2 is presented. The energy dependences of the RXS intensity with polarization analysis are analyzed by considering the interference between the resonances of dipolar (E1) and quadrupolar (E2) transition processes. It is found that the structure factors…
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Experimental evidence of the d-f Coulomb interaction responsible for the resonant x-ray scattering (RXS) from antiferroquadrupolar order in DyB2C2 is presented. The energy dependences of the RXS intensity with polarization analysis are analyzed by considering the interference between the resonances of dipolar (E1) and quadrupolar (E2) transition processes. It is found that the structure factors for the E1 and E2 processes have the same sign for sigma-pi' but the opposite sign for sigma-sigma' channel. This result, when compared with the calculated structure factors, means that the quadrupolar moments of the 4f and 5d electrons have opposite signs to each other. Interference between nonresonant Thomson scattering from the lattice distortion and the resonant scatterings is also studied and a direct coupling between 4f and the lattice is concluded.
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Submitted 22 September, 2004;
originally announced September 2004.