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We performed high-magnetic-field magnetization, polarization, and ultrasonic measurements in Ba$_2$CuGe$_2$O$_7$ to investigate field-induced multiferroic properties arising from a cross-correlation between electric dipoles and electric quadrupoles in addition to cross-correlation between magnetic dipoles and electric dipoles. Magnetization $M$ shows saturation behavior above 20 T for several magnetic field directions, however, electric polarization $P_c$ exhibits an increase, and elastic constants show a softening above 20 T. Based on quantum states with a crystalline electric field for the $D_{2d}$ point group and $d$-$p$ hybridization between Cu-$3d$ and O-$2p$ electrons, we confirmed that the matrix of an electric dipole $P_z$ was proportional to that of an electric quadrupole $O_{xy}$. Furthermore, considering the spin-orbit coupling of $3d$ electrons and the Zeeman effect, we showed that $P_z$ and $O_{xy}$ simultaneously exhibited field-induced responses. These findings indicate that the orbital degrees of freedom, in addition to the spin degrees of freedom, contribute to the high-field multiferroicity in Ba$_2$CuGe$_2$O$_7$., Comment: 28 pages, 13 figures, accepted in Phys. Rev. B (20 Feb. 2024)

We investigated Fe-substitution effects on ferromagnetic fluctuations in the superconducting overdoped and non-superconducting heavily overdoped regimes of the Bi-2201 cuprates by the magnetization and electrical-resistivity measurements. It was found that the spin-glass state was induced at low temperatures by the Fe substitution. The Curie constant and the effective Bohr magneton, estimated from the magnetic susceptibility, as well as the dimensionality of the ferromagnetic fluctuations from the resistivity, suggest the enhancement of the ferromagnetic fluctuations owing to the Fe substitution. A ferromagnetic spin-cluster model is proposed in the heavily overdoped regime of Bi-2201, while an antiferromagnetic spin-cluster model has been proposed in the overdoped regime of Bi-2201 [Hiraka et al., Phys. Rev. B 81, 144501 (2010)]., Comment: 5 pages, 4 figures

We have investigated the Mn-site substitution effect in Nd$_{0.45}$Sr$_{0.55}$MnO$_3$ single crystal, which has an $A$-type layered antiferromagnetic ($A$-AFM) phase with the 3$d_{x^2-y^2}$-type orbital-order. Substitution of Fe or Ga for Mn-site suppresses both the $A$-AFM order and competing ferromagnetic (FM) correlation whereas Cr substitution suppresses only the $A$-AFM order but reactivates the underlying FM correlation via double-exchange mechanism along the AFM coupled $c$-direction. In Nd$_{0.45}$Sr$_{0.55}$Mn$_{0.95}$Cr$_{0.05}$O$_3$, the $A$-AFM state with the orbital-order is changed into the orbital-disordered three-dimensional FM metallic state by applying magnetic field of $\mu_0 H = 12$ T, which is much smaller than that of the parent compound Nd$_{0.45}$Sr$_{0.55}$MnO$_3$., Comment: 5 pages, 4 figures, to appear in APL Materials

We present the muon spin relaxation/rotation spectra in the multiferroic compound (Cu,Zn)$_{3}$Mo$_{2}$O$_{9}$. The parent material Cu$_{3}$Mo$_{2}$O$_{9}$ has a multiferroic phase below $T_{\rm N}$ = 8.0 K, where the canted antiferromagnetism and the ferroelectricity coexist. The asymmetry time spectra taken at RIKEN-RAL pulsed muon facility show a drastic change at $T_{\rm N}$. At low temperatures the weakly beating oscillation caused by the static internal magnetic fields in the antiferromagnetic phase was observed in Cu$_{3}$Mo$_{2}$O$_{9}$ and the lightly ($0.5\%$) Zn-doped sample. From the fitting of the oscillating term, we obtain the order parameter in these samples: ferromagnetic moment in two sublattices of antiferromagnet. In the heavily ($5.0\%$) Zn-doped sample, the muon-spin oscillation is rapidly damped. The frequency-domain spectrum of this sample suggests a formation of magnetic superstructure., Comment: 8 pages, 5 figures, in press in JPS Conf. Proc. as a part of USM2013 Proceedings

The magnetic and dielectric properties under high magnetic fields are studied in the single crystal of Cu3Mo2O9. This multiferroic compound has distorted tetrahedral spin chains. The effects of the quasi-one dimensionality and the geometrical spin frustration are expected to appear simultaneously. We measure the magnetoelectric current and the differential magnetization under the pulsed magnetic field up to 74 T. We also measure the electric polarization versus the electric field curve/loop under the static field up to 23 T. Dielectric properties change at the magnetic fields where the magnetization jumps are observed in the magnetization curve. Moreover, the magnetization plateaus are found at high magnetic fields., Comment: 6 pages, 3 figures, in press in JPS Conf. Proc. as a part of SCES2013 Proceedings

The magnetic and dielectric properties of \aa kermanite Sr$_2$CoSi$_2$O$_7$ single crystals in high magnetic fields were investigated. We have observed finite induced electric polarization along the c axis in high fields, wherein all Co spins were forcibly aligned to the magnetic field direction. Existence of the induced polarization in the spin-polarized state accompanied with the finite slope in the magnetization curve suggests the possible role of the orbital angular momenta in the excited states as its microscopic origin. The emergence of the field-induced polarization without particular magnetic order can be regarded as the magnetoelectric effects of the second order from the symmetry point of view. A low magnetic field-driven electric polarization flip induced by a rotating field, even at room temperature, has been successfully demonstrated., Comment: 12 pages, 4 figures

We have investigated the $R$-site randomness effect of $R$/Ba-ordered $R$BaMn$_{2}$O$_{6}$ ($R$ = rare earth) by using Y$_{1-y}$La$_y$BaMn$_2$O$_6$ (0 (\leq) $y$ (\leq) 1) in which $R$ (Y,La) and Ba are regularly arranged while Y and La randomly occupy the $R$-site. YBaMn$_2$O$_6$ ($y$ = 0) undergoes charge/orbital ordering (CO) transition at $T_{\rm CO}$ = 500 K while LaBaMn$_{2}$O$_{6}$ ($y$ = 1) shows ferromagnetic metallic (FM) behavior below 350 K\@. In 0 (\leq) $y$ (\leq) 0.6, $T_{\rm CO}$ decreases with an increase in $y$. In 0.6 (\leq) $y$ (\leq) 0.8, $R$-site randomness causes strong phase separation tendencies among the FM, antiferromagnetic (AFM), and CO insulating (COI) states. The large magnetoresistance is observed in the phase separated region., Comment: 4 pages, 2 figures, proceeding of International Conference on Magnetism 2009

We have investigated the $Ln^{3+}$-substitution ($Ln$ = lanthanoid) effect of a quasi two-dimensional ferromagnet Sr$_3$Fe$_{2-x}$Co$_x$O$_{7-\delta}$ ($x$$ = $0.5). %$Ln^{3+}$-substitution creates antiferromagnetic insulating clusters around $Ln^{3+}$. With increasing $Ln^{3+}$-concentration, the ferromagnetism is gradually suppressed and the resistivity is increasing, which are ascribed to an increase in antiferromagnetic (AFM) clusters created by $Ln^{3+}$-substitution. In Sr$_{2.7}$Gd$_{0.3}$Fe$_{1.5}$Co$_{0.5}$O$_{7-\delta}$, the magnetoresistance (MR) is enhanced by about 20 % compared with that of Sr$_3$Fe$_{1.5}$Co$_{0.5}$O$_{7-\delta}$. Coexistence of ferromagnetic (FM) and AFM phases is essential for the enhancement of the MR\@. Applied magnetic fields align the FM clusters in the same direction, resulting in a reduction in the resistivity. A metamagnetic transition observed in the $Ln^{3+}$-doped samples also contributes to the enhancement of the MR., Comment: 4 pages

We have investigated the magnetoelectric properties of (Ca$_{1-x}$Sr$_{x}$)$_2$CoSi$_2$O$_7$ ($0\leq x\leq 1$) crystals with a quasi-two-dimensional structure. In Ca$_2$CoSi$_2$O$_7$ ($x=0$), a canted antiferromagnetic transition occurs at 5.6 K. The transition temperature $T_{\rm N}$ is increasing with increasing Sr concentration, and the rises of the magnetization and dielectric constant become larger. Since the dielectric constant shows large change at $T_{\rm N}$ and the magnetocapacitance effect is observed below $T_{\rm N}$, a coupling between the magnetism and dielectricity is strong in (Ca$_{1-x}$Sr$_{x}$)$_2$CoSi$_2$O$_7$. The positive magnetocapacitance is reduced by Sr substitution, and is not observed in $x\geq 0.5$. Namely, the compound of $x\geq 0.5$ does not show the magnetic-field-induced electric polarization. On the other hand, the negative magnetocapacitance is enhanced by Sr substitution., Comment: 4 pages, 2figures, proceeding of International Conference on Magnetism 2009

We have investigated the magnetic and dielectric properties of Ca$_2$CoSi$_2$O$_7$ crystal. The dielectricity and magnetism of Ca$_2$CoSi$_2$O$_7$ are strongly coupled below a canted antiferromagnetic transition temperature ($T_{\rm N}$): Magnetic fields induce electric polarization below $T_{\rm N}$. Interestingly, the magnetic-field-induced electric polarization is detected even without poling electric fields. Below $T_{\rm N}$, a canted antiferromagnetic-paramagnetic transition is induced by magnetic fields. The large magnetocapacitance is observed around $T_{\rm N}$. The origin of the large magnetocapacitance is due to the magnetic-field-induced the canted antiferromagnetic-paramagnetic transition., Comment: 3 pages, 3 figures. accepted to Applied Physics Letters

We have investigated the Cr-doping effect of Nd0.375Sr0.625MnO3 near the phase boundary between the x2-y2 and 3z2-r2 orbital ordered states, where a ferromagnetic correlation and concomitant large magnetoresistance are observed owing to orbital fluctuation. Cr-doping steeply suppresses the ferromagnetic correlation and magnetoresistance in Nd0.375Sr0.625Mn1-yCryO3 with 0 < y < 0.05, while they reappear in 0.05 < y < 0.10. Such a reentrant behavior implies that a phase boundary is located at y = 0.05, or a phase crossover occurs across y = 0.05., Comment: 3 pages, 3 figures, to be published in Journal of Applied Physics

We have investigated temperature and magnetic-field dependence of dielectric properties in the orthorhombic GdMnO$_3$ single crystal which is located near the phase boundary between the ferroelectric/spiral-antiferromagnetic phase and the paraelectric/$A$-type-antiferromagnetic one. In this compound, strong phase competition between these two phases results in a unique phase diagram with large temperature and magnetic-field hystereses. Based on the phase diagram, we have successfully demonstrated the persistent and reversible phase switching between them by application of magnetic fields., Comment: 4 pages, 2 figures, proceeding of 25th International Conference on Low Temperature Physics LT25

We have investigated the magnetic and dielectric properties of $A_2$CoSi$_2$O$_7$ ($A$=Ca, Sr, and Ba) crystals with a two-dimensional network of CoO$_4$ and SiO$_4$ tetrahedra connected with each other through the corners. In Ca$_2$CoSi$_2$O$_7$, a weak ferromagnetic transition occurs at 5.7 K, where the dielectric constant parallel to the c axis shows a concomitant anomaly. The large magnetocapacitance effect is observed below 5.7 K; $\Delta \varepsilon (H)/\varepsilon (0) \equiv [\varepsilon (H)-\varepsilon (0)]/\varepsilon (0)$ reaches 13 % at 5.1 K\@. These results indicate a strong coupling between the magnetism and dielectricity in Ca$_2$CoSi$_2$O$_7$. Sr$_2$CoSi$_2$O$_7$ shows a similar magnetoelectric behavior to that of Ca$_2$CoSi$_2$O$_7$. In contrast, in Ba$_2$CoSi$_2$O$_7$, which has the different arrangement of SiO$_4$ and CoO$_4$ tetrahedra from that of Ca$_2$CoSi$_2$O$_7$, the magnetocapacitance is hardly observed. The key for the magnetocapacitance effect of $A_2$CoSi$_2$O$_7$ lies in the quasi-two-dimensional crystal structure., Comment: 4 pages, 2 figures, proceeding of 25th International Conference on Low Temperature Physics LT25

We have studied the effects of band filling and bandwidth control on the chemical potential in perovskite manganites $R_{1-x}A_x$MnO$_3$ ($R$ : rare earth, $A$ : alkaline earth) by measurements of core-level photoemission spectra. A suppression of the doping-dependent chemical potential shift was observed in and around the CE-type charge-ordered composition range, indicating that there is charge self-organization such as stripe formation or its fluctuations. As a function of bandwidth, we observed a downward chemical potential shift with increasing bandwidth due to the reduction of the orthorhombic distortion. After subtracting the latter contribution, we found an upward chemical potential shift in the ferromagnetic metallic region $0.3

We have succeeded in preparing A-site ordered- and disordered-Y1/4Sr3/4CoO3-d with various oxygen deficiencies delta, and have made comparative study of their structural and physical properties. In the A-site ordered structure, oxygen vacancies order, and d = 0.34 sample shows a weak ferromagnetic transition beyond 300 K. On the other hand, in the A-site disordered structure, no oxygen vacancy ordering is observed, and d = 0.16 sample shows a ferromagnetic metallic transition around 150 K. A-site disordering destroys the orderings of oxygen-vacancies and orbitals, leading to the strong modification of the electronic phases., Comment: 3 pages, 3 figures, proceeding of 52nd Mangetism and Magnetic Materials Conference (MMM 2007), published in Journal of Applied Physics

We have studied the chemical potential shift as a function of temperature in Nd$_{1-x}$Sr$_x$MnO$_3$ (NSMO) by measurements of core-level photoemission spectra. For ferromagnetic samples ($x=0.4$ and 0.45), we observed an unusually large upward chemical potential shift with decreasing temperature in the low-temperature region of the ferromagnetic metallic (FM) phase. This can be explained by the double-exchange (DE) mechanism if the $e_g$ band is split by dynamical/local Jahn-Teller effect. The shift was suppressed near the Curie temperature ($T_C$), which we attribute to the crossover from the DE to lattice-polaron regimes., Comment: 5 pages, 6 figures

We have investigated the role of the 4$f$ moment on the magnetoelectric (ME) effect of orthorhombic $R$MnO$_{3}$ ($R$=rare earth ions). In order to clarify the role of the 4$f$ moment, we prepared three samples: (Eu,Y)MnO$_{3}$ without the 4$f$ moment, TbMnO$_{3}$ with the anisotropic 4$f$ moment, and (Gd,Y)MnO$_{3}$ with the isotropic 4$f$ moment. The ferroelectric behaviors of these samples are different from each other in a zero magnetic field. (Eu,Y)MnO$_{3}$ and (Gd,Y)MnO$_{3}$ show the ferroelectric polarization along the a axis in the ground state, while TbMnO$_{3}$ shows it along the c axis. Such difference may arise from the influence of the anisotropic Tb$^{3+}$ 4$f$ moment. The direction of the ferroelectric polarization of $R$MnO$_{3}$ is determined by the internal magnetic field arising from the 4$f$ moment., Comment: 2 pages, 1 figure, the proceeding of International Conference of Magnetism, to be published in the Journal of Magnetism and Magnetic Materials

We have investigated orthorhombic $R$MnO$_{3}$ ($R$=(Gd$_{1-y}$Tb$_{y}$)) crystals near the phase boundary between the paraelectric $A$-type-antiferromagnetic (AF) phase (PA) and the ferroelectric transverse-spiral-AF one (FS). The spiral AF structure breaks inversion symmetry and induces the ferroelectric polarization through the inverse Dzyaloshinskii-Moriya (DM) interaction. We have found that the PA-FS phase boundary is located at around 0.15$<$$y$$<$0.2. In $y$=0.15 compound, PA and FS phases appear in cooling scan, while FS is not observed in warming scan. This result suggests that FS observed in $y$=0.15 is a metastable state arising from the competition between PA and FS. Furthermore, we demonstrate the phase control between these competing phases by the application of the external magnetic field and external quasihydrostatic pressure., Comment: 6 pages, 3 figures, proceeding of Highly Frustrated Magnetism 2006,to be published in the Journal of Physics: Condensed Matter

We have investigated the dielectric and magnetic properties of Eu$_{0.595}$Y$_{0.405}$MnO$_{3}$ $without$ the presence of the 4$f$ magnetic moments of the rare earth ions, and have found two ferroelectric phases with polarization along the $a$ and $c$ axes in a zero magnetic field. A magnetic field induced switching from one to the other ferroelectric phase took plase in which the direction of ferroelectric polarization changed from the a axis to the c axis by the application of magnetic fields parallel to the a axis. In contrast to the case of TbMnO$_{3}$, in which the 4$f$ moments of Tb$^{3+}$ ions play an important role in such a ferroelectric phase switching, the magnetic-field-induced switching between ferroelectric phases in Eu$_{0.595}$Y$_{0.405}$MnO$_{3}$ does not originate from the magnetic transition of the rare-earth 4$f$ moments, but from that of the Mn 3$d$ spins., Comment: 8 pages, 3 figures, RevTeX4, Proceedings of MMM 2005, to appear in J. Appl. Phys

The Hall resistivity and magnetization have been investigated in the ferromagnetic state of the bilayered manganite La(2-2x)Sr(1+2x)Mn2O7 (x=0.36). The Hall resistivity shows an increase in both the ordinary and anomalous Hall coefficients at low temperatures below 50K, a region in which experimental evidence for the spin glass state has been found in a low magnetic field of 1mT. The origin of the anomalous behavior of the Hall resistivity relevant to magnetic states may lie in the intrinsic microscopic inhomogeneity in a quasi-two-dimensional electron system., Comment: 7 pages, 4 figures, Solid State Communications (in press)

We have investigated the dielectric properties of Gd$_{1-x}$Tb$_{x}$MnO$_{3}$ crystals in magnetic fields to clarify the crossover between two distinct ferroelectric phases, GdMnO$_{3}$-type (first-order displacive) and TbMnO$_{3}$-type (second-order order-disorder). We have found that the compositional phase boundary between the phases exists around 0.3$<$$x$$<$0.4. For the $x$=0.1 sample exposed to magnetic fields above 3T, we have discovered successive ferroelectric phase transitions that occur at two different temperatures. We have determined the electric and magnetic phase diagram for $x$$=$0, 0.1, and 0.3 in the plane of temperature and field in order to demonstrate the change in the ferroelectric phases., Comment: 3 pages, 3 figures, IEEEtran, Proceedings of INTERMAG 2005, appear in IEEE Transactions on Magnetics

We have investigated dielectric properties in a series of crystals of $R$MnO$_{3}$ ($R$ is a rare earth ion) under magnetic fields and quasihydrostatic pressure. We have found that ferroelectric phase appeared in GdMnO$_3$ crystal below 13K. We have confirmed that a small spontaneous polarization exists along a axis ($P_a$) in the orthorhombic $Pbnm$ setting and that $P_a$ can be reversed by the dc electric field. The dielectric anomaly due to the ferroelectric transition accompanied thermal hysteresis and lattice striction. The ferroelectric transition temperature decreased with quasihydrostatic pressure. These results indicate that the ferroelectric transition is improper and is of the first-order displacement-type one. $P_a$ was easily collapsed by application of magnetic field of 0.4T parallel to the spin-canting direction ($H \| c$) while it was enhanced parallel to the easy axis ($H \| b$)., Comment: 2 pages, 1 figure. Proceedings of SCES'04, to appear in Physica B

We have investigated dielectric properties in Mott insulators GdMnO$_{3}$ and TbMnO$_{3}$ under magnetic fields and external quasihydrostatic pressures. In the case of GdMnO$_{3}$, thermal hysteresis for dielectric constant $\epsilon$ and discontinuous lattice distortion were observed at ferroelectric transition temperature ($T_{C}$), and ferroelectric spontaneous polarization was suppressed by application of external pressure. These results indicate that the ferroelectric transition in GdMnO$_{3}$ is a first-order displacive-type one. On the other hand, the thermal hysteresis and discontinuous lattice striction were not observed at $T_{C}$ in TbMnO$_{3}$. The peak of $\epsilon$ corresponding to ferroelectric transition was shifted toward higher temperatures by application of external pressure in TbMnO$_{3}$. The ferroelectric transition of TbMnO$_{3}$ was thought to be a second-order order-disorder-type one., Comment: 4 pages, 3 figures, RevTeX4, Proceedings of MMM 2004, appear in J. Appl. Phys

Photoinduced effects in a single crystal of bilayered manganites, La2-2xSr1+2xMn2O7 (x=0.38), were investigated in a wide range of temperatures by pump-probe measurement at a photon energy of 1.6eV. In a ferromagnetic metallic state, significant enhancement of positive rise in differential reflectivity with a slow relaxing time of hundred picoseconds was observed just below Tc=127K, indicating that the reflectivity change with the slow relaxation time constant is induced by laser heating. We have also observed an unconventional fast relaxing component that has a time constant of the order of ten picoseconds. This fast relaxing component, whose absolute value has an asymmetric peak at Tc, is presumably due to short-range correlation of Jahn-Teller distortion., Comment: 13 pages, 4 figures, accepted to Solid State Communications

Unusual temperature and doping dependence of the Mn 3d spectral functions of manganese perovskites Nd1-xSrxMnO3 has been revealed by the high-resolution Mn 2p-3d resonance photoemission. The temperature-dependent spectra cannot be explained by any theoretical model currently under debate, while showing evidence for a microscopic and dynamic phase segregation. The experimental results strongly suggest that the competition of both the dynamical and static Jahn-Teller effects with ferromagnetic ordering at high and low temperatures, respectively, is responsible for the actual electronic states., Comment: 4 pages, 2 figures

Spin wave excitations were measured in the ferromagnetic phase of Nd$_{1/2}$Sr$_{1/2}$MnO$_{3}$ by neutron scattering. This compound is located in proximity to the A-type antiferromagnetic state, and it shows a clear anisotropy and anomalous softening of the spin wave excitations. The softening in the ferromagnetic phase is induced by the orbital ordering., Comment: 2 pages, 1 figure, proceeding of ICM2000. Corrected typos

In order to study the magnetic and crystal structures in the Nd{1-x}Sr{x}MnO{3} system, we have peformed neutron diffraction measurements on melt-grown polycrystalline samples with 0.49 < x < 0.75. As a function of hole concentration x, the system shows systematic transformation of magnetic and crystal structures, which is consistently explained by the change of the character of Mn eg orbitals. With increasing x, the Nd{1-x}Sr{x}MnO{3} system exhibits a metallic ferromagnetic state, a metallic A-type AFM state, and then an insulating C-type AFM state. The CE-type charge-ordered AFM state was observed only in the vicinity of x=1/2, and it coexists with the A-type AFM state for x > 1/2, indicating that the energy difference between these two states is extremely small. We also found that the MnO{6} octahedra are apically compressed in the CE-type and A-type AFM states due to the d(3x2-r2)/d(3y2-r2) or d(x2-y2) orbital orderings, respectively, whereas they are apically elongated by the rod-type d(3z2-r2) orbital ordering in the C-type AFM state. In addition, a selective broadening of Bragg peaks was observed in the C-type AFM phase, and its x dependence strongly suggests the charge ordering for a commsurate value of the hole concentration at either x=3/4 or x=4/5., Comment: REVTeX, 13 pages, 10 figures, submitted to Phys. Rev. B

We report inelastic neutron scattering results on the spin dynamics in the 50 % hole-doped manganites, Pr{1/2}Sr{1/2}MnO3 and Nd{1/2}Sr{1/2}MnO3. In the paramagnetic phase, these systems exhibit a ridge-type diffuse scattering, indicating a two-dimensional ferromagnetic (FM) correlation. With decreasing temperature, the systems enter the FM state, but simultaneously they develop A-type antiferromagnetic spin fluctuations. The spin wave dispersion in the FM state is strongly anisotropic. These behaviors can be consistently interpreted from a viewpoint of the underlying orbital ordering., Comment: REVTeX, 4 pages, 4 figures, submitted to Phys. Rev. Lett