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ABSTRACT: The complete magnetic and multiferroic phase diagram of
Mn$_{1-x}$Co$_{x}$WO$_4$ single crystals is investigated by means of magnetic,
heat capacity, and polarization experiments. We show that the ferroelectric
polarization $\overrightarrow{P}$ in the multiferroic state abruptly changes
its direction twice upon increasing Co content, x. At x$_{c1}$=0.075,
$\overrightarrow{P}$ rotates from the $b-$axis into the $a-c$ plane and at
x$_{c2}$=0.15 it flips back to the $b-$axis. The origin of the multiple
polarization flops is identified as an effect of the Co anisotropy on the
orientation and shape of the spin helix leading to thermodynamic instabilities
caused by the decrease of the magnitude of the polarization in the
corresponding phases. A qualitative description of the ferroelectric
polarization is derived by taking into account the intrachain ($c-$axis) as
well as the interchain ($a-$axis) exchange pathways connecting the magnetic
ions. In a narrow Co concentration range (0.1$\leq$x$\leq$0.15), an
intermediate phase, sandwiched between the collinear high-temperature and the
helical low-temperature phases, is discovered. The new phase exhibits a
collinear and commensurate spin modulation similar to the low-temperature
magnetic structure of MnWO$_4$.
06/2012;
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ABSTRACT: The magnetic and multiferroic phase diagram of Mn0.85Co0.15WO4 single crystals is investigated by means of magnetic, heat-capacity, dielectric, polarization, and neutron-scattering experiments. Three magnetic phase transitions are detected through distinct anomalies in all physical quantities. The ferroelectric polarization is observed only along the b axis below 10 K but not along the a axis as recently suggested. The magnetic phases studied by neutron scattering are very complex. Up to four different magnetic structures, partially coexisting at certain temperature ranges, have been identified. Upon decreasing temperature two commensurate phases (AF4, AF1) are followed by an incommensurate phase (AF5) and a second incommensurate phase (AF2) is detected as a minor phase. The ferroelectric polarization is possibly associated with both (AF2 and AF5) phases.
Phys. Rev. B. 11/2010; 82(18).
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ABSTRACT: We report on the remarkably robust ferroelectric state in the multiferroic compound Mn1-xZnxWO4. Substitution of the magnetic Mn2+ with nonmagnetic Zn2+ reduces the magnetic exchange and provides control of the various magnetic and multiferroic states of MnWO4. Only 5% of Zn substitution results in complete suppression of the frustrated collinear (paraelectric) low-temperature phase. The helical magnetic and ferroelectric phase develops as the ground state. The multiferroic state is stable up to a high level of substitution of more than 50%. The magnetic, thermodynamic, and dielectric properties, as well as the ferroelectric polarization of single crystals of Mn1-xZnxWO4, are studied for different substitutions up to x=0.5. The magnetic phases have been identified in single-crystal neutron-scattering experiments. The ferroelectric polarization scales with the neutron intensity of the incommensurate peak of the helical phase.
Phys. Rev. B. 11/2010; 83(1).
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ABSTRACT: We report inelastic neutron scattering measurements that provide a distinct dynamical "fingerprint" for the multiferroic ground state of 3.5% Ga-doped CuFeO_2. The complex ground state is stabilized by the displacement of the oxygen atoms, which are also responsible for the multiferroic coupling predicted by Arima. By comparing the observed and calculated spectrum of spin excitations, we conclude that the magnetic ground state is a distorted screw-type spin configuration that requires a mechanism for magnetoelectric coupling different from the generally accepted spin-current model. Comment: 4 pages, 4 figures, Submitted to Physical Review Letters
06/2010;
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ABSTRACT: We use neutron scattering to investigate the doping evolution of the magnetic correlations in the single-layer manganite Pr1-xCa1+xMnO4, away from the x=0.5 composition where the CE-type commensurate antiferromagnetic (AF) structure is stable. We find that short-range incommensurate spin correlations develop as the system is electron doped (x<0.5), which coexist with the CE-type AF order. This suggests that electron doping in this system induces an inhomogeneous electronic self-organization, where commensurate AF patches with x=0.5 are separated by electron-rich domain walls with short-range magnetic correlations. This behavior is strikingly different than for the perovskite Pr1-xCaxMnO3, where the long-range CE-type commensurate AF structure is stable over a wide range of electron or hole doping around x=0.5.
Physical Review Letters 10/2009; 103(16):167202. · 7.37 Impact Factor
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ABSTRACT: We use neutron scattering to investigate the doping evolution of the magnetic correlations in the single-layer manganite $\rm Pr_{\it 1-x}Ca_{\it 1+x}MnO_4$, away from the $x=0.5$ composition where the CE-type commensurate antiferromagnetic (AF) structure is stable. We find that short-range incommensurate spin correlations develop as the system is electron doped ($x<0.5$), which coexist with the CE-type AF order. This suggests that electron doping in this system induces an inhomogeneous electronic self-organization, where commensurate AF patches with $x=0.5$ are separated by electron-rich domain walls with short range magnetic correlations. This behavior is strikingly different than for the perovksite $\rm Pr_{\it 1-x}Ca_{\it x}MnO_3$, where the long-range CE-type commensurate AF structure is stable over a wide range of electron or hole doping around $x=0.5$. Comment: 4 figures. To be published in Phys. Rev. Lett
09/2009;
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ABSTRACT: We report the observation of a re-entrant spiral (noncollinear) magnetic order and ferroelectricity below 6 K in Mn <sub>0.965</sub> Fe <sub>0.035</sub> WO <sub>4</sub> under applied magnetic fields above 3.6 T. At zero field, this compound shows a transition into the spiral magnetic and ferroelectric phase at 12 K, and it becomes paraelectric at 10.5 K with the entrance into the commensurate magnetic phase, which is the ground state at H=0 . Under magnetic field above 3.6 T, however, the spiral magnetic phases with a larger FE polarization reappears below 6 K. The re-entrant magnetic/ferroelectric phase behavior is further studied by single crystal neutron scattering and the H-T phase diagram is completely resolved from neutron, dielectric constant, polarization, and magnetic measurements.
Journal of Applied Physics 05/2009; · 2.17 Impact Factor
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ABSTRACT: Elastic neutron scattering is used to study the spin correlations in the multiferroic Mn1−xFexWO4 with x=0.035, 0.05, and 0.10. The noncollinear incommensurate (ICM) magnetic structure associated with the ferroelectric (FE) phase in pure MnWO4 is suppressed at x=0.035 and completely absent at x=0.10. The ICM spin order and FE phase can be restored by applying a magnetic field along the spin easy axis. The low-T commensurate magnetic structure extends in both H/T with increasing Fe concentration. The systematic evolution of the magnetic and electric properties indicates that the noncollinear ICM spin order results from competing magnetic interactions and its stabilization can be tuned by the internal (x) or external (magnetic-field) perturbations.
Phys. Rev. B. 11/2008; 78(19).
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ABSTRACT: Neutron scattering has been used to investigate the evolution of long- and short-range charge-ordered (CO), ferromagnetic, and antiferromagnetic (AF) correlations in single crystals of Pr1−xCaxMnO3. The existence and population of spin clusters as reflected by short-range correlations are found to drastically depend on the doping and temperature. Concentrated spin clusters coexist with long-range canted AF order in a wide temperature range in the x=0.3 while clusters do not appear in the x=0.4 crystal. In contrast, both CO and AF order parameters in the x=0.35 crystal show a precipitous decrease below ∼35 K where spin clusters form. These results provide direct evidence of magnetic phase separation and demonstrate a critical doping xc (close to x=0.35) that divides the inhomogeneous from homogeneous CO ground state.
Phys. Rev. B. 08/2008; 78(5).
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ABSTRACT: The correct stacking of hexagonal layers is used to obtain accurate estimates for the exchange and anisotropy parameters of the geometrically-frustrated antiferromagnet CuFeO$_2$. Those parameters are highly constrained by the stability of a collinear metamagnetic phase between fields of 13.5 and 20 T. Constrained fits of the spin-wave frequencies of the collinear $\uudd $ phase below 7 T are used to identify the magnetic unit cell of the metamagnetic $\uuudd $ phase, which contains two hexagonal layers and 10 Fe$^{3+}$ spins.
08/2008;
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ABSTRACT: Neutron scattering has been used to investigate the evolution of the long- and short-range charge-ordered (CO), ferromagnetic (FM), and antiferromagnetic (AF) correlations in single crystals of Pr1-xCaxMnO3. The existence and population of spin clusters as refected by short-range correlations are found to drastically depend on the doping (x) and temperature (T). Concentrated spin clusters coexist with long-range canted AF order in a wide temperature range in x = 0.3 while clusters do not appear in x = 0.4 crystal. In contrast, both CO and AF order parameters in the x = 0.35 crystal show a precipitous decrease below ~ 35 K where spin clusters form. These results provide direct evidence of magnetic phase separation and indicate that there is a critical doping x_c (close to x = 0.35) that divides the phase-separated site-centered from the homogeneous bond-centered or charge-disproportionated CO ground state. Comment: 4 pages, 4 figures, submitted to Phys. Rev. Letters
04/2008;
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ABSTRACT: We use neutron scattering to study the Pr$^{3+}$ crystalline electric field (CEF) excitations in the filled skutterudite PrOs$_4$As$_{12}$. By comparing the observed levels and their strengths under neutron excitation with the theoretical spectrum and neutron excitation intensities, we identify the Pr$^{3+}$ CEF levels, and show that the ground state is a magnetic $\Gamma_4^{(2)}$ triplet, and the excited states $\Gamma_1$, $\Gamma_4^{(1)}$ and $\Gamma_{23}$ are at 0.4, 13 and 23 meV, respectively. A comparison of the observed CEF levels in PrOs$_4$As$_{12}$ with the heavy fermion superconductor PrOs$_4$Sb$_{12}$ reveals the microscopic origin of the differences in the ground states of these two filled skutterudites.
03/2008;
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ABSTRACT: The spin-wave excitations of the geometrically frustrated triangular lattice antiferromagnet CuFeO2 have been measured using high resolution inelastic neutron scattering. Antiferromagnetic interactions up to third nearest neighbors in the ab plane (J1, J2, J3, with J{2}/J{1} approximately 0.44 and J{3}/J{1} approximately 0.57), as well as out-of-plane coupling (J{z}, with J{z}/J{1} approximately 0.29) are required to describe the spin-wave dispersion relations, indicating a three-dimensional character of the magnetic interactions. Two energy dips in the spin-wave dispersion occur at the incommensurate wave vectors associated with multiferroic phase and can be interpreted as dynamic precursors to the magnetoelectric behavior in this system.
Physical Review Letters 11/2007; 99(15):157201. · 7.37 Impact Factor
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ABSTRACT: The spin wave excitations of the geometrically frustrated triangular lattice antiferromagnet (TLA) $\rm CuFeO_2$ have been measured using high resolution inelastic neutron scattering. Antiferromagnetic interactions up to third nearest neighbors in the ab plane (J_1, J_2, J_3, with $J_2/J_1 \approx 0.44$ and $J_3/J_1 \approx 0.57$), as well as out-of-plane coupling (J_z, with $J_z/J_1 \approx 0.29$) are required to describe the spin wave dispersion relations, indicating a three dimensional character of the magnetic interactions. Two energy dips in the spin wave dispersion occur at the incommensurate wavevectors associated with multiferroic phase, and can be interpreted as dynamic precursors to the magnetoelectric behavior in this system.
09/2007;
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ABSTRACT: Ferromagnetic (FM) manganites, a group of likely half-metallic oxides, are of special interest not only because they are a testing ground for the classical double-exchange interaction mechanism for the 'colossal' magnetoresistance, but also because they exhibit an extraordinary arena of emergent phenomena. These emergent phenomena are related to the complexity associated with strong interplay between charge, spin, orbital, and lattice. In this review, we focus on the use of inelastic neutron scattering to study the spin dynamics, mainly the magnon excitations in this class of FM metallic materials. In particular, we discuss the unusual magnon softening and damping near the Brillouin zone boundary in relatively narrow-band compounds with strong Jahn-Teller lattice distortion and charge-orbital correlations. The anomalous behaviours of magnons in these compounds indicate the likelihood of cooperative excitations involving spin and lattice as well as orbital degrees of freedom.
Journal of Physics Condensed Matter 08/2007; 19(31):315204. · 2.55 Impact Factor
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ABSTRACT: By combining dielectric, specific heat, and magnetization measurements and high-resolution neutron powder diffraction, we have investigated the thermodynamic and magnetic/structural properties of the metastable orthorhombic perovskite ErMnO_3 prepared by high-pressure synthesis. The system becomes antiferromagnetically correlated below 42 K and undergoes a lock-in transition at 28 K with propagation wave vector (0,k_b,0), which remains incommensurate at low temperature. The intercorrelation between the magnetic structure and electric properties and the role of the rare earth moment are discussed.
08/2007;
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ABSTRACT: We use neutron scattering to study the lattice and magnetic structure of the layered half-doped manganite Pr(0.5)Ca(1.5)MnO(4). On cooling from high temperature, the system first becomes charge-and orbital-ordered (CO/OO) near T(CO) = 300 K and then develops checkerboard-like antiferromagnetic (AF) order below T(N) = 130 K. At temperatures above T(N) but below T(CO) (T(N)<T<T(CO)), the appearance of short-range AF spin correlations suppresses the CO/OO-induced orthorhombic strain, contrasting with other half-doped manganites, where AF order has no observable effect on the lattice distortion. These results suggest that a strong spin-lattice coupling and the competition between AF exchange and CO/OO ordering ultimately determines the low-temperature properties of the system.
Proceedings of the National Academy of Sciences 07/2007; 104(26):10796-801. · 9.68 Impact Factor
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ABSTRACT: Using time-of-flight and triple-axis inelastic neutron spectroscopy, we determine spin wave excitations throughout the Brillouin zone for ferromagnetic manganites La$_{1-x}$Ca$_x$MnO$_3$ ($x=0.25,0.3$) in their low temperature metallic states. While spin wave excitations in the long wavelength limit (spin stiffness $D$) have similar values for both compounds, the excitations near the Brillouin zone boundary of La$_{0.7}$Ca$_{0.3}$MnO$_3$ are considerable softened in all symmetry directions compared to that of La$_{0.75}$Ca$_{0.25}$MnO$_3$. A Heisenberg model with the nearest neighbor and the fourth neighbor exchange interactions can describe the overall dispersion curves fairly well. We compare the data with various theoretical models describing the spin excitations of ferromagnetic manganites.
03/2007;
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ABSTRACT: Neutron scattering results are presented for spin-wave excitations of three ferromagnetic metallic A1-xA'xMnO3 manganites (where A and A' are rare- and alkaline-earth-metal ions), which when combined with previous work elucidate the systematics of the interactions as a function of carrier concentration x, on-site disorder, and strength of the lattice distortion. The long-wavelength spin dynamics show only a very weak dependence across the series. The ratio of fourth to first neighbor exchange (J4/J1) that controls the zone boundary magnon softening changes systematically with x, but does not depend on the other parameters. None of the prevailing models can account for these behaviors.
Physical Review Letters 03/2006; 96(4):047204. · 7.37 Impact Factor
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ABSTRACT: We use neutron scattering to study the spin and charge-orbital ordering (CO-OO) in the nearly half-doped perovskite manganite Pr0.55(Ca0.8Sr0.2)0.45MnO3 (PCSMO). On cooling from room temperature, PCSMO first enters into a CO-OO state below TCO and then becomes a CE-type long-range ordered antiferromagnet below TN. At temperatures above TN but below TCO (TN<T<TCO), the spins in PCSMO form highly anisotropic smectic liquid-crystal-like texture with ferromagnetic (FM) quasi-long-range ordered one-dimensional zigzag chains weakly coupled antiferromagnetically. Such a magnetic smecticlike phase results directly from the spin-orbit interaction and demonstrates the presence of textured “electronic soft” phases in doped Mott insulators.
Phys. Rev. B. 12/2005; 72(21).
