Unravelling the complex magnetic structure of multiferroic pyroxene NaFeGe2O6: A combined experimental and theoretical study

Magnetic order and the underlying magnetic model of the multiferroic pyroxene NaFeGe2O6 are systematically investigated by neutron powder diffraction, thermodynamic measurements, density-functional bandstructure calculations, and Monte-Carlo simulations. Upon cooling, NaFeGe2O6 first reveals one-dimensional spin-spin correlations in the paramagnetic state below about 50 K, revealed by magnetic diffuse scattering. The sinusoidal spin-density wave with spins along the a-direction sets in at 13 K, followed by the cycloidal configuration with spins lying in the (ac) plane below 11.6 K. Microscopically, the strongest magnetic coupling runs along the structural chains, J1 ' 12 K, which is likely related to the one-dimensional spin-spin correlations. The interchain couplings J2 ' 3:8K and J3 ' 2:1K are energetically well balanced and compete, thus giving rise to the incommensurate order in sharp contrast to other transition-metal pyroxenes, where one type of the interchain couplings prevails. The magnetic model of NaFeGe2O6 is further completed by the weak single-ion anisotropy along the a-direction. Our results resolve the earlier controversies regarding the magnetic order in NaFeGe2O6 and establish relevant symmetries of the magnetic structures. These results, combined with symmetry analysis, enable us to identify the possible mechanisms of the magnetoelectric coupling in this compound. We also elucidate microscopic conditions for the formation of incommensurate magnetic order in pyroxenes.Comment: 10 pages 10 figures, PRB(accepted

Weak ferromagnetism and spin reorientation in antiferroelectric BiCrO3

BiCrO3 is an antiferroelectric perovskite known to exhibit an unconventional spin reorientation transition between antiferromagnetic structures, accompanied by a large jump in weak ferromagnetism. Using a combination of neutron powder diffraction, magnetometry, and symmetry analysis, we confirm the dominant G-type antiferromagnetic order below TN = 111 K and identify the magnetic phase transition with a spontaneous rotation of Cr3+ moments from the b axis to a particular direction in the ac plane. We demonstrate the role of antiferroelectric displacements produced by the Bi3+ lone-pair electrons and octahedral rotations in establishing spin canting via the antisymmetric Dzyaloshinskii-Moriya interaction. This mechanism results in weak ferromagnetism above and below the spin-reorientation and explains the dramatic increase in net magnetization on cooling

Magnetic order in the frustrated Ising-like chain compound Sr3_3NiIrO6_6

We have studied the field and temperature dependence of the magnetization of single crystals of Sr3NiIrO6. These measurements evidence the presence of an easy axis of anisotropy and two anomalies in the magnetic susceptibility. Neutron powder diffraction realized on a polycrystalline sample reveals the emergence of magnetic reflections below 75 K with magnetic propagation vector k ~ (0, 0, 1), undetected in previous neutron studies [T.N. Nguyen and H.-C zur Loye, J. Solid State Chem., 117, 300 (1995)]. The nature of the magnetic ground state, and the presence of two anomalies common to this family of material, are discussed on the basis of the results obtained by neutron diffraction, magnetization measurements, and symmetry arguments

First-order multi-k phase transitions and magnetoelectric effects in multiferroic Co3TeO6

A theoretical description of the sequence of magnetic phases in Co3TeO6 is presented. The strongly first-order character of the transition to the commensurate multiferroic ground state, induced by coupled order parameters corresponding to different wavevectors, is related to a large magnetoelastic effect with an exchange energy critically sensitive to the interatomic spacing. The monoclinic magnetic symmetry C2' of the multiferroic phase permits spontaneous polarization and magnetization as well as the linear magnetoelectric effect. The existence of weakly ferromagnetic domains is verified experimentally by second harmonic generation measurements

Magnetic frustration and spontaneous rotational symmetry breaking in PdCrO2

In the triangular layered magnet PdCrO2 the intralayer magnetic interactions are strong, however the lattice structure frustrates interlayer interactions. In spite of this, long-range, 120$^\circ$ antiferromagnetic order condenses at $T_N = 38$~K. We show here through neutron scattering measurements under in-plane uniaxial stress and in-plane magnetic field that this occurs through a spontaneous lifting of the three-fold rotational symmetry of the nonmagnetic lattice, which relieves the interlayer frustration. We also show through resistivity measurements that uniaxial stress can suppress thermal magnetic disorder within the antiferromagnetic phase.Comment: 9 pages, 9 figure