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At least 343 records · Page 19

Effect of Sequential Heat Impacts on the Formation of a Stable State of the xLPM–(1 – x)PT Multiferroic Composites

The effect of thermal cycling and sintering temperature on the chemical and thermodynamic stability of the bulk multiferroic xLa{sub 0.7}Pb{sub 0.3}MnO{sub 3}–(1 – x)PbTiO{sub 3} quasi-ceramic and ceramic composites has been experimentally investigated. It is shown that the limiting temperature of the long-term sample firing should not exceed 1070 K. It has been found that sintering at this temperature and/or short-term exposure of the samples at higher temperatures (up to 1220 K) significantly increase the sample compactness, stabilize the thermal expansion, and enhance the quality of the composites. It has been established that the component grain integrity is violated by shrinkage of the samples and a sharp change in their volume during the phase transition of a ferroelectric component.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetostructural Phase Diagram of Multiferroic (ND 4 ) 2 FeCl 5 .H 2 O

Spin and polarization flop transitions are fascinating, especially when controlled by external stimuli like magnetic and electric field and accompanied by large material responses involving multiple degrees of freedom. Multiferroics like MnWO 4 , TbMnO 3 , and Ni 3 TeO 6 are flagship examples and owe their remarkable properties, for instance field control of polarization and polarization flops combined with spin helix reorientation, to the anisotropy and heavy centers that bring in spin-orbit coupling. The family of A 2 FeX 5 .H 2 O erythrosiderites (A = K, Rb, NH 4 ; B = Fe, Mn, Co; X = Cl, Br, H 2 O) drew our attention due to the rich chemical tuning possibilities, complex phase diagrams, and topological similarities to oxide multiferroics.1 (NH 4 ) 2 FeCl 5 .H 2 O is the flagship example (Fig. 1(a)). It displays a high temperature order-disorder transition involving long-range hydrogen bonding of the NH 4 + group and two successive low temperature magnetic transitions below which non-collinear magnetic order and ferroelectricity are established.1 In addition to the magnetically-induced electric polarization that arises below 6.9 K (P = 3 μC/m 2 along a and a smaller component along b), applied field reveals a peculiar hysteretic spin flop transition near 4.5 T above which polarization flops from the a- to the c-axis. There are elastic components as well. Taken together, these findings raise questions about the interactions that induce this behavior and whether additional non-equilibrium phases might be accessed under even higher magnetic fields.

36 MATERIALS SCIENCE↗

Lack of multiferroic behavior in BaCuSi 2 O 6 is consistent with the frustrated magnetic scenario for this material

BaCuSi 2 O 6 is a well-known quantum magnet that exhibits a Bose-Einstein Condensation quantum phase transition in applied magnetic fields. It contains Cu dimers that form singlets in zero magnetic field, and in applied fields as the singlet-triplet gap is suppressed a quantum phase transition occurs to canted XY antiferromagnetism between critical fields H c1 = 23 T and H c2 = 59 T. In addition, as the temperature is lowered, a rare frustrationinduced dimensional reduction has been proposed from three to two dimensions. Recently, however, a controversy has arisen about the details of the magnetic ordering due to the discovery of a tetragonal to orthorhombic structural transition at 100 K with an incommensurate modulation along the b-axis. Multiple magnon modes were observed in neutron diffraction studies, while NMR found modulation of the spin structure along both the ab plane and the c-axis. In this scenario the material is still a Bose-Einstein condensate system but the frustration is not perfect, calling into question the dimension reduction scenario. A recent study of BaCuSi 2 O 6 combining inelastic neutron diffraction and density functional theory suggest that the material isn’t even frustrated at all and that the spins are ordered ferromagnetically in the a-b plane and antiferromagnetically along the c-axis. After a detailed symmetry analysis we have concluded that the magnetic scenario postulated by this most recent unfrustrated theory6 will render BaCuSi 2 O 6 a multiferroic between H c1 and H c2 , with electric polarization in easy axis of the a-b plane for magnetic fields along the c-axis via an inverse Dzyaloshinskii-Moriya mechanism. Electric polarization is a sensitive symmetry probe of magnetic order, since magnetic systems that break spatial inversion symmetry can induce an overall ferroelectricity in the crystalline lattice. In pulsed magnetic fields we can detect electric polarizations with unique sensitivity to sub-pC/m 2 , which is orders of magnitude more sensitive than what can be detected in DC magnetic field.

36 MATERIALS SCIENCE↗

Organic Multiferroics

This project addresses the physical properties of organic multiferroics, with the understanding of room temperature organic magnetism, magneto-transport, magnetic field effects and magnetoelectric coupling, which could have potential impacts on the flexible electronics, and potentially high T c organic superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Intertwining of Frustration with Magneto-Elastic Coupling in the Multiferroic LuMnO3

Residual magnetic frustration in the multiferroic LuMnO3 may be key towards understanding magneto-elastic coupling in hexagonal manganites. Critical magnetic scattering present well above the magnetic ordering temperature TN persists below, as observed by inelastic neutron scattering. The magnetic fluctuations are confined in two dimensions implied by the characteristic wavevector dependence of the magnetic structure factor that changes from symmetric to asymmetric across TN. The low dimensionality of the magnetic structure is also evident in the temperature dependence of the commensurate antiferromagnetic intensity which follows a mean field exponent of 0.2.

Yano, Shin-ichiro↗

Neutron polarization analysis of the anisotropic spin wave excitations in multiferroic BiFeO 3

A multiferroic material BiFeO 3 shows a cycloidal spin structure below 640 K. Anisotropy of the magnetic excitations below 6 meV was previously studied using neutron polarization analysis (Zhang et al. 2022 Phys. Rev. B 105 144426). The magnetic excitations in and out of the cycloidal plane were separated and compared to those calculated based on the linear spin-wave theory. The overall feature of the observed excitations was found to be consistent with those calculated. Further polarized neutron study with extended energy range has been performed. The anisotropy of the magnetic excitations is present at least up to 15 meV. The out-of-plane mode is constantly more intense by ~50% than the in-plane mode in the energy range between 3 and 15 meV. The anisotropic excitations in the wide energy range are unexpected since multiple in-plane and out-of-plane modes are mixed at higher energies and the excitations are expected to become more isotropic.

Matsuda, Masaaki↗

Single-domain multiferroic BiFeO 3 films

The strong coupling between antiferromagnetism and ferroelectricity at room temperature found in BiFeO 3 generates high expectations for the design and development of technological devices with novel functionalities. However, the multi-domain nature of the material tends to nullify the properties of interest and complicates the thorough understanding of the mechanisms that are responsible for those properties. Here we report the realization of a BiFeO 3 material in thin film form with single-domain behaviour in both its magnetism and ferroelectricity: the entire film shows its antiferromagnetic axis aligned along the crystallographic b axis and its ferroelectric polarization along the c axis. With this we are able to reveal that the canted ferromagnetic moment due to the Dzyaloshinskii–Moriya interaction is parallel to the a axis. Moreover, by fabricating a Co/BiFeO 3 heterostructure, we demonstrate that the ferromagnetic moment of the Co film does couple directly to the canted moment of BiFeO 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Pressure-induced transformations of multiferroic relaxor PbFe 0.5 Nb 0.5 O 3

The effects of hydrostatic pressure at ambient temperature on the structural and dielectric properties of PbFe 0.5 Nb 0.5 O 3 (PFN) were investigated using second harmonic generation (SHG) and powder x-ray diffraction measurements to 31 GPa. The results demonstrate that PFN undergoes a pressure-induced structural transition from the R3$m$ ferroelectric to the $R$$\bar{3}m$ paraelectric phase. SHG measurements showed a continuous decrease in the signal with pressure and complete disappearance at 7.1 GPa. Effective nonlinear optical coefficients were determined from the SHG data, and their pressure behavior was used to infer the nature of the transition. The loss of the SHG signal is accompanied by drastic changes in line widths of Bragg reflections, but no discontinuous change in volume was observed. The pressure-volume data were fit to various equations of state, and a bulk modulus $K_0$ = 136 (±2) GPa, bulk modulus pressure derivative $K_0$ ' = 4.0 (±0.2), and initial volume $V_0$ = 64.5 (±0.1) Å 3 were obtained.

36 MATERIALS SCIENCE↗

Ultrafast light-induced shear strain probed by time-resolved x-ray diffraction: Multiferroic BiFeO 3 as a case study

Enabling the light control of complex systems on ultrashort timescales gives rise to rich physics with promising applications. Although crucial, the quantitative determination of both the longitudinal and the shear photoinduced strains still remains challenging. Here, by scrutinizing asymmetric Bragg peaks pairs (±h01) in BiFeO 3 using picosecond time-resolved x-ray diffraction experiments, we simultaneously determine the longitudinal and shear strains. Importantly, we reveal a difference in the dynamical response of the longitudinal strain with respect to the shear one due to an interplay of quasilongitudinal and quasitransverse acoustic modes, well reproduced by our model. Lastly, we show that the relative amplitude of those strains can be explained only if both thermal and nonthermal processes contribute to the acoustic phonon photogeneration process.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Selection rules and dynamic magnetoelectric effect of the spin waves in multiferroic Bi Fe O 3

Here, we report the magnetic-field dependence of the THz absorption and nonreciprocal directional dichroism spectra of BiFeO 3 measured on the three principal crystal cuts for fields applied along the three principal directions of each cut. From the systematic study of the light polarization dependence, we deduced the optical selection rules of the spin-wave excitations. Our THz data, combined with small-angle neutron scattering results showed that (i) an in-plane magnetic field rotates the q vectors of the cycloids perpendicular to the magnetic field and (ii) the selection rules are mostly determined by the orientation of the q vector with respect to the electromagnetic fields. We observed a magnetic field history-dependent change in the strength and the frequency of the spin-wave modes, which we attributed to the change of the orientation and the length of the cycloidal q vector, respectively. Finally, we compared our experimental data with the results of linear spin-wave theory that reproduces the magnetic-field dependence of the spin-wave frequencies and most of the selection rules, from which we identified the spin-polarization coupling terms relevant for the optical magnetoelectric effect.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Spin dynamics in natural multiferroic pyroxene NaFeSi 2 ⁢O 6

Spin dynamics in the natural mineral aegirine, NaFeSi 2⁢ O 6 , a member of the pyroxene family, was studied by elastic and inelastic neutron scattering. Magnetization and specific-heat measurements as well as single-crystal neutron diffraction maps, taken in the temperature range 2–20 K, confirm two successive magnetic transitions at 8.8 and 5.8 K, consistent with previous studies. The observed spin-wave excitations emerge from the incommensurate magnetic Bragg peaks corresponding to the propagation vector 𝑘 ICM = (0,0.77,0), and extend up to energies of about 1.5 meV. In the low-temperature helical phase, the spin dynamics of the Fe3+ ions is well described by a simple linear spin-wave model. The observed excitations can be modeled using a spin Hamiltonian that includes three primary exchange interactions—intrachain coupling 𝐽 = 0.142⁢(2) ⁢meV, and interchain couplings 𝐽 1 = 0.083⁢(1) ⁢meV and 𝐽 2 = 0.186⁢(1) meV—and an easy-plane anisotropy 𝐷 = 0.020⁢(6)⁢ meV. Furthermore, our results show that no single exchange interaction dominates the spin dynamics. The similar strengths of the intrachain and interchain couplings point to the fact that the magnetic interactions in aegirine are three dimensional rather than confined along one direction. As a result, the system cannot be considered quasi one dimensional, as previously suggested, and calls for further investigations.

Magnetic coupling↗

High P-T Raman study of transitions in relaxor multiferroic Pb(Fe 0.5 Nb 0.5 )O 3

The vibrational and structural properties of Pb(Fe 0.5 Nb 0.5 )O 3 have been investigated using Raman spectroscopy up to 40 GPa at 300 K and from 300 to 415 K at selected pressures. The measurements reveal three phase transitions at 5.5, 8.7 and 24 GPa at room temperature. The temperature dependences of the spectra indicated transitions at 1.5 GPa, at 335 and 365 K. The results support the appearance of an intermediate tetragonal P 4mm phase between ferroelectric R 3m and paraelectric P m-3m phases. Furthermore, a P-T phase diagram is proposed that allows further insight into the magnetoelectric coupling present in this material.

36 MATERIALS SCIENCE↗