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Piezo-magnetoelectric effect, namely simultaneous induction of both the ferromagnetic moment and electric polarization by an application of uniaxial stress, was achieved in the non-ferroelectric and antiferromagnetic ground state of DyFeO$_3$. The in duced electric polarization and ferromagnetic moment are coupled with each other, and monotonically increase with increasing uniaxial stress. The present work provides a new way to design spin-driven multiferroic states, that is, magnetic symmetry breaking forced by external uniaxial stress.
We have investigated spin-wave excitations in a magnetic-field-induced 1/5-magnetization plateau phase in a triangular lattice antiferromagnet CuFeO2 (CFO), by means of inelastic neutron scattering measurements under applied magnetic fields of up to 13.4 T. Comparing the observed spectra with the calculations in which spin-lattice coupling effects for the nearest neighbor exchange interactions are taken into account, we have determined the Hamiltonian parameters in the field-induced 1/5- plateau phase, which directly show that CFO exhibits a bond order associated with the magnetic structure in this phase.
We have investigated spin-wave excitations in a four-sublattice (4SL) magnetic ground state of a frustrated magnet CuFeO2, in which `electromagnon (electric-field-active magnon) excitation has been discovered by recent terahertz time-domain spectrosc opy [Seki et al. Phys. Rev. Lett. 105 097207 (2010)]. In previous study, we have identified two spin-wave branches in the 4SL phase by means of inelastic neutron scattering measurements under applied uniaxial pressure. [T. Nakajima et al. J. Phys. Soc. Jpn. 80 014714 (2011) ] In the present study, we have performed high-energy-resolution inelastic neutron scattering measurements in the 4SL phase, resolving fine structures of the lower-energy spin-wave branch near the zone center. Taking account of the spin-driven lattice distortions in the 4SL phase, we have developed a model Hamiltonian to describe the spin-wave excitations. The determined Hamiltonian parameters have successfully reproduced the spin-wave dispersion relations and intensity maps obtained in the inelastic neutron scattering measurements. The results of the spin-wave analysis have also revealed physical pictures of the magnon and electromagnon modes in the 4SL phase, suggesting that collinear and noncollinear characters of the two spin-wave modes are the keys to understand the dynamical coupling between the spins and electric dipole moments in this system.
We have demonstrated that ferroelectric polarization in a spin-driven multiferroic CuFe1-xGaxO2 with x = 0.035 can be controlled by the application of uniaxial pressure. Our neutron diffraction and in-situ ferroelectric polarization measurements have revealed that the pressure dependence of the ferroelectric polarization is explained by repopulation of three types of magnetic domains originating from the trigonal symmetry of the crystal. We conclude that the spin-driven anisotropic lattice distortion and the fixed relationship between the directions of the magnetic modulation wave vector and the ferroelectric polarization are the keys to this spin-mediated piezoelectric effect.
By means of neutron scattering measurements, we have investigated spin-wave excitation in a collinear four-sublattice (4SL) magnetic ground state of a triangular lattice antiferromagnet CuFeO2, which has been of recent interest as a strongly frustrat ed magnet, a spin-lattice coupled system and a multiferroic. To avoid mixing of spin-wave spectrum from magnetic domains having three different orientations reflecting trigonal symmetry of the crystal structure, we have applied uniaxial pressure on [1-10] direction of a single crystal CuFeO2. By elastic neutron scattering measurements, we have found that only 10 MPa of the uniaxial pressure results in almost single domain state in the 4SL phase. We have thus performed inelastic neutron scattering measurements using the single domain sample, and have identified two distinct spin- wave branches. The dispersion relation of the upper spin-wave branch cannot be explained by the previous theoretical model [R. S. Fishman: J. Appl. Phys. 103 (2008) 07B109]. This implies the importance of the lattice degree of freedom in the spin-wave excitation in this system, because the previous calculation neglected the effect of the spin-driven lattice distortion in the 4SL phase. We have also discussed relationship between the present results and the recently discovered electromagnon excitation.
We have investigated magnetic field dependences of a ferroelectric incommensurate-helimagnetic order in a trigonal magneto-electric (ME) multiferroic CuFe1-xAlxO2 with x=0.015, which exhibits the ferroelectric phase as a ground state, by means of neu tron diffraction, magnetization and dielectric polarization measurements under magnetic fields applied along various directions. From the present results, we have established the H-T magnetic phase diagrams for the three principal directions of magnetic fields; (i) parallel to the c axis, (ii) parallel to the helical axis, and (iii) perpendicular to the c and the helical axes. While the previous dielectric polarization (P) measurements on CuFe1-xGaxO2 with x=0.035 have demonstrated that the magnetic field dependence of the `magnetic domain structure results in distinct magnetic field responses of P [S. Seki et al., Phys. Rev. Lett., 103 237601 (2009)], the present study have revealed that the anisotropic magnetic field dependence of the ferroelectric helimagnetic order `in each magnetic domain can be also a source of a variety of magnetic field responses of P in CuFe1-xAxO2 systems (A=Al, Ga).
We have performed synchrotron radiation X-ray and neutron diffraction measurements on magnetoelectric multiferroic CuFe1-xAlxO2 (x=0.0155), which has a proper helical magnetic structure with incommensurate propagation wave vector in the ferroelectric phase. The present measurements revealed that the ferroelectric phase is accompanied by lattice modulation with a wave number 2q, where q is the magnetic modulation wave number. We have calculated the Fourier spectrum of the spatial modulations in the local electric polarization using a microscopic model proposed by Arima [T. Arima, J. Phys. Soc. Jpn. 76, 073702 (2007)]. Comparing the experimental results with the calculation results, we found that the origin of the 2q-lattice modulation is not conventional magnetostriction but the variation in the metal-ligand hybridization between the magnetic Fe^3+ ions and ligand O^2- ions. Combining the present results with the results of a previous polarized neutron diffraction study [Nakajima et al., Phys. Rev. B 77 052401 (2008)], we conclude that the microscopic origin of the ferroelectricity in CuFe1-xAlxO2 is the variation in the metal-ligand hybridization with spin-orbit coupling.
Multiferroic CuFe1-xAlxO2 (x=0.02) exhibits a ferroelectric ordering accompanied by a proper helical magnetic ordering below T=7K under zero magnetic field. By polarized neutron diffraction and pyroelectric measurements, we have revealed a one-to-one correspondence between the spin helicity and the direction of the spontaneous electric polarization. This result indicates that the spin helicity of the proper helical magnetic ordering is essential for the ferroelectricity in CuFe1-xAlxO2. The induction of the electric polarization by the proper helical magnetic ordering is, however, cannot be explained by the Katsura-Nagaosa-Balatsky model, which successfully explains the ferroelectricity in the recently explored ferroelectric helimagnets, such as TbMnO3. We thus conclude that CuFe1-xAlxO2 is a new class of magnetic ferroelectrics.
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