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Register a new userIdentification of microscopic spin-polarization coupling in the ferroelectric phase of a magnetoelectric multiferroic CuFe1-xAlxO2
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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.
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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 neutron 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).
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.
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.
We have discovered strong magnetoelectric (ME) effects in the single chiral-helical magnetic state of single-crystalline langasite Ba3NbFe3Si2O14 that is crystallographically chiral. The ferroelectric polarization, predominantly aligned along the a axis below the Neel temperature of ~27 K, changes in a highly non-linear fashion in the presence of in-plane magnetic fields (H) perpendicular to the a axis (H//b*). This ME effect as well as smaller ME effects in other directions exhibit no poling dependence, suggesting the presence of a self-formed single ME domain. In addition, these ME effects accompany no-measurable hysteresis, which is crucial for many technological applications.
We present a unique example of giant magnetoelectric effect in a conventional multiferroic HoMnO3, where polarization is very large (~56 mC/m2) and the ferroelectric transition temperature is higher than the magnetic ordering temperature by an order. We attribute the uniqueness of the giant magnetoelectric effect to the ferroelectricity induced entirely by the off-center displacement of rare earth ions with large magnetic moments. This finding suggests a new avenue to design multiferroics with large polarization and higher ferroelectric transition temperature as well as large magnetoelectric effects.
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