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Electric Polarization Induced by a Proper Helical Magnetic Ordering in a Delafossite Multiferroic CuFe1-xAlxO2

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 Added by Taro Nakajima
 Publication date 2007
  fields Physics
and research's language is English




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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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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).
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.
All-electrical control of a dynamic magnetoelectric effect is demonstrated in a classical multiferroic manganite DyMnO3, a material containing coupled antiferromagnetic and ferroelectric orders. Due to intrinsic magnetoelectric coupling with electromagnons a linearly polarized terahertz light rotates upon passing through the sample. The amplitude and the direction of the polarization rotation are defined by the orientation of ferroelectric domains and can be switched by static voltage. These experiments allow the terahertz polarization to be tuned using the dynamic magnetoelectric effect.
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.
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We report unusual effects of nonmagnetic impurities on the spin-triplet superconductor Sr2RuO4. The substitution of nonmagnetic Ti4+ for Ru4+ induces localized-moment magnetism characterized by unexpected Ising anisotropy with the easy axis along the interlayer c direction. Furthermore, for x(Ti) > 0.03 magnetic ordering occurs in the metallic state with the remnant magnetization along the c-axis. We argue that the localized moments are induced in the Ru4+ and/or oxygen ions surrounding Ti4+ and that the ordering is due to their interaction mediated by itinerant Ru-4d electrons with strong spin fluctuations.
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