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Magnetoelectric coupling in the cubic ferrimagnet Cu2OSeO3

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 Added by Jan-Willem Bos
 Publication date 2008
  fields Physics
and research's language is English




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We have investigated the magnetoelectric coupling in the lone pair containing piezoelectric ferrimagnet Cu2OSeO3. Significant magnetocapacitance develops in the magnetically ordered state (TC = 60 K). We find critical behavior near TC and a divergence near the metamagnetic transition at 500 Oe. High-resolution X-ray and neutron powder diffraction measurements show that Cu2OSeO3 is metrically cubic down to 10 K but that the ferrimagnetic ordering reduces the symmetry to rhombohedral R3. The metric cubic lattice dimensions exclude a magnetoelectric coupling mechanism involving spontaneous lattice strain, and this is unique among magnetoelectric and multiferroic materials.



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We present magnetodielectric measurements in single crystals of the cubic spin-1/2 compound Cu$_2$OSeO$_3$. A magnetic field-induced electric polarization ($vec{P}$) and a finite magnetocapacitance (MC) is observed at the onset of the magnetically ordered state ($T_c = 59$ K). Both $vec{P}$ and MC are explored in considerable detail as a function of temperature (T), applied field $vec{H}_a$, and relative field orientations with respect to the crystallographic axes. The magnetodielectric data show a number of anomalies which signal magnetic phase transitions, and allow to map out the phase diagram of the system in the $H_a$-T plane. Below the 3up-1down collinear ferrimagnetic phase, we find two additional magnetic phases. We demonstrate that these are related to the field-driven evolution of a long-period helical phase, which is stabilized by the chiral Dzyalozinskii-Moriya term $D vec{M} cdot(bs{ abla}timesvec{M})$ that is present in this non-centrosymmetric compound. We also present a phenomenological Landau-Ginzburg theory for the ME$_H$ effect, which is in excellent agreement with experimental data, and shows three novel features: (i) the polarization $vec{P}$ has a uniform as well as a long-wavelength spatial component that is given by the pitch of the magnetic helices, (ii) the uniform component of $vec{P}$ points along the vector $(H^yH^z, H^zH^x, H^xH^y)$, and (iii) its strength is proportional to $eta_parallel^2-eta_perp^2/2$, where $eta_parallel$ is the longitudinal and $eta_perp$ is the transverse (and spiraling) component of the magnetic ordering. Hence, the field dependence of P provides a clear signature of the evolution of a conical helix under a magnetic field. A similar phenomenological theory is discussed for the MC.
A detailed zero and transverse field (ZF&TF) muon spin rotation (muSR) investigation of magnetism and the magneto-electric coupling in Cu2OSeO3 is reported. An internal magnetic field B_int(T=0) = 85.37(25) mT was found, in agreement with a ferrimagnetic state below Tc = 57.0(1) K. The temperature dependence of the magnetic order parameter is well described by the relation B_int = B(0)(1-(T/Tc)^2)^b with an effective exponent b = 0.39(1) which is close to the critical exponent B ~ 1/3 for a three dimensional (3D) magnetic system. Just above Tc the muon relaxation rate follows the power low lambda (T)propto (T/Tc - 1)^omega with omega = 1.06(9), which is characteristic for 3D ferromagnets. Measurements of B_int(T) with and without an applied electrostatic field E = 1.66 x 10^5 V/m suggest a possible electric field effect of magnitude Delta Bv = Bv(0 V)-Bv(500 V) = - 0.4(4) mT.
We experimentally study the magnon-photon coupling in a system consitsing of the compensating ferrimagnet gadolinium iron garnet (GdIG) and a three-dimensional microwave cavity. The temperature is varied in order to tune the GdIG magnetization and to observe the transition from the weak coupling regime to the strong coupling regime. By measuring and modelling the complex reflection parameter of the system the effective coupling rate g eff and the magnetization M eff of the sample are extracted. Comparing g eff with the magnon and the cavity decay rate we conclude that the strong coupling regime is easily accessible using GdIG. We show that the effective coupling strength follows the predicted square root dependence on the magnetization.
The ultrastrong coupling of (quasi-)particles has gained considerable attention due to its application potential and richness of the underlying physics. Coupling phenomena arising due to electromagnetic interactions are well explored. In magnetically ordered systems, the quantum-mechanical exchange-interaction should furthermore enable a fundamentally different coupling mechanism. Here, we report the observation of ultrastrong intralayer exchange-enhanced magnon-magnon coupling in a compensated ferrimagnet. We experimentally study the spin dynamics in a gadolinium iron garnet single crystal using broadband ferromagnetic resonance. Close to the ferrimagnetic compensation temperature, we observe ultrastrong coupling of clockwise and anticlockwise magnon modes. The magnon-magnon coupling strength reaches more than 30% of the mode frequency and can be tuned by varying the direction of the external magnetic field. We theoretically explain the observed phenomenon in terms of an exchange-enhanced mode-coupling mediated by a weak cubic anisotropy.
The effect of Cr doping with nominal compositions Mn2-xCrxO3 (0 less than equal to x less than equal to 0.10) has been undertaken to investigate its effect on structural, magnetic, dielectric and magnetoelectric properties. The Cr doping transformed the room temperature crystal structure from orthorhombic to cubic symmetry. Similar to alpha-Mn2O3, two magnetic transitions have been observed in the Cr doped samples. The effect of Cr doping is significant on the low temperature transition i.e. the lower magnetic transition shifted towards higher temperature (25 K for pristine to 40 K for x=0.10) whereas the high temperature transition decreases slightly with increasing Cr content. A clear frequency independent transition is observed in complex dielectric measurements for all compositions around high temperature magnetic ordering. Interestingly, the magnetodielectric behaviour enhanced enormously approx 21% with Cr substitution as compared to pristine Mn2O3.
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