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Register a new userMagnetic order, hysteresis and phase coexistence in magnetoelectric LiCoPO$_4$
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The magnetic phase diagram of magnetoelectric LiCoPO$_4$ is established using neutron diffraction and magnetometry in fields up to 25.9T applied along the crystallographic $b$-axis. For fields greater than 11.9T the magnetic unit cell triples in size with propagation vector Q = (0, 1/3, 0). A magnetized elliptic cycloid is formed with spins in the $(b,c)$-plane and the major axis oriented along $b$. Such a structure allows for the magnetoelectric effect with an electric polarization along $c$ induced by magnetic fields applied along $b$. Intriguingly, additional ordering vectors Q $approx$ (0, 1/4, 0) and Q $approx$ (0, 1/2, 0) appear for increasing fields in the hysteresis region below the transition field. Traces of this behavior are also observed in the magnetization. A simple model based on a mean-field approach is proposed to explain these additional ordering vectors. In the field interval 20.5-21.0T, the propagation vector Q = (0, 1/3, 0) remains but the spins orient differently compared to the cycloid phase. Above 21.0T and up until saturation a commensurate magnetic structure exists with a ferromagnetic component along $b$ and an antiferromagnetic component along $c$.
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Magnetic structures are investigated by means of neutron diffraction to shine a light on the intricate details that are believed to be key to understanding the magnetoelectric effect in LiCoPO$_4$ . At zero field, a spontaneous spin canting of $varphi = 7(1)^{circ}$ is found. The spins tilt away from the easy $b$-axis toward $c$. Symmetry considerations lead to the magnetic point group $m_z$, which is consistent with the previously observed magnetoelectric tensor form and weak ferromagnetic moment along $b$. For magnetic fields applied along $a$, the induced ferromagnetic moment couples via the Dzyaloshinskii-Moriya interaction to yield an additional field-induced spin canting. An upper limit to the size of the interaction is estimated from the canting angle.
Inelastic neutron scattering (INS) experiments were performed to investigate the spin dynamics in magnetoelectric effect (ME) LiCoPO$_4$ single crystals. Weak dispersion was detected in the magnetic excitation spectra along the three principal crystallographic axes measured around the (0 1 0) magnetic reflection. Analysis of the data using linear spin-wave theory indicate that single-ion anisotropy in LiCoPO$_4$ is as important as the strongest nearest-neighbor exchange coupling. Our results suggest that Co$^{2+}$ single-ion anisotropy plays an important role in the spin dynamics of LiCoPO$_4$ and must be taken into account in understanding its physical properties. High resolution INS measurements reveal an anomalous low energy excitation that we hypothesize may be related to the magnetoelectric effect of LiCoPO$_4$.
Neutron diffraction with static and pulsed magnetic fields is used to directly probe the magnetic structures in LiNiPO$_4$ up to 25T and 42T, respectively. By combining these results with magnetometry and electric polarization measurements under pulsed fields, the magnetic and magnetoelectric phases are investigated up to 56T applied along the easy $c$-axis. In addition to the already known transitions at lower fields, three new ones are reported at 37.6, 39.4 and 54T. Ordering vectors are identified with ${bf Q}_{mathrm{VI}}$ = (0, 1/3, 0) in the interval 37.6--39.4T and ${bf Q}_{mathrm{VII}}$ = (0, 0, 0) in the interval 39.4-54T. A quadratic magnetoelectric effect is discovered in the ${bf Q}_{mathrm{VII}}$ = (0, 0, 0) phase and the field-dependence of the induced electric polarization is described using a simple mean-field model. The observed magnetic structure and magnetoelectric tensor elements point to a change in the lattice symmetry in this phase. We speculate on the possible physical mechanism responsible for the magnetoelectric effect in LiNiPO4.
A theoretical description of the sequence of magnetic phases in Co3TeO6 is presented. The strongly first-order character of the transition to the commensurate multiferroic ground state, induced by coupled order parameters corresponding to different wavevectors, is related to a large magnetoelastic effect with an exchange energy critically sensitive to the interatomic spacing. The monoclinic magnetic symmetry C2 of the multiferroic phase permits spontaneous polarization and magnetization as well as the linear magnetoelectric effect. The existence of weakly ferromagnetic domains is verified experimentally by second harmonic generation measurements.
Combining quasistatic and time-resolved transport measurements with X-ray and neutron diffraction experiments we study the non-equilibrium states that arise in pure and in Ti substituted Ca$_2$RuO$_4$ under the application of current densities. Time-resolved studies of the current-induced switching find a slow conductance relaxation that can be identified with heating and a fast one that unambiguously proves an intrinsic mechanism. The current-induced phase transition leads to complex diffraction patterns. Separated Bragg reflections that can be associated with the metallic and insulating phases by their lattice parameters, indicate a real structure with phase coexistence that strongly varies with temperature and current strength. A third contribution with a $c$ lattice constant in between those of metallic and insulating phases appears upon cooling. At low current densities, this additional phase appears below $sim$100 K and is accompanied by a suppression of the antiferromagnetic order that otherwise can coexist with current carrying states. A possible origin of the intermediate phase is discussed.
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