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Register a new userCompeting Exchange Interactions in the Multiferroic and Ferrimagnetic CaBaCo$_4$O$_7$
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Competing exchange interactions can produce complex magnetic states together with spin-induced electric polarizations. With competing interactions on alternating triangular and kagome layers, the swedenborgite CBO may have one of the largest measured spin-induced polarizations of about 1700 nC/cm$^2$ below its ferrimagnetic transition temperature at 70 K. Powder neutron-diffraction data, magnetization measurements, and spin-wave resonance frequencies in the THz range reveal that the complex spin order of multiferroic CBO can be described as a triangular array of c-axis chains ferrimagnetically coupled to each other in the ab plane. Magnetostriction on bonds that couple those chains produces the large spin-induced polarization of CBO.
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We present a study of terahertz frequency magnetoelectric effect in ferrimagnetic pyroelectric CaBaCo$_4$O$_7$ and its Ni-doped variants. The terahertz absorption spectrum of these materials consists of spin excitations and low-frequency infrared-active phonons. We studied the magnetic-field-induced changes in the terahertz refractive index and absorption in magnetic fields up to 17 T. We find that the magnetic field modulates the strength of infrared-active optical phonons near 1.2 and 1.6 THz. We use the Lorentz model of the dielectric function to analyze the measured magnetic-field dependence of the refractive index and absorption. We propose that most of the magnetoelectric effect is contributed by the optical phonons near 1.6 THz and higher-frequency resonances. Our experimental results can be used to construct and validate more detailed theoretical descriptions of magnetoelectricity in CaBaCo$_{4-x}$Ni$_x$O$_7$.
Distinctive effects of dopant valency is discussed using an impurity level 1% doping each of Cr$^{3+}$ and Ni$^{2+}$ in CaBaCo$_4$O$_7$. Through a comparative study of the magnetic and dielectric properties of multiferroic CaBaCo$_{3.96}$Cr$_{0.04}$O$_7$ and CaBaCo$_{3.96}$Ni$_{0.04}$O$_7$, we highlight that Cr doping does not significantly alter the properties in spite of differences in magnetic spin and ionic radius compared to Co$^{3+}$ and Co$^{2+}$ while Ni doping induces spectacular changes. Particularly, a manifold increase of electric polarization change up to 650 ${rm mu}$C/m$^2$ at 5.6 kV/cm is observed in CaBaCo$_{3.96}$Ni$_{0.04}$O$_7$ compared to CaBaCo$_{3.96}$Cr$_{0.04}$O$_7$ and a stronger magnetoelectric coupling leading to a polarization change of $sim$ 12% in 15 T magnetic field and below 40 K. Further, magnetodielectric effects hint to competing magnetic phases over the temperature range of magnetic transitions. We discuss the observed disparity in the light of a possible site selective doping of Cr$^{3+}$ and Ni$^{2+}$ in the triangular and kagome layers, respectively, of the parent compound.
The formation of conducting channels of Ti${}_4$O${}_7$ inside TiO${}_2$-based memristors is believed to be the origin for the change in electric resistivity of these devices. While the properties of the bulk materials are reasonably known, the interface between them has not been studied up to now mostly due to their different crystalline structures. In this work we present a way to match the interfaces between TiO${}_2$ and Ti${}_4$O${}_7$ and subsequently the band offset between these materials is obtained from density functional theory based calculations. The results show that while the valence band is located at the Ti${}_4$O${}_7$, the conduction band is found at the TiO${}_2$ structure, resulting into a type II interface. In this case, the Ti${}_4$O${}_7$ would act as a donor to the TiO${}_2$ matrix.
We report a neutron scattering study of the magnetic order and dynamics of the bilayer perovskite Sr$_3$Fe$_2$O$_7$, which exhibits a temperature-driven metal-insulator transition at 340 K. We show that the Fe$^{4+}$ moments adopt incommensurate spiral order below $T_text{N}=115$ K and provide a comprehensive description of the corresponding spin wave excitations. The observed magnetic order and excitation spectra can be well understood in terms of an effective spin Hamiltonian with interactions ranging up to third nearest-neighbor pairs. The results indicate that the helical magnetism in Sr$_3$Fe$_2$O$_7$ results from competition between ferromagnetic double-exchange and antiferromagnetic superexchange interactions whose strengths become comparable near the metal-insulator transition. They thus confirm a decades-old theoretical prediction and provide a firm experimental basis for models of magnetic correlations in strongly correlated metals.
The quadruple perovskite CaMn$_7$O$_{12}$ is a topical multiferroic, in which the hierarchy of electronic correlations driving structural distortions, modulated magnetism, and orbital order is not well known and may vary with temperature. x-ray resonant elastic scattering (XRES) provides a momentum-resolved tool to study these phenomena, even in very small single crystals, with valuable information encoded in its polarization- and energy-dependence. We present an application of this technique to CaMn$_7$O$_{12}$. By polarization analysis, it is possible to distinguish superstructure reflections associated with magnetic order and orbital order. Given the high momentum resolution, we resolve a previously unknown splitting of an orbital order superstructure peak, associated with a distinct textit{locked-in} phase at low temperatures. A second set of orbital order superstructure peaks can then be interpreted as a second-harmonic orbital signal. Surprisingly, the intensities of the first- and second-harmonic orbital signal show disparate temperature and polarization dependence. This orbital re-ordering may be driven by an exchange mechanism, that becomes dominant over the Jahn-Teller instability at low temperature.
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