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Register a new userRemarkable effects of dopant valency $-$ a comparative study of CaBaCo$_{3.96}$Cr$_{0.04}$O$_7$ and CaBaCo$_{3.96}$Ni$_{0.04}$O$_7$
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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.
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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$_7$.
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.
Using maximally localized Wannier functions obtained from DFT calculations, we derive an effective Hubbard Hamiltonian for a bilayer of Sr$_3$Cr$_2$O$_7$, the $n=2$ member of the Ruddlesden-Popper Sr$_{n+1}$Cr$_n$O$_{3n+1}$ system. The model consists of effective $t_{2g}$ orbitals of Cr in two square lattices, one above the other. The model is further reduced at low energies and two electrons per site, to an effective Kugel-Khomskii Hamiltonian that describes interacting spins 1 and pseudospins 1/2 at each site describing spin and orbitals degrees of freedom respectively. We solve this Hamiltonian at zero temperature using pseudospin bond operators and spin waves. Our results confirm a previous experimental and theoretical study that proposes spin ordering antiferromagnetic in the planes and ferromagnetic between planes, while pseudospins form vertical singlets, although the interplane separation is larger than the nearest-neighbor distance in the plane. We explain the physics behind this rather unexpected behavior.
Magnetic materials with pyrochlore crystal structure form exotic magnetic states due to the high lattice frustration. In this work we follow the effects of coupling of the lattice and electronic and magnetic degrees of freedom in two Praseodymium-based pyrochlores Pr$_2$Zr$_2$O$_7$ and Pr$_2$Ir$_2$O$_7$. In both materials the presence of magnetic interactions does not lead to magnetically ordered low temperature states, however their electronic properties are different. A comparison of Raman phonon spectra of Pr$_2$Zr$_2$O$_7$ and Pr$_2$Ir$_2$O$_7$ allows us to identify magneto-elastic coupling in Pr$_2$Zr$_2$O$_7$ that elucidates its magnetic properties at intermediate temperatures, and allows us to characterize phonon-electron coupling in the semimetallic Pr$_2$Ir$_2$O$_7$. We also show that the effects of random disorder on the Raman phonon spectra is small.
Recently, the bi-layer Kagome lattice material Ca$_{10}$Cr$_7$O$_{28}$ has been shown to be a quasi-two-dimensional quantum spin liquid (QSL) where the frustration arises from a balance between competing ferromagnetic and antiferromagnetic exchange within a bi-layer. In an attempt to understand what happens when this balance is disturbed, we present a magnetic dilution study. Specifically, we have synthesized Ca$_{10}$(Cr$_{1-x}$V$_x$)$_7$O$_{28}$ (0 $leq$ x $leq$ 0.5) where magnetic Cr$^{5+}$ ($S = 1/2$) is partially replaced by non-magnetic V$^{5+}$ ($S = 0$). We also synthesized the fully non-magnetic isostructural material Ca$_{10}$V$_7$O$_{27.5}$. We report a detailed structural, magnetic and heat capacity study on these materials. A monotonic increase in the unit cell parameters is found for the Ca$_{10}$(Cr$_{1-x}$V$_x$)$_7$O$_{28}$ materials with increasing $x$. An order of magnitude decrease in the Curie-Weiss temperature from $4$ to $0.5$~ K is found for the partial V substituted samples, which indicates a relative increase in antiferromagnetic exchange with increase in V content. However, despite this change in the relative balance in the exchange interactions and the large disorder introduced, no magnetic ordering or spin-glass state is observed down to $2$~K in the V substituted samples. The QSL state of the parent compound thus seems surprisingly robust against these large perturbations.
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