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Register a new userInfrared phonon spectrum of the tetragonal helimagnet Ba$_2$CuGe$_2$O$_7$
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The lattice dynamics of Ba$_2$CuGe$_2$O$_7$, a compound which develops Dzyaloshinsky-Moriya (DM) helical magnetism below $T_N$ = 3.2 K, has been studied by measuring the infrared reflectivity of a single crystal with the radiation polarized both in the $ab$ plane and along the $c$ axis of its tetragonal cell, from 7 K to 300 K. In this compound, where the unit cell has no inversion symmetry, fourteen $E$ phonon modes of the $ab$ plane, out of the eighteen predicted, and all the ten $B_2$ modes of the $c$ axis, have been observed. They have been assigned to the atomic motions by a comparison with shell-model calculations, which provided vibrational frequencies in good agreement with the experiment, while most calculated intensities turned to be much lower than the experimental values. This discrepancy has been tentatively explained by assuming strong electron-phonon interactions, a hypothesis supported by the failure of the $f$- sum rule if restricted to the phonon region. Indeed, we observe a remarkable increase in the oscillator strengths at $T$s low but higher than $T_N$, which suggests that the dielectric constant of Ba$_2$CuGe$_2$O$_7$ may increase at those temperatures.
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The single-site anisotropy vanishes for the spin-1/2 as a consequence of Kramers degeneracy. We argue that similar property holds for the magnetically induced electric polarization P, which should depend only on the relative orientation of spins in the bonds but not on the direction of each individual spin. Thus, for insulating multiferroic compounds, P can be decomposed in terms of pairwise isotropic, antisymmetric, and anisotropic contributions, which can be rigorously derived in the framework of the superexchange (SE) theory, in an analogy with the spin Hamiltonian. The SE theory also allows us to identify the microscopic mechanism, which stands behind each contribution. The most controversial and intriguing one is antisymmetric or spin-current mechanism. In this work, we propose that the disputed magnetoelectric (ME) properties of Ba2CuGe2O7 can be explained solely by the spin-current mechanism, while other contributions are either small or forbidden by symmetry. First we explicitly show how the cycloidal spin order induces the experimentally observed P in the direction perpendicular to the xy plane, which can be naturally explained by the spin-current mechanism operating in the out-of-plane bonds. Then, we unveil previously overlooked ME effect, where the application of the magnetic field perpendicular to the plane not only causes the incommensurate-commensurate transition, but also flips P into the plane due to the spin-current mechanism operating in the neighboring bonds within this plane. In both cases, the magnitude and direction of P can be controlled by rotating the spin pattern in the xy plane. Our analysis is based on a realistic spin model, which was rigorously derived from the first-principles calculations and supplemented with the new algorithm for the construction of localized Wannier functions obeying the crystallographic symmetry of Ba2CuGe2O7.
Neutron diffraction on a triple-axis spectrometer and a small-angle neutron scattering instrument is used to study the magnetic phase transition in tetragonal Ba$_2$CuGe$_2$O$_7$ at zero magnetic field. In addition to the incommensurate cycloidal antiferromagnetic (AFM) long-range order, we establish that weak incommensurate ferromagnetism (FM) also arises below the transition temperature $T_N$ identified by sharp Bragg peaks close to the $Gamma$ point. The intensities of both the incommensurate AFM and FM Bragg peaks vanish abruptly at $T_N$ indicative of a weak first-order transition. Above $T_N$, evidence is presented that the magnetic intensity within the tetragonal $(a,b)$ plane is distributed on a ring in momentum space whose radius is determined by the incommensurate wavevector of the cycloidal order. We speculate that the associated soft fluctuations are at the origin of the weak first-order transition in the spirit of a scenario proposed by Brazovskii.
We have investigated the microwave non-reciprocity for a non-centrosymmetric antiferromagnet Ba$_2$MnGe$_2$O$_7$. The magnon modes expected by the conventional spin wave theory for staggered antiferromagnets are certainly observed. The magnitudes of exchange interaction and magnetic anisotropy are obtained by the comparison with the theory. The microwave non-reciprocity is identified for one of these mode. The relative magnitude of microwave non-reciprocity can be explained with use of spin wave theory and Kubo formula.
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.
Terbium titanate (Tb$_2$Ti$_2$O$_7$) is a spin-ice material with remarkable magneto-optical properties. It has a high Verdet constant and is a promising substrate crystal for the epitaxy of quantum materials with the pyrochlore structure. Large single crystals with adequate quality of Tb$_2$Ti$_2$O$_7$ or any pyrochlore are not available so far. Here we report the growth of high-quality bulk crystals using the Czochralski method to pull crystals from the melt. Prior work using the automated Czochralski method has suffered from growth instabilities like diameter fluctuation, foot formation and subsequent spiraling shortly after the seeding stage. In this study, the volumes of the crystals were strongly increased to several cubic centimeters by means of manual growth control, leading to crystal diameters up to 40 mm and crystal lengths up to 10 mm. Rocking curve measurements revealed full width at half maximum values between 28 and 40 for 222 reflections. The specific heat capacity c$_p$ was measured between room temperature and 1573 K by dynamic differential scanning calorimetry and shows the typical slow parabolic rise. In contrast, the thermal conductivity kappa(T) shows a minimum near 700 K and increases at higher temperature T. Optical spectroscopy was performed at room temperature from the ultraviolet to the near infrared region, and additionally in the near infrared region up to 1623 K. The optical transmission properties and the crystal color are interpreted to be influenced by partial oxidation of Tb$^{3+}$ to Tb$^{4+}$.
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