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Register a new userOptical phonons, spin correlations, and spin-phonon coupling in the frustrated pyrochlore magnets CdCr2O4 and ZnCr2O4
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We report on infrared, Raman, magnetic susceptibility, and specific heat measurements on CdCr2O4 and ZnCr2O4 single crystals. We estimate the nearest-neighbor and next-nearest neighbor exchange constants from the magnetic susceptibility and extract the spin-spin correlation functions obtained from the magnetic susceptibility and the magnetic contribution to the specific heat. By comparing with the frequency shift of the infrared optical phonons above TN , we derive estimates for the spin-phonon coupling constants in these systems. The observation of phonon modes which are both Raman and infrared active suggest the loss of inversion symmetry below the Neel temperature in CdCr2O4 in agreement with theoretical predictions by Chern and coworkers [Phys. Rev. B 74, 060405 (2006)]. In ZnCr2O4 several new modes appear below TN, but no phonon modes could be detected which are both Raman and infrared active indicating the conservation of inversion symmetry in the low temperature phase.
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We analyzed the magnetic susceptibilities of several Cr spinels using two recent models for the geometrically frustrated pyrochlore lattice, the Quantum Tetrahedral Mean Field model and a Generalized Constant Coupling model. Both models can describe the experimental data for ACr2 O4 (with A = Zn, Mg, and Cd) satisfactorily, with the former yielding a somewhat better agreement with experiment for A = Zn, Mg. The obtained exchange constants for nearest and next-nearest neighbors are discussed.
We report neutron scattering studies of the spin correlations of the geometrically frustrated pyrochlore Tb2Mo2O7 using single crystal samples. This material undergoes a spin-freezing transition below Tg~24 K, similar to Y2Mo2O7, and has little apparent chemical disorder. Diffuse elastic peaks are observed at low temperatures, indicating short-range ordering of the Tb moments in an arrangement where the Tb moments are slightly rotated from the preferred directions of the spin ice structure. In addition, a Q-independent signal is observed which likely originates from frozen, but completely uncorrelated, Tb moments. Inelastic measurements show the absence of sharp peaks due to crystal field excitations. These data show how the physics of the Tb sublattice responds to the glassy behavior of the Mo sublattice with the associated effects of lattice disorder.
Using synchrotron X-rays and neutron diffraction we disentangle spin-lattice order in highly frustrated ZnCr$_2$O$_4$ where magnetic chromium ions occupy the vertices of regular tetrahedra. Upon cooling below 12.5 K the quandary of anti-aligning spins surrounding the triangular faces of tetrahedra is resolved by establishing weak interactions on each triangle through an intricate lattice distortion. The resulting spin order is however, not simply a N{e}el state on strong bonds. A complex co-planar spin structure indicates that antisymmetric and/or further neighbor exchange interactions also play a role as ZnCr$_2$O$_4$ resolves conflicting magnetic interactions.
We report on optical transmission spectroscopy of the Cr-based frustrated triangular antiferromagnets CuCrO2 and alpha-CaCr2O4, and the spinels CdCr2O4 and ZnCr2O4 in the near-infrared to visible-light frequency range. We explore the possibility to search for spin correlations far above the magnetic ordering temperature and for anomalies in the magnon lifetime in the magnetically ordered state by probing exciton-magnon sidebands of the spin-forbidden crystal-field transitions of the Cr3+ ions (spin S = 3/2). In CuCrO2 and alpha-CaCr2O4 the appearance of fine structures below T_N is assigned to magnon sidebands by comparison with neutron scattering results. The temperature dependence of the line width of the most intense sidebands in both compounds can be described by an Arrhenius law. For CuCrO2 the sideband associated with the 4A2 -> 2T2 transition can be observed even above T_N. Its line width does not show a kink at the magnetic ordering temperature and can alternatively be described by a Z2 vortex scenario proposed previously for similar materials. The exciton-magnon features in alpha-CaCr2O4 are more complex due to the orthorhombic distortion. While for CdCr2O4 magnon sidebands are identified below T_N and one sideband excitation is found to persist across the magnetic ordering transition, only a weak fine structure related to magnetic ordering has been observed in ZnCr2O4.
Polar phonons of HgCr2S4 and CdCr2S4 are studied by far-infrared spectroscopy as a function of temperature and external magnetic field. Eigenfrequencies, damping constants, effective plasma frequencies and Lyddane-Sachs-Teller relations, and effective charges are determined. Ferromagnetic CdCr2S4 and antiferromagnetic HgCr2S4 behave rather similar. Both compounds are dominated by ferromagnetic exchange and although HgCr2S4 is an antiferromagnet, no phonon splitting can be observed at the magnetic phase transition. Temperature and magnetic field dependence of the eigenfrequencies show no anomalies indicating displacive polar soft mode behavior. However, significant effects are detected in the temperature dependence of the plasma frequencies indicating changes in the nature of the bonds and significant charge transfer. In HgCr2S4 we provide experimental evidence that the magnetic field dependence of specific polar modes reveal shifts exactly correlated with the magnetization showing significant magneto-dielectric effects even at infrared frequencies.
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