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Register a new userRearrangement of Sodium ordering and its effect on physical properties in $Na_xCoO_2$ system
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We systematically study Raman spectroscopy of cleaved Na$_x$CoO$_2$ single crystals with 0.37 $leq$ x $leq$ 0.80. The Raman shift of A$_{1g}$ mode is found to be linearly dependent on Na content, while the Raman shift of E$_{1g}$ mode has an abnormal shift to high frequency around x = 0.5. The abnormal shift is ascribed to the occurrence of Na rearrangement in O1 structure. Temperature dependent Raman spectrum for x = 0.56 sample shows that Na rearrangement transition from O1 structure to H1 structure occurs around 240 K. Electronic transport and susceptibility for the sample with $x=0.56$ show a response to the Na rearrangement transition from O1 to H1 structure, and that different Na ordering pattern causes distinct physical properties. These results give a direct evidence to proved Na ordering effect on physical properties of Co-O plane.
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Synchrotron X-ray diffraction investigations of two single crystals of Na_xCoO_2 from different batches with composition x = 0.525-0.530 reveal homogeneous incommensurate sodium ordering with propagation vector (0.53 0.53 0) at room-temperature. The incommensurate (qq0) superstructure exists between 220 K and 430 K. The value of q varies between q = 0.514 and 0.529, showing a broad plateau at the latter value between 260 K and 360 K. On cooling, unusual reversible phase segregation into two volume fractions is observed. Below 220 K, one volume fraction shows the well-known commensurate orthorhombic x = 0.50 superstructure, while a second volume fraction with x = 0.55 exhibits another commensurate superstructure, presumably with a 6a x 6a x c hexagonal supercell. We argue that the commensurate-to-incommensurate transition is an intrinsic feature of samples with Na concentrations x = 0.5 + d with d ~ 0.03.
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We develop the cluster self-consistent field method incorporating both electronic and lattice degrees of freedom to study the origin of ferromagnetism in Cs$_{2}$AgF$_{4}$. After self-consistently determining the harmonic and anharmonic Jahn-Teller distortions, we show that the anharmonic distortion stabilizes the staggered x$^{2}$-z$^{2}$/y$^{2}$-z$^{2}$ orbital and ferromagnetic ground state, rather than the antiferromagnetic one. The amplitudes of lattice distortions, Q$_{2}$ and Q$_{3}$, the magnetic coupling strengthes, J$_{x,y}$, and the magnetic moment, are in good agreement with the experimental observation.
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