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Anisotropic uniaxial pressure response of the Mott insulator Ca2RuO4

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 Added by Haruka Taniguchi
 Publication date 2013
  fields Physics
and research's language is English




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We have investigated the in-plane uniaxial pressure effect on the antiferromagnetic Mott insulator Ca2RuO4 from resistivity and magnetization measurements. We succeeded in inducing the ferromagnetic metallic phase at lower critical pressure than by hydrostatic pressure, indicating that the flattening distortion of the RuO6 octahedra is more easily released under in-plane uniaxial pressure. We also found a striking in-plane anisotropy in the pressure responses of various magnetic phases: Although the magnetization increases monotonically with pressure diagonal to the orthorhombic principal axes, the magnetization exhibits peculiar dependence on pressure along the in-plane orthorhombic principal axes. This peculiar dependence can be explained by a qualitative difference between the uniaxial pressure effects along the orthorhombic a and b axes, as well as by the presence of twin domain structures.

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We have performed nuclear quadrupole resonance and nuclear magnetic resonance measurements on UCoAl with strong Ising-type anisotropy under $b$- and $c$-axes uniaxial pressure. In the $b$-axis uniaxial pressure ($P_{parallel b}$) measurement, we observed an increase in the metamagnetic transition field with increasing $P_{parallel b}$. In the $c$-axis uniaxial pressure ($P_{parallel c}$) measurement, on the other hand, we observed a ferromagnetic transition in zero magnetic field along the $c$-axis above $P_{parallel c}$ = 0.08 GPa. The anomaly of the nuclear spin-lattice relaxation rate divided by the temperature $left[ (T_1 T)^{-1} right]$ at $T$ = 20 K is suppressed by $P_{parallel b}$ and slightly enhanced by $P_{parallel c}$. The anisotropic uniaxial pressure response indicates that uniaxial pressure is a good parameter for tuning the Ising magnetism in UCoAl.
We study the origin of the temperature-induced Mott transition in Ca2RuO4. As a method we use the local-density approximation+dynamical mean-field theory. We show the following. (i) The Mott transition is driven by the change in structure from long to short c-axis layered perovskite (L-Pbca to S-Pbca); it occurs together with orbital order, which follows, rather than produces, the structural transition. (ii) In the metallic L-Pbca phase the orbital polarization is ~0. (iii) In the insulating S-Pbca phase the lower energy orbital, ~xy, is full. (iv) The spin-flip and pair-hopping Coulomb terms reduce the effective masses in the metallic phase. Our results indicate that a similar scenario applies to Ca_{2-x}Sr_xRuO_4 (x<0.2). In the metallic x< 0.5 structures electrons are progressively transferred to the xz/yz bands with increasing x, however we find no orbital-selective Mott transition down to ~300 K.
The surprisingly low current densities required for inducing the insulator to metal transition has made Ca$_2$RuO$_4$ an attractive candidate material for developing novel Mott-based electronics devices. The mechanism underlying the resistive switching, however, remains to be a controversial topic in the field of correlated electron systems. Here we report a four orders of magnitude increase in the current density required for driving Ca$_2$RuO$_4$ out of the insulating state upon decreasing the crystal size. We investigate this unprecedented effect by conducting an extensive size-dependent study of electrical transport in high-purity Ca$_2$RuO$_4$ single crystals. We establish that the size dependence is not a result of Joule heating, by integrating a microscopic platinum thermometer. Our detailed study demonstrates that the universally observed transport characteristics of Ca$_2$RuO$_4$ are a result of a strongly inhomogenous current distribution in the nominally homogeneous crystal.
We studied the crystal and magnetic structure of Ca2RuO4 by different diffraction techniques under high pressure. The observed first order phase transition at moderate pressure (0.5 GPa) between the insulating phase and the metallic high pressure phase is characterized by a broad region of phase coexistence. The following structural changes are observed as function of pressure: a) a discontinuous change of both the tilt and rotation angle of the RuO6-Octahedra at this transition, b) a gradual decrease of the tilt angle in the high pressure phase (p>0.5 GPa) and c) the disappearance of the tilt above 5.5GPa leading to a higher symmetry structure. By single crystal neutron diffraction at low temperature, the ferromagnetic component of the high pressure phase and a rearrangement of antiferromagnetic order in the low pressure phase was observed.
We define, compute and analyze the nonequilibrium differential optical conductivity of the one-dimensional extended Hubbard model at half-filling after applying a pump pulse, using the time-dependent density matrix renormalization group method. The melting of the Mott insulator is accompanied by a suppression of the local magnetic moment and ensuing photogeneration of doublon-holon pairs. The differential optical conductivity reveals $(i)$ mid-gap states related to parity-forbidden optical states, and $(ii)$ strong renormalization and hybridization of the excitonic resonance and the absorption band, yielding a Fano resonance. We offer evidence and interpret such a resonance as a signature of nonequilibrium optical excitations resembling excitonic strings, (bi)excitons, and unbound doublon-holon pairs, depending on the magnitude of the intersite Coulomb repulsion. We discuss our results in the context of pump and probe spectroscopy experiments on organic Mott insulators.
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