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Register a new userBand-width control in a perovskite-type 3d^1 correlated metal Ca_{1-x}Sr_xVO_3. I. Evolution of the electronic properties and effective mass
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Single crystals of the perovskite-type $3d^{1}$ metallic alloy system Ca$_{1-x}$Sr$_x$VO$_3$ were synthesized in order to investigate metallic properties near the Mott transition. The substitution of a Ca$^{2+}$ ion for a Sr$^{2+}$ ion reduces the band width $W$ due to a buckling of the V-O-V bond angle from $sim180^circ$ for SrVO$_3$ to $sim160^circ$ for CaVO$_3$. Thus, the value of $W$ can be systematically controlled without changing the number of electrons making Ca$_{1-x}$Sr$_x$VO$_3$: one of the most ideal systems for studying band-width effects. The Sommerfeld-Wilsons ratio ($simeq2$), the Kadowaki-Woods ratio (in the same region as heavy Fermion systems), and a large $T^{2}$ term in the electric resistivity, even at 300 K, substantiate a large electron correlation in this system, though the effective mass, obtained by thermodynamic and magnetic measurements, shows only a systematic but moderate increase in going from SrVO$_3$ to CaVO$_3$, in contrast to the critical enhancement expected from the Brinkmann-Rice picture. It is proposed that the metallic properties observed in this system near the Mott transition can be explained by considering the effect of a non-local electron correlation.
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Optical conductivity spectra of single crystals of Ca_1-xSr_xVO_3 have been studied to elucidate how the electronic behavior depends on the strength of the electron correlation without changing the nominal number of electrons per vanadium atom. The effective mass deduced by the analysis of the Drude-like contribution do not show critical enhancement, even though the system is close to the Mott transition. Besides the Drude-like contribution, two anomalous features were observed in the optical conductivity spectra of the intraband transition within the 3d band. These features can be assigned to transitions involving the incoherent and coherent bands near the Fermi level. The large spectral weight redistribution in this system, however, does not involve a large mass enhancement.
We investigated the electronic properties of epitaxially stabilized perovskite SrIrO3 and demonstrated the effective strain-control on its electronic structure. Comprehensive transport measurements showed that the strong spin-orbit coupling renders a novel semimetallic phase for the J_eff=1/2 electrons rather than an ordinary correlated metal, elucidating the nontrivial mechanism underlying the dimensionality-controlled metal-insulator transition in iridates. The electron-hole symmetry of this correlated semimetal was found to exhibit drastic variation when subject to bi-axial strain. Under compressive strain, substantial electron-hole asymmetry is observed in contrast to the tensile side, where the electron and hole effective masses are comparable, illustrating the susceptivity of the J_eff=1/2 to structural distortion. Tensile strain also shrinks the Fermi surface, indicative of an increasing degree of correlation which is consistent with optical measurements. These results pave a pathway to investigate and manipulate the electronic states in spin-orbit-coupled correlated oxides, and lay the foundation for constructing 5d transition metal heterostructures.
We have investigated the electronic structure of meta-stable perovskite Ca1-xSrxIrO3 (x = 0, 0.5, and 1) thin films using transport measurements, optical spectroscopy, and first-principles calculations. We artificially fabricated the perovskite phase of Ca1-xSrxIrO3, which has a hexagonal or post perovskite crystal structure in bulk form, by growing epitaxial thin films on perovskite GdScO3 substrates using epi-stabilization technique. The transport properties of the perovskite Ca1-xSrxIrO3 films systematically changed from nearly insulating (or semi-metallic) for x = 0 to bad metallic for x = 1. Due to the extended wavefunctions, 5d electrons are usually delocalized. However, the strong spin-orbit coupling in Ca1-xSrxIrO3 results in the formation of effective total angular momentum Jeff = 1/2 and 3/2 states, which puts Ca1-xSrxIrO3 in the vicinity of a metal-insulator phase boundary. As a result, the electrical properties of the Ca1-xSrxIrO3 films are found to be sensitive to x and strain.
The LDA+DMFT (local density approximation combined with dynamical mean-field theory) computation scheme has been used to study spectral and magnetic properties of FeSi and Fe$_{1-x}$Co$_{x}$Si. Having compared different models we conclude that a correlated band insulator scenario in contrast to Kondo insulator model agrees with FeSi band structure as well as experimental data. Coulomb correlation effects lead to band narrowing of the states near the Fermi level with mass renormalization parameter $m^*approx 2$ in agreement with the results of angle-resolved photoemission spectroscopy (ARPES). Temperature dependence of spectral functions and magnetic susceptibility calculated in DMFT reproduces transition from nonmagnetic semiconductor to metal with local magnetic moments observed experimentally. Cobalt doping leads to ferromagnetism that has itinerant nature and can be successfully described by LDA+DMFT method.
We measured thermal conductivity, k, thermoelectric power, S, and dc electric conductivity, sigma, of La_{5/8-x}Pr_{x}Ca_{3/8}MnO_{3}, showing an intricate interplay between metallic ferromagnetism (FM) and charge ordering (CO) instability. The change of k, S and sigma with temperature (T) and x agrees well with the effective medium theories for binary metal-insulator mixtures. This agreement clearly demonstrates that with the variation of T as well as x, the relative volumes of FM and CO phases drastically change and percolative metal-insulator transition occurs in the mixture of FM and CO domains.
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