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Register a new userBand-width control in a perovskite-type 3d^1 correlated metal Ca_1-xSr_xVO_3. II. Optical spectroscopy investigation
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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.
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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.
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 report x-ray scattering studies of broad peaks located at a (0.5 0 0)/(0 0.5 0)-type wavevector in the paramagnetic insulating phases of La_{0.7}Ca_{0.3}MnO_{3} and Pr_{0.7}Ca_{0.3}MnO_{3}. We interpret the scattering in terms of correlated polarons and measure isotropic correlation lengths of 1-2 lattice constants in both samples. Based on the wavevector and correlation lengths, the correlated polarons are found to be consistent with CE-type bipolarons. Differences in behavior between the samples arise as they are cooled through their respective transition temperatures and become ferromagnetic metallic (La_{0.7}Ca_{0.3}MnO_{3}) or charge and orbitally ordered insulating (Pr_{0.7}Ca_{0.3}MnO_{3}). Since the primary difference between the two samples is the trivalent cation size, these results illustrate the robust nature of the correlated polarons to variations in the relative strength of the electron-phonon coupling, and the sensitivity of the low-temperature ground state to such variations.
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.
Ultrafast electron delocalization induced by a fs laser pulse is a well-known process and is the initial step for important applications such as fragmentation of molecules or laser ablation in solids. It is well understood that an intense fs laser pulse can remove several electrons from an atom within its pulse duration. [1] However, the speed of electron localization out of an electron gas, the capture of an electron by ion, is unknown. Here, we demonstrate that electronic localization out of the conduction band can occur within only a few hundred femtoseconds. This ultrafast electron localization into 4f states has been directly quantified by transient x-ray absorption spectroscopy following photo-excitation of a Eu based correlated metal with a fs laser pulse. Our x-ray experiments show that the driving force for this process is either an ultrafast reduction of the energy of the 4f states, a change of their bandwidth or an increase of the hybridization between the 4f and the 3d states. The observed ultrafast electron localization process raises further basic questions for our understanding of electron correlations and their coupling to the lattice.
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