The anomalous charge transport observed in some strongly correlated metals raises questions as to the universal applicability of Landau Fermi liquid theory. The coherence temperature $T_{FL}$ for normal metals is usually taken to be the temperature below which $T^2$ is observed in the resistivity. Below this temperature, a Fermi liquid with well-defined quasiparticles is expected. However, metallic ruthenates in the Ruddlesden-Popper family, frequently show non-Drude low-energy optical conductivity and unusual $ω/T$ scaling, despite the frequent observation of $T^2$ dc resistivity. Herein we report time-domain THz spectroscopy measurements of several different high-quality metallic ruthenate thin films and show that the optical conductivity can be interpreted in more conventional terms. In all materials, the conductivity has a two-Drude peak lineshape at low temperature and a crossover to a one-Drude peak lineshape at higher temperatures. The two-component low-temperature conductivity is indicative of two well-separated current relaxation rates for different conduction channels. We discuss three particular possibilities for the separation of rates: (a) Strongly energy-dependent inelastic scattering; (b) an almost-conserved pseudomomentum operator that overlaps with the current, giving rise to the narrower Drude peak; (c) the presence of multiple conduction channels that undergoes a crossover to stronger interband scattering at higher temperatures. None of these scenarios require the existence of exotic quasiparticles. The results may give insight into the possible significance of Hund's coupling in determining interband coupling in these materials. Our results also show a route towards understanding the violation of Matthiessen's rule in this class of materials and deviations from the "Gurzhi" scaling relations in Fermi liquids.
We have measured the change in the resistivity of thin films of ${\rm SrRuO_3}$ and ${\rm CaRuO_3}$ upon introducing point defects by electron irradiation at low temperatures, and we find significant deviations from Matthiessen's rule. For a fixed irradiation dose, the induced change in resistivity {\it decreases} with increasing temperature. Moreover, for a fixed temperature, the increase in resistivity with irradiation is found to be {\it sublinear}. We suggest that the observed behavior is due to the marked anisotropic scattering of the electrons together with their relatively short mean fr…
A comparative density functional plus dynamical mean field theory study of the pseudocubic ruthenate materials CaRuO$_3$ and SrRuO$_3$ is presented. Phase diagrams are determined for both materials as a function of Hubbard repulsion $U$ and Hund's rule coupling $J$. Metallic and insulating phases are found, as are ferromagnetic and paramagnetic states. The locations of the relevant phase boundaries are determined. Based on the computed phase diagrams, Mott-dominated and Hund's dominated regimes of strong correlation are distinguished. Comparison of calculated properties to experiments indicate…
We investigated the electronic structures of the bandwidth-controlled ruthenates, Y$_{2}$Ru$_{2}$O$_{7}$, CaRuO$_{3}$, SrRuO$_{3}$, and Bi$_{2}$Ru$% _{2}$O$_{7}$, by optical conductivity analysis in a wide energy region of 5 meV $\sim $ 12 eV. We could assign optical transitions from the systematic changes of the spectra and by comparison with the O 1$s$ x-ray absorption data. We estimated some physical parameters, such as the on-site Coulomb repulsion energy and the crystal-field splitting energy. These parameters show that the 4$d$ orbitals should be more extended than 3$d$ ones. These resul…
We investigate the temperature evolution of the electronic states in the vicinity of the Fermi level of a non-Fermi liquid (NFL) system, CaRuO3 using ultra high-resolution photoemission spectroscopy; isostructural SrRuO3 exhibiting Fermi liquid behavior despite similar electron interaction parameters as that of CaRuO3, is used as a reference. High-energy resolution in this study helps to reveal particle-hole asymmetry in the excitation spectra of CaRuO3 in contrast to that in SrRuO3. In addition, we observe signature of phonon excitations in the photoemission spectra of CaRuO3 at finite temper…
We investigate the role of long range ferromagnetic order in the electronic structure of Sr$_{1-x}$Ca$_x$RuO$_3$ using high resolution photoemission spectroscopy. SrRuO$_3$ is a ferromagnetic metal but isostructural, isoelectronic CaRuO$_3$ is an enhanced paramagnet. Surface spectra of CaRuO$_3$ exhibit temperature induced modifications. This is not significant in other compositions. This may be attributed to the structural changes observed in previous studies. Interestingly, the bulk spectra reveal unusual spectral changes exhibiting large decrease in the coherent feature intensity correspond…
Optical conductivity spectra $σ_1(ω)$ of paramagnetic CaRuO$_3$ are investigated at various temperatures. At T=10 K, it shows a non-Fermi liquid behavior of $σ_1(ω)\sim 1/ω^{\frac 12}$, similar to the case of a ferromagnet SrRuO$_3$. As the temperature ($T$) is increased, on the other hand, $σ_1(ω)$ in the low frequency region is progressively suppressed, deviating from the $1/ω^{\frac 12%}$-dependence. Interestingly, the suppression of $σ_1(ω)$ is found to scale with $ω/T$ at all temperatures. The origin of the $% ω/T$ scaling behavior coupled with the non-Fermi liquid behavior is discussed.
We report calorimetric, magnetic and electric transport properties of single-crystal CaRuO3 and SrRuO3 as a function of temperature T and applied magnetic field B. We find that CaRuO3 is a non-Fermi-liquid metal near a magnetic instability, as characterized by the following properties: (1) the heat capacity C(T,B) ~ -T log T is readily enhanced in low applied fields, and exhibits a Schottky peak at 2.3 K that exhibits field dependence when T is reduced; (2) the magnetic susceptibility diverges as T^-x at low temperatures with 1/2 < x < 1, depending on the applied field; and (3) the electrical …
Hartree-Fock calculations are presented of a theoretical model describing the Sr/CaRuO$_4$ family of compounds. Both commensurate and incommensurate magnetic states are considered, along with orbital ordering and the effect of lattice distortions. For reasonable parameter values, interactions disfavor orbital disproportionation. A coherent description of the observed phase diagram is obtained.
Srn+1RunO3n+1 represents a class of layered materials whose physical properties are a strong function of the number of Ru-O layers per unit cell, n. This series includes the p-wave superconductor Sr2RuO4 (n=1), enhanced paramagnetic Sr3Ru2O7 (n=2), nearly ferromagnetic Sr4Ru3O10 (n=3) and itinerant ferromagnetic SrRuO3 (n=infinity). In spite of a wide spectrum of physical phenomena, this series of materials along with paramagnetic CaRuO3 shares two major characteristics, namely, robust Fermi liquid behavior at low temperatures and anomalous transport behavior featured by linear temperature dep…
Using quasiparticle self-consistent $GW$ calculations, we re-examined the electronic structure of Sr$_2$RuO$_4$ and SrRuO$_3$. Our calculations show that the correlation effects beyond the conventional LDA (local density approximation) and GGA (generalized gradient approximation) are reasonably well captured by QS$GW$ self-energy without any {\it ad hoc} parameter or any ambiguity related to the double-counting and the downfolding issues. While the spectral weight transfer to the lower and upper Hubbard band is not observed, the noticeable bandwidth reduction and effective mass enhancement are…
We show that a ferromagnetic (FM) order in the orthorhombic CaRuO3, which is a non-magnetic and iso-structural analog of FM system SrRuO3, can be established and stabilized by the means of tensile epitaxial strain. Investigations on the structural and magnetic property correlations in the CaRuO3 films with different degrees of strain reveal that the FM moment increases with increasing the tensile strain. This is an experimental verification to the theoretical predictions of scaling of the tensile epitaxial strain and the magnetic order in this system. Our studies further establish that the ten…
There is intense controversy around the unconventional superconductivity in strontium ruthenate, where the various theoretical and experimental studies suggest diverse and mutually exclusive pairing symmetries. Currently, the investigation is solely focused on only one material, Sr2RuO4, and the field suffers from the lack of comparison targets. Here, employing a density functional theory based analysis, we show that the heterostructure composed of SrRuO3 and SrTiO3 is endowed with all the key characteristics of Sr2RuO4, and, in principle, can host superconductivity. Furthermore, we show that …
The magnetic properties of (Ca,Sr)RuO_3 and Sr_2YRuO_6 are studied within the context of band structure based Stoner theory. LSDA calculations without recourse to strong correlation effects yield the correct magnetic behavior and order in all cases. Insulating character of Sr_2YRuO_6 is reproduced. The different magnetic states of SrRuO_3 and CaRuO_3 are shown to be due to the different structural distortions. CaRuO_3 is found to be on the verge of a ferromagnetic instability. O p states hybridize strongly with Ru d states in all three compounds, and O, through this hybridization plays an unus…
The electronic structure of SrRuO$_3$ thin film with thickness from 50 to 1 unit cell (u.c.) is investigated via the resonant inelastic x-ray scattering (RIXS) technique at the O K-edge to unravel the intriguing interplay of orbital and charge degrees of freedom. We found that orbital-selective quantum confinement effect (QCE) induces the splitting of Ru $4d$ orbitals. At the same time, we observed a clear suppression of the electron-hole continuum across the metal-to-insulator transition (MIT) occurring at the 4 u.c. sample. From these two clear observations we conclude that QCE gives rise to…
Magnetic excitations in \srruo ~ have been studied by inelastic neutron scattering. The magnetic fluctuations are dominated by incommensurate peaks related to the Fermi surface nesting of the quasi-one-dimensional $d_{xz}$- and $d_{yz}$-bands. The shape of the incommensurate signal agrees well with RPA calculations. At the incommensurate {\bf Q}-positions the energy spectrum considerably softens upon cooling pointing to a close magnetic instability : \srruo ~does not exhibit quantum criticality but is very close to it. $ω/ T$-scaling may be fitted to the data for temperatures above 30 K. Below…
The ferromagnetic quantum phase transition in the perovskite ruthenate Sr$_{1-x}$Ca$_x$RuO$_3$ is studied by low-temperature magnetization and electrical resistivity measurements on thin films. The films were grown epitaxially on SrTiO$_3$ substrates using metalorganic aerosol deposition and characterized by X-ray diffraction and room temperature scanning tunneling microscopy. High residual resistivity ratios of 29 and 16 for $x=0$ and $x=1$, respectively, prove the high quality of the investigated samples. We observe a continuous suppression of the ferromagnetic Curie temperature from $T_C=16…
Lattice structure can dictate electronic and magnetic properties of a material. Especially, reconstruction at a surface or heterointerface can create properties that are fundamentally different from those of the corresponding bulk material. We have investigated the lattice structure on the surface and in the thin films of epitaxial SrRuO3 with the film thickness up to 22 pseudo-cubic unit cells (u.c.), using the combination of surface sensitive low energy electron diffraction and bulk sensitive scanning transmission electron microscopy. Our analysis indicates that, in contrast to many perovski…
We present a systematical theoretical study on the transport properties of an archetypal family of Hund's metals, Sr$_2$RuO$_4$,Sr$_3$Ru$_2$O$_7$, SrRuO$_3$ and CaRuO$_3$, within the combination of first principles density functional theory and dynamical mean field theory. The agreement between theory and experiments for optical conductivity and resistivity is good, which indicates that electron-electron scattering dominates the transport of ruthenates. We demonstrate that in the single-site dynamical mean field approach the transport properties of Hund's metals fall into the scenario of "resi…
We investigate the optical conductivity of Sr$_{1-x}$Ca$_x$RuO$_3$ across the ferromagnetic to paramagnetic transition that occurs at $x=0.8$. The thin films were grown by metalorganic aerosol deposition with $0 \leq x \leq 1$ onto NdGaO$_3$ substrates. We performed THz frequency domain spectroscopy in a frequency range from 3~cm$^{-1}$ to 40~cm$^{-1}$ (100~GHz to 1.4~THz) and at temperatures ranging from 5~K to 300~K, measuring transmittivity and phase shift through the films. From this we obtained real and imaginary parts of the optical conductivity. The end-members, ferromagnetic SrRuO$_3$ …
A series of epitaxial films were grown across the solid solution Ca(x)Sr(1-x)RuO(3) in order to pinpoint the ferromagnetic to paramagnetic quantum phase transition in this system and to study the evolution of transport and magnetic properties in its vicinity. The ferromagnetic Tc of SrRuO(3) was found to decrease linearly with Ca doping levels up to 70%. Further doping resulted in the abrupt elimination of ferromagnetic order, and the onset of low temperature (< 10K) non-Fermi liquid (NFL) resistivity of the form rho ~ rho(0 + AT^(1.5) for samples with x <= 0.75 <= 1.0. The resistivity exponen…
Atomically thin ferromagnetic and conducting electron systems are highly desired for spintronics, because they can be controlled with both magnetic and electric fields. We present (SrRuO3)1-(SrTiO3)5 superlattices and single-unit-cell-thick SrRuO3 samples that are capped with SrTiO3. We achieve samples of exceptional quality. In these samples, the electron systems comprise only a single RuO2 plane. We observe conductivity down to 50 mK, a ferromagnetic state with a Curie temperature of 25 K, and signals of magnetism persisting up to approximately 100 K.
In oxide heterostructures, different materials are integrated into a single artificial crystal, resulting in a breaking of inversion-symmetry across the heterointerfaces. A notable example is the interface between polar and non-polar materials, where valence discontinuities lead to otherwise inaccessible charge and spin states. This approach paved the way to the discovery of numerous unconventional properties absent in the bulk constituents. However, control of the geometric structure of the electronic wavefunctions in correlated oxides remains an open challenge. Here, we create heterostructur…
