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 $T_C=160$ K at $x=0$ towards $T_C\to 0$ at $x_c\approx 0.8$. The analysis of the electrical resistivity between 2 and 10 K reveals $T^2$ and $T^{3/2}$ behavior at $x\leq 0.6$ and $x\geq 0.7$, respectively. For undoped CaRuO$_3$, the measurement has been extended down to 60 mK, revealing a crossover to $T^2$ behavior around 2 K, which suggests a Fermi-liquid ground state in this system.
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…
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…
We report the synthesis of Ca$_2$RuO$_4$ thin films on NdCaAlO$_{4}$ (110), LaAlO$_3$ (100) and LaSrAlO$_4$ (001) substrates and show that epitaxial strain induces a transition from the Mott-insulating phase of bulk Ca$_2$RuO$_4$ into a metallic phase. Magnetometry and spin-polarized neutron reflectometry reveal a low-temperature, small-moment ferromagnetic state in metallic Ca$_2$RuO$_4$ films.
We show that the pressure-temperature phase diagram of the Mott insulator Ca$_{2}$RuO$_{4}$ features a metal-insulator transition at 0.5GPa: at 300K from paramagnetic insulator to paramagnetic quasi-two-dimensional metal; at $T \leq$ 12K from antiferromagnetic insulator to ferromagnetic, highly anisotropic, three-dimensional metal. % We compare the metallic state to that of the structurally related p-wave superconductor Sr$_{2}$RuO$_{4}$, and discuss the importance of structural distortions, which are expected to couple strongly to pressure.
We studied the magnetic ordering of thin films and bulk crystals of rutile RuO$_2$ using resonant X-ray scattering across the Ru L$_2$ absorption edge. Combining polarization analysis and azimuthal-angle dependence of the magnetic Bragg signal, we have established the presence of G-type antiferromagnetism in RuO$_2$ with T$_N$ $>$ 300 K. In addition to revealing a spin-ordered ground state in the simplest ruthenium oxide compound, the persistence of magnetic order even in nanometer-thick films lays the ground for potential applications of RuO$_2$ in antiferromagnetic spintronics.
The microscopic origin of triplet superconductivity in Sr$_2$RuO$_4$ is discussed, paying attention to the role of Coulomb interaction, $U_{pp}$, at the O site. It is shown on the $d$-$p$ model that $U_{pp}$ induces a ferromagnetic exchange interaction between "d-electrons" (molecular orbital with $d_{xy}$-symmetry) at adjacent Ru sites, leading to short-range ferromagnetic correlations and promoting Cooper pairing with ($\sin p_x\pm\ii\sin p_y$)-symmetry on the $γ$-band. The reason why such ferromagnetic correlations work effectively may be traced back to the fact that the level of 4d-electro…
Strain engineering vanadium dioxide thin films is one way to alter this material's characteristic first order transition from semiconductor to metal. In this study we extend the exploitable strain regime by utilizing the very large lattice mismatch of 8.78 % occurring in the VO$_2$/RuO$_2$ system along the c axis of the rutile structure. We have grown VO$_2$ thin films on single domain RuO$_2$ islands of two distinct surface orientations by atomic oxygen-supported reactive MBE. These films were examined by spatially resolved photoelectron and x-ray absorption spectroscopy, confirming the corre…
By inelastic neutron scattering, we have analyzed the magnetic correlations in the paramagnetic metallic region of the series Ca(2-x)Sr(x)RuO(4), 0.2<=x<=0.62. We find different contributions that correspond to 2D ferromagnetic fluctuations and to fluctuations at incommensurate wave vectors (0.11,0,0), (0.26,0,0) and (0.3,0.3,0). These components constitute the measured response as function of the Sr-concentration x, of the magnetic field and of the temperature. A generic model is applicable to metallic Ca(2-x)Sr(x)RuO(4) close to the Mott transition, in spite of their strongly varying physica…
We measure the Shubnikov-de Haas effect in thin-film Sr$_2$RuO$_4$ grown on an (LaAlO$_3$)$_{0.29}$-(SrAl$_{1/2}$Ta$_{1/2}$O$_3$)$_{0.71}$ (LSAT) substrate. We detect all three known Fermi surfaces and extract the Fermi surface volumes, cyclotron effective masses, and quantum lifetimes. We show that the electronic structure is nearly identical to that of single-crystal Sr$_2$RuO$_4$, and that the quasiparticle lifetime is consistent with the Tc of comparably clean, single-crystal Sr$_2$RuO$_4$. Unlike single-crystal Sr$_2$RuO$_4$, where the quantum and transport lifetimes are roughly equal, we…
The synthesis of stoichiometric Sr$_2$RuO$_4$ thin films has been a challenge because of the high volatility of ruthenium oxide precursors, which gives rise to ruthenium vacancies in the films. Ru vacancies greatly affect the transport properties and electronic phase behavior of Sr$_2$RuO$_4$, but their direct detection is difficult due to their atomic dimensions and low concentration. We applied polarized X-ray absorption spectroscopy at the oxygen K-edge and confocal Raman spectroscopy to Sr$_2$RuO$_4$ thin films synthesized under different conditions. The results show that these methods can…
Motivated by the success of experimental manipulation of the band structure through biaxial strain in Sr$_2$RuO$_4$ thin film grown on a mismatched substrate, we investigate theoretically the effects of biaxial strain on the electronic instabilities, such as superconductivity (SC) and spin density wave (SDW), by functional renormalization group. According to the experiment, the positive strain (from lattice expansion) causes charge transfer to the $γ$-band and consequently Lifshitz reconstruction of the Fermi surface. Our theoretical calculations show that within a limited range of positive st…
Observation of mirror-odd and mirror-even spin texture in ultrathin epitaxially strained RuO2 films
University of Minnesota-Twin Cities（明尼苏达大学双城分校）；Kyung Hee University（庆熙大学）；Rice University（莱斯大学）；Paul Scherrer Institute（保罗谢勒研究所）；Gwangju Institute of Science and Technology (GIST)（光州科学技术院）
The layered perovskite Sr$_2$RuO$_4$ is a most intensively studied superconductor, but its pairing mechanism, which is often coupled intimately with magnetic fluctuations in correlated materials, is still an open question. Here we present a systematic evolution of the Seebeck coefficient in Co- and Mn-substituted Sr$_2$RuO$_4$ single crystals, in which ferromagnetic and antiferromagnetic glassy states respectively emerge in proximity to the superconducting phase of the parent compound. We find that the Seebeck coefficient $S$ divided by temperature $T$, $S/T$, shows a maximum near characterist…
We investigated the optical properties of (Ca,Sr)RuO_3 films on the borderline of a metal-insulator (M-I) transition. Our results show all of the predicted characteristics for a metallic Mott-Hubbard system, including (i) a mass enhancement in dc-limit, (ii) an U/2 excitation, and (iii) an U excitation. Also, a self-consistency is found within the Gutzwiller-Brinkman-Rice picture for the Mott transition. Our finding displays that electron correlation should be important even in 4d materials.
We demonstrate that the cluster-glass state emerges as ferromagnetic quantum criticality is avoided in itinerant ferromagnet Sr1-x(La0.5K0.5)xRuO3. In this compound, the ferromagnetic order is suppressed by increasing x, and then disappears at the critical concentration: x=0.5. In this x range, the present study reveals that no prominent feature is ascribed to the quantum critical fluctuations in specific heat. Instead, ac magnetic susceptibility exhibits a broad peak due to spontaneous spin freezing, and the peak temperature depends significantly on the frequency of the applied ac magnetic fi…
We present a general methodology that enables the disentanglement of the electronic and lattice contributions to the metal-insulator transition by building an energy landscape from numerical solutions of the equation of state. The methodology works with any electronic structure method that provides electronic expectation values at given atomic positions. Applying the theory to rare-earth perovskite nickelates ($R$NiO$_3$) and Ruddlesden-Popper calcium ruthenates (Ca$_2$RuO$_4$) in bulk, heterostructure and epitaxially strained thin film forms using equation of state results from density functi…
The alloy Ca$_{2-x}$Sr$_x$RuO$_4$ exhibits a complex phase diagram with peculiar magnetic metallic phases. In this paper some aspects of this alloy are discussed based on a mean field theory for an effective Kugel-Khomskii model of localized orbital and spin degrees of freedom. This model results from an orbital selective Mott transition which in the three-band system localized two orbitals while leaving the third one itinerant. Special attention is given to the region around a structure quantum phase transition at $ x \approx 0.5 $ where the crystal lattice changes from tetragonal to orthorho…
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$_3$ …
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 r…
Layered perovskite ruthenium oxides exhibit a striking series of metal-insulator and magnetic-nonmagnetic phase transitions easily tuned by temperature, pressure, epitaxy, and nonlinear drive. In this work, we combine results from two complementary state of the art many-body methods, Auxiliary Field Quantum Monte Carlo and Dynamical Mean Field Theory, to determine the low-temperature phase diagram of Ca$_2$RuO$_4$. Both methods predict a low temperature, pressure-driven metal-insulator transition accompanied by a ferromagnetic-antiferromagnetic transition. The properties of the ferromagnetic s…
We develop a procedure for calculating the magnetic properties of a ferromagnetic Heisenberg film with single-ion anisotropy which is valid for arbitrary spin and film thickness. Applied to sc(100) and fcc(100) films with spin S=7/2 the theory yields the layer dependent magnetizations and Curie temperatures of films of various thicknesses making it possible to investigate magnetic properties of films at the interesting 2D-3D transition.
There have been two different proposals for the spin-triplet order parameter of the superconducting phase in Sr$_2$RuO$_4$; an $f$-wave order parameter and the multigap model where some of the bands have the line node. In an effort to propose an experiment that can distinguish two cases, we study the behavior of the supercurrent and compute the critical current for these order parameters when the sample is a thin film with the thickness $d \ll ξ$ where $ξ$ is the coherence length. It is found that the supercurrent behaves very differently in two models. This will serve as a sharp test for the …
The anomalous Hall effect (AHE) of ferromagnetic thin films of Sr$_{1-x}$Ca$_{x}$RuO$_3$ (0 $\leq x \leq$ 0.4) is studied as a function of $x$ and temperature $T$. As $x$ increases, both the transition temperature $T_c$ and the magnetization $M$ are reduced and vanish near $x \sim$ 0.7. For all compositions, the transverse resistivity $ρ_{H}$ varies non-monotonously with $T$, and even changes sign, thus violating the conventional expression $ρ_{H}=R_o B + 4πR_s M(T)$ ($B$ is the magnetic induction, while $R_o$ and $R_s$ are the ordinary and anomalous Hall coefficients). From the rather complic…
We present magnetoresistance (MR) measurements performed on magnetic tunnel junctions in which one of the electrodes is a granular ferromagnetic film. These junctions exhibit a zero field resistance dip. The dip magnitude depends on the size of the grains. We interpret these results as a consequence of the orange peel effect between the continuous ferromagnetic film and the magnetic grains. The coupling is found to be much stronger than that between continuous ferromagnetic layers.
We studied the ferromagnetic topology in a Y$_{0.67}$Ca$_{0.33}$MnO$_3$ thin film with a combination of magnetic force microscopy and magnetization measurements. Our results show that the spin-glass like behavior, reported previously for this system, could be attributed to frustrated interfaces of the ferromagnetic clusters embedded in a non-ferromagnetic matrix. We found temperature dependent changes of the magnetic topology at low temperatures, which suggests a non-static Mn$^{3+}$/Mn$^{4+}$ ratio.
Bulk magnetization in Pr_{0.6}Ca_{0.4}MnO_3 thin films with tensile (SrTiO_3) and compressive (LaAlO_3) substrate-induced strain is compared to the magnetooptical Kerr effect (MOKE) measurements. In the absence of an external magnetic field, in both films, a stable ferromagnetic insulating majority phase coexists with an antiferromagnetic insulating phase below ~120K. MOKE measurements indicate that at 5K a metastable ferromagnetic metallic (FM) phase is formed at the surface of the stretched film in a magnetic field below 1.1T already, while in the bulk the FM phase starts to form in the fiel…
Experimental efforts to stabilize ferromagnetism in ultrathin films of transition metal oxides have so far failed, despite expectations based on density functional theory (DFT) and DFT+U. Here, we investigate one of the most promising materials, SrRuO$_3$, and include correlation effects beyond DFT by means of dynamical mean field theory. In agreement with experiment we find an intrinsic thickness limitation for metallic ferromagnetism in SrRuO$_3$ thin films. Indeed, we demonstrate that the realization of ultrathin ferromagnetic films is out of reach of standard thin-film techniques. Proposin…
Spin currents have been shown to play a key role in the ultrafast laser-driven demagnetization process in ferromagnetic thin films. Here, we show that an oscillating spin current can be generated in the film via the application of a femtosecond laser pulse in the visible range. In particular, we prove that the spin current is due to ballistic electrons traveling back and forth in the film. The dependence of the current intensity on the driving electric field is also investigated.
The authors investigated the structure and properties of GdBaCo$_{2}$O$_{5.5+δ}$ thin films epitaxially grown on SrTiO$_{3}$ (001) single crystal substrates. The thin films were found to have a notable remnant magnetization above room temperature, which is much higher than that observed in bulk material. Transmission electron microscopy and x-ray diffraction patterns reveal that phase separation occurs in these films, and the phase responsible for the enhanced ferromagnetic order is $a$-oriented. The enhanced ferromagnetic order is attributed to the enhanced orbital order of Co$^{3+}$ in CoO$_…
Ferromagnetic-paramagnetic phase transitions in classical and quantum thin films have been studied up to 50 mono-layers using effective field theory with two-site cluster approximation. Variation of the Curie temperature as a function of film thickness has been examined. The relative shift of the Curie temperature from the corresponding bulk value has been investigated in terms of the shift exponent $λ$. We have found that shift exponent $λ$ clearly depends on the strength of the ferromagnetic exchange coupling of the surface. Moreover, we have not observed any significant difference between c…
In this paper we have created a strain driven single crystal like ferromagnetic insulating (FMI) state in a PLD grown thin film of low doped LCMO(X = 0.15)on NGO(100) substrate and make a thorough study of strain effects on the electric and magnetic transport of this film. We have studied and compared the FMI state, ferromagnetic transition temperature (TC), ferromagnetic insulating temperature (TFMI) and the resistivity of the film in details with bulk single crystals of X=0.18 to 0.22 doping region. We have found that TFMI and the localisation length of the carriers are increased and there i…
Ferromagnetic SrRuO3 thin films are deposited on the ab-surface of single crystals of the spin-triplet superconductor Sr2RuO4 as substrates using pulsed laser deposition. The films are under a severe in-plane compressive strain. Nevertheless, the films exhibit ferromagnetic order with the easy axis along the c-direction below the Curie temperature of 158 K. The electrical transport reveals that the SrRuO3/Sr2RuO4 interface is highly conducting, in contrast with the interface between other normal-metals and the ab-surface of Sr2RuO4. Our results will stimulate the investigations on proximity ef…
