The internal structure of the superconducting state in Sr$_2$RuO$_4$ remains elusive at present, and exhibits evidence for time-reversal symmetry breaking. Recent muon spin relaxation measurements under uniaxial strain have revealed an increasing splitting between the superconducting critical temperature $T_c$ and the onset of time-reversal symmetry breaking $T_{\rm TRSB}$ with applied strain [Grinenko et al., arXiv:2001.08152]. In addition, static magnetic order is induced by the uniaxial strain beyond $\sim$1 GPa, indicating that unstrained Sr$_2$RuO$_4$ is close to a magnetic quantum critical point. Here, we perform a theoretical study of the magnetic susceptibility and the associated pairing structure as a function of uniaxial strain. It is found that the recent muon relaxation data can be qualitatively explained from the perspective of spin-fluctuation mediated pairing and the associated strain-dependence of accidentally degenerate pair states in unstrained Sr$_2$RuO$_4$. In addition, while unstrained Sr$_2$RuO$_4$ features mainly $(2π/3,2π/3)$ magnetic fluctuations, uniaxial strain promotes $(π,\pmπ/2)$ magnetism.
There is considerable evidence that the superconducting state of Sr$_2$RuO$_4$ breaks time reversal symmetry. In the experiments showing time reversal symmetry breaking its onset temperature, $T_\text{TRSB}$, is generally found to match the critical temperature, $T_\text{c}$, within resolution. In combination with evidence for even parity, this result has led to consideration of a $d_{xz} \pm id_{yz}$ order parameter. The degeneracy of the two components of this order parameter is protected by symmetry, yielding $T_\text{TRSB} = T_\text{c}$, but it has a hard-to-explain horizontal line node at…
Muon spin rotation/relaxation ($μ$SR) and polar Kerr effect measurements provide evidence for a time-reversal symmetry breaking (TRSB) superconducting state in Sr$_2$RuO$_4$. However, the absence of a cusp in the superconducting transition temperature ($T_{\rm c}$) vs. stress and the absence of a resolvable specific heat anomaly at TRSB transition temperature ($T_{\rm TRSB}$) under uniaxial stress challenge a hypothesis of TRSB superconductivity. Recent $μ$SR studies under pressure and with disorder indicate that the splitting between $T_{\rm c}$ and $T_{\rm TRSB}$ occurs only when the structu…
Uniaxial strain experiments have become a powerful tool to unveil the character of unconventional phases of electronic matter. Here we propose a combination of the superconducting fitness analysis and density functional theory (DFT) calculations in order to dissect the effects of strain in complex multi-orbital quantum materials from a microscopic perspective. We apply this framework to the superconducting state of Sr$_2$RuO$_4$, and argue that the recently proposed orbitally anti-symmetric spin-triplet (OAST) order parameter candidate has unique signatures under strain which are in agreement …
In the light of the recently discussed mechanism for suppression of superconductivity in multi-orbital systems called inter-orbital effect, here we extend our analysis of the upper critical field in Sr$_2$RuO$_4$ now under strain. We show that the presence of the standard orbital effect and the new mechanism can consistently account for the qualitative changes observed in the upper critical field for the strained system, in particular, combining the overall enhancement of the critical field with the reduction in the anisotropy. The proposed picture holds for a triplet superconducting state, sh…
Sr$_2$RuO$_4$ is a leading candidate for chiral $p$-wave superconductivity. The detailed mechanism of superconductivity in this material is still the subject of intense investigations. Since superconductivity is sensitive to the topology of the Fermi surface (the contour of zero-energy quasi-particle excitations in the momentum space in the normal state), changing this topology can provide a strong test of theory. Recent experiments tuned the Fermi surface topology efficiently by applying planar anisotropic strain. Using functional renormalization group theory, we study the superconductivity a…
Strontium ruthenate (Sr$_2$RuO$_4$) is a multiband superconductor that displays evidence of topological superconductivity, although a model of the order parameter that is consistent with all experiments remains elusive. We integrated a piezoelectric-based strain apparatus with a scanning superconducting quantum interference device (SQUID) microscope to map the diamagnetic response of single-crystal Sr$_2$RuO$_4$ as a function of temperature, uniaxial pressure, and position with micron-scale spatial resolution. We thereby obtained local measurements of the superconducting transition temperature…
The search for broken time reversal symmetry (TRSB) in unconventional superconductors intensified in the past year as more systems have been predicted to possess such a state. Following our pioneering study of TRSB states in Sr$_2$RuO$_4$ using magneto-optic probes, we embarked on a systematic study of several other of these candidate systems. The primary instrument for our studies is the Sagnac magneto-optic interferometer, which we recently developed. This instrument can measure magneto-optic Faraday or Kerr effects with an unprecedented sensitivity of 10 nanoradians at temperatures as low a…
It has been shown [1] that many seemingly contradictory experimental findings concerning the superconducting state in Sr$_2$RuO$_4$ can be accounted for as resulting from the existence of an assumed tetra-critical point at near ambient pressure at which $d_{x^2-y^2}$ and $g_{xy(x^2-y^2)}$ superconducting states are degenerate. We perform both a Landau-Ginzburg and a microscopic mean-field analysis of the effect of spatially varying strain on such a state. In the presence of finite $xy$ shear strain, the superconducting state consists of two possible symmetry-related time-reversal symmetry (TRS…
Motivated by recent measurements of strain effects on the transition temperature (T$_c$) of Sr$_2$RuO$_4$, we study the strain response of a two-dimensional chiral p-wave supercoductor. We focus on the effects of inhomgeneous strain fields, which are always present in any such experiment, and which have been neglected in previous theoretical treatments. We show that the response of T$_c$ of a chiral superconductor to strain chages from being linear without inhomogeneity, to quadratic in the presence of inhomogeneity. We discuss our results in the context of the ongoing debate of superconductiv…
We report a combined experimental and theoretical study of the dependence of the superconductivity of the unconventional superconductor Sr$_2$RuO$_4$ on anisotropic strain. Novel piezoelectric apparatus is used to apply uniaxial pressures of up to $\sim$1~GPa along a $\langle 100 \rangle$ direction ($a$-axis) of the crystal lattice. $T_c$ increases from 1.5~K in unstrained material to 3.4~K at compression by $\approx$0.6\%, then falls steeply. The $c$-axis upper critical field for the strained $T_c$ = 3.4~K material is a factor of twenty larger than that of the unstrained crystal, whereas the …
Shortly after the discovery of superconductivity in Sr$_2$RuO$_4$, spin-triplet pairing was proposed and further corroborated by a constant Knight shift ($K$) across the transition temperature (T$_c$). However, a recent experiment observed a drop in $K$ at T$_c$ which becomes larger under uniaxial strain, ruling out several spin-triplet scenarios. Here we show that inter-orbital spin-triplet pairing features a d-vector that rotates when uniaxial strain is applied, leading to a larger drop in the spin polarization perpendicular to the strain direction, distinct from spin-singlet pairing. We pro…
The binary ruthenate, RuO$_2$, has been the subject of intense interest due to its itinerant antiferromagnetism and strain-induced superconductivity. The strain mechanism and its effect on the microscopic electronic states leading to the normal and superconducting state, however, remain undisclosed. Here, we investigate highly-strained epitaxial (110) RuO$_2$ films using polarization-dependent oxygen K-edge X-ray absorption spectroscopy (XAS). Through the detection of pre-edge peaks, arising from O:$2p$ - Ru:$4d$ hybridization, we uncover the effects of epitaxial strain on the orbital/electron…
We show that the observed time-reversal symmetry breaking (TRSB) of the superconducting state in $\mathrm{Sr}_{2}\mathrm{Ru}\mathrm{O}_{4}$ can be understood as originating from inhomogeneous strain fields near edge dislocations of the crystal. Specifically, we argue that, without strain inhomogeneities, $\mathrm{Sr}_{2}\mathrm{Ru}\mathrm{O}_{4}$ is a single-component, time-reversal symmetric superconductor, likely with $d_{x^{2}-y^{2}}$ symmetry. However, due to the strong strain inhomogeneities generated by dislocations, a slowly-decaying sub-leading pairing state contributes to the condensa…
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…
In its ground state, RuO2 was long thought to be an ordinary metallic paramagnet. Recent neutron and x-ray diffraction revealed that bulk RuO2 is an antiferromagnet (AFM) with TN above 300 K. Furthermore, epitaxial strain induces novel superconductivity in thin films of RuO2 below 2 K. Here, we present a resonant elastic x-ray scattering (REXS) study at the Ru L2 edge of the strained RuO2 films exhibiting the strain-induced superconductivity. We observe an azimuthal modulation of the 100 Bragg peak consistent with canted AFM found in bulk. Most notably, in the strained films displaying novel s…
In-plane uniaxial pressure has been shown to strongly tune the superconducting state of Sr2RuO4 by approaching a Lifshitz transition and associated Van Hove singularity (VHS) in the density of states. At the VHS, $T_c$ and the in- and out-of-plane upper critical fields are all strongly enhanced, and the latter has changed its curvature as a function of temperature from convex to concave. However, due to strain inhomogeneity it has not been possible so far to determine how the upper critical fields change with strain. Here, we show the strain dependence of both upper critical fields, which was …
The superconducting state in the quasi-two-dimensional and strongly correlated Sr$_2$RuO$_4$ is uniquely held up as a solid state analog to superfluid $^3$He-$A$, with an odd-parity order parameter that also breaks time reversal symmetry, and for which the vector order parameter has the same direction in spin space for all electron momenta. The recent discovery that uniaxial pressure causes a steep rise and maximum in transition temperature ($T_c$) in strained samples motivated the study of $^{17}$O nuclear magnetic resonance (NMR) that we describe in this article. A reduction of Knight shifts…
We analyze the spin anisotropy of the magnetic susceptibility of Sr$_2$RuO$4$ in presence of spin-orbit coupling and anisotropic strain using quasi-two-dimensional tight-binding parametrization fitted to the ARPES results. Similar to the previous observations we find the in-plane polarization of the low ${\bf q}$ magnetic fluctuations and the out-of-plane polarization of the incommensurate magnetic fluctuation at the nesting wave vector ${\bf Q}_1 = (2/3 π,2/3 π)$ but also nearly isotropic fluctuations near ${\bf Q}_2=(π/6,π/6)$. Furthermore, one finds that apart from the high-symmetry directi…
Due to the presence of a nontrivial three-dimensional spin-orbital entanglement, Sr$_2$RuO$_4$ may be a time-reversal invariant nematic $p$-wave superconductor with coexisting in-plane and out-of-plane pairings. Here we discuss various signatures of such a state if the out-of-plane pairing component is dominant. First, the enhancement of the superconducting $T_c$ under in-plane uniaxial strains is nearly a quadratic function of the strain, because the out-of-plane pairing lacks a linear-order coupling to the strain. Second, when the strain applies along a certain in-plane direction, the nemati…
SrRuO$_3$ (SRO113) is an important material for device physics particularly as one of the best metallic oxide electrodes for ferroelectric devices. This oxide has moderate electron correlations with novel properties including ferromagnetic ordering, which can be utilized in future to spintronics and superconducting spintronics devices. Recently, we observed strongly enhanced magnetization of SRO113 thin films grown on single crystals of the spin-triplet superconductor Sr$_2$RuO$_4$ (SRO214). To clarify the origin of such an enhancement, we conducted systematic investigations of magnetic proper…
Pressure represents a clean tuning parameter for traversing the complex phase diagrams of interacting electron systems and as such has proved of key importance in the study of quantum materials. Application of controlled uniaxial pressure has recently been shown to more than double the transition temperature of the unconventional superconductor Sr$_{2}$RuO$_{4}$ for example, leading to a pronounced peak in $T_\mathrm{c}$ vs. strain whose origin is still under active debate. Here, we develop a simple and compact method to apply large uniaxial pressures passively in restricted sample environment…
The superconducting pairing in Sr$_2$RuO$_4$ is widely considered to be chiral $p$-wave with $\vec{d}_{\boldsymbol k} \sim (k_x + ik_y)\hat{z}$, which belongs to the $E_u$ representation of the crystalline $D_{4h}$ group. However, this superconducting order appears hard to reconcile with a number of key experiments. In this paper, based on symmetry analysis we discuss the possibility of odd-parity pairing with inherent three-dimensional (3D) character enforced by the inter-orbital interlayer coupling and the sizable spin-orbit coupling (SOC) in the material. We focus on a yet unexplored $E_u$ …
Single crystals of the Sr$_2$RuO$_4$-Ru eutectic system are known to exhibit enhanced superconductivity at 3~K, in addition to the bulk superconductivity of Sr$_2$RuO$_4$ at 1.5~K. The 1.5-K phase is believed to be a spin-triplet, chiral $p$-wave state with the multi-component order parameter, giving rise to chiral domain structure. In contrast, the 3-K phase is attributable to enhanced superconductivity of Sr$_2$RuO$_4$ in the strained interface region between Ru inclusion of a few to tens of micrometers in size and the surrounding Sr$_2$RuO$_4$. We investigate the dynamic behavior of a topol…
The exact nature of unconventional superconductivity in Sr$_2$RuO$_4$ remains a mystery. At the phenomenological level, no superconducting order parameter proposed thus far seems able to coherently account for all essential experimental signatures. Among the latter is the prominent polar Kerr effect, which implies a nonzero ac anomalous Hall conductivity. Assuming the Kerr effect is intrinsic, it can be accounted for by a bulk chiral Cooper pairing with nonzero orbital angular momentum, such as $p+ip$ or $d+id$, which, however, has difficulties in being reconciled with other experimental resul…
Recent experiments suggest that the superconducting order parameter of Sr$_2$RuO$_4$ has two components. A two-component order parameter has multiple degrees of freedom in the superconducting state that can result in low-energy collective modes or the formation of domain walls -- a possibility that would explain a number of experimental observations including the smallness of the time reversal symmetry breaking signal at T$_\mathrm{c}$ and telegraph noise in critical current experiments. We perform ultrasound attenuation measurements across the superconducting transition of Sr$_2$RuO$_4$ using…
We report the evolution of the electronic structure at the surface of the layered perovskite Sr$_2$RuO$_4$ under large in-plane uniaxial compression, leading to anisotropic $B_{1g}$ strains of ${\varepsilon_{xx}-\varepsilon_{yy}=-0.9\pm0.1\%}$. From angle-resolved photoemission, we show how this drives a sequence of Lifshitz transitions, reshaping the low-energy electronic structure and the rich spectrum of van Hove singularities that the surface layer of Sr$_2$RuO$_4$ hosts. From comparison to tight-binding modelling, we find that the strain is accommodated predominantly by bond-length change…
For a tetragonal material, order parameters of $p_x$ and $p_y$ symmetry are related by rotation and hence have the same $T_{\rm c}$ at a mean-field level. This degeneracy can be lifted by a symmetry-breaking field, like (uniaxial) in-plane strain, such that at $T_{\rm c}$, the order parameter is only of $p_x$ or $p_y$ symmetry. Only at a lower temperature also the respective other order parameter condenses to form a chiral $p$-wave state. At the mean-field level, the derivative of $T_{\rm c}$ with strain is discontinuous at zero strain. We analyze consequences of (thermal) fluctuations on the …
Here we demonstrate how the Fermi surface topology and quantum many-body interactions can be manipulated via epitaxial strain in the spin-triplet superconductor Sr$_2$RuO$_4$ and its isoelectronic counterpart Ba$_2$RuO$_4$ using oxide molecular beam epitaxy (MBE), \emph{in situ} angle-resolved photoemission spectroscopy (ARPES), and transport measurements. Near the topological transition of the $γ$ Fermi surface sheet, we observe clear signatures of critical fluctuations, while the quasiparticle mass enhancement is found to increase rapidly and monotonically with increasing Ru-O bond distance.…
The effects of uniaxial compressive stress on the normal state $^{17}$O nuclear magnetic resonance properties of the unconventional superconductor Sr$_{2}$RuO$_{4}$ are reported. The paramagnetic shifts of both planar and apical oxygen sites show pronounced anomalies near the nominal $\mathbf{a}$-axis strain $\varepsilon_{aa}\equiv\varepsilon_v$, that maximizes the superconducting transition temperature, $T_{c}$. The spin susceptibility weakly increases on lowering the temperature below $T$$\simeq$10 K, consistent with an enhanced density of states associated with passing the Fermi energy thro…
Recently, rutile RuO$_2$ has raised interest for its itinerant antiferromagnetism, crystal Hall effect, and strain-induced superconductivity. Understanding and manipulating these properties demands resolving the electronic structure and the relative roles of the rutile crystal field and $4d$ spin-orbit coupling (SOC). Here, we use O-K and Ru $M_3$ x-ray absorption (XAS) and Ru $M_3$ resonant inelastic x-ray scattering (RIXS) to disentangle the contributions of crystal field, SOC, and electronic correlations in RuO$_2$. The locally orthorhombic site symmetry of the Ru ions introduces significan…
We propose to realize second-order topological superconductivity in bilayer spin-polarized Fermi gas superfluids. We focus on systems with intralayer chiral $p$-wave pairing and with tunable interlayer hopping and interlayer interactions. Under appropriate circumstances, an interlayer even-parity $s$- or $d$-wave pairing may coexist with the intralayer $p$-wave. Our model supports localized Majorana zero modes not only at the corners of the system geometry, but also at the terminations of certain one-dimensional defects, such as lattice line defects and superfluid domain walls. We show how suc…
Standard superconductors display a ubiquitous discontinuous jump in the electronic specific heat at the critical superconducting transition temperature. In a growing class of unconventional superconductors, however, a second order parameter component may get stabilized and produce a second heat capacity jump at a lower temperature, typically associated with the spontaneous breaking of time-reversal symmetry. The splitting of the two specific heat discontinuities can be controlled by external perturbations such as chemical substitution, hydrostatic pressure, or uniaxial strain. We develop a the…
Superconductivity is among the most fascinating and well-studied quantum states of matter. Despite over 100 years of research, a detailed understanding of how features of the normal-state electronic structure determine superconducting properties has remained elusive. For instance, the ability to deterministically enhance the superconducting transition temperature by design, rather than by serendipity, has been a long sought-after goal in condensed matter physics and materials science, but achieving this objective may require new tools, techniques and approaches. Here, we report the first insta…
Entropy mapping under uniaxial pressure utilizing the elastocaloric effect
Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Scottish Universities Physics Alliance, School of Physics and Astronomy, University of St Andrews（圣安德鲁斯大学物理与天文学学院苏格兰大学物理联盟）；Department of Physics, National Taiwan University（台湾大学物理学系）；National Institute for Materials Science（国立材料研究所）
