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D. A. Sokolov

Publications and source records attributed to D. A. Sokolov.

At least 19 recordsLinked to original sources

Non-Fermi liquid quasiparticles in strain-tuned Sr2RuO4

Interacting electrons can form metallic states beyond the Fermi liquid paradigm, a conceptual frontier of many-body physics mainly explored via bulk thermodynamics and transport. In contrast, the microscopics of anomalous single-particle excitations underlying non-Fermi liquid properties have largely remained in the dark. Here we spectroscopically map such quantum-critical excitations in Sr$_2$RuO$_4$ under uniaxial pressure, an experimental challenge overcome by technical advances combining focused ion beam micro-milling with laser angle resolved photoemission. We show that quasiparticle excitations acquire a non-Fermi liquid scattering rate near the critical point but remain remarkably robust throughout the transition. These experiments serve as a benchmark for the theory of anomalous metals and settle the long-standing question if quantum-critical systems host quasiparticle excitations.

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Evidence for vertical line nodes in Sr$_2$RuO$_4$ from nonlocal electrodynamics

By determining the superconducting lower and upper critical fields $H_\mathrm{c1}(T)$ and $H_\mathrm{c2}(T)$, respectively, in a high-purity spherical Sr$_2$RuO$_4$ sample via ac-susceptibility measurements, we obtain the temperature dependence of the coherence length $ξ$ and the penetration depth $λ$ down to 0.04$T_c$. Given the high sample quality, the observed $T^2$ dependence of $λ$ at low temperatures cannot be explained in terms of impurity effects. Instead, we argue that the weak type-II superconductor Sr$_2$RuO$_4$ has to be treated in the non-local limit. In that limit, the penetration depth data agree with a gap structure having vertical line nodes, while horizontal line nodes cannot account for the observation.

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The fate of quasiparticles at high-temperature

We study the temperature evolution of quasiparticles in the correlated metal Sr$_2$RuO$_4$. Our angle resolved photoemission data show that quasiparticles persist up to temperatures above 200~K, far beyond the Fermi liquid regime. Extracting the quasiparticle self-energy we demonstrate that the quasiparticle residue $Z$ increases with increasing temperature. Quasiparticles eventually disappear on approaching the bad metal state of Sr$_2$RuO$_4$ not by losing weight but via excessive broadening from super-Planckian scattering. We further show that the Fermi surface of Sr$_2$RuO$_4$ - defined as the loci where the spectral function peaks - deflates with increasing temperature. These findings are in semi-quantitative agreement with dynamical mean field theory calculations.

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Spin-density-wave order controlled by uniaxial stress in CeAuSb$_2$

The tetragonal heavy-fermion compound CeAuSb$_2$ (space group $P4/nmm$) exhibits incommensurate spin density wave (SDW) order below $T_{N}\approx6.5~K$ with the propagation vector $\mathbf{q}_A = (δ_A,δ_A,1/2)$. The application of uniaxial stress along the [010] direction induces a sudden change in the resistivity ratio $ρ_a/ρ_b$ at a compressive strain of $ε\approx -0.5$\%. Here we use neutron scattering to show that the uniaxial stress induces a first-order transition to a SDW state with a different propagation vector $(0,δ_B,1/2)$ with $δ_B=0.25$. The magnetic structure of the new (B) phase consists of Ce layers with ordered moments alternating with layers with zero moment stacked along the $c$-axis. The ordered layers have an up-up-down-down configuration along the $b$-axis. This is an unusual situation in which the loss of spatial inversion is driven by the magnetic order. We argue that the change in SDW wavevector leads to Fermi surface reconstruction and a concomitant change in the transport properties.

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In-plane magnetic penetration depth in Sr$_2$RuO$_4$: muon-spin rotation/relaxation study

We report on measurements of the in-plane magnetic penetration depth ($λ_{\rm ab}$) in single crystals of Sr$_2$RuO$_4$ down to $\simeq 0.015$ K by means of muon-spin rotation/relaxation. The linear temperature dependence of $λ^{-2}_{\rm ab}$ for $T\lesssim 0.7$ K suggests the presence of nodes in the superconducting gap. This statement is further substantiated by observation of the Volovik effect, $i.e.$ the reduction of $λ_{ab}^{-2}$ as a function of the applied magnetic field. The experimental zero-field and zero-temperature value of $λ_{\rm ab}=124(3)$ nm agrees with $λ_{\rm ab}\simeq 130$ nm, calculated based on results of electronic structure measurements reported in [Phys. Rev X 9, 021048 (2019)]. Our analysis reveals that a simple nodal superconducting energy gap, described by the lowest possible harmonic of a gap function, does not capture the dependence of $λ_{\rm ab}^{-2}$ on $T$, so the higher angular harmonics of the energy gap function need to be introduced.

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A spatially resolved optical method to measure thermal diffusivity

We describe an optical method to directly measure position-dependent thermal diffusivity of reflective single crystal samples across a broad range of temperatures for condensed matter physics research. Two laser beams are used, one as a source to locally modulate the sample temperature, and the other as a probe of sample reflectivity, which is a function of the modulated temperature. Thermal diffusivity is obtained from the phase delay between source and probe signals. We combine this technique with a microscope setup in an optical cryostat, in which the sample is placed on a 3-axis piezo-stage, allowing for spatially resolved measurements. Furthermore, we demonstrate experimentally and mathematically that isotropic in-plane diffusivity can be obtained when overlapping the two laser beams instead of separating them in the traditional way, which further enhances the spatial resolution to a micron scale, especially valuable when studying inhomogeneous or multidomain samples. We discuss in detail the experimental conditions under which this technique is valuable, and demonstrate its performance on two stoichiometric bilayer ruthenates: Sr3Ru2O7 and Ca3Ru2O7. The spatial resolution allowed us to study the diffusivity in single domains of the latter, and we uncovered a temperature-dependent in-plane diffusivity anisotropy. Finally, we used the enhanced spatial resolution enabled by overlapping the two beams to measure temperature-dependent diffusivity of Ti-doped Ca3Ru2O7, which exhibits a metal-insulator transition. We observed large variations of transition temperature over the same sample, originating from doping inhomogeneity, and pointing to the power of spatially resolved techniques in accessing inherent properties.

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Magnetic field-induced softening of spin waves and hard-axis order in Kondo-lattice ferromagnet CeAgSb$_{2}$

A significant number of Kondo-lattice ferromagnets order perpendicular to the easy magnetization axis dictated by the crystalline electric field. The nature of this phenomenon has attracted considerable attention, but remains poorly understood. In the present paper we use inelastic neutron scattering supported by magnetization and specific heat measurements to study the spin dynamics in the hard-axis ferromagnet CeAgSb2. In the zero field state we observed two sharp magnon modes, which are associated with Ce ordering and extended up to $\approx 3 meV with a considerable spin gap of 0.6 meV. Application of a magnetic field perpendicular to the moment direction reduces the spectral intensity and suppresses the gap and significantly enhances the low-temperature specific heat at a critical field of Bc ~ 2.8 T via a mean-field-like transition. Above the transition, in the field polarized state, the gap eventually reopens due to the Zeeman effect. We modeled the observed dispersion using linear spin-wave theory (LSWT) taking into account the ground state Gamma 6 doublet and exchange anisotropy. Our model correctly captures the essential features of the spin dynamics including magnetic dispersion, distribution of the spectral intensity as well as the field-induced behavior, although several minor features remain obscure. The observed spectra do not show significant broadening due to the finite lifetime of the quasiparticles. Along with a moderate electronic specific heat coefficient gamma = 46 mJ/mol K2 this indicates that the Kondo coupling is relatively weak and the Ce moments are well localized. Altogether, our results provide profound insight into the spin dynamics of the hard-axis ferromagnet CeAgSb2 and can be used as solid ground for studying magnetic interactions in isostructural compounds including CeAuSb2, which exhibits nematicity and unusual mesoscale magnetic textures.

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The planar triangular $S=3/2$ magnet AgCrSe$_2$: magnetic frustration, short range correlations, and field tuned anisotropic cycloidal magnetic order

Our studies evidence an anisotropic magnetic order below $T_N = 32$~K. Susceptibility data in small fields of about 1~T reveal an antiferromagnetic (AFM) order for $H \perp c$, whereas for $H \parallel c$ the data are reminiscent of a field-induced ferromagnetic (FM) structure. At low temperatures and for $H \perp c$, the field-dependent magnetization and AC susceptibility data evidence a metamagnetic transition at $H^+ = 5$~T, which is absent for $H \parallel c$. We assign this to a transition from a planar cycloidal spin structure at low fields to a planar fan-like arrangement above $H^+$. A fully FM polarized state is obtained above the saturation field of $H_{\perp S} = 23.7$~T at 2~K with a magnetization of $M_s = 2.8$~$μ_{\rm B}{\rm /Cr}$. For $H \parallel c$, $M(H)$ monotonously increases and saturates at the same $M_s$ value at $H_{\parallel S} = 25.1$~T at 4.2~K. Above $T_N $, the magnetic susceptibility and specific heat indicate signatures of two dimensional (2D) frustration related to the presence of planar ferromagnetic and antiferromagnetic exchange interactions. We found a pronounced nearly isotropic maximum in both properties at about $T^* = 45$~K, which is a clear fingerprint of short-range correlations and emergent spin fluctuations. Calculations based on a planar 2D Heisenberg model support our experimental findings and suggest a predominant FM exchange among nearest and AFM exchange among third-nearest neighbors. Only a minor contribution might be assigned to the antisymmetric Dzyaloshinskii-Moriya interaction possible related to the non-centrosymmetric polar space group $R3m$. Due to these competing interactions, the magnetism in AgCrSe$_{2}$, in contrast to the oxygen based delafossites, can be tuned by relatively small, experimentally accessible, magnetic fields, allowing us to establish the complete anisotropic magnetic $H-T$ phase diagram in detail.

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Scale-Invariance of a Spin Liquid in High Magnetic Fields

In RuCl$_3$, inelastic neutron scattering and Raman spectroscopy reveal a continuum of non-spin-wave excitations that persists to high temperature, suggesting the presence of a spin liquid state on a honeycomb lattice. In the context of the Kitaev model, magnetic fields introduce finite interactions between the elementary excitations, and thus the effects of high magnetic fields - comparable to the spin exchange energy scale - must be explored. Here we report measurements of the magnetotropic coefficient - the second derivative of the free energy with respect to magnetic field orientation - over a wide range of magnetic fields and temperatures. We find that magnetic field and temperature compete to determine the magnetic response in a way that is independent of the large intrinsic exchange interaction energy. This emergent scale-invariant magnetic anisotropy provides evidence for a high degree of exchange frustration that favors the formation of a spin liquid state in RuCl$_3$.

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Scale-invariant magnetic anisotropy in RuCl$_3$ at high magnetic fields

In RuCl$_3$, inelastic neutron scattering and Raman spectroscopy reveal a continuum of non-spin-wave excitations that persists to high temperature, suggesting the presence of a spin liquid state on a honeycomb lattice. In the context of the Kitaev model, magnetic fields introduce finite interactions between the elementary excitations, and thus the effects of high magnetic fields - comparable to the spin exchange energy scale - must be explored. Here we report measurements of the magnetotropic coefficient - the second derivative of the free energy with respect to magnetic field orientation - over a wide range of magnetic fields and temperatures. We find that magnetic field and temperature compete to determine the magnetic response in a way that is independent of the large intrinsic exchange interaction energy. This emergent scale-invariant magnetic anisotropy provides evidence for a high degree of exchange frustration that favors the formation of a spin liquid state in RuCl$_3$.

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High sensitivity heat capacity measurements on Sr2RuO4 under uniaxial pressure

A key question regarding the unconventional superconductivity of Sr$_2$RuO$_4$ remains whether the order parameter is single- or two-component. Under a hypothesis of two-component superconductivity, uniaxial pressure is expected to lift their degeneracy, resulting in a split transition. The most direct and fundamental probe of a split transition is heat capacity. Here, we report development of new high-frequency methodology for measurement of heat capacity of samples subject to large and highly homogeneous uniaxial pressure. We place an upper limit on the heat capacity signature of any second transition of a few per cent of the primary superconducting transition. The normalized jump in heat capacity, $ΔC/C$, grows smoothly as a function of uniaxial pressure, but we find no qualitative evidence of a pressure-induced order parameter transition. Thanks to the high precision of our measurements, these findings place stringent constraints on theories of the superconductivity of Sr$_2$RuO$_4$.

cond-mat.supr-con↗

Electronically driven spin-reorientation transition of the correlated polar metal Ca$_3$Ru$_2$O$_7$

Polar distortions in solids give rise to the well-known functionality of switchable macroscopic polarisation in ferroelectrics and, when combined with strong spin-orbit coupling, can mediate giant spin splittings of electronic states. While typically found in insulators, ferroelectric-like distortions can remain robust against increasing itineracy, giving rise to so-called "polar metals". Here, we investigate the temperature-dependent electronic structure of Ca$_3$Ru$_2$O$_7$, a correlated oxide metal in which octahedral tilts and rotations combine to mediate pronounced polar distortions. Our angle-resolved photoemission measurements reveal the destruction of a large hole-like Fermi surface upon cooling through a coupled structural and spin-reorientation transition at 48 K, accompanied by a sudden onset of quasiparticle coherence. We demonstrate how these result from band hybridisation mediated by a hidden Rashba-type spin-orbit coupling. This is enabled by the bulk structural distortions and unlocked when the spin reorients perpendicular to the local symmetry-breaking potential at the Ru sites. We argue that the electronic energy gain associated with the band hybridisation is actually the key driver for the phase transition, reflecting a delicate interplay between spin-orbit coupling and strong electronic correlations, and revealing a new route to control magnetic ordering in solids.

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Metamagnetic texture in a polar antiferromagnet

The notion of a simple ordered state implies homogeneity. If the order is established by a broken symmetry, elementary Landau theory of phase transitions shows that only one symmetry mode describes this state. Precisely at points of phase coexistence domain states formed of large regions of different phases can be stabilized by long range interactions. In uniaxial antiferromagnets the so-called metamagnetism is an example of such a behavior, when an antiferromagnetic and field-induced spin-polarized paramagnetic/ferromagnetic state co-exist at a jump-like transition in the magnetic phase diagram. Here, combining experiment with theoretical analysis, we show that a different type of mixed state between antiferromagnetism and ferromagnetism can be created in certain acentric materials. In the small-angle neutron scattering experiments we observe a field-driven spin-state in the layered antiferromagnet Ca3Ru2O7, which is modulated on a scale between 8 and 20 nm and has both antiferromagnetic and ferromagnetic parts. We call this state a metamagnetic texture and explain its appearance by the chiral twisting effects of the asymmetric Dzyaloshinskii-Moriya (DM) exchange. The observation can be understood as an extraordinary coexistence, in one thermodynamic state, of spin orders belonging to different symmetries. Experimentally, the complex nature of this metamagnetic state is demonstrated by measurements of anomalies in electronic transport which reflect the spin-polarization in the metamagnetic texture, determination of the magnetic orbital moments, which supports the existence of strong spin-orbit effects, a pre-requisite for the mechanism of twisted magnetic states in this material.

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Normal state $^{17}$O NMR studies of Sr$_{2}$RuO$_{4}$ under uniaxial stress

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 through a van Hove singularity. Although such a Lifshitz transition occurs in the $γ$ band, formed by the Ru $d_{xy}$ states hybridized with in-plane O $p_π$ orbitals, the large Hund's coupling renormalizes the uniform spin susceptibilty, which, in turn, affects the hyperfine fields of all nuclei. We estimate this \textquotedblleft Stoner\textquotedblright\ renormalization, $S,$ by combining the data with first-principles calculations and conclude that this is an important part of the strain effect, with implications for superconductivity.

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Pronounced drop of $^{17}$O NMR Knight shift in superconducting state of Sr$_2$RuO$_4$

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 $K$ was observed for all strain values and temperatures $T<T_c$, consistent with a drop in spin polarization in the superconducting state. In unstrained samples, our results are in contradiction with a body of previous NMR work, and with the most prominent previous proposals for the order parameter of Sr$_2$RuO$_4$. Possible alternative scenarios are discussed.

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Direct Observation of a Uniaxial Stress-driven Lifshitz Transition in Sr$_{2}$RuO$_{4}$

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 environments, and utilize this to study the evolution of the electronic structure of Sr$_{2}$RuO$_{4}$ using angle-resolved photoemission. We directly visualize how uniaxial stress drives a Lifshitz transition of the $γ$-band Fermi surface, pointing to the key role of strain-tuning its associated van Hove singularity to the Fermi level in mediating the peak in $T_\mathrm{c}$. Our measurements provide stringent constraints for theoretical models of the strain-tuned electronic structure evolution of Sr$_{2}$RuO$_{4}$. More generally, our novel experimental approach opens the door to future studies of strain-tuned phase transitions not only using photoemission, but also other experimental techniques where large pressure cells or piezoelectric-based devices may be difficult to implement.

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Ferromagnetic ordering along the hard axis in the Kondo lattice YbIr3Ge7

Ferromagnetic Kondo lattice compounds are far less common than their antiferromagnetic analogs. In this work, we report the discovery of a new ferromagnetic Kondo lattice compound, YbIr3Ge7. Like almost all ferromagnetic Kondo lattice systems, YbIr3Ge7 shows magnetic order with moments aligned orthogonal to the crystal electric field (CEF) easy axis. YbIr3Ge7 is unique in that it is the only member of this class of compounds that crystallizes in a rhombohedral structure with a trigonal point symmetry of the magnetic site, and it lacks broken inversion symmetry at the local moment site. AC magnetic susceptibility, magnetization, and specific heat measurements show that YbIr3Ge7 has a Kondo temperature TK = 14 K and a Curie temperature TC = 2.4 K. Ferromagnetic order occurs along the crystallographic [100] hard CEF axis despite the large CEF anisotropy of the ground state Kramers doublet with a saturation moment along [001] almost four times larger than the one along [100]. This implies that a mechanism which considers the anisotropy in the exchange interaction to explain the hard axis ordering is unlikely. On the other hand, the broad second-order phase transition at TC favors a fluctuation-induced mechanism.

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Improved Single-Crystal Growth of Sr$_2$RuO$_4$

High-quality single crystals are essentially needed for the investigation of the novel bulk properties of unconventional superconductors. The availability of such crystals grown by the floating-zone method has helped to unveil the unconventional superconductivity of the layered perovskite Sr$_2$RuO$_4$, which is considered as a strong candidate of a topological spin-triplet superconductor. Yet, recent progress of investigations urges further efforts to obtain ultimately high-quality crystalline samples. In this paper, we focus on the method of preparation of feed rods for the floating-zone melting and report on the improvements of the crystal growth. We present details of the improved methods used to obtain crystals with superconducting transition temperatures $T_\mathrm{c}$ that are consistently as high as 1.4 K, as well as the properties of these crystals.

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