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D. Pelc

Publications and source records attributed to D. Pelc.

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Dynamic nanoscale structural correlations in strontium ruthenate

Strontium ruthenate (Sr$_2$RuO$_4$, SRO) has been the subject of intense research as a model quasi-two-dimensional metal with strong electronic correlations and potential exotic multi-component superconductor. Yet the nature of the superconducting state and its emergence remain debated, despite highly detailed knowledge of the normal-state electronic properties. Here we use diffuse neutron and x-ray scattering to uncover self-organized structural fluctuations on the picosecond timescale in SRO. We show that these nanoscale correlations do not originate from extrinsic disorder but rather involve cooperative displacements of oxygen atoms in the quintessential RuO$_2$ planes. Moreover, the observed displacement pattern is consistent with distortions due to incipient orbital order that we obtain in first-principles calculations, which suggests that orbital effects could play a pivotal role in the physics of SRO. Similar dynamic correlations may play a role in the physical properties of a wide range of prominent oxides with closely-related lamellar structures, such as the cuprates and nickelates.

cond-mat.str-el

Spin-chiral electron-phonon coupling in metallic strontium titanate

Electron-phonon coupling (EPC) - the interaction between conduction electrons and quantized atomic vibrations - plays a central role in condensed matter physics and determines some of the most important properties of materials, such as electrical resistivity and superconductivity. Conventionally, EPC is assumed to be induced by the ionic electrostatic background, and electronic spin plays no role in the process. In stark contrast with this view, here we uncover a direct spin-mediated coupling mechanism between electrons and transverse polar phonons in a metal. Using far-infrared light absorption measurements of the model system SrTiO$_3$ in a magnetic field, we observe a strong spin-mediated EPC that is quantitatively consistent with recent theoretical predictions, and that generates chiral phonon modes with large effective magnetic moments. The extracted coupling strength is in good agreement with ab initio estimates and sufficiently high to explain superconductivity in SrTiO$_3$, thereby resolving a long-standing conundrum. Spin-chiral EPC should generically appear in all metals with polar phonons, and the present work could be of relevance to spintronics applications and to uncovering the origins of superconductivity in layered materials, metals with Dirac points in their electronic dispersions, and nearly ferroelectric superconductors.

cond-mat.str-el

Evidence for rare-region physics in the structural and electronic degrees of freedom of the nickelate La$_{2-x}$Sr$_x$NiO$_4$

We present a diffuse neutron and x-ray scattering study of structural as well as spin- and charge-density-wave fluctuations in the electrical insulator La$_{2-x}$Sr$_x$NiO$_4$. This lamellar nickelate is an isostructural analogue of the high-temperature cuprate superconductor La$_{2-x}$Sr$_x$CuO$_4$, for which recent experiments uncovered evidence for unusual structural and superconducting fluctuations indicative of rare-region physics due to inherent inhomogeneity unrelated to common point disorder effects. We find closely analogous nanoscale orthorhombic fluctuation behavior in La$_{2-x}$Sr$_x$NiO$_4$, including exponential scaling of the diffuse scattering intensity and power-law scaling of the characteristic length with relative temperature. Moreover, our neutron and x-ray scattering data reveal similar behavior for short-range magnetic and charge fluctuations above the respective ordering temperatures. These observations indicate that rare-region effects are a generic feature of perovskite-related structures and lead to universal fluctuations of both structural and electronic degrees of freedom over extended temperature ranges.

cond-mat.str-el

Uniaxial strain tuning of polar lattice vibrations in KTaO$_3$ and SrTiO$_3$

The interplay of electronic and structural degrees of freedom is a prominent feature of many quantum materials and of particular interest in systems with strong ferroelectric fluctuations, such as SrTiO$_3$ (STO) and KTaO$_3$ (KTO). Both materials are close to a ferroelectric transition, but despite six decades of extensive research, pivotal questions regarding the nature of this transition and of the associated fluctuations remain debated. Here we combine inelastic neutron scattering, Raman spectroscopy, and ab initio calculations to study the evolution of soft polar phonons across the strain-induced ferroelectric transition in STO and KTO. We find that the modes remain underdamped and at nonzero energy, consistent with a first-order quantum phase transition. We also reveal a strong violation of the well-known Lyddane-Sachs-Teller relation between the phonon energies and static dielectric permittivities in insulating KTO and STO, which is not captured by ab initio calculations and points to the presence of slow mesoscale fluctuations induced by long-range interactions. In metallic STO, we uncover a first-order transition at a remarkably low critical stress, in qualitative agreement with recent theoretical predictions. The present work resolves several long-standing questions pertaining to the model systems STO and KTO and is relevant to numerous other materials with soft polar phonons.

cond-mat.mtrl-sci

Pervasive symmetry-lowering nanoscale structural fluctuations in the cuprate La$_{2-x}$Sr$_{x}$CuO$_{4}$

The cuprate superconductors are among the most widely studied quantum materials, yet there remain fundamental open questions regarding their electronic properties and the role of the structural degrees of freedom. Recent neutron and x-ray scattering measurements uncovered exponential scaling with temperature of the strength of orthorhombic fluctuations in the tetragonal phase of $La_{2-x}Sr_xCuO_4$ and $Tl_2Ba_2CuO_{6+y}$, unusual behavior that closely resembles prior results for the emergence of superconducting fluctuations, and that points to a common origin rooted in inherent correlated structural inhomogeneity. Here we extend the measurements of $La_{2-x}Sr_xCuO_4$ to higher temperatures in the parent compound (x=0) and to optimal doping (x=0.155), and we furthermore investigate the effects of in-situ in-plane uniaxial stress. Our neutron scattering result for undoped $La_2CuO_4$ complement prior x-ray data and reveal that the structural fluctuations persist to the maximum experimental temperature of nearly 1000K, i.e., to a significant fraction of the melting point. At this temperature, the spatial correlation length extracted from the momentum-space data is still about three lattice constants. The neutron scattering experiment enables quasistatic discrimination and reveals that the response is increasingly dynamic at higher temperatures. We also find that uniaxial stress up to 500 MPa along the tetragonal [110] direction, which corresponds to a strain of about 0.2%, does not significantly alter this robust behavior. Overall, these results support the notion that subtle, underlying inhomogeneity underpins the cuprate phase diagram. Finally, we uncover (for x=0.2) low-energy structural fluctuations at a nominally forbidden reflection. While the origin of these fluctuations is not clear, they might be related to the presence of extended defects such as dislocations or stacking faults.

cond-mat.supr-con

Continuous-wave cryogenic optical absorption spectrometer for sub-THz frequencies

We present the design of a continuous-wave, highly sensitive optical spectrometer for millimeter-wave frequencies between 50 and 1000 GHz. The spectrometer uses photomixing of near-infrared light to generate radiation in a wide frequency range, and the absorbed optical power is determined directly through measurements of the sample temperature. This enables relative sensitivities of up to $10^6$ for the sample absorption coefficient below liquid-helium temperatures, suitable for measurements on highly reflective samples. The instrument is also compatible with high magnetic fields. In order to validate its performance, we measure the ferromagnetic resonance in the Mott insulator YTiO$_3$, the electron spin resonance in a standard free-radical reference compound, and the antiferromagnetic resonance in a van der Waals magnetic material.

physics.ins-det

Electronic spin susceptibility in metallic strontium titanate

Metallic strontium titanate (SrTiO$_3$) is known to have both normal-state and superconducting properties that vary strongly over a wide range of charge carrier densities. This indicates the importance of nonlinear dynamics, and has hindered the development of a clear qualitative description of the observed behaviour. A major challenge is to understand how the charge carriers themselves evolve with doping and temperature, with possible polaronic effects and evidence of an effective mass that strongly increases with temperature. Here we use $^{47,49}$Ti nuclear magnetic resonance (NMR) to perform a comprehensive study of the electronic spin susceptibility in the dilute metallic state of strontium titanate across the doping-temperature phase diagram. We find a temperature-dependent Knight shift that can be quantitatively understood within a non-degenerate Fermi gas model that fully takes into account the complex band structure of SrTiO$_3$. Our data are consistent with a temperature-independent effective mass, and we show that the behavior of the spin susceptibility is universal in a wide range of temperatures and carrier concentrations. These results provide a microscopic foundation for the understanding of the properties of the unconventional low-density metallic state in strontium titanate and related materials.

cond-mat.str-el

Local inversion-symmetry breaking in a bismuthate high-$T_c$ superconductor

The doped perovskite BaBiO$_3$ exhibits a maximum superconducting transition temperature ($T_c$) of 34 K and was the first high-$T_c$ oxide to be discovered, yet pivotal questions regarding the nature of both the metallic and superconducting states remain unresolved. Although it is generally thought that superconductivity in the bismuthates is of the conventional s-wave type, the pairing mechanism is still debated, with strong electron-phonon coupling and bismuth valence or bond disproportionation possibly playing a role. Here we use diffuse x-ray scattering and Monte Carlo modeling to study the local structure of Ba$_{1-x}$K$_x$BiO$_3$ across its insulator-metal boundary. We find no evidence for either long- or short-range disproportionation, which resolves a major conundrum, as disproportionation and the related polaronic effects are likely not relevant for the metallic and superconducting states. Instead, we uncover nanoscale structural correlations that break inversion symmetry, which has far-reaching implications for the electronic physics, including the pairing mechanism. This unexpected finding furthermore establishes that the bismuthates belong to the broader classes of materials with hidden spin-orbit coupling and a tendency towards inversion-breaking displacements.

cond-mat.supr-con

Unconventional short-range structural fluctuations in cuprate high-$T_c$ superconductors

The interplay between structural and electronic degrees of freedom in complex materials is the subject of extensive debate in physics and materials science. Particularly interesting questions pertain to the nature and extent of pre-transitional short-range order in diverse systems ranging from shape-memory alloys to unconventional superconductors, and how this microstructure affects macroscopic properties. Here we use neutron and X-ray diffuse scattering to uncover universal structural fluctuations in La$_{2-x}$Sr$_x$CuO$_4$ and Tl$_2$Ba$_2$CuO$_{6+\delta}$, two cuprate superconductors with distinct point disorder effects and optimal superconducting transition temperatures. The fluctuations are present in wide doping and temperature ranges, including compositions that maintain high average structural symmetry, and they exhibit unusual, yet simple scaling behavior. The scaling regime is robust and universal, similar to the well-known critical fluctuations close to second-order phase transitions, but with a distinctly different physical origin. We relate this behavior to pre-transitional phenomena in a broad class of systems with structural and magnetic transitions, and propose an explanation based on rare structural fluctuations caused by intrinsic nanoscale inhomogeneity. We also uncover parallels with superconducting fluctuations, which indicates that the underlying inhomogeneity plays an important role in cuprate physics.

cond-mat.supr-con

Ferroelectric quantum criticality and enhanced superconductivity in plastically deformed strontium titanate

The properties of quantum materials are commonly tuned using experimental variables such as pressure, magnetic field and doping. Here we explore a different approach: irreversible, plastic deformation of single crystals. We show for the superconductor SrTiO$_3$ that compressive plastic deformation induces low-dimensional superconductivity significantly above the superconducting transition temperature ($T_c$) of undeformed samples, with evidence of superconducting correlations at temperatures two orders of magnitude above the bulk $T_c$. The superconductivity enhancement is correlated with the appearance of self-organized dislocation structures, as revealed by diffuse neutron and X-ray scattering. We also observe signatures of deformation-induced quantum-critical ferroelectric fluctuations and inhomogeneous ferroelectric order via Raman scattering. These results suggest that the strain surrounding the self-organized dislocation structures induces local ferroelectricity and quantum-critical dynamics that strongly influence $T_c$, consistent with a theory of superconductivity enhanced by soft polar fluctuations. More broadly, our results demonstrate the promise of plastic deformation and dislocation engineering as tools to manipulate electronic properties of quantum materials.

cond-mat.supr-con

Resistivity phase diagram of cuprates revisited

The phase diagram of the cuprate superconductors has posed a formidable scientific challenge for more than three decades. This challenge is perhaps best exemplified by the need to understand the normal-state charge transport as the system evolves from Mott insulator to Fermi-liquid metal with doping. Here we report a detailed analysis of the temperature (T) and doping (p) dependence of the planar resistivity of simple-tetragonal HgBa$_2$CuO$_{4+\delta}$ (Hg1201), the single-CuO$_2$-layer cuprate with the highest optimal $T_c$. The data allow us to test a recently proposed phenomenological model for the cuprate phase diagram that combines a universal transport scattering rate with spatially inhomogeneous (de)localization of the Mott-localized hole. We find that the model provides an excellent description of the data. We then extend this analysis to prior transport results for several other cuprates, including the Hall number in the overdoped part of the phase diagram, and find little compound-to-compound variation in (de)localization gap scale. The results point to a robust, universal structural origin of the inherent gap inhomogeneity that is unrelated to doping-related disorder. They are inconsistent with the notion that much of the phase diagram is controlled by a quantum critical point, and instead indicate that the unusual electronic properties exhibited by the cuprates are fundamentally related to strong nonlinearities associated with subtle nanoscale inhomogeneity.

cond-mat.str-el

Universal superconducting precursor in the cuprates

The nature of the superconducting (SC) precursor in the cuprates has been the subject of intense interest, with profound implications for both the normal and the SC states. Different experimental probes have led to vastly disparate conclusions on the temperature range of superconducting fluctuations. The main challenges have been to separate the SC response from complex normal-state behavior, and to distinguish the underlying behavior of the quintessential CuO$_{2}$ layers from compound-specific properties. Here we reveal remarkably simple and universal behavior of the SC precursor using torque magnetometry, a unique thermodynamic probe with extremely high sensitivity to SC diamagnetism. We comprehensively study four distinct cuprate compounds: single-CuO$_{2}$-layer La$_{2-x}$Sr$_{x}$CuO$_{4}$ (LSCO), Bi$_{2}$(Sr,La)$_{2}$CuO$_{6+\delta}$ (Bi2201) and HgBa$_{2}$CuO$_{4+\delta}$ (Hg1201), and double-layer Bi$_{2}$Sr$_{2}$Ca$_{0.95}$Y$_{0.05}$CuO$_{8+\delta}$ (Bi2212). Our approach, which focuses on the nonlinear diamagnetic response, completely removes normal-state contributions and thus allows us to trace the diamagnetic signal above Tc with great precision. We find that SC diamagnetism vanishes in an unusual, yet surprisingly simple exponential manner, marked by a universal temperature scale that is independent of compound and Tc. We discuss the distinct possibility that this unusual behavior signifies the proliferation of SC clusters as a result of the intrinsic inhomogeneity known to be an inherent property of the cuprates.

cond-mat.supr-con

Unusual behavior of cuprates explained by heterogeneous charge localization

The cuprate high-temperature superconductors are among the most intensively studied materials, yet essential questions regarding their principal phases and the transitions between them remain unanswered. Generally thought of as doped charge-transfer insulators, these complex lamellar oxides exhibit pseudogap, strange-metal, superconducting and Fermi-liquid behaviour with increasing hole-dopant concentration. Here we propose a simple inhomogeneous Mott-like (de)localization model wherein exactly one hole per copper-oxygen unit is gradually delocalized with increasing doping and temperature. The model is percolative in nature, with parameters that are experimentally constrained. It comprehensively captures pivotal unconventional experimental results, including the temperature and doping dependence of the pseudogap phenomenon, the strange-metal linear temperature dependence of the planar resistivity, and the doping dependence of the superfluid density. The success and simplicity of our model greatly demystify the cuprate phase diagram and point to a local superconducting pairing mechanism involving the (de)localized hole.

cond-mat.supr-con

Effective numbers of charge carriers in doped graphene: The generalized Fermi liquid approach

The single-band current-dipole Kubo formula for the dynamical conductivity of heavily doped graphene from Kupčić [Phys. Rev. B 91, 205428 (2015)] is extended to a two-band model for conduction $π$ electrons in lightly doped graphene. Using a posteriori relaxation-time approximation in the two-band quantum transport equations, with two different relaxation rates and one quasi-particle lifetime, we explain a seemingly inconsistent dependence of the dc conductivity $σ^{\rm dc}_{αα}$ of ultraclean and dirty lightly doped graphene samples on electron doping, in a way consistent with the charge continuity equation. It is also shown that the intraband contribution to the effective number of conduction electrons in $σ^{\rm dc}_{αα}$ vanishes at $T=0$ K in the ultraclean regime, but it remains finite in the dirty regime. The present model is shown to be consistent with a picture in which the intraband and interband contributions to $σ^{\rm dc}_{αα}$ are characterized by two different mobilities of conduction electrons, the values of which are well below the widely accepted value of mobility in ultraclean graphene. The dispersions of Dirac and $π$ plasmon resonances are reexamined to show that the present, relatively simple expression for the dynamical conductivity tensor can be used to study simultaneously single-particle excitations in the dc and optical conductivity and collective excitations in energy loss spectroscopy experiments.

cond-mat.mes-hall

17O-NMR Knight shift study of the interplay between superconductivity and pseudogap in (Ca_xLa_{1-x})(Ba_{1.75 - x}La_{0.25 + x})Cu_3O_y

We report systematic 17O-NMR measurements on the high-Tc cuprate (Ca_xLa_{1-x})(Ba_{1.75 - x}La_{0.25 + x})Cu_3O_y, for four different families (different x). Using Knight shift data, we show that the pseudogap lines for all families are inconsistent with a quantum critical point inside the superconducting dome. In addition, at constant doping the pseudogap temperature does not vary with x, in contrast to Tc. We therefore argue that pseudogap and superconductivity are separate phenomena in these cuprates. Using Knight shift data, we show that the pseudogap opening temperature T* is much higher than Tc near optimal doping, unlike structurally similar YBCO. In addition, at constant doping the pseudogap temperature does not vary with x, in contrast to Tc. This puts constraints on the nature of the pseudogap and position of the quantum critical point inside the superconducting dome.

cond-mat.supr-con