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N. Barišić

Publications and source records attributed to N. Barišić.

At least 19 recordsLinked to original sources

Robustness of the Verwey transition against remanent strain-induced defects in magnetite

The Verwey transition in magnetite is a benchmark electronically driven phase transition that is highly sensitive to lattice imperfections and external perturbations. Doping, deviations from oxygen stoichiometry, and irradiation-induced point defects are known to lower the Verwey transition temperature, $T_{\rm V}$. By contrast, the role of remanent strain fields and extended defect structures generated by uniaxial stress has remained largely unexplored. Here we combine dark-field x-ray microscopy (DFXM) and ac magnetic susceptibility to determine how strain-induced defects affect the Verwey transition in stoichiometric single-crystalline magnetite after uniaxial compression and unloading. The DFXM measurements were performed on two samples compressed along the same $[011]$ direction: loading to $200~\mathrm{MPa}$ generated stable line-like defects and remanent strain fields, whereas loading beyond the fracture threshold produced denser defect networks and mechanical fracture. To test the effect of a different loading geometry, we also measured the ac susceptibility of a sample fractured by compression along $[001]$. Real-space DFXM imaging, lattice-orientation mapping, and residual strain mapping show substantial remanent structural disorder after compression. Nevertheless, neither the transition temperature $T_{\rm V}$ nor the sharpness of the transition changes measurably in any of the compressed or fractured samples. This behavior contrasts with the strong suppression of $T_{\rm V}$ by point-like disorder. Our results show that extended line-like defects and remanent strain fields produced by plastic deformation do not measurably perturb the macroscopic electronic ordering responsible for the Verwey transition, thereby distinguishing the effects of point defects from those of extended slip-related defects in magnetite.

cond-mat.str-el↗

Strain-tunable charge localization coupled to complex magnetic orders in EuAl$_4$

Charge localization is particularly interesting when coupled to antiferromagnetic spin structures. Coupled spin-charge orders are well established in elemental chromium and correlated oxide superconductors, yet the interplay between charge order and more complex magnetic textures -- such as skyrmion lattices and chiral spin structures -- remains largely unexplored. Here we report a comprehensive study of how charge localization couples to the unusually rich sequence of magnetic phases in EuAl$_4$. Using x-ray diffraction under applied magnetic field and uniaxial pressure, we demonstrate a direct coupling between the charge and spin order parameters. In the absence of external stimuli, charge localization is markedly enhanced upon entering the magnetically ordered phases. Strikingly, this effect is highly susceptible to strain: uniaxial pressure applied along the charge-order propagation direction further enhances localization, whereas pressure applied perpendicular to it weakens it. Application of magnetic field reveals both competitive and possible collaborative interactions between spin and charge ordering.This flexible coupling between spin and charge ordering opens a new route to designing symmetry-breaking states. Chiral charge order may for example be patterned from spin structures with that symmetry.

cond-mat.str-el↗

Optical conductivity of layered topological semimetal TaNiTe$_5$

We present an infrared spectroscopy study of the layered topological semimetal TaNiTe$_5$, a material with a quasi-one-dimensional structure and strong in-plane anisotropy. Despite its structural features, infrared reflectivity and electronic transport measurements along the $a$ and $c$ crystallographic axes show metallic behavior without evidence of reduced dimensionality. Optical conductivity reveals an anisotropic but conventional metallic response with low scattering rates and a single sharp infrared-active phonon mode at $396$ cm$^{-1}$ ($49$ meV). Ab initio calculations closely match the experimental optical data and confirm a three-dimensional electronic structure. Our results demonstrate that TaNiTe$_5$ behaves as a three-dimensional anisotropic semimetal in its electronic and optical properties.

cond-mat.str-el↗

Cuprates, Pnictides and Sulfosalts: Lessons in Functional Materials

Murunskite K$_2$Cu$_3$FeS$_4$ is a representative sulfosalt, isostructural to the pnictides, but with electronic properties more similar to the insulating parent compounds of the cuprates. We use it as a bridge to compare the chemical and physical roles of metal and ligand orbitals in cuprates and pnictides. In cuprates, ionicity, covalency, and metallicity are tightly interwoven to give rise to high-temperature superconductivity (SC). Their most remarkable property is the interaction of an ionically localized hole on the copper (Cu) with a Fermi liquid (FL) on the oxygens (O), which is critically important for understanding all key properties of these materials. The localization is due to strong correlations on the Cu $3d$ orbital. We describe a scenario in which the localized hole gives rise both to SC by Cooper scattering of O holes, and to Fermi arcs, as observed in cuprate spectroscopy, the latter by a purely kinematic projection of the static local disorder, without invoking any residual interactions between the mobile O FL carriers. In the pnictides, the orbitals responsible for binding and metallic conduction appear to be separate. The Fe $3d$ $e_{g}$ orbitals hybridized with the ligands set the lattice spacing. The $3d$ $t_{2g}$ orbitals overlap directly between the Fe atoms, resulting in several electronic bands appearing at the Fermi level. The ensuing Fermi liquid exhibits both charge and magnetic correlations. We argue that a similar SC scenario as in the cuprates is plausible in the pnictides, except that a light FL scatters on a slow nearly-antiferromagnetic (AF) one, rather than on localized holes as in the cuprates.

cond-mat.supr-con↗

High-entropy magnetism of murunskite

Murunskite (K$_2$FeCu$_3$S$_4$) is a bridging compound between the only two known families of high-temperature superconductors. It is a semiconductor like the parent compounds of cuprates, yet isostructural to metallic iron-pnictides. Moreover, like both families, it has an antiferromagnetic (AF)-like response with an ordered phase occurring below $\approx$ 100 K. Through comprehensive neutron, Mössbauer, and XPS measurements on single crystals, we unveil AF with a nearly commensurate quarter-zone wave vector. Intriguingly, the only identifiable magnetic atoms, iron, are randomly distributed over one-quarter of available crystallographic sites in 2D planes, while the remaining sites are occupied by closed-shell copper. Notably, any interpretation in terms of a spin-density wave is challenging, in contrast to the metallic iron-pnictides where Fermi-surface nesting can occur. Our findings align with a disordered-alloy picture featuring magnetic interactions up to second neighbors. Moreover, in the paramagnetic state, iron ions are either in Fe$^{3+}$ or Fe$^{2+}$ oxidation states, associated with two distinct paramagnetic sites identified by Mössbauer spectroscopy. Upon decreasing the temperature below the appearance of magnetic interactions, these two signals merge completely into a third, implying an orbital transition. It completes the cascade of (local) transitions that transform iron atoms from fully orbitally and magnetically disordered to homogeneously ordered in inverse space, but still randomly distributed in real space.

cond-mat.str-el↗

Evidence of 3D Dirac conical bands in TlBiSSe by optical and magneto-optical spectroscopy

TlBiSSe is a rare realization of a 3D semimetal with a conically dispersing band that has an optical response which is well isolated from other contributions in a broad range of photon eneries. We report optical and magneto-optical spectroscopy on this material. When the compound is chemically tuned into a state of the lowest carrier concentration, we find a nearly linear frequency dependence of the optical conductivity below 0.5~eV. Landau level spectroscopy allows us to describe the system with a massive Dirac model, giving a gap $2Δ=32$~meV and an in-plane velocity parameter $v= 4.0\times 10^5$~m/s. % Finally, we provide a theoretical recipe to extract all parameters of the anisotropic Dirac band, including the Fermi energy and band degeneracy.

cond-mat.mtrl-sci↗

Arc-to-pocket transition and quantitative understanding of transport properties in cuprate superconductors

Despite immense efforts, the cuprate Fermi surface (FS) has been unambiguously determined in only two distinct, low-temperature regions of the phase diagram: a large hole-like FS at high doping, and a small electron-like pocket associated with charge-density-wave driven FS reconstruction at moderate doping. Moreover, there exists incomplete understanding of the reconstructed state, which is stabilized by high magnetic fields, and its connection with the normal state that consists of arc-like remnants of the large underlying FS. Part of the problem is that compound-specific idiosyncrasies, such as disorder effects and low structural symmetry, can obscure the fundamental properties of the quintessential CuO$_2$ planes. Here we present planar magnetotransport measurements for moderately-doped HgBa$_2$CuO$_{4+δ}$ that enable a quantitative understanding of the phase transition between the normal and reconstructed states and of the charge transport in the latter, and that demonstrate that the quasiparticle scattering rate in both states is due to Umklapp scattering. Building on prior insights, we furthermore arrive at a comprehensive understanding of the evolution of the planar transport properties throughout the entire cuprate phase diagram.

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$_{4+δ}$ (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↗

Hole-pocket-driven superconductivity and its universal features in the electron-doped cuprates

After three decades of enormous scientific inquiry, the emergence of superconductivity in the cuprates remains an unsolved puzzle. One major challenge has been to arrive at a satisfactory understanding of the unusual metallic normal state from which the superconducting state emerges upon cooling. A second challenge has been to achieve a unified understanding of hole- and electron-doped compounds. Here we report detailed magnetoresistivity measurements for the archetypal electron-doped cuprate Nd$_{2-x}$Ce$_x$CuO$_{4+δ}$ that, in combination with prior data, provide crucial links between the normal and superconducting states and between the electron- and hole-doped parts of the phase diagram. The characteristics of the normal state (magnetoresistivity, quantum oscillations, and Hall coefficient) and those of the superconducting state (superfluid density and upper critical field) consistently indicate two-band (electron and hole) features and clearly point to hole-pocket-driven superconductivity in these nominally electron-doped materials. We show that the approximate Uemura scaling between the superconducting transition temperature and the superfluid density found for hole-doped cuprates also holds for the small hole component of the superfluid density in the electron-doped cuprates.

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$_{6+δ}$ (Bi2201) and HgBa$_{2}$CuO$_{4+δ}$ (Hg1201), and double-layer Bi$_{2}$Sr$_{2}$Ca$_{0.95}$Y$_{0.05}$CuO$_{8+δ}$ (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↗

Synchrotron x-ray scattering study of charge-density-wave order in HgBa$_2$CuO$_{4+δ}$

We present a detailed synchrotron x-ray scattering study of the charge-density-wave (CDW) order in simple tetragonal HgBa$_2$CuO$_{4+δ}$ (Hg1201). Resonant soft x-ray scattering measurements reveal that short-range order appears at a temperature that is distinctly lower than the pseudogap temperature and in excellent agreement with a prior transient reflectivity result. Despite considerable structural differences between Hg1201 and YBa$_2$Cu$_3$O$_{6+δ}$, the CDW correlations exhibit similar doping dependencies, and we demonstrate a universal relationship between the CDW wave vector and the size of the reconstructed Fermi pocket observed in quantum oscillation experiments. The CDW correlations in Hg1201 vanish already below optimal doping, once the correlation length is comparable to the CDW modulation period, and they appear to be limited by the disorder potential from unit cells hosting two interstitial oxygen atoms. A complementary hard x-ray diffraction measurement, performed on an underdoped Hg1201 sample in magnetic fields along the crystallographic $c$ axis of up to 16 T, provides information about the form factor of the CDW order. As expected from the single-CuO$_2$-layer structure of Hg1201, the CDW correlations vanish at half-integer values of $L$ and appear to be peaked at integer $L$. We conclude that the atomic displacements associated with the short-range CDW order are mainly planar, within the CuO$_2$ layers.

cond-mat.supr-con↗

Evidence for a universal Fermi-liquid scattering rate throughout the phase diagram of the copper-oxide superconductors

The phase diagram of the cuprate superconductors continues to pose formidable scientific challenges. While these materials are typically viewed as doped Mott insulators, it is well known that they are Fermi liquids at high hole-dopant concentrations. It was recently demonstrated that at moderate doping, in the pseudogap region of the phase diagram, the charge carriers are also best described as Fermi liquid. Nevertheless, the relationship between the two Fermi-liquid regions and the nature of the strange-metal state at intermediate doping have remained unsolved. Here we show in the case of the model cuprate superconductor HgBa2CuO4+δ that the scattering rate measured by the cotangent of the Hall angle remains quadratic in temperature across the pseudogap temperature, upon entering the strange-metal state, and that it is doping-independent below optimal doping. Analysis of the published results for other cuprates reveals that this behavior is universal throughout the entire phase diagram and points to a pervasive Fermi-liquid transport scattering rate. We argue that these observations can be reconciled with other data upon considering the possibility that the pseudogap phenomenon signifies the completion of the gradual, non-uniform localization of one hole per planar CuO2 unit upon cooling.

cond-mat.supr-con↗

Hidden Fermi-liquid charge transport in the antiferromagnetic phase of the electron-doped cuprates

Systematic analysis of the planar resistivity, Hall effect and cotangent of the Hall angle for the electron-doped cuprates reveals underlying Fermi-liquid behavior even deep in the antiferromagnetic part of the phase diagram. The transport scattering rate exhibits a quadratic temperature dependence, and is nearly independent of doping, compound and carrier type (electrons vs. holes), and hence universal. Our analysis moreover indicates that the material-specific resistivity upturn at low temperatures and low doping has the same origin in both electron- and hole-doped cuprates.

cond-mat.supr-con↗

Connection between charge-density-wave order and charge transport in the cuprate superconductors

Charge-density-wave (CDW) correlations within the quintessential CuO$_2$ planes have been argued to either cause [1] or compete with [2] the superconductivity in the cuprates, and they might furthermore drive the Fermi-surface reconstruction in high magnetic fields implied by quantum oscillation (QO) experiments for YBa$_2$Cu$_3$O$_{6+δ}$ (YBCO) [3] and HgBa$_2$CuO$_{4+δ}$ (Hg1201) [4]. Consequently, the observation of bulk CDW order in YBCO was a significant development [5,6,7]. Hg1201 features particularly high structural symmetry and recently has been demonstrated to exhibit Fermi-liquid charge transport in the relevant temperature-doping range of the phase diagram, whereas for YBCO and other cuprates this underlying property of the CuO$_2$ planes is partially or fully masked [8-10]. It therefore is imperative to establish if the pristine transport behavior of Hg1201 is compatible with CDW order. Here we investigate Hg1201 ($T_c$ = 72 K) via bulk Cu L-edge resonant X-ray scattering. We indeed observe CDW correlations in the absence of a magnetic field, although the correlations and competition with superconductivity are weaker than in YBCO. Interestingly, at the measured hole-doping level, both the short-range CDW and Fermi-liquid transport appear below the same temperature of about 200 K. Our result points to a unifying picture in which the CDW formation is preceded at the higher pseudogap temperature by $q$ = 0 magnetic order [11,12] and the build-up of significant dynamic antiferromagnetic correlations [13]. Furthermore, the smaller CDW modulation wave vector observed for Hg1201 is consistent with the larger electron pocket implied by both QO [4] and Hall-effect [14] measurements, which suggests that CDW correlations are indeed responsible for the low-temperature QO phenomenon.

cond-mat.supr-con↗

Validity of Kohler's rule in the pseudogap phase of the cuprate superconductors

We report in-plane resistivity ($ρ$) and transverse magnetoresistance (MR) measurements in underdoped HgBa$_2$CuO$_{4+δ}$ (Hg1201). Contrary to the longstanding view that Kohler's rule is strongly violated in underdoped cuprates, we find that it is in fact satisfied in the pseudogap phase of Hg1201. The transverse MR shows a quadratic field dependence, $δρ/ρ_o=a H^{2}$, with $a(T)\propto T^{-4}$. In combination with the observed $ρ\propto T^2$ dependence, this is consistent with a single Fermi-liquid quasiparticle scattering rate. We show that this behavior is universal, yet typically masked in cuprates with lower structural symmetry or strong disorder effects.

cond-mat.supr-con↗

Angle-resolved photoemission spectroscopy study of HgBa$_{2}$CuO$_{4+δ}$

HgBa$_{2}$CuO$_{4+δ}$ (Hg1201) has been shown to be a model cuprate for scattering, optical, and transport experiments, but angle-resolved photoemission spectroscopy (ARPES) data are still lacking owing to the absence of a charge-neutral cleavage plane. We report on progress in achieving the experimental conditions for which quasiparticles can be observed in the near-nodal region of the Fermi surface. The d-wave superconducting gap is measured and found to have a maximum of 39 meV. At low temperature, a kink is detected in the nodal dispersion at approximately 51 meV below the Fermi level, an energy that is different from other cuprates with comparable T$_c$. The superconducting gap, Fermi surface, and nodal band renormalization measured here provide a crucial momentum-space complement to other experimental probes.

cond-mat.supr-con↗

Universal sheet resistance and revised phase diagram of the cuprate high-temperature superconductors

Upon introducing charge carriers into the copper-oxygen sheets of the enigmatic lamellar cuprates the ground state evolves from an insulator into a superconductor, and eventually into a seemingly conventional metal (a Fermi liquid). Much has remained elusive about the nature of this evolution and about the peculiar metallic state at intermediate hole-carrier concentrations (p). The planar resistivity of this unconventional metal exhibits a linear temperature dependence (ρ$\propto$ T) that is disrupted upon cooling toward the superconducting state by the opening of a partial gap (the pseudogap) on the Fermi surface. Here we first demonstrate for the quintessential compound HgBa$_2$CuO$_{4+δ}$ a dramatic switch from linear to purely quadratic (Fermi-liquid-like, ρ$\propto$ T$^2$) resistive behavior in the pseudogap regime. Despite the considerable variation in crystal structures and disorder among different compounds, our result together with prior work gives new insight into the p-T phase diagram and reveals the fundamental resistance per copper-oxygen sheet in both linear (ρ_S = A_{1S} T) and quadratic (ρ_S = A_{2S} T$^2$) regimes, with A_{1S} $\propto$ A_{2S} $\propto$ 1/p. Theoretical models can now be benchmarked against this remarkably simple universal behavior. Deviations from this underlying behavior can be expected to lead to new insights into the non-universal features exhibited by certain compounds.

cond-mat.supr-con↗