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I. Biało

Publications and source records attributed to I. Biało.

14 recordsLinked to original sources

Autonomous Diffractometry Enabled by Visual Reinforcement Learning

Automation underpins progress across scientific and industrial disciplines. Yet, automating tasks requiring interpretation of abstract visual information remain challenging. For example, crystal alignment strongly relies on humans with the ability to comprehend diffraction patterns. Here we introduce an autonomous system that aligns single crystals without access to crystallography and diffraction theory. Using a model-free reinforcement learning framework, an agent learns to identify and navigate towards high-symmetry orientations directly from Laue diffraction patterns. Despite the absence of human supervision, the agent develops human-like strategies to achieve time-efficient alignment across different crystal symmetry classes. With this, we provide a computational framework for intelligent diffractometers. As such, our approach advances the development of automated experimental workflows in materials science.

cs.LG↗

Correlated charge order intertwined with time-reversal symmetry-breaking nodal superconductivity in the dual flat band kagome superconductor CeRu$_{3}$Si$_{2}$

Kagome materials provide a powerful platform for exploring how flat electronic bands promote symmetry-breaking quantum states, yet studies have so far focused mainly on kagome-derived $d$-electron flat bands. In this paper, we introduce CeRu$_{3}$Si$_{2}$, a kagome superconductor in which our first-principles calculations show the coexistence of Ru $d$-orbital kagome flat bands and heavy-fermion flat bands derived from Ce$^{4+}$ $4f$-states. X-ray diffraction reveals a dominant 1/2 charge order with a much weaker 1/3 component persisting up to room temperature. Theoretical calculations further highlight the correlated nature of these charge-order states. Deep within the charge-ordered state, magnetoresistance emerges below 80 K and strengthens further below 30 K. Zero-field muon spin-rotation measurements show no time-reversal symmetry (TRS) breaking in the normal state, in contrast to LaRu$_{3}$Si$_{2}$ and YRu$_{3}$Si$_{2}$. However, an applied magnetic field induces weak magnetism. Across the $A$Ru$_{3}$Si$_{2}$ family ($A$ = La, Y, and Ce), the superconducting transition temperature $T_{\rm c}$ scales linearly with the onset temperature of normal-state TRS breaking $T_{\rm {TRSB}}$ and the magnitude of the field-induced magnetic response, revealing a direct positive correlation between normal-state symmetry breaking and superconductivity. Furthermore, we identify that CeRu$_{3}$Si$_{2}$ is the first 132-type kagome compound to host nodal superconductivity together with spontaneous internal magnetic fields, providing clear evidence for intrinsic TRS breaking in the superconducting state. These results establish CeRu$_{3}$Si$_{2}$ as a unique platform where intertwined kagome $d$- and heavy fermion $f$-electron flat bands generate a rich hierarchy of electronic orders.

cond-mat.supr-con↗

Magnetic Excitations of a Half-Filled Tl-based Cuprate

Strong electron correlations drive Mott insulator transitions. Yet, there exists no framework to classify Mott insulators by their degree of correlation. Cuprate superconductors, with their tunable doping and rich phase diagrams, offer a unique platform to investigate the evolution of these interactions. However, spectroscopic access to a clean half-filled Mott-insulating state is lacking in compounds with the highest superconducting onset temperature. To fill this gap, we introduce a pristine, half-filled thallium-based cuprate system, Tl$_2$Ba$_5$Cu$_4$O$_{x}$. Using high-resolution resonant inelastic x-ray scattering, we probe long-lived magnon excitations and uncover a pronounced kink in the magnon dispersion, marked by a simultaneous change in group velocity and lifetime broadening. Modeling the dispersion within a Hubbard-Heisenberg approach, we extract the interaction strength and compare it with other cuprate systems. Our results establish a cuprate universal relation between electron-electron interaction and magnon zone-boundary dispersion. Superconductivity seems to be optimal at intermediate correlation strength, suggesting an optimal balance between localization and itinerancy.

cond-mat.supr-con↗

Orbital Separation of Charge Order and Superconductivity in La$_{2-x}$Sr$_{x}$CuO$_4$

We report a combined x-ray absorption (XAS) and oxygen $K$-edge resonant inelastic x-ray scattering (RIXS) study of charge order in underdoped La$_{2-x}$Sr$_x$CuO$_4$ ($x=0.125$) under uniaxial $c$-axis pressure. We find that compressive $c$-axis strain modifies the charge order only within the superconducting state, with a striking polarization dependence: suppression in the $d_{x^2-y^2}$ channel and enhancement in the $d_{z^2}$ channel. X-ray absorption spectra reveal concomitant strain-induced modifications of the oxygen pre-edge and upper Hubbard band, consistent with increased $d_{z^2}$ orbital admixture. Our results suggest that $c$-axis pressure drives an orbital separation between superconductivity, rooted in $d_{x^2-y^2}$ states, and charge order, which gradually shifts to the $d_{z^2}$ channel. This orbital separation reveals a way for superconductivity and charge order to coexist in the cuprates with minimal competition. Furthermore, it suggests that the multi-order phase diagram of La$_{2-x}$Sr$_{x}$CuO$_4$ cannot be realistically described within single band models usually used to describe cuprate physics.

cond-mat.supr-con↗

Impact of Electron Correlations on Infinite-Layer Cuprates and Nickelates

Optimization of unconventional superconductivity involves a balance of interaction strengths. Precise determination of correlation strength across different material families is therefore important. Here, we present a combined X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) study of infinite-layer PrNiO$_2$ and SrCuO$_2$ that enables fair comparison of their interaction strengths. For both compounds, we study the orbital and magnetic excitations and extract their dispersions along high-symmetry directions. Using a single-band Hubbard model and including higher-order exchange interactions, we derive the correlation factor $U/t$ for both compounds. A key finding is that despite a smaller Coulomb repulsion $U$, PrNiO$_2$ exhibits a correlation strength that is 20% stronger than that of its isostructural cuprate counterpart SrCuO$_2$. This indicates that a moderation of the correlation strength may further optimize superconductivity in nickelates.

cond-mat.supr-con↗

Decoupling of Static and Dynamic Charge Correlations revealed by Uniaxial Strain in a Cuprate Superconductor

We use uniaxial strain in combination with ultra-high-resolution Resonant Inelastic X-ray Scattering (RIXS) at the oxygen K- and copper L3-edges to study the excitations stemming from the charge ordering wave vector in La1.875Sr0.125CuO4. By detwinning stripe ordering, we demonstrate that the optical phonon anomalies do not show any stripe anisotropy. The low-energy charge excitations also retain an in-plane four-fold symmetry. As such, we find that both phonon and charge excitations are decoupled entirely from the strength of static charge ordering. The almost isotropic character of charge excitations is indicative of a quantum critical behaviour and remains a possible source for the strange metal properties found in the normal state of cuprate superconductors.

cond-mat.str-el↗

Engineering Phase Competition Between Stripe Order and Superconductivity in La$_{1.88}$Sr$_{0.12}$CuO$_4$

Unconventional superconductivity often couples to other electronic orders in a cooperative or competing fashion. Identifying external stimuli that tune between these two limits is of fundamental interest. Here, we show that strain perpendicular to the copper-oxide planes couples directly to the competing interaction between charge stripe order and superconductivity in La$_{1.88}$Sr$_{0.12}$CuO$_4$ (LSCO). Compressive $c$-axis pressure amplifies stripe order within the superconducting state, while having no impact on the normal state. By contrast, strain dramatically diminishes the magnetic field enhancement of stripe order in the superconducting state. These results suggest that $c$-axis strain acts as tuning parameter of the competing interaction between charge stripe order and superconductivity. This interpretation implies a uniaxial pressure-induced ground state in which the competition between charge order and superconductivity is reduced.

cond-mat.str-el↗

Strain-Tuned Magnetic Frustration in a Square Lattice $J_1$-$J_2$ Material

Magnetic frustration is a route that can lead to the emergence of novel ground states, including spin liquids and spin ices. Such frustration can be introduced through either the geometry of lattice structures or by incompatible exchange interactions. Identifying suitable strategies to control the degree of magnetic frustration in real systems is an active field of research. In this study, we devise a design principle for the tuning of frustrated magnetism on the square lattice through the manipulation of nearest (NN) and next-nearest neighbor (NNN) antiferromagnetic (AF) exchange interactions. By studying the magnon excitations in epitaxially-strained La$_2$NiO$_4$ films using resonant inelastic x-ray scattering (RIXS) we show that, in contrast to the cuprates, the dispersion peaks at the AF zone boundary. This indicates the presence of an AF-NNN spin interaction. Using first principles simulations and an effective spin-model, we demonstrate the AF-NNN coupling to be a consequence of the two-orbital nature of La$_2$NiO$_4$. Our results demonstrate that compressive strain can enhance this coupling, providing a design principle for the tunability of frustrated magnetism on a square lattice.

cond-mat.str-el↗

Magnon interactions in a moderately correlated Mott insulator

Quantum fluctuations in low-dimensional systems and near quantum phase transitions have significant influences on material properties. Yet, it is difficult to experimentally gauge the strength and importance of quantum fluctuations. Here we provide a resonant inelastic x-ray scattering study of magnon excitations in Mott insulating cuprates. From the thin film of SrCuO$_2$, single- and bi-magnon dispersions are derived. Using an effective Heisenberg Hamiltonian generated from the Hubbard model, we show that the single-magnon dispersion is only described satisfactorily when including significant quantum corrections stemming from magnon-magnon interactions. Comparative results on La$_2$CuO$_4$ indicate that quantum fluctuations are much stronger in SrCuO$_2$ suggesting closer proximity to a magnetic quantum critical point. Monte Carlo calculations reveal that other magnetic orders may compete with the antiferromagnetic Néel order as the ground state. Our results indicate that SrCuO$_2$ - due to strong quantum fluctuations - is a unique starting point for the exploration of novel magnetic ground states.

cond-mat.str-el↗

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↗

Discovery of Giant Unit-Cell Super-Structure in the Infinite-Layer Nickelate PrNiO$_2$

Spectacular quantum phenomena such as superconductivity often emerge in flat-band systems where Coulomb interactions overpower electron kinetics. Engineering strategies for flat-band physics is therefore of great importance. Here, using high-energy grazing-incidence x-ray diffraction, we demonstrate how in-situ temperature annealing of the infinite-layer nickelate PrNiO$_2$ induces a giant superlattice structure. The annealing effect has a maximum well above room temperature. By covering a large scattering volume, we show a rare period-six in-plane (bi-axial) symmetry and a period-four symmetry in the out-of-plane direction. This giant unit-cell superstructure likely stems from ordering of diffusive oxygen. The stability of this superlattice structure suggests a connection to an energetically favorable electronic state of matter. As such, our study provides a new pathway - different from Moiré structures - to ultra-small Brillouin zone electronics.

cond-mat.supr-con↗

Two-Dimensional Phase-Fluctuating Superconductivity in Bulk-Crystalline NdO$_{0.5}$F$_{0.5}$BiS$_2$

We present a combined growth and transport study of superconducting single-crystalline NdO$_{0.5}$F$_{0.5}$BiS$_2$. Evidence of two-dimensional superconductivity with significant phase fluctuations of preformed Cooper pairs preceding the superconducting transition is reported. This result is based on three key observations. (1) The resistive superconducting transition temperature $T_c$ (defined by resistivity $ρ\rightarrow 0$) increases with increasing disorder. (2) As $T\rightarrow T_c$, the conductivity diverges significantly faster than what is expected from Gaussian fluctuations in two and three dimensions. (3) Non-Ohmic resistance behavior is observed in the superconducting state. Altogether, our observations are consistent with a temperature regime of phase-fluctuating superconductivity. The crystal structure with magnetic ordering tendencies in the NdO$_{0.5}$F$_{0.5}$ layers and (super)conductivity in the BiS$_2$ layers is likely responsible for the two-dimensional phase fluctuations. As such, NdO$_{0.5}$F$_{0.5}$BiS$_2$ falls into the class of unconventional ``laminar" bulk superconductors that include cuprate materials and 4Hb-TaS$_2$.

cond-mat.supr-con↗

The impact of hydrostatic pressure, nonstoichiometry, and doping on trimeron lattice excitations in magnetite during axis switching

Trimeron lattice excitations in single crystalline magnetite, in the form of the $c$ axis switching (i.e. the reorganization of the lattice caused by external magnetic field) at temperatures below the Verwey temperature $T_V$ are observed by magnetization experiments. These excitations exhibit strong sensitivity to doping (with Zn, Al, and Ti), nonstoichiometry and hydrostatic pressure ($p < 1.2$ GPa). The considered indicators of the axis switching (AS) are: the switching field $B_{sw}$, the energy density needed to switch the axis $E_{sw}$ and the activation energy $U$. Our results show that hydrostatic pressure $p$ weakens the low$-T$ magnetite structure (decreases $T_V$) and has roughly similar effects on AS in Zn-doped Fe$_3$O$_4$ and, in much less extent, in stoichiometric magnetite. We have, however, found that while doping/nonstoichiometry also lowers $T_V$, making it more prone to temperature chaos, it drastically increases the switching field, activation and switching energies suggesting that the trimeron order, subject to change while AS occurs, is more robust. Consequently, we conclude that the manipulation of trimerons in the process of axis switching and the mechanisms leading to the Verwey transition are distinct phenomena.

cond-mat.str-el↗

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↗