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Understanding and manipulating emergent phases, which are themes at the forefront of quantum-materials research, rely on identifying their underlying symmetries. This general principle has been particularly prominent in materials with coupled electronic and magnetic degrees of freedom, in which magnetic order influences the electronic band structure and can lead to exotic topological effects. However, identifying symmetry of a magnetically ordered phase can pose a challenge, particularly in the presence of small domains. Here we introduce a multimodal approach for determining magnetic structures, which combines symmetry-sensitive optical probes, scattering, and group-theoretical analysis. We apply it to EuIn_{2}As_{2}, a material that has received attention as a candidate axion insulator. While first-principles calculations predict this state on the assumption of a simple collinear antiferromagnetic structure, subsequent neutron-scattering measurements reveal a much more intricate magnetic ground state characterized by two coexisting magnetic wave vectors reached by successive thermal phase transitions. The proposed high- and low-temperature phases are a spin helix and a state with interpenetrating helical and Néel antiferromagnetic order termed a “broken helix,” respectively. Employing a multimodal approach, we identify the magnetic structure associated with these two phases of EuIn_{2}As_{2}. We find that the higher-temperature phase is characterized by a variation of the magnetic moment amplitude from layer to layer, with the moment vanishing entirely in every third Eu layer. The lower-temperature structure is similar to the broken helix, with one important difference: Because of local strain, the relative orientation of the magnetic structure and the lattice is not fixed. Consequently, the symmetry required to protect the axion phase is not generically protected in EuIn_{2}As_{2}, but we show that it can be restored if the magnetic structure is tuned with uniaxial strain. Finally, we present a spin Hamiltonian that identifies the spin interactions that account for the complex magnetic order in EuIn_{2}As_{2}. Our work highlights the importance of a multimodal approach in determining the symmetry of complex order parameters.

Abstract Controlling spin wave excitations in magnetic materials underpins the burgeoning field of magnonics. Yet, little is known about how magnons interact with the conduction electrons of itinerant magnets, or how this interplay can be controlled. Via a surface-sensitive spectroscopic approach, we demonstrate a strong electron–magnon coupling at the Pd-terminated surface of the delafossite oxide PdCoO2, where a polar surface charge mediates a Stoner transition to itinerant surface ferromagnetism. We show how the coupling is enhanced sevenfold with increasing surface disorder, and concomitant charge carrier doping, becoming sufficiently strong to drive the system into a polaronic regime, accompanied by a significant quasiparticle mass enhancement. Our study thus sheds light on electron–magnon interactions in solid-state materials, and the ways in which these can be controlled.

The origin of intertwined electronic orders in transition-metal dichalcogenides has long been debated. Here, Bawden et al. report that the normal state, from which these phases emerge, is unexpectedly spin-polarized, with spins locked to both valley and layer pseudospins.

The delafossite metals PdCoO_{2}, PtCoO_{2}, and PdCrO_{2} are among the highest conductivity materials known, with low-temperature mean free paths of tens of microns in the best as-grown single crystals. A key question is whether these very low resistive scattering rates result from strongly suppressed backscattering due to special features of the electronic structure or are a consequence of highly unusual levels of crystalline perfection. We report the results of experiments in which high-energy electron irradiation was used to introduce point disorder to the Pd and Pt layers in which the conduction occurs. We obtain the cross section for formation of Frenkel pairs in absolute units, and cross-check our analysis with first-principles calculations of the relevant atomic displacement energies. We observe an increase of resistivity that is linear in defect density with a slope consistent with scattering in the unitary limit. Our results enable us to deduce that the as-grown crystals contain extremely low levels of in-plane defects of approximately 0.001%. This confirms that crystalline perfection is the most important factor in realizing the long mean free paths and highlights how unusual these delafossite metals are in comparison with the vast majority of other multicomponent oxides and alloys. We discuss the implications of our findings for future materials research.

In many physical situations in which many-body assemblies exist at temperature T , a characteristic quantum-mechanical time scale of approximately [Formula: see text] can be identified in both theory and experiment, leading to speculation that it may be the shortest meaningful time in such circumstances. This behavior can be investigated by probing the scattering rate of electrons in a broad class of materials often referred to as "strongly correlated metals". It is clear that in some cases only electron-electron scattering can be its cause, while in others it arises from high-temperature scattering of electrons from quantized lattice vibrations, i.e., phonons. In metallic oxides, which are among the most studied materials, analysis of electrical transport does not satisfactorily identify the relevant scattering mechanism at "high" temperatures near room temperature. We therefore employ a contactless optical method to measure thermal diffusivity in two Ru-based layered perovskites, Sr 3 Ru 2 O 7 and Sr 2 RuO 4 , and use the measurements to extract the dimensionless Lorenz ratio. By comparing our results to the literature data on both conventional and unconventional metals, we show how the analysis of high-temperature thermal transport can both give important insight into dominant scattering mechanisms and be offered as a stringent test of theories attempting to explain anomalous scattering., Competing Interests: Competing interests statement:The authors declare no competing interest.

The adiabatic elastocaloric effect measures the temperature change of a given system with strain and provides a thermodynamic probe of the entropic landscape in the temperature-strain space. Here, we demonstrate that the DC bias strain-dependence of AC elastocaloric effect allows decomposition of the latter into symmetric (rotation-symmetry-preserving) and antisymmetric (rotation-symmetry-breaking) strain channels, using a tetragonal [Formula: see text]-electron intermetallic DyB[Formula: see text]C[Formula: see text]-whose antiferroquadrupolar order breaks local fourfold rotational symmetries while globally remaining tetragonal-as a showcase example. We capture the strain evolution of its quadrupolar and magnetic phase transitions using both singularities in the elastocaloric coefficient and its jumps at the transitions, and the latter we show follows a modified Ehrenfest relation. We find that antisymmetric strain couples to the underlying order parameter in a biquadratic (linear-quadratic) manner in the antiferroquadrupolar (canted antiferromagnetic) phase, which are attributed to a preserved (broken) global tetragonal symmetry, respectively. The broken tetragonal symmetry in the magnetic phase is further evidenced by elastocaloric strain-hysteresis and optical birefringence. Additionally, within the staggered quadrupolar order, the observed elastocaloric response reflects a quadratic increase of entropy with antisymmetric strain, analogous to the role magnetic field plays for Ising antiferromagnetic orders by promoting pseudospin flips. Our results demonstrate AC elastocaloric effect as a compact and incisive thermodynamic probe into the coupling between electronic degrees of freedom and strain in free energy, which holds the potential for investigating and understanding the symmetry of a wide variety of ordered phases in broader classes of quantum materials.

We describe an optical method to directly measure the 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 three-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 the 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., (© 2023 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).)

Microstructures can be carefully designed to reveal the quantum phase of the wave-like nature of electrons in a metal. Here, we report phase-coherent oscillations of out-of-plane magnetoresistance in the layered delafossites PdCoO 2 and PtCoO 2 The oscillation period is equivalent to that determined by the magnetic flux quantum, h/e , threading an area defined by the atomic interlayer separation and the sample width, where h is Planck's constant and e is the charge of an electron. The phase of the electron wave function appears robust over length scales exceeding 10 micrometers and persisting up to temperatures of T > 50 kelvin. We show that the experimental signal stems from a periodic field modulation of the out-of-plane hopping. These results demonstrate extraordinary single-particle quantum coherence lengths in delafossites., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.)

A nearly free electron metal and a Mott insulating state can be thought of as opposite ends of the spectrum of possibilities for the motion of electrons in a solid. Understanding their interaction lies at the heart of the correlated electron problem. In the magnetic oxide metal PdCrO 2 , nearly free and Mott-localized electrons exist in alternating layers, forming natural heterostructures. Using angle-resolved photoemission spectroscopy, quantitatively supported by a strong coupling analysis, we show that the coupling between these layers leads to an "intertwined" excitation that is a convolution of the charge spectrum of the metallic layer and the spin susceptibility of the Mott layer. Our findings establish PdCrO 2 as a model system in which to probe Kondo lattice physics and also open new routes to use the a priori nonmagnetic probe of photoemission to gain insights into the spin susceptibility of correlated electron materials., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY).)

We revisit the enduring problem of the 2×2×2 charge density wave (CDW) order in TiSe_{2}, utilizing photon energy-dependent angle-resolved photoemission spectroscopy to probe the full three-dimensional high- and low-temperature electronic structure. Our measurements demonstrate how a mismatch of dimensionality between the 3D conduction bands and the quasi-2D valence bands in this system leads to a hybridization that is strongly k_{z} dependent. While such a momentum-selective coupling can provide the energy gain required to form the CDW, we show how additional "passenger" states remain, which couple only weakly to the CDW and thus dominate the low-energy physics in the ordered phase of TiSe_{2}.

The ability to modulate the collective properties of correlated electron systems at their interfaces and surfaces underpins the burgeoning field of "designer" quantum materials. Here, we show how an electronic reconstruction driven by surface polarity mediates a Stoner-like magnetic instability to itinerant ferromagnetism at the Pd-terminated surface of the nonmagnetic delafossite oxide metal PdCoO 2 Combining angle-resolved photoemission spectroscopy and density-functional theory calculations, we show how this leads to a rich multiband surface electronic structure. We find similar surface state dispersions in PdCrO 2 , suggesting surface ferromagnetism persists in this sister compound despite its bulk antiferromagnetic order., Competing Interests: The authors declare no conflict of interest.

We study the low-energy surface electronic structure of the transition-metal dichalcogenide superconductor PdTe_{2} by spin- and angle-resolved photoemission, scanning tunneling microscopy, and density-functional theory-based supercell calculations. Comparing PdTe_{2} with its sister compound PtSe_{2}, we demonstrate how enhanced interlayer hopping in the Te-based material drives a band inversion within the antibonding p-orbital manifold well above the Fermi level. We show how this mediates spin-polarized topological surface states which form rich multivalley Fermi surfaces with complex spin textures. Scanning tunneling spectroscopy reveals type-II superconductivity at the surface, and moreover shows no evidence for an unconventional component of its superconducting order parameter, despite the presence of topological surface states.

Transition-metal dichalcogenides (TMDs) are renowned for their rich and varied bulk properties, while their single-layer variants have become one of the most prominent examples of two-dimensional materials beyond graphene. Their disparate ground states largely depend on transition metal d-electron-derived electronic states, on which the vast majority of attention has been concentrated to date. Here, we focus on the chalcogen-derived states. From density-functional theory calculations together with spin- and angle-resolved photoemission, we find that these generically host a co-existence of type-I and type-II three-dimensional bulk Dirac fermions as well as ladders of topological surface states and surface resonances. We demonstrate how these naturally arise within a single p-orbital manifold as a general consequence of a trigonal crystal field, and as such can be expected across a large number of compounds. Already, we demonstrate their existence in six separate TMDs, opening routes to tune, and ultimately exploit, their topological physics.

Engineering and enhancing the breaking of inversion symmetry in solids-that is, allowing electrons to differentiate between 'up' and 'down'-is a key goal in condensed-matter physics and materials science because it can be used to stabilize states that are of fundamental interest and also have potential practical applications. Examples include improved ferroelectrics for memory devices and materials that host Majorana zero modes for quantum computing. Although inversion symmetry is naturally broken in several crystalline environments, such as at surfaces and interfaces, maximizing the influence of this effect on the electronic states of interest remains a challenge. Here we present a mechanism for realizing a much larger coupling of inversion-symmetry breaking to itinerant surface electrons than is typically achieved. The key element is a pronounced asymmetry of surface hopping energies-that is, a kinetic-energy-coupled inversion-symmetry breaking, the energy scale of which is a substantial fraction of the bandwidth. Using spin- and angle-resolved photoemission spectroscopy, we demonstrate that such a strong inversion-symmetry breaking, when combined with spin-orbit interactions, can mediate Rashba-like spin splittings that are much larger than would typically be expected. The energy scale of the inversion-symmetry breaking that we achieve is so large that the spin splitting in the CoO 2 - and RhO 2 -derived surface states of delafossite oxides becomes controlled by the full atomic spin-orbit coupling of the 3d and 4d transition metals, resulting in some of the largest known Rashba-like spin splittings. The core structural building blocks that facilitate the bandwidth-scaled inversion-symmetry breaking are common to numerous materials. Our findings therefore provide opportunities for creating spin-textured states and suggest routes to interfacial control of inversion-symmetry breaking in designer heterostructures of oxides and other material classes.

Metallic transition-metal dichalcogenides (TMDCs) are benchmark systems for studying and controlling intertwined electronic orders in solids, with superconductivity developing from a charge-density wave state. The interplay between such phases is thought to play a critical role in the unconventional superconductivity of cuprates, Fe-based and heavy-fermion systems, yet even for the more moderately-correlated TMDCs, their nature and origins have proved controversial. Here, we study a prototypical example, 2H-NbSe2, by spin- and angle-resolved photoemission and first-principles theory. We find that the normal state, from which its hallmark collective phases emerge, is characterized by quasiparticles whose spin is locked to their valley pseudospin. This results from a combination of strong spin-orbit interactions and local inversion symmetry breaking, while interlayer coupling further drives a rich three-dimensional momentum dependence of the underlying Fermi-surface spin texture. These findings necessitate a re-investigation of the nature of charge order and superconducting pairing in NbSe2 and related TMDCs.

Understanding the role of electron correlations in strong spin-orbit transition-metal oxides is key to the realization of numerous exotic phases including spin-orbit-assisted Mott insulators, correlated topological solids, and prospective new high-temperature superconductors. To date, most attention has been focused on the 5d iridium-based oxides. We instead consider the Pt-based delafossite oxide PtCoO2. Our transport measurements, performed on single-crystal samples etched to well-defined geometries using focused ion beam techniques, yield a room temperature resistivity of only 2.1 microhm·cm (μΩ-cm), establishing PtCoO2 as the most conductive oxide known. From angle-resolved photoemission and density functional theory, we show that the underlying Fermi surface is a single cylinder of nearly hexagonal cross-section, with very weak dispersion along k z . Despite being predominantly composed of d-orbital character, the conduction band is remarkably steep, with an average effective mass of only 1.14m e. Moreover, the sharp spectral features observed in photoemission remain well defined with little additional broadening for more than 500 meV below E F, pointing to suppressed electron-electron scattering. Together, our findings establish PtCoO2 as a model nearly-free-electron system in a 5d delafossite transition-metal oxide.