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We present an experimental and theoretical study which compares the phonon anomalies and the electronic gap features in the infrared response of the weakly coupled two-leg-ladders in Sr14-xCaxCu24O41(SCCO) with those of the underdoped high-Tcsuperconductor YBa2Cu3O6+x(YBCO) and thereby reveals some surprising analogies. Specifically, we present a phenomenological model that describes the anomalous doping- and temperature-dependence of some of the phonon features in thea-axis response (field along the rungs of the ladders) of SCCO. It assumes that the phonons are coupled to charge oscillations within the ladders. Their changes with decreasing temperature reveal the formation of a crystal (density wave) of hole pairs that are oriented along the rungs. We also discuss the analogy to a similar model that was previously used to explain the phonon anomalies and an electronic plasma mode in thec-axis response (field perpendicular to the CuO2planes) of YBCO. We further confirm that an insulator-like pseudogap develops in thea-axis conductivity of SCCO which closely resembles that in thec-axis conductivity of YBCO. Most surprisingly, we find that thec-axis conductivity (field along the legs of the ladders) of SCCO is strikingly similar to the in-plane one (field parallel to the CuO2planes) of YBCO. Notably, in both cases a dip feature develops in the normal state spectra that is connected with a spectral weight shift toward low frequencies and can thus be associated with precursor superconducting pairing correlations that are lacking macroscopic phase coherence. This SCCO-YBCO analogy indicates that collective degrees of freedom contribute to the low-energy response of underdoped highTccuprates and it even suggests that the charges in the CuO2planes tend to segregate forming quasi-one-dimensional structures similar to the two-leg ladders, as predicted for the stripe-scenario or certain intertwinned states.
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The role of the crystal lattice for the electronic properties of cuprates and other high-temperature superconductors remains controversial despite decades of theoretical and experimental efforts. While the paradigm of strong electronic correlations suggests a purely electronic mechanism behind the insulator-to-metal transition, recently the mutual enhancement of the electron-electron and the electron-phonon interaction and its relevance to the formation of the ordered phases have also been emphasized. Here, we combine polarization-resolved ultrafast optical spectroscopy and state-of-the-art dynamical mean-field theory to show the importance of the crystal lattice in the breakdown of the correlated insulating state in an archetypal undoped cuprate. We identify signatures of electron-phonon coupling to specific fully symmetric optical modes during the buildup of a three-dimensional (3D) metallic state that follows charge photodoping. Calculations for coherently displaced crystal structures along the relevant phonon coordinates indicate that the insulating state is remarkably unstable toward metallization despite the seemingly large charge-transfer energy scale. This hitherto unobserved insulator-to-metal transition mediated by fully symmetric lattice modes can find extensive application in a plethora of correlated solids.
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In the high spin-orbit-coupled Sr2IrO4, the high sensitivity of the ground state to the details of the local lattice structure shows a large potential for the manipulation of the functional properties by inducing local lattice distortions. We use epitaxial strain to modify the Ir-O bond geometry in Sr2IrO4 and perform momentum-dependent resonant inelastic X-ray scattering (RIXS) at the metal and at the ligand sites to unveil the response of the low-energy elementary excitations. We observe that the pseudospin-wave dispersion for tensile-strained Sr2IrO4 films displays large softening along the [h,0] direction, while along the [h,h] direction it shows hardening. This evolution reveals a renormalization of the magnetic interactions caused by a strain-driven cross-over from anisotropic to isotropic interactions between the magnetic moments. Moreover, we detect dispersive electron-hole pair excitations which shift to lower (higher) energies upon compressive (tensile) strain, manifesting a reduction (increase) in the size of the charge gap. This behavior shows an intimate coupling between charge excitations and lattice distortions in Sr2IrO4, originating from the modified hopping elements between the t2g orbitals. Our work highlights the central role played by the lattice degrees of freedom in determining both the pseudospin and charge excitations of Sr2IrO4 and provides valuable information toward the control of the ground state of complex oxides in the presence of high spin-orbit coupling.
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The interplay between a topological electronic structure and magnetism may result in intricate physics. In this work, we describe a case of rather peculiar coexistence or competition of several magnetic phases below seemingly single antiferromagnetic transition in LnSbTe (Ln = Ho and Tb) topological semimetals, the magnetic members of the ZrSiS/PbFCl structure type (space group P4/nmm). Neutron diffraction experiments reveal a complex multi-step order below TN = 3.8 K (Ln = Ho) and TN = 6.4 K (Ln = Tb). Magnetic phases can be described using four propagation vectors k1 = (1/2 0 0) and k2 = (1/2 0 1/4) at a base temperature of 1.7 K, which transform into incommensurate vectors k1' = (1/2 - δ 0 0) and k3 = (1/2 - δ 0 1/2) at elevated temperatures in both compounds. Together with the refined models of magnetic structures, we present the group theoretical analysis of magnetic symmetry of the proposed solutions. These results prompt further investigations of the relation between the electronic structure of those semimetals and the determined antiferromagnetic ordering existing therein.
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The role of the perovskite lattice oxygen in the oxygen evolution reaction (OER) is systematically studied in the PrBaCo2 O5+δ family. The reduced number of physical/chemical variables combined with in-depth characterizations such as neutron dif-fraction, O K-edge X-ray absorption spectroscopy (XAS), electron energy loss spectroscopy (EELS), magnetization and scanning transmission electron microscopy (STEM) studies, helps investigating the complex correlation between OER activity and a single perovskite property, such as the oxygen content. Larger amount of oxygen vacancies appears to facilitate the OER, possibly contributing to the mechanism involving the oxidation of lattice oxygen, i.e., the lattice oxygen evolution reaction (LOER). Furthermore, not only the number of vacancies but also their local arrangement in the perovskite lattice influences the OER activity, with a clear drop for the more stable, ordered stoichiometry.
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We report the discovery of topological magnetism in the candidate magnetic Weyl semimetal CeAlGe. Using neutron scattering we find this system to host several incommensurate, square-coordinated multi-k[over â] magnetic phases below T_{N}. The topological properties of a phase stable at intermediate magnetic fields parallel to the c axis are suggested by observation of a topological Hall effect. Our findings highlight CeAlGe as an exceptional system for exploiting the interplay between the nontrivial topologies of the magnetization in real space and Weyl nodes in momentum space.
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In this work, we present a new chemical route to synthesize Tm2Mn2O7 pyrochlore, which a compound that is thermodynamically unstable at ambient pressure. Differently from the reported in the past high-pressure synthesis of the same compound applying oxides as starting materials, we have obtained a pure Tm2Mn2O7 phase by a converting TmMnO3 at 1100 °C and an oxygen pressure of 1300 bar. The studies of Tm2Mn2O7 performed by a high-resolution neutron powder diffraction have shown that a pure pyrochlore cubic phase Tm2Mn2O7 (space group Fd3¯m) have been obtained. Upon cooling below 25 K, there is a transition to a ferromagnetically (FM) ordered phase observed with an additional antiferromagnetic (AFM) canting, suggesting a lowering of the initial cubic crystal symmetry. The magnetic transition is accompanied by a small but very visible magnetostriction effect. Using symmetry analysis, we have found a solution for the AFM structure in the maximal Shubnikov subgroup I41/am'd'.
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In quantum magnetic materials, ordered phases induced by an applied magnetic field can be described as the Bose-Einstein condensation (BEC) of magnon excitations. In the strongly frustrated system SrCu2(BO3)2, no clear magnon BEC could be observed, pointing to an alternative mechanism, but the high fields required to probe this physics have remained a barrier to detailed investigation. Here we exploit the first purpose-built high-field neutron scattering facility to measure the spin excitations of SrCu2(BO3)2 up to 25.9 T and use cylinder matrix-product-states (MPS) calculations to reproduce the experimental spectra with high accuracy. Multiple unconventional features point to a condensation of S = 2 bound states into a spin-nematic phase, including the gradients of the one-magnon branches and the persistence of a one-magnon spin gap. This gap reflects a direct analogy with superconductivity, suggesting that the spin-nematic phase in SrCu2(BO3)2 is best understood as a condensate of bosonic Cooper pairs.
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Co-based perovskite oxides are intensively studied as promising catalysts for electrochemical water splitting in an alkaline environment. However, the increasing Co demand by the battery industry is pushing the search for Co-free alternatives. Here we report a systematic study of the Co-free layered perovskite family RBaCuFeO5+δ (R = 4f lanthanide), where we uncover the existence of clear correlations between electrochemical properties and several physicochemical descriptors. Using a combination of advanced neutron and X-ray synchrotron techniques with ab initio DFT calculations we demonstrate and rationalize the positive impact of a large R ionic radius in their oxygen evolution reaction (OER) activity. We also reveal that, in these materials, Fe3+ is the transition metal cation the most prone to donate electrons. We also show that similar R3+/Ba2+ ionic radii favor the incorporation and mobility of oxygen in the layered perovskite structure and increase the number of available O diffusion paths, which have an additional, positive impact on both, the electric conductivity and the OER process. An unexpected result is the observation of a clear surface reconstruction exclusively in oxygen-rich samples (δ > 0), a fact that could be related to their superior OER activity. The encouraging intrinsic OER values obtained for the most active electrocatalyst (LaBaCuFeO5.49), together with the possibility of industrially producing this material in nanocrystalline form should inspire the design of other Co-free oxide catalysts with optimal properties for electrochemical water splitting.
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Charge density wave (CDW) orders in vanadium-based kagome metals have recently received tremendous attention, yet their origin remains a topic of debate. The discovery of ScV6Sn6, a bilayer kagome metal featuring an intriguing [Formula: see text] CDW order, offers a novel platform to explore the underlying mechanism behind the unconventional CDW. Here, we combine high-resolution angle-resolved photoemission spectroscopy, Raman scattering and density functional theory to investigate the electronic structure and phonon modes of ScV6Sn6. We identify topologically nontrivial surface states and multiple van Hove singularities (VHSs) in the vicinity of the Fermi level, with one VHS aligning with the in-plane component of the CDW vector near the [Formula: see text] point. Additionally, Raman measurements indicate a strong electron-phonon coupling, as evidenced by a two-phonon mode and new emergent modes. Our findings highlight the fundamental role of lattice degrees of freedom in promoting the CDW in ScV6Sn6.
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Magnetic skyrmions, topological vortex-like spin textures, garner significant interest due to their unique properties and potential applications in nanotechnology. While they typically form a hexagonal crystal with distinct internal magnetisation textures known as Bloch- or Néel-type, recent theories suggest the possibility for direct transitions between skyrmion crystals of different lattice structures and internal textures. To date however, experimental evidence for these potentially useful phenomena have remained scarce. Here, we discover the polar tetragonal magnet EuNiGe3 to host two hybrid skyrmion phases, each with distinct internal textures characterised by anisotropic combinations of Bloch- and Néel-type windings. Variation of the magnetic field drives a direct transition between the two phases, with the modification of the hybrid texture concomitant with a hexagonal-to-square skyrmion crystal transformation. We explain these observations with a theory that includes the key ingredients of momentum-resolved Ruderman-Kittel-Kasuya-Yosida and Dzyaloshinskii-Moriya interactions that compete at the observed low symmetry magnetic skyrmion crystal wavevectors. Our findings underscore the potential of polar magnets with rich interaction schemes as promising for discovering new topological magnetic phases.
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The microscopic mechanism of heavy band formation, relevant for unconventional superconductivity in CeCoIn5 and other Ce-based heavy fermion materials, depends strongly on the efficiency with which f electrons are delocalized from the rare earth sites and participate in a Kondo lattice. Replacing Ce3+ (4f1, J = 5/2) with Sm3+ (4f5, J = 5/2), we show that a combination of the crystal electric field and on-site Coulomb repulsion causes SmCoIn5 to exhibit a Γ7 ground state similar to CeCoIn5 with multiple f electrons. We show that with this single-ion ground state, SmCoIn5 exhibits a temperature-induced valence crossover consistent with a Kondo scenario, leading to increased delocalization of f holes below a temperature scale set by the crystal field, Tv ≈ 60 K. Our result provides evidence that in the case of many f electrons, the crystal field remains the dominant tuning knob in controlling the efficiency of delocalization near a heavy fermion quantum critical point, and additionally clarifies that charge fluctuations play a general role in the ground state of "115" materials.
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Crystalline symmetry is a defining factor of the electronic band topology in solids, where many-body interactions often induce a spontaneous breaking of symmetry. Superconductors lacking an inversion center are among the best systems to study such effects or even to achieve topological superconductivity. Here, we demonstrate that TRuSi materials (with T a transition metal) belong to this class. Their bulk normal states behave as three-dimensional Kramers nodal-line semimetals, characterized by large antisymmetric spin-orbit couplings and by hourglass-like dispersions. Our muon-spin spectroscopy measurements show that certain TRuSi compounds spontaneously break the time-reversal symmetry at the superconducting transition, while unexpectedly showing a fully gapped superconductivity. Their unconventional behavior is consistent with a unitary (s + ip) pairing, reflecting a mixture of spin singlets and spin triplets. By combining an intrinsic time-reversal symmetry-breaking superconductivity with nontrivial electronic bands, TRuSi compounds provide an ideal platform for investigating the rich interplay between unconventional superconductivity and the exotic properties of Kramers nodal-line/hourglass fermions.
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A state of matter with a multi-component order parameter can give rise to vestigial order. In the vestigial phase, the primary order is only partially melted, leaving a remaining symmetry breaking behind, an effect driven by strong classical or quantum fluctuations. Vestigial states due to primary spin and charge-density-wave order have been discussed in iron-based and cuprate materials. Here we present the observation of a partially melted superconductivity in which pairing fluctuations condense at a separate phase transition and form a nematic state with broken Z3, i.e., three-state Potts-model symmetry. Thermal expansion, specific heat and magnetization measurements of the doped topological insulators NbxBi2Se3 and CuxBi2Se3 reveal that this symmetry breaking occurs at [Formula: see text] above [Formula: see text], along with an onset of superconducting fluctuations. Thus, before Cooper pairs establish long-range coherence at Tc, they fluctuate in a way that breaks the rotational invariance at Tnem and induces a crystalline distortion.
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This article presents a measurement technique and data analysis tool to perform 3D grain distribution mapping and indexing of oligocrystalline samples using neutrons: Laue three-dimensional neutron diffraction (Laue3DND). The approach builds on forward modelling used for correlation and multiple fitting of the measured diffraction spots relative to individual grains. This enables not only to identify individual grains, but also their position and orientation in the sample. The feasibility and performance of the Laue3DND approach are tested using multi-grain synthetic datasets from cubic (α-Fe) and tetragonal (YBaCuFeO5) symmetries. Next, experimental results from two data sets measured at the FALCON instrument of Helmholtz-Zentrum Berlin are presented: A cylindrical alpha iron (α-Fe) reference sample with 5 mm diameter and 5 mm height, as well as a 2 mm3 layered perovskite (YBaCuFeO5). Using Laue3DND, we were able to retrieve the position and orientation of 97 out of 100 grains from a synthetic α-Fe data set, as well as 24 and 9 grains respectively from the α-Fe and YBaCuFeO5 sample measured at FALCON. Results from the synthetic tests also indicate that Laue3DND is capable of indexing 10 out of 10 grains for both symmetries in two extreme scenarios: using only 6 Laue projections and using 360 projections with extremely noisy data. The precision achieved in terms of spatial and orientation resolution for the current version of the method is 430 µm and 1° respectively. Based on these results obtained, we are confident to present a tool that expands the capabilities of standard Laue diffraction, providing the number, position, orientation and relative size of grains in oligocrystalline samples.
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In insulating materials with ordered magnetic spiral phases, ferroelectricity can emerge owing to the breaking of inversion symmetry. This property is of both fundamental and practical interest, particularly with a view to exploiting it in low-power electronic devices. Advances toward technological applications have been hindered, however, by the relatively low ordering temperatures T spiral of most magnetic spiral phases, which rarely exceed 100 K. We have recently established that the ordering temperature of a magnetic spiral can be increased up to 310 K by the introduction of chemical disorder. Here, we explore the design space opened up by this novel mechanism by combining it with a targeted lattice control of some magnetic interactions. In Cu-Fe layered perovskites, we obtain T spiral values close to 400 K, comfortably far from room temperature and almost 100 K higher than using chemical disorder alone. Moreover, we reveal a linear relationship between the spiral's wave vector and the onset temperature of the spiral phase. This linear law ends at a paramagnetic-collinear-spiral triple point, which defines the highest spiral ordering temperature that can be achieved in this class of materials. On the basis of these findings, we propose a general set of rules for designing magnetic spirals in layered perovskites using external pressure, chemical substitutions, and/or epitaxial strain, which should guide future efforts to engineer magnetic spiral phases with ordering temperatures suitable for technological applications.
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In the past years, magnetism-driven ferroelectricity and gigantic magnetoelectric effects have been reported for a number of frustrated magnets featuring ordered spiral magnetic phases. Such materials are of high-current interest due to their potential for spintronics and low-power magnetoelectric devices. However, their low-magnetic ordering temperatures (typically <100 K) greatly restrict their fields of application. Here we demonstrate that the onset temperature of the spiral phase in the perovskite YBaCuFeO5 can be increased by more than 150 K through a controlled manipulation of the Fe/Cu chemical disorder. Moreover, we show that this novel mechanism can stabilize the magnetic spiral state of YBaCuFeO5 above the symbolic value of 25 °C at zero magnetic field. Our findings demonstrate that the properties of magnetic spirals, including its wavelength and stability range, can be engineered through the control of chemical disorder, offering a great potential for the design of materials with magnetoelectric properties beyond room temperature.