Discerning charge patterns in a cuprate Copper oxides are well known to be able to achieve the order required for superconductivity. They can also achieve another order—one that produces patterns in their charge density. Experiments using nuclear magnetic resonanceand resonant x-ray scattering have both detected this so-called charge density wave (CDW) in yttrium-based cuprates. However, the nature of the CDW appeared to be different in the two types of measurement. Gerber et al. used pulsed magnetic fields of up to 28 T, combined with scattering, to bridge the gap (see the Perspective by Julien). As the magnetic field increased, a two-dimensional CDW gave way to a three-dimensional one. Science , this issue p. 949 ; see also p. 914
The interactions that lead to the emergence of superconductivity in iron-based materials remain a subject of debate. It has been suggested that electron-electron correlations enhance electron-phonon coupling in iron selenide (FeSe) and related pnictides, but direct experimental verification has been lacking. Here we show that the electron-phonon coupling strength in FeSe can be quantified by combining two time-domain experiments into a "coherent lock-in" measurement in the terahertz regime. X-ray diffraction tracks the light-induced femtosecond coherent lattice motion at a single phonon frequency, and photoemission monitors the subsequent coherent changes in the electronic band structure. Comparison with theory reveals a strong enhancement of the coupling strength in FeSe owing to correlation effects. Given that the electron-phonon coupling affects superconductivity exponentially, this enhancement highlights the importance of the cooperative interplay between electron-electron and electron-phonon interactions.
The existence of charge-density-wave (CDW) correlations in cuprate superconductors has now been established. However, the nature of the CDW ground state has remained uncertain because disorder and the presence of superconductivity typically limit the CDW correlation lengths to only a dozen unit cells or less. Here we explore the field-induced 3D CDW correlations in extremely pure detwinned crystals of YBa 2 Cu 3 Ox (YBCO) ortho-II and ortho-VIII at magnetic fields in excess of the resistive upper critical field (H c2 ) where superconductivity is heavily suppressed. We observe that the 3D CDW is unidirectional and possesses a long in-plane correlation length as well as significant correlations between neighboring CuO 2 planes. It is significant that we observe only a single sharply defined transition at a critical field proportional to H c2 , given that the field range used in this investigation overlaps with other high-field experiments including quantum oscillation measurements. The correlation volume is at least two to three orders of magnitude larger than that of the zero-field CDW. This is by far the largest CDW correlation volume observed in any cuprate crystal and so is presumably representative of the high-field ground state of an "ideal" disorder-free cuprate.high-temperature superconductors | charge-density-wave order | high magnetic field X-ray scattering | vestigial nematic order | competing order C harge-density-wave (CDW) order has been found to exist universally in the hole-doped superconducting cuprates (1-18), and the common characteristics at zero magnetic field include bidirectionality, quasi-2D and short-ranged correlations (7-17). More specifically, the CDW diffraction patterns are found in both directions of Cu-O bonds in the CuO2 plane (Fig. 1A), and the CDW correlation lengths parallel and perpendicular to the planes (i.e., along the a-or b-axes and the c axis) are less than ∼ 20 and ∼ 1 lattice constants, respectively (7-16), corresponding to a correlation volume of order 10 2 unit cells (UCs). Thus, the properties of the quasi-2D CDW are likely strongly affected by disorder and only indirectly represent the true nature of the underlying CDW correlations. Indeed, X-ray scattering shows that the onset of the quasi-2D order is gradual without a sharp transition (7-17), consistent with the influence of quenched disorder on an incommensurate CDW (19-21). Furthermore, whereas Y-based and La-based cuprates exhibit a clear competition between CDW and superconductivity (7,8,(12)(13)(14)(15), such competition is not apparent in the families of Bi-based and Hg-based cuprate compounds (9-11)-a discrepancy that probably reflects different degrees of quenched disorder among cuprate families.Recently, a CDW with significantly longer correlation lengths was observed in superconducting YBCO (Fig. 1B) via X-ray scattering at high magnetic fields (13,14). This reveals the character (i.e., 3D) of the high-field charge ordering previously inferred by other measurements (3-6). At a magnetic field of ∼ 30 T, i...
The electrochemical oxygen evolution reaction (OER) is an important anodic process in water splitting and CO2 reduction applications. Precious metals including Ir, Ru. and Pt are traditional OER catalysts, but recent emphasis has been placed on finding less expensive, earth-abundant materials with high OER activity. Ni-based materials are promising next-generation OER catalysts because they show high reaction rates and good long-term stability. Unfortunately, most catalyst samples contain heterogeneous particle sizes and surface structures that produce a range of reaction rates and rate-determining steps. Here we use a combination of experimental and computational techniques to study the OER at a supported organometallic nickel complex with a precisely known crystal structure. The Ni6(PET)12 (PET = phenylethyl thiol) complex out performed bulk NiO and Pt and showed OER activity comparable to Ir. Density functional theory (DFT) analysis of electrochemical OER at a realistic Ni6(SCH3)12 model determined the Gibbs free energy change (ΔG) associated with each mechanistic step. This allowed computational prediction of potential determining steps and OER onset potentials that were in excellent agreement with experimentally determined values. Moreover, DFT found that small changes in adsorbate binding configuration can shift the potential determining step within the OER mechanism and drastically change onset potentials. Our work shows that atomically precise nanocatalysts like Ni6(PET)12 facilitate joint experimental and computational studies because experimentalists and theorists can study nearly identical systems. These types of efforts can identify atomic-level structure–property relationships that would be difficult to obtain with traditional heterogeneous catalyst samples.
Heavy-fermion metals exhibit a plethora of low-temperature ordering phenomena . Among these are the so-called hidden-order phases that, in contrast to conventional magnetic order, are invisible to standard neutron diffraction experiments. One of the structurally most simple hidden-order compounds, CeB6, has been intensively studied for an elusive phase that was attributed to the antiferroquadrupolar ordering of cerium-4f moments . As the ground state of CeB6 is characterized by a more conventional antiferromagnetic (AFM) order , the low-temperature physics of this system has generally been assumed to be governed solely by AFM interactions between the dipolar and multipolar Ce moments . Here we overturn this established picture by observing an intense ferromagnetic (FM) low-energy collective mode that dominates the magnetic excitation spectrum of CeB6. Inelastic neutron-scattering data reveal that the intensity of this FM excitation significantly exceeds that of conventional spin-wave magnons emanating from the AFM wavevectors, thus placing CeB6 much closer to a FM instability than previously anticipated. This propensity for ferromagnetism may account for much of the unexplained behaviour of CeB6, and should lead to a re-examination of existing theories that have so far largely neglected the role of FM interactions.
Non-noble-metal, thin-film oxides are widely investigated as promising catalysts for oxygen evolution reactions (OER). Amorphous cobalt oxide films electrochemically formed in the presence of borate (CoBi) and phosphate (CoPi) share a common cobaltate domain building block, but differ significantly in OER performance that derives from different electron-proton charge transport properties. Here, we use a combination of L edge synchrotron X-ray absorption (XAS), resonant X-ray emission (RXES), resonant inelastic X-ray scattering (RIXS), resonant Raman (RR) scattering, and high-energy X-ray pair distribution function (PDF) analyses that identify electronic and structural factors correlated to the charge transport differences for CoPi and CoBi. The analyses show that CoBi is composed primarily of cobalt in octahedral coordination, whereas CoPi contains approximately 17% tetrahedral Co(II), with the remainder in octahedral coordination. Oxygen-mediated 4 p-3 d hybridization through Co-O-Co bonding was detected by RXES and the intersite dd excitation was observed by RIXS in CoBi, but not in CoPi. RR shows that CoBi resembles a disordered layered LiCoO-like structure, whereas CoPi is amorphous. Distinct domain models in the nanometer range for CoBi and CoPi have been proposed on the basis of the PDF analysis coupled to XAS data. The observed differences provide information on electronic and structural factors that enhance oxygen evolving catalysis performance.
The discovery of charge- and spin-density-wave (CDW/SDW) orders in superconducting cuprates has altered our perspective on the nature of high-temperature superconductivity (SC). However, it has proven difficult to fully elucidate the relationship between the density wave orders and SC. Here, using resonant soft X-ray scattering, we study the archetypal cuprate La 2- x Sr x CuO 4 (LSCO) over a broad doping range. We reveal the existence of two types of CDW orders in LSCO, namely CDW stripe order and CDW short-range order (SRO). While the CDW-SRO is suppressed by SC, it is partially transformed into the CDW stripe order with developing SDW stripe order near the superconducting T c . These findings indicate that the stripe orders and SC are inhomogeneously distributed in the superconducting CuO 2 planes of LSCO. This further suggests a new perspective on the putative pair-density-wave order that coexists with SC, SDW, and CDW orders.
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