X-ray techniques have been used for more than a century to study the atomic and electronic structure in practically any type of material. The advent of correlated electron systems, in particular ...complex oxides, brought about new scientific challenges and opportunities for the advancement of conventional X-ray methods. In this context, the need for new approaches capable of selectively sensing new forms of orders involving all degrees of freedom-charge, orbital, spin, and lattice-paved the way for the emergence and success of resonant X-ray scattering, which has become an increasingly popular and powerful tool for the study of electronic ordering phenomena in solids. We review the recent resonant X-ray scattering breakthroughs in the copper oxide high-temperature superconductors, in particular regarding the phenomenon of charge order, a broken-symmetry state occurring when valence electrons self-organize into periodic structures. After a brief historical perspective on charge order, we outline the milestones in the development of resonant X-ray scattering as well as the basic theoretical formalism underlying its unique capabilities. The rest of the review focuses on the recent contributions of resonant scattering to the advancements in our description and understanding of charge order. To conclude, we propose a series of present and upcoming challenges and discuss the future outlook for this technique.
Electronic flat bands in momentum space, arising from strong localization of electrons in real space, are an ideal stage to realize strongly-correlated phenomena. Theoretically, the flat bands can ...naturally arise in certain geometrically frustrated lattices, often with nontrivial topology if combined with spin-orbit coupling. Here, we report the observation of topological flat bands in frustrated kagome metal CoSn, using angle-resolved photoemission spectroscopy and band structure calculations. Throughout the entire Brillouin zone, the bandwidth of the flat band is suppressed by an order of magnitude compared to the Dirac bands originating from the same orbitals. The frustration-driven nature of the flat band is directly confirmed by the chiral d-orbital texture of the corresponding real-space Wannier functions. Spin-orbit coupling opens a large gap of 80 meV at the quadratic touching point between the Dirac and flat bands, endowing a nonzero Z
invariant to the flat band. These findings demonstrate that kagome-derived flat bands are a promising platform for novel emergent phases of matter at the confluence of strong correlation and topology.
Photovoltaic devices based on lead iodide perovskite films have seen rapid advancements, recently achieving an impressive 17.9% certified solar power conversion efficiency. Reports have consistently ...emphasized that the specific choice of growth conditions and chemical precursors is central to achieving superior performance from these materials; yet the roles and mechanisms underlying the selection of materials processing route is poorly understood. Here we show that films grown under iodine-rich conditions are prone to a high density of deep electronic traps (recombination centers), while the use of a chloride precursor avoids the formation of key defects (Pb atom substituted by I) responsible for short diffusion lengths and poor photovoltaic performance. Furthermore, the lowest-energy surfaces of perovskite crystals are found to be entirely trap-free, preserving both electron and hole delocalization to a remarkable degree, helping to account for explaining the success of polycrystalline perovskite films. We construct perovskite films from I-poor conditions using a lead acetate precursor, and our measurement of a long (600 ± 40 nm) diffusion length confirms this new picture of the importance of growth conditions.
Hybrid perovskites are promising semiconductors for optoelectronic applications. However, they suffer from morphological disorder that limits their optoelectronic properties and, ultimately, device ...performance. Recently, perovskite single crystals have been shown to overcome this problem and exhibit impressive improvements: low trap density, low intrinsic carrier concentration, high mobility, and long diffusion length that outperform perovskite-based thin films. These characteristics make the material ideal for realizing photodetection that is simultaneously fast and sensitive; unfortunately, these macroscopic single crystals cannot be grown on a planar substrate, curtailing their potential for optoelectronic integration. Here we produce large-area planar-integrated films made up of large perovskite single crystals. These crystalline films exhibit mobility and diffusion length comparable with those of single crystals. Using this technique, we produced a high-performance light detector showing high gain (above 10(4) electrons per photon) and high gain-bandwidth product (above 10(8) Hz) relative to other perovskite-based optical sensors.
A two‐step ligand‐exchange strategy is developed, in which the long‐carbon‐ chain ligands on all‐inorganic perovskite (CsPbX3, X = Br, Cl) quantum dots (QDs) are replaced with halide‐ion‐pair ...ligands. Green and blue light‐emitting diodes made from the halide‐ion‐pair‐capped quantum dots exhibit high external quantum efficiencies compared with the untreated QDs.
The fundamental properties and ultimate performance limits of organolead trihalide MAPbX3 (MA = CH3NH3+; X = Br– or I–) perovskites remain obscured by extensive disorder in polycrystalline MAPbX3 ...films. We report an antisolvent vapor-assisted crystallization approach that enables us to create sizable crack-free MAPbX3 single crystals with volumes exceeding 100 cubic millimeters. These large single crystals enabled a detailed characterization of their optical and charge transport characteristics. We observed exceptionally low trap-state densities on the order of 109 to 1010 per cubic centimeter in MAPbX3 single crystals (comparable to the best photovoltaic-quality silicon) and charge carrier diffusion lengths exceeding 10 micrometers. These results were validated with density functional theory calculations.
Abstract
In ultrathin films of FeSe grown on SrTiO
3
(FeSe/STO), the superconducting transition temperature
T
c
is increased by almost an order of magnitude, raising questions on the pairing ...mechanism. As in other superconductors, antiferromagnetic spin fluctuations have been proposed to mediate SC making it essential to study the evolution of the spin dynamics of FeSe from the bulk to the ultrathin limit. Here, we investigate the spin excitations in bulk and monolayer FeSe/STO using resonant inelastic x-ray scattering (RIXS) and quantum Monte Carlo (QMC) calculations. Despite the absence of long-range magnetic order, bulk FeSe displays dispersive magnetic excitations reminiscent of other Fe-pnictides. Conversely, the spin excitations in FeSe/STO are gapped, dispersionless, and significantly hardened relative to its bulk counterpart. By comparing our RIXS results with simulations of a bilayer Hubbard model, we connect the evolution of the spin excitations to the Fermiology of the two systems revealing a remarkable reconfiguration of spin excitations in FeSe/STO, essential to understand the role of spin fluctuations in the pairing mechanism.
Earth-abundant first-row (3d) transition metal–based catalysts have been developed for the oxygen-evolution reaction (OER); however, they operate at overpotentials substantially above thermodynamic ...requirements. Density functional theory suggested that non-3d high-valency metals such as tungsten can modulate 3d metal oxides, providing near-optimal adsorption energies for OER intermediates. We developed a room-temperature synthesis to produce gelled oxyhydroxides materials with an atomically homogeneous metal distribution. These gelled FeCoW oxyhydroxides exhibit the lowest overpotential (191 millivolts) reported at 10 milliamperes per square centimeter in alkaline electrolyte. The catalyst shows no evidence of degradation after more than 500 hours of operation. X-ray absorption and computational studies reveal a synergistic interplay between tungsten, iron, and cobalt in producing a favorable local coordination environment and electronic structure that enhance the energetics for OER.
PDF
