Local negative permittivity and topological phase transition in polar skyrmions.

Topological solitons such as magnetic skyrmions have drawn attention as stable quasi-particle-like objects. The recent discovery of polar vortices and skyrmions in ferroelectric oxide superlattices has opened up new vistas to explore topology, emergent phenomena and approaches for manipulating such features with electric fields. Using macroscopic dielectric measurements, coupled with direct scanning convergent beam electron diffraction imaging on the atomic scale, theoretical phase-field simulations and second-principles calculations, we demonstrate that polar skyrmions in (PbTiO3)n/(SrTiO3)n superlattices are distinguished by a sheath of negative permittivity at the periphery of each skyrmion. This enhances the effective dielectric permittivity compared with the individual SrTiO3 and PbTiO3 layers. Moreover, the response of these topologically protected structures to electric field and temperature shows a reversible phase transition from the skyrmion state to a trivial uniform ferroelectric state, accompanied by large tunability of the dielectric permittivity. Pulsed switching measurements show a time-dependent evolution and recovery of the skyrmion state (and macroscopic dielectric response). The interrelationship between topological and dielectric properties presents an opportunity to simultaneously manipulate both by a single, and easily controlled, stimulus, the applied electric field.

Charge Condensation and Lattice Coupling Drives Stripe Formation in Nickelates.

Revealing the predominant driving force behind symmetry breaking in correlated materials is sometimes a formidable task due to the intertwined nature of different degrees of freedom. This is the case for La_{2-x}Sr_{x}NiO_{4+δ}, in which coupled incommensurate charge and spin stripes form at low temperatures. Here, we use resonant x-ray photon correlation spectroscopy to study the temporal stability and domain memory of the charge and spin stripes in La_{2-x}Sr_{x}NiO_{4+δ}. Although spin stripes are more spatially correlated, charge stripes maintain a better temporal stability against temperature change. More intriguingly, charge order shows robust domain memory with thermal cycling up to 250 K, far above the ordering temperature. These results demonstrate the pinning of charge stripes to the lattice and that charge condensation is the predominant factor in the formation of stripe orders in nickelates.

Strong Superexchange in a d

The discovery of superconductivity in a d^{9-δ} nickelate has inspired disparate theoretical perspectives regarding the essential physics of this class of materials. A key issue is the magnitude of the magnetic superexchange, which relates to whether cuprate-like high-temperature nickelate superconductivity could be realized. We address this question using Ni L-edge and O K-edge spectroscopy of the reduced d^{9-1/3} trilayer nickelates R_{4}Ni_{3}O_{8} (where R=La, Pr) and associated theoretical modeling. A magnon energy scale of ∼80 meV resulting from a nearest-neighbor magnetic exchange of J=69(4) meV is observed, proving that d^{9-δ} nickelates can host a large superexchange. This value, along with that of the Ni-O hybridization estimated from our O K-edge data, implies that trilayer nickelates represent an intermediate case between the infinite-layer nickelates and the cuprates. Layered nickelates thus provide a route to testing the relevance of superexchange to nickelate superconductivity.

Nucleation and Growth Bottleneck in the Conductivity Recovery Dynamics of Nickelate Ultrathin Films.

We investigate THz conductivity dynamics in NdNiO3 and EuNiO3 ultrathin films (15 unit cells, u.c., ∼5.7 nm thick) following a photoinduced thermal quench into the metallic state and reveal a clear contrast between first- and second-order dynamics. While in EuNiO3 the conductivity recovers exponentially, in NdNiO3 the recovery is nonexponential and slower than a simple thermal model. Crucially, it is consistent with first-order dynamics and well-described by a 2d Avrami model, with supercooling leading to metastable phase coexistence on the nano- to mesoscopic scale. This novel observation is a fundamentally dynamic manifestation of the first-order character of the insulator-to-metal transition, which the nanoscale thickness of our films and their fast cooling rate enable us to detect. The large transients seen in our films are promising for fast electronic (and magnetic) switching applications.

Direct Evidence of the Competing Nature between Electronic and Lattice Breathing Order in Rare-Earth Nickelates.

Correlated electrons give rise to both exotic electronic and magnetic properties in rare-earth nickelates. Here we present evidence of the interfacial coupling between two nickelate systems, EuNiO_{3} (ENO) and LaNiO_{3} (LNO), with different electronic and magnetic properties but with compatible structural registry giving rise to an electrostructural transition, unobserved in each constituent. Nominally, LNO remains in a paramagnetic-metallic R3[over ¯]c phase while orthorhombic ENO undergoes antiferromagnetic and insulating transitions. However, the ENO/LNO heterostructure displays a uniform rotational symmetry set by an entwined interface. This leads to an anomalous reduction of bond disproportionation in the ENO layer through the metal to insulator transition and concomitantly charge disproportionation opens the gap accompanied by antiferromagnetic ordering. Our results resolve a long-standing question in the physics of rare-earth nickelates, herein demonstrating that charge and bond disproportionation are competing mechanisms for the charge localization process in the rare-earth nickelate system.

Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective.

Many remarkable properties of quantum materials emerge from states with intricate coupling between the charge, spin and orbital degrees of freedom. Ultrafast photo-excitation of these materials holds great promise for understanding and controlling the properties of these states. Here, we introduce time-resolved resonant inelastic X-ray scattering (tr-RIXS) as a means of measuring the charge, spin and orbital excitations out of equilibrium. These excitations encode the correlations and interactions that determine the detailed properties of the states generated. After outlining the basic principles and instrumentations of tr-RIXS, we review our first observations of transient antiferromagnetic correlations in quasi two dimensions in a photo-excited Mott insulator and present possible future routes of this fast-developing technique. The increasing number of X-ray free electron laser facilities not only enables tackling long-standing fundamental scientific problems, but also promises to unleash novel inelastic X-ray scattering spectroscopies. This article is part of the theme issue 'Measurement of ultrafast electronic and structural dynamics with X-rays'.

Complex association patterns for inflammatory mediators in induced sputum from subjects with asthma.

BACKGROUND: The release of various inflammatory mediators into the bronchial lumen is thought to reflect both the type and degree of airway inflammation, eosinophilic Th2, and Th9, or neutrophilic Th1, and Th17, in patients with asthma. AIMS: We investigated whether cytokines and chemokines differed in sputum from subjects with more severe compared with milder asthma and whether unbiased factor analysis of cytokine and chemokine groupings indicates specific inflammatory pathways. METHODS: Cell-free supernatants from induced sputum were obtained from subjects with a broad range of asthma severity (n = 158) and assessed using Milliplex® Cytokines/Chemokine kits I, II and III, measuring 75 individual proteins. Each cytokine, chemokine or growth factor concentration was examined for differences between asthma severity groups, for association with leucocyte counts, and by factor analysis. RESULTS: Severe asthma subjects had 9 increased and 4 decreased proteins compared to mild asthma subjects and fewer differences compared to moderate asthma. Twenty-six mediators were significantly associated with an increasing single leucocyte type: 16 with neutrophils (3 interleukins [IL], 3 CC chemokines, 4 CXC chemokines, 4 growth factors, TNF-α and CX3CL1/Fractalkine); 5 with lymphocytes (IL-7, IL-16, IL-23, IFN-α2 and CCL4/MIP1ß); IL-15 and CCL15/MIP1δ with macrophages; IL-5 with eosinophils; and IL-4 and TNFSF10/TRAIL with airway epithelial cells. Factor analysis grouped 43 cytokines, chemokines and growth factors which had no missing data onto the first 10 factors, containing mixes of Th1, Th2, Th9 and Th17 inflammatory and anti-inflammatory proteins. CONCLUSIONS: Sputum cytokines, chemokines and growth factors were increased in severe asthma, primarily with increased neutrophils. Factor analysis identified complex inflammatory protein interactions, suggesting airway inflammation in asthma is characterized by overlapping immune pathways. Thus, focus on a single specific inflammatory mediator or pathway may limit understanding the complexity of inflammation underlying airway changes in asthma and selection of appropriate therapy.

Observation of Double Weyl Phonons in Parity-Breaking FeSi.

Condensed matter systems have now become a fertile ground to discover emerging topological quasiparticles with symmetry protected modes. While many studies have focused on fermionic excitations, the same conceptual framework can also be applied to bosons yielding new types of topological states. Motivated by Zhang et al.'s recent theoretical prediction of double Weyl phonons in transition metal monosilicides [Phys. Rev. Lett. 120, 016401 (2018)PRLTAO0031-900710.1103/PhysRevLett.120.016401], we directly measure the phonon dispersion in parity-breaking FeSi using inelastic x-ray scattering. By comparing the experimental data with theoretical calculations, we make the first observation of double Weyl points in FeSi, which will be an ideal material to explore emerging bosonic excitations and its topologically nontrivial properties.

Disentangled Cooperative Orderings in Artificial Rare-Earth Nickelates.

Coupled transitions between distinct ordered phases are important aspects behind the rich phase complexity of correlated oxides that hinder our understanding of the underlying phenomena. For this reason, fundamental control over complex transitions has become a leading motivation of the designer approach to materials. We have devised a series of new superlattices by combining a Mott insulator and a correlated metal to form ultrashort period superlattices, which allow one to disentangle the simultaneous orderings in RENiO_{3}. Tailoring an incommensurate heterostructure period relative to the bulk charge ordering pattern suppresses the charge order transition while preserving metal-insulator and antiferromagnetic transitions. Such selective decoupling of the entangled phases resolves the long-standing puzzle about the driving force behind the metal-insulator transition and points to the site-selective Mott transition as the operative mechanism. This designer approach emphasizes the potential of heterointerfaces for selective control of simultaneous transitions in complex materials with entwined broken symmetries.

Decoupling Carrier Concentration and Electron-Phonon Coupling in Oxide Heterostructures Observed with Resonant Inelastic X-Ray Scattering.

We report the observation of multiple phonon satellite features in ultrathin superlattices of the form nSrIrO_{3}/mSrTiO_{3} using resonant inelastic x-ray scattering (RIXS). As the values of n and m vary, the energy loss spectra show a systematic evolution in the relative intensity of the phonon satellites. Using a closed-form solution for the RIXS cross section, we extract the variation in the electron-phonon coupling strength as a function of n and m. Combined with the negligible carrier doping into the SrTiO_{3} layers, these results indicate that the tuning of the electron-phonon coupling can be effectively decoupled from doping. This work both showcases a feasible method to extract the electron-phonon coupling in superlattices and unveils a potential route for tuning this coupling, which is often associated with superconductivity in SrTiO_{3}-based systems.

Two-Dimensional J_{eff}=1/2 Antiferromagnetic Insulator Unraveled from Interlayer Exchange Coupling in Artificial Perovskite Iridate Superlattices.

We report an experimental investigation of the two-dimensional J_{eff}=1/2 antiferromagnetic Mott insulator by varying the interlayer exchange coupling in [(SrIrO_{3})_{1}, (SrTiO_{3})_{m}] (m=1, 2 and 3) superlattices. Although all samples exhibited an insulating ground state with long-range magnetic order, temperature-dependent resistivity measurements showed a stronger insulating behavior in the m=2 and m=3 samples than the m=1 sample which displayed a clear kink at the magnetic transition. This difference indicates that the blocking effect of the excessive SrTiO_{3} layer enhances the effective electron-electron correlation and strengthens the Mott phase. The significant reduction of the Néel temperature from 150 K for m=1 to 40 K for m=2 demonstrates that the long-range order stability in the former is boosted by a substantial interlayer exchange coupling. Resonant x-ray magnetic scattering revealed that the interlayer exchange coupling has a switchable sign, depending on the SrTiO_{3} layer number m, for maintaining canting-induced weak ferromagnetism. The nearly unaltered transition temperature between the m=2 and the m=3 demonstrated that we have realized a two-dimensional antiferromagnet at finite temperatures with diminishing interlayer exchange coupling.

Doping Dependence of Collective Spin and Orbital Excitations in the Spin-1 Quantum Antiferromagnet La_{2-x}Sr_{x}NiO_{4} Observed by X Rays.

We report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to collective magnetic excitations in S=1 systems by probing the Ni L_{3} edge of La_{2-x}Sr_{x}NiO_{4} (x=0, 0.33, 0.45). The magnetic excitation peak is asymmetric, indicating the presence of single and multi-spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. This work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultrafast pump-probe experiments.

Magnetic Interactions at the Nanoscale in Trilayer Titanates.

We report on the phase diagram of competing magnetic interactions at the nanoscale in engineered ultrathin trilayer heterostructures of LaTiO_{3}/SrTiO_{3}/YTiO_{3}, in which the interfacial inversion symmetry is explicitly broken. Combined atomic layer resolved scanning transmission electron microscopy with electron energy loss spectroscopy and electrical transport have confirmed the formation of a spatially separated two-dimensional electron liquid and high density two-dimensional localized magnetic moments at the LaTiO_{3}/SrTiO_{3} and SrTiO_{3}/YTiO_{3} interfaces, respectively. Resonant soft x-ray linear dichroism spectroscopy has demonstrated the presence of orbital polarization of the conductive LaTiO_{3}/SrTiO_{3} and localized SrTiO_{3}/YTiO_{3} electrons. Our results provide a route with prospects for exploring new magnetic interfaces, designing a tunable two-dimensional d-electron Kondo lattice, and potential spin Hall applications.

Mott Electrons in an Artificial Graphenelike Crystal of Rare-Earth Nickelate.

Deterministic control over the periodic geometrical arrangement of the constituent atoms is the backbone of the material properties, which, along with the interactions, define the electronic and magnetic ground state. Following this notion, a bilayer of a prototypical rare-earth nickelate, NdNiO_{3}, combined with a dielectric spacer, LaAlO_{3}, has been layered along the pseudocubic [111] direction. The resulting artificial graphenelike Mott crystal with magnetic 3d electrons has antiferromagnetic correlations. In addition, a combination of resonant X-ray linear dichroism measurements and ab initio calculations reveal the presence of an ordered orbital pattern, which is unattainable in either bulk nickelates or nickelate based heterostructures grown along the [001] direction. These findings highlight another promising venue towards designing new quantum many-body states by virtue of geometrical engineering.

Orbital Engineering in Nickelate Heterostructures Driven by Anisotropic Oxygen Hybridization rather than Orbital Energy Levels.

Resonant inelastic x-ray scattering is used to investigate the electronic origin of orbital polarization in nickelate heterostructures taking LaTiO_{3}-LaNiO_{3}-3×(LaAlO_{3}), a system with exceptionally large polarization, as a model system. We find that heterostructuring generates only minor changes in the Ni 3d orbital energy levels, contradicting the often-invoked picture in which changes in orbital energy levels generate orbital polarization. Instead, O K-edge x-ray absorption spectroscopy demonstrates that orbital polarization is caused by an anisotropic reconstruction of the oxygen ligand hole states. This provides an explanation for the limited success of theoretical predictions based on tuning orbital energy levels and implies that future theories should focus on anisotropic hybridization as the most effective means to drive large changes in electronic structure and realize novel emergent phenomena.

Slater Insulator in Iridate Perovskites with Strong Spin-Orbit Coupling.

The perovskite SrIrO_{3} is an exotic narrow-band metal owing to a confluence of the strengths of the spin-orbit coupling (SOC) and the electron-electron correlations. It has been proposed that topological and magnetic insulating phases can be achieved by tuning the SOC, Hubbard interactions, and/or lattice symmetry. Here, we report that the substitution of nonmagnetic, isovalent Sn^{4+} for Ir^{4+} in the SrIr_{1-x}Sn_{x}O_{3} perovskites synthesized under high pressure leads to a metal-insulator transition to an antiferromagnetic (AF) phase at T_{N}≥225 K. The continuous change of the cell volume as detected by x-ray diffraction and the λ-shape transition of the specific heat on cooling through T_{N} demonstrate that the metal-insulator transition is of second order. Neutron powder diffraction results indicate that the Sn substitution enlarges an octahedral-site distortion that reduces the SOC relative to the spin-spin exchange interaction and results in the type-G AF spin ordering below T_{N}. Measurement of high-temperature magnetic susceptibility shows the evolution of magnetic coupling in the paramagnetic phase typical of weak itinerant-electron magnetism in the Sn-substituted samples. A reduced structural symmetry in the magnetically ordered phase leads to an electron gap opening at the Brillouin zone boundary below T_{N} in the same way as proposed by Slater.

Novel Electronic Behavior Driving NdNiO3 Metal-Insulator Transition.

We present evidence that the metal-insulator transition (MIT) in a tensile-strained NdNiO3 (NNO) film is facilitated by a redistribution of electronic density and that it neither requires Ni charge disproportionation nor a symmetry change [U. Staub et al., Phys. Rev. Lett. 88, 126402 (2002); R. Jaramillo et al., Nat. Phys. 10, 304 (2014)]. Given that epitaxial tensile strain in thin NNO films induces preferential occupancy of the e(g) d(x(2)-y(2)) orbital we propose that the larger transfer integral of this orbital state with the O 2p orbital state mediates a redistribution of electronic density from the Ni atom. A decrease in the Ni d(x(2)-y(2)) orbital occupation is directly observed by resonant inelastic x-ray scattering below the MIT temperature. Furthermore, an increase in the Nd charge occupancy is measured by x-ray absorption at the Nd L(3) edge. Both spin-orbit coupling and crystal field effects combine to break the degeneracy of the Nd 5d states, shifting the energy of the Nd e(g) d(x(2)-y(2)) orbit towards the Fermi level, allowing the A site to become an active acceptor during the MIT. This work identifies the relocation of electrons from the Ni 3d to the Nd 5d orbitals across the MIT. We propose that the insulating gap opens between the Ni 3d and O 2p states, resulting from Ni 3d electron localization. The transition seems to be neither a purely Mott-Hubbard transition nor a simple charge transfer.

eQTL of bronchial epithelial cells and bronchial alveolar lavage deciphers GWAS-identified asthma genes.

BACKGROUND: Genome-wide association studies (GWASs) have identified various genes associated with asthma, yet, causal genes or single nucleotide polymorphisms (SNPs) remain elusive. We sought to dissect functional genes/SNPs for asthma by combining expression quantitative trait loci (eQTLs) and GWASs. METHODS: Cis-eQTL analyses of 34 asthma genes were performed in cells from human bronchial epithelial biopsy (BEC, n = 107) and from bronchial alveolar lavage (BAL, n = 94). RESULTS: For TSLP-WDR36 region, rs3806932 (G allele protective against eosinophilic esophagitis) and rs2416257 (A allele associated with lower eosinophil counts and protective against asthma) were correlated with decreased expression of TSLP in BAL (P = 7.9 × 10(-11) and 5.4 × 10(-4) , respectively) and BEC, but not WDR36. Surprisingly, rs1837253 (consistently associated with asthma) showed no correlation with TSLP expression levels. For ORMDL3-GSDMB region, rs8067378 (G allele protective against asthma) was correlated with decreased expression of GSDMB in BEC and BAL (P = 1.3 × 10(-4) and 0.04) but not ORMDL3. rs992969 in the promoter region of IL33 (A allele associated with higher eosinophil counts and risk for asthma) was correlated with increased expression of IL33 in BEC (P = 1.3 × 10(-6) ) but not in BAL. CONCLUSIONS: Our study illustrates cell-type-specific regulation of the expression of asthma-related genes documenting SNPs in TSLP, GSDMB, IL33, HLA-DQB1, C11orf30, DEXI, CDHR3, and ZBTB10 affect asthma risk through cis-regulation of its gene expression. Whenever possible, disease-relevant tissues should be used for transcription analysis. SNPs in TSLP may affect asthma risk through up-regulating TSLP mRNA expression or protein secretion. Further functional studies are warranted.

Preponderance of toxigenic Escherichia coli in stool pathogens correlates with toxin detection in accessible drinking-water sources.

Since early detection of pathogens and their virulence factors contribute to intervention and control strategies, we assessed the enteropathogens in diarrhoea disease and investigated the link between toxigenic strains of Escherichia coli from stool and drinking-water sources; and determined the expression of toxin genes by antibiotic-resistant E. coli in Lagos, Nigeria. This was compared with isolates from diarrhoeal stool and water from Wisconsin, USA. The new Luminex xTAG GPP (Gastroplex) technique and conventional real-time PCR were used to profile enteric pathogens and E. coli toxin gene isolates, respectively. Results showed the pathogen profile of stool and indicated a relationship between E. coli toxin genes in water and stool from Lagos which was absent in Wisconsin isolates. The Gastroplex technique was efficient for multiple enteric pathogens and toxin gene detection. The co-existence of antibiotic resistance with enteroinvasive E. coli toxin genes suggests an additional prognostic burden on patients.