Absence of 3a0 charge density wave order in the infinite-layer nickelate NdNiO2.

A hallmark of many unconventional superconductors is the presence of many-body interactions that give rise to broken-symmetry states intertwined with superconductivity. Recent resonant soft X-ray scattering experiments report commensurate 3a0 charge density wave order in infinite-layer nickelates, which has important implications regarding the universal interplay between charge order and superconductivity in both cuprates and nickelates. Here we present X-ray scattering and spectroscopy measurements on a series of NdNiO2+x samples, which reveal that the signatures of charge density wave order are absent in fully reduced, single-phase NdNiO2. The 3a0 superlattice peak instead originates from a partially reduced impurity phase where excess apical oxygens form ordered rows with three-unit-cell periodicity. The absence of any observable charge density wave order in NdNiO2 highlights a crucial difference between the phase diagrams of cuprate and nickelate superconductors.

Evolution of superconductivity in K2-xFe4+ySe5: Spectroscopic studies of X-ray absorption and emission.

This study investigates the evolution of superconductivity in K2-xFe4+ySe5 using temperature-dependent X-ray absorption and resonant inelastic X-ray scattering techniques. Magnetization measurements show that polycrystalline superconducting (SC) K1.9Fe4.2Se5 has a critical temperature (T c) of ∼31 K with a varying superconducting volume fraction, which strongly depends on its synthesis temperature. An increase in Fe-structural/vacancy disorder in SC samples with more Fe atoms occupying vacant 4d sites is found to be closely related to the decrease in the spin magnetic moment of Fe. Moreover, the nearest-neighbor Fe-Se bond length in SC samples exceeds that in the non-SC (NS) sample, K2Fe4Se5, which indicates a weaker hybridization between the Fe 3d and Se 4p states in SC samples. These results clearly demonstrate the correlations among the local electronic and atomic structures and the magnetic properties of K2-xFe4+ySe5 superconductors, providing deeper insight into the electron pairing mechanisms of superconductivity.

Publisher Correction: Electronic structure of the parent compound of superconducting infinite-layer nickelates.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Electronic structure of the parent compound of superconducting infinite-layer nickelates.

The search continues for nickel oxide-based materials with electronic properties similar to cuprate high-temperature superconductors1-10. The recent discovery of superconductivity in the doped infinite-layer nickelate NdNiO2 (refs. 11,12) has strengthened these efforts. Here, we use X-ray spectroscopy and density functional theory to show that the electronic structure of LaNiO2 and NdNiO2, while similar to the cuprates, includes significant distinctions. Unlike cuprates, the rare-earth spacer layer in the infinite-layer nickelate supports a weakly interacting three-dimensional 5d metallic state, which hybridizes with a quasi-two-dimensional, strongly correlated state with [Formula: see text] symmetry in the NiO2 layers. Thus, the infinite-layer nickelate can be regarded as a sibling of the rare-earth intermetallics13-15, which are well known for heavy fermion behaviour, where the NiO2 correlated layers play an analogous role to the 4f states in rare-earth heavy fermion compounds. This Kondo- or Anderson-lattice-like 'oxide-intermetallic' replaces the Mott insulator as the reference state from which superconductivity emerges upon doping.

Nonlinear Ultrafast Spin Scattering in the Skyrmion Phase of Cu_{2}OSeO_{3}.

Ultrafast x-ray scattering studies of the topological Skyrmion phase in Cu_{2}OSeO_{3} show the dynamics to be strongly dependent on the excitation energy and fluence. At high photon energies, where the electron-spin scattering cross section is relatively high, the excitation of the topological Skyrmion phase shows a nonlinear dependence on the excitation fluence, in contrast to the excitation of the conical phase which is linearly dependent on the excitation fluence. The excitation of the Skyrmion order parameter is nonlinear in the magnetic excitation resulting from scattering during electron-hole recombination, indicating different dominant scattering processes in the conical and Skyrmion phases.

Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface.

Static strain in complex oxide heterostructures has been extensively used to engineer electronic and magnetic properties at equilibrium. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across heterointerfaces dynamically. Here, by exciting large-amplitude infrared-active vibrations in a LaAlO3 substrate we induce magnetic order melting in a NdNiO3 film across a heterointerface. Femtosecond resonant soft X-ray diffraction is used to determine the spatiotemporal evolution of the magnetic disordering. We observe a magnetic melt front that propagates from the substrate interface into the film, at a speed that suggests electronically driven motion. Light control and ultrafast phase front propagation at heterointerfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.

Speed limit of the insulator-metal transition in magnetite.

As the oldest known magnetic material, magnetite (Fe3O4) has fascinated mankind for millennia. As the first oxide in which a relationship between electrical conductivity and fluctuating/localized electronic order was shown, magnetite represents a model system for understanding correlated oxides in general. Nevertheless, the exact mechanism of the insulator-metal, or Verwey, transition has long remained inaccessible. Recently, three-Fe-site lattice distortions called trimerons were identified as the characteristic building blocks of the low-temperature insulating electronically ordered phase. Here we investigate the Verwey transition with pump-probe X-ray diffraction and optical reflectivity techniques, and show how trimerons become mobile across the insulator-metal transition. We find this to be a two-step process. After an initial 300 fs destruction of individual trimerons, phase separation occurs on a 1.5±0.2 ps timescale to yield residual insulating and metallic regions. This work establishes the speed limit for switching in future oxide electronics.

Coupled Skyrmion sublattices in Cu(2)OSeO(3).

We report the observation of a Skyrmion lattice in the chiral multiferroic insulator Cu2OSeO3 using Cu L3-edge resonant soft x-ray diffraction. We observe the unexpected existence of two distinct Skyrmion sublattices that arise from inequivalent Cu sites with chemically identical coordination numbers but different magnetically active orbitals. The Skyrmion sublattices are rotated with respect to each other, implying a long wavelength modulation of the lattice. The modulation vector is controlled with an applied magnetic field, associating this moirélike phase with a continuous phase transition. Our findings will open up a new class of science involving manipulation of quantum topological states.

Melting of charge stripes in vibrationally driven La(1.875)Ba(0.125)CuO4: assessing the respective roles of electronic and lattice order in frustrated superconductors.

We report femtosecond resonant soft x-ray diffraction measurements of the dynamics of the charge order and of the crystal lattice in nonsuperconducting, stripe-ordered La1.875Ba0.125CuO4. Excitation of the in-plane Cu-O stretching phonon with a midinfrared pulse has been previously shown to induce a transient superconducting state in the closely related compound La1.675Eu0.2Sr0.125CuO4. In La1.875Ba0.125CuO4, we find that the charge stripe order melts promptly on a subpicosecond time scale. Surprisingly, the low temperature tetragonal (LTT) distortion is only weakly reduced, reacting on significantly longer time scales that do not correlate with light-induced superconductivity. This experiment suggests that charge modulations alone, and not the LTT distortion, prevent superconductivity in equilibrium.

Real-time manifestation of strongly coupled spin and charge order parameters in stripe-ordered La(1.75)Sr(0.25)NiO(4) nickelate crystals using time-resolved resonant x-ray diffraction.

We investigate the order parameter dynamics of the stripe-ordered nickelate, La(1.75)Sr(0.25)NiO(4), using time-resolved resonant x-ray diffraction. In spite of distinct spin and charge energy scales, the two order parameters' amplitude dynamics are found to be linked together due to strong coupling. Additionally, the vector nature of the spin sector introduces a longer reorientation time scale which is absent in the charge sector. These findings demonstrate that the correlation linking the symmetry-broken states does not unbind during the nonequilibrium process, and the time scales are not necessarily associated with the characteristic energy scales of individual degrees of freedom.

Imaging the first-order magnetic transition in La0.35Pr0.275Ca0.375MnO3.

The nature of the ferromagnetic, charge, orbital, and antiferromagnetic order in La0.35Pr0.275Ca0.375MnO3 on the nano- and microscale was investigated by photoemission electron microscopy (PEEM) and resonant elastic soft x-ray scattering (RSXS). The structure of the ferromagnetic domains around the Curie temperature T(C) indicates that they nucleate under a high degree of lattice strain, which is brought about by the charge, orbital, and antiferromagnetic order. The combined temperature-dependent PEEM and RSXS measurements suggest that the lattice distortions associated with charge and orbital order are glassy in nature and that phase separation is driven by the interplay between it and the more itinerant charge carriers associated with ferromagnetic metallic order, even well below T(C).

Femtosecond dynamics of the collinear-to-spiral antiferromagnetic phase transition in CuO.

We report on the ultrafast dynamics of magnetic order in a single crystal of CuO at a temperature of 207 K in response to strong optical excitation using femtosecond resonant x-ray diffraction. In the experiment, a femtosecond laser pulse induces a sudden, nonequilibrium increase in magnetic disorder. After a short delay ranging from 400 fs to 2 ps, we observe changes in the relative intensity of the magnetic ordering diffraction peaks that indicate a shift from a collinear commensurate phase to a spiral incommensurate phase. These results indicate that the ultimate speed for this antiferromagnetic reorientation transition in CuO is limited by the long-wavelength magnetic excitation connecting the two phases.

Ferromagnetic enhancement of CE-type spin ordering in (Pr,Ca)MnO3.

We present resonant soft x-ray scattering results from small bandwidth manganites (Pr,Ca)MnO(3), which show that the CE-type spin ordering (SO) at the phase boundary is stabilized only below the canted antiferromagnetic transition temperature and enhanced by ferromagnetism in the macroscopically insulating state (FM-I). Our results reveal the fragility of the CE-type ordering that underpins the colossal magnetoresistance effect in this system, as well as an unexpected cooperative interplay between FM-I and CE-type SO which is in contrast to the competitive interplay between the ferromagnetic metallic state and CE-type ordering.

Spectroscopic Determination of Key Energy Scales for the Base Hamiltonian of Chromium Trihalides.

The van der Waals (vdW) chromium trihalides (CrX3) exhibit field-tunable, two-dimensional magnetic orders that vary with the halogen species and the number of layers. Their magnetic ground states with proximity in energies are sensitive to the degree of ligand-metal (p-d) hybridization and relevant modulations in the Cr d-orbital interactions. We use soft X-ray absorption (XAS) and resonant inelastic X-ray scattering (RIXS) spectroscopy at Cr L-edge along with the atomic multiplet simulations to determine the key energy scales such as the crystal field 10 Dq and interorbital Coulomb interactions under different ligand metal charge transfer (LMCT) in CrX3 (X= Cl, Br, and I). Through this systematic study, we show that our approach compared to the literature has yielded a set of more reliably determined parameters for establishing a base Hamiltonian for CrX3.

Dynamic electron correlations with charge order wavelength along all directions in the copper oxide plane.

In strongly correlated systems the strength of Coulomb interactions between electrons, relative to their kinetic energy, plays a central role in determining their emergent quantum mechanical phases. We perform resonant x-ray scattering on Bi2Sr2CaCu2O8+δ, a prototypical cuprate superconductor, to probe electronic correlations within the CuO2 plane. We discover a dynamic quasi-circular pattern in the x-y scattering plane with a radius that matches the wave vector magnitude of the well-known static charge order. Along with doping- and temperature-dependent measurements, our experiments reveal a picture of charge order competing with superconductivity where short-range domains along x and y can dynamically rotate into any other in-plane direction. This quasi-circular spectrum, a hallmark of Brazovskii-type fluctuations, has immediate consequences to our understanding of rotational and translational symmetry breaking in the cuprates. We discuss how the combination of short- and long-range Coulomb interactions results in an effective non-monotonic potential that may determine the quasi-circular pattern.

Time-resolved RIXS experiment with pulse-by-pulse parallel readout data collection using X-ray free electron laser.

Time-resolved resonant inelastic X-ray scattering (RIXS) is one of the developing techniques enabled by the advent of X-ray free electron laser (FEL). It is important to evaluate how the FEL jitter, which is inherent in the self-amplified spontaneous emission process, influences the RIXS measurement. Here, we use a microchannel plate (MCP) based Timepix soft X-ray detector to conduct a time-resolved RIXS measurement at the Ti L3-edge on a charge-density-wave material TiSe2. The fast parallel Timepix readout and single photon sensitivity enable pulse-by-pulse data acquisition and analysis. Due to the FEL jitter, low detection efficiency of spectrometer, and low quantum yield of RIXS process, we find that less than 2% of the X-ray FEL pulses produce signals, preventing acquiring sufficient data statistics while maintaining temporal and energy resolution in this measurement. These limitations can be mitigated by using future X-ray FELs with high repetition rates, approaching MHz such as the European XFEL in Germany and LCLS-II in the USA, as well as by utilizing advanced detectors, such as the prototype used in this study.

Fermi surface nesting and nanoscale fluctuating charge/orbital ordering in colossal magnetoresistive oxides.

We used high-resolution angle-resolved photoemission spectroscopy to reveal the Fermi surface and key transport parameters of the metallic state of the layered colossal magnetoresistive oxide La1.2Sr1.8Mn2O7. With these parameters, the calculated in-plane conductivity is nearly one order of magnitude larger than the measured direct current conductivity. This discrepancy can be accounted for by including the pseudogap, which removes at least 90% of the spectral weight at the Fermi energy. Key to the pseudogap and to many other properties are the parallel straight Fermi surface sections, which are highly susceptible to nesting instabilities. These nesting instabilities produce nanoscale fluctuating charge/orbital modulations, which cooperate with Jahn-Teller distortions and compete with the electron itinerancy favored by double exchange.

Polaronic effect in the x-ray absorption spectra of La1-x Ca x MnO3 manganites.

X-ray absorption spectroscopy (XAS) is performed to study changes in the electronic structures of colossal magnetoresistance (CMR) and charged ordered (CO) La1-x Ca x MnO3 manganites with respect to temperature. The pre-edge features in O and Mn K-edge XAS spectra, which are highly sensitive to the local distortion of MnO6 octahedral, exhibit contrasting temperature dependence between CMR and CO samples. The seemingly counter-intuitive XAS temperature dependence can be reconciled in the context of polarons. These results help identify the most relevant orbital states associated with polarons and highlight the crucial role played by polarons in understanding the electronic structures of manganites.

Femtosecond electron-phonon lock-in by photoemission and x-ray free-electron laser.

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.