Search

The shape of 3d-orbitals often governs the electronic and magnetic properties of correlated transition metal oxides. In the superconducting cuprates, the planar confinement of the $${d}_{{x}^{2}-{y}^{2}}$$ d x 2 − y 2 orbital dictates the two-dimensional nature of the unconventional superconductivity and a competing charge order. Achieving orbital-specific control of the electronic structure to allow coupling pathways across adjacent planes would enable direct assessment of the role of dimensionality in the intertwined orders. Using Cu L3 and Pr M5 resonant x-ray scattering and first-principles calculations, we report a highly correlated three-dimensional charge order in Pr-substituted YBa2Cu3O7, where the Pr f-electrons create a direct orbital bridge between CuO2 planes. With this we demonstrate that interplanar orbital engineering can be used to surgically control electronic phases in correlated oxides and other layered materials.

The detection and manipulation of antiferromagnetic domains and topological antiferromagnetic textures are of central interest to solid-state physics. A fundamental step is identifying tools to probe the mesoscopic texture of an antiferromagnetic order parameter. In this work, we demonstrate that Bragg coherent diffractive imaging can be extended to study the mesoscopic texture of an antiferromagnetic order parameter using resonant magnetic x-ray scattering. We study the onset of the antiferromagnet transition in PrNiO 3 , focusing on a temperature regime in which the antiferromagnetic domains are dilute in the beam spot and the coherent diffraction pattern modulating the antiferromagnetic peak is greatly simplified. We demonstrate that it is possible to extract the arrangements and sizes of these domains from single diffraction patterns and show that the approach could be extended to a time-structured light source to study the motion of dilute domains or the motion of topological defects in an antiferromagnetic spin texture.

The shape of 3d-orbitals often governs the electronic and magnetic properties of correlated transition metal oxides. In the superconducting cuprates, the planar confinement of the [Formula: see text] orbital dictates the two-dimensional nature of the unconventional superconductivity and a competing charge order. Achieving orbital-specific control of the electronic structure to allow coupling pathways across adjacent planes would enable direct assessment of the role of dimensionality in the intertwined orders. Using Cu L

Neuromorphic computing which aims to mimic the collective and emergent behavior of the brain's neurons, synapses, axons, dendrites offers an intriguing, potentially disruptive solution to society's ever-growing computational needs. Although much progress has been made in designing circuit elements that mimic the behavior of neurons and synapses, challenges remain in designing networks of elements that feature a collective response behavior. We present simulations of networks of circuits and devices based on superconducting and Mott-insulating oxides that display a multiplicity of emergent states that depend on the spatial configuration of the network. Our proposed network designs are based on experimentally known ways of tuning the properties of these oxides using light ions. We show how neuronal and synaptic behavior can be achieved with arrays of superconducting Josephson junction loops, all within the same device. We also show how a multiplicity of synaptic states could be achieved by designing arrays of devices based on hydrogenated rare-earth nickelates. Together, our results demonstrate a new research platform that utilizes the collective macroscopic properties of quantum materials to mimic the emergent behavior found in biological systems., Comment: 11 pages, 8 figures

We report the structural and magnetic ground state properties of the monoclinic compound barium iridium oxide ${\mathrm{Ba}}_{4}{\mathrm{Ir}}_{3}{\mathrm{O}}_{10}$ using a combination of resonant x-ray scattering, magnetometry, and thermodynamic techniques. Magnetic susceptibility exhibits a pronounced antiferromagnetic transition at ${T}_{\text{N}}\ensuremath{\approx}25$ K, a weaker anomaly at ${T}_{\text{S}}\ensuremath{\approx}142$ K, and strong magnetic anisotropy at all temperatures. Resonant elastic x-ray scattering experiments reveal a second order structural phase transition at ${T}_{\text{S}}$ and a magnetic transition at ${T}_{\text{N}}$. Both structural and magnetic superlattice peaks are observed at $L$ = half integer values. The magnetization anomaly at ${T}_{\text{S}}$ implies the presence of magnetoelastic coupling, which conceivably facilitates the symmetry lowering. Mean field critical scattering is observed above ${T}_{\text{S}}$. The magnetic structure of the antiferromagnetic ground state is discussed based on the measured magnetic superlattice peak intensity. Our study not only presents essential information for understanding the intertwined structural and magnetic properties in ${\mathrm{Ba}}_{4}{\mathrm{Ir}}_{3}{\mathrm{O}}_{10}$ but also highlights the necessary ingredients for exploring novel ground states with octahedra trimers.

The spin-orbit entangled nature of the magnetic moments in Kitaev materials is expected to give rise to a quantum spin liquid (QSL) state with fractional excitations. Using resonant inelastic x-ray scattering under a magnetic field, here the authors map the excitation spectra of $\ensuremath{\beta}$-Li${}_{2}$IrO${}_{3}$. They observe a dichotomy between a magnon-like response at low energies, originating from intertwined field-induced ground states, and a multi-spinon-like continuum at higher energies, originating from pairwise excitations of long-lived Majorana fermions of the proximate QSL.

The authors measure the effects of uniaxial tensile-stress on a prototypical stripe-ordered cuprate, showing that a modest amount of stress creates large changes in the phase diagram.

Interactions between nematic fluctuations, magnetic order and superconductivity are central to the physics of iron-based superconductors. Here we report on in-plane transverse acoustic phonons in hole-doped ${\mathrm{Sr}}_{1\ensuremath{-}x}{\mathrm{Na}}_{x}{\mathrm{Fe}}_{2}{\mathrm{As}}_{2}$ measured via inelastic x-ray scattering, and extract both the nematic susceptibility and the nematic correlation length. By a self-contained method of analysis, for the underdoped ($x=0.36$) sample, which harbors a magnetically ordered tetragonal phase, we find it hosts a short nematic correlation length $\ensuremath{\xi}\ensuremath{\sim}10\text{ }\text{ }\AA{}$ and a large nematic susceptibility ${\ensuremath{\chi}}_{\mathrm{nem}}$. The optimal-doped ($x=0.55$) sample exhibits weaker phonon softening effects, indicative of both reduced $\ensuremath{\xi}$ and ${\ensuremath{\chi}}_{\mathrm{nem}}$. Our results suggest short-range nematic fluctuations may favor superconductivity, placing emphasis on the nematic correlation length for understanding the iron-based superconductors.

Neuromorphic computing approaches become increasingly important as we address future needs for efficiently processing massive amounts of data. The unique attributes of quantum materials can help address these needs by enabling new energy-efficient device concepts that implement neuromorphic ideas at the hardware level. In particular, strong correlations give rise to highly non-linear responses, such as conductive phase transitions that can be harnessed for short- and long-term plasticity. Similarly, magnetization dynamics are strongly non-linear and can be utilized for data classification. This Perspective discusses select examples of these approaches and provides an outlook on the current opportunities and challenges for assembling quantum-material-based devices for neuromorphic functionalities into larger emergent complex network systems.

A momentum resolved resonant inelastic X-ray scattering (qRIXS) experimental station with continuously rotatable spectrometers and parallel detection is designed to operate at different beamlines at synchrotron and free electron laser (FEL) facilities. This endstation, currently located at the Advanced Light Source (ALS), has five emission ports on the experimental chamber for mounting the high-throughput modular soft X-ray spectrometers (MXS) [24]. Coupled to the rotation from the supporting hexapod, the scattered X-rays from 27.5° (forward scattering) to 152.5° (backward scattering) relative to the incident photon beam can be recorded, enabling the momentum-resolved RIXS spectroscopy. The components of this endstation are described in details, and the preliminary RIXS measurements on highly oriented pyrolytic graphite (HOPG) reveal the low energy vibronic excitations from the strong electron-phonon coupling at C K edge around σ* band. The grating upgrade option to enhance the performance at low photon energies is presented and the potential of this spectroscopy is discussed in summary.

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 Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$, a prototypical cuprate superconductor, to probe electronic correlations within the CuO$_2$ 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., Comment: This is a post-peer-review, pre-copyedit version of an article published in Nature Communications. The final authenticated version is available online at: https://doi.org/10.1038/s41467-020-20824-7. Supplementary materials are available through the published version in Nature Communications

We use a 30-nm x-ray beam to study the spatially resolved properties of a ${\mathrm{SmNiO}}_{3}$-based nanodevice that is doped with protons. The x-ray absorption spectra supported by density-functional theory simulations show partial reduction of nickel valence in the region with high proton concentration, which leads to the insulating behavior. Concurrently, x-ray diffraction reveals only a small lattice distortion in the doped regions. Together, our results directly show that the knob which proton doping modifies is the electronic valency and not the crystal lattice. The studies are relevant to ongoing efforts to disentangle structural and electronic effects across metal-insulator phase transitions in correlated oxides.

Interactions between nematic fluctuations, magnetic order and superconductivity are central to the physics of iron-based superconductors. Here we report on in-plane transverse acoustic phonons in hole-doped Sr_{1-x}Na_{x}Fe_{2}As_{2} measured via inelastic x-ray scattering, and extract both the nematic susceptibility and the nematic correlation length. By a self-contained method of analysis, for the underdoped (x=0.36) sample, which harbors a magnetically ordered tetragonal phase, we find it hosts a short nematic correlation length ξ∼10 Å and a large nematic susceptibility χ_{nem}. The optimal-doped (x=0.55) sample exhibits weaker phonon softening effects, indicative of both reduced ξ and χ_{nem}. Our results suggest short-range nematic fluctuations may favor superconductivity, placing emphasis on the nematic correlation length for understanding the iron-based superconductors.

Trees are used by animals, humans and machines to classify information and make decisions. Natural tree structures displayed by synapses of the brain involves potentiation and depression capable of branching and is essential for survival and learning. Demonstration of such features in synthetic matter is challenging due to the need to host a complex energy landscape capable of learning, memory and electrical interrogation. We report experimental realization of tree-like conductance states at room temperature in strongly correlated perovskite nickelates by modulating proton distribution under high speed electric pulses. This demonstration represents physical realization of ultrametric trees, a concept from number theory applied to the study of spin glasses in physics that inspired early neural network theory dating almost forty years ago. We apply the tree-like memory features in spiking neural networks to demonstrate high fidelity object recognition, and in future can open new directions for neuromorphic computing and artificial intelligence., Designing energy efficient and scalable artificial networks for neuromorphic computing remains a challenge. Here, the authors demonstrate tree-like conductance states at room temperature in strongly correlated perovskite nickelates by modulating proton distribution under high speed electric pulses.

Author(s): Ruiz, A; Nagarajan, V; Vranas, M; Lopez, G; McCandless, GT; Kimchi, I; Chan, JY; Breznay, NP; Frano, A; Frandsen, BA; Analytis, JG | Abstract: We report the existence of a high-temperature magnetic anomaly in the three-dimensional Kitaev candidate material, β-Li2IrO3. Signatures of the anomaly appear in magnetization, heat capacity, and muon spin relaxation measurements. The onset coincides with a reordering of the principal axes of magnetization, which is thought to be connected to the onset of Kitaev-like correlations in the system. The anomaly also shows magnetic hysteresis with a spatially anisotropic magnitude that follows the spin-anisotropic exchange anisotropy of the underlying Kitaev Hamiltonian. We discuss possible scenarios for a bulk and impurity origin.

Author(s): Breznay, NP; Hayes, IM; Nair, NL; Helm, T; Analytis, JG; McDonald, RD; Zhu, Z; Krockenberger, Y; Irie, H; Yamamoto, H; Modic, KA; Frano, A; Shafer, P; Arenholz, E | Abstract: The discovery of quantum oscillations in hole- A nd electron-doped cuprate families has underscored the importance of the Fermi surface in cuprate superconductivity. While the observed quantum oscillations in both families have revealed the presence of reconstructed Fermi surfaces, there remains an important distinction between the two. In hole-doped cuprates the oscillations are thought to arise from the effects of a charge density wave, while in the electron-doped cuprates it is thought that these oscillations occur from an antiferromagnetically reconstructed Fermi surface, despite the fact that the oscillations are observed in overdoped compounds, far from the putative antiferromagnetic critical point. In this work we study thin films of Pr2CuO4±δ, whose apparent doping can be finely tuned by annealing, allowing studies of quantum oscillations in samples straddling the critical point. We show that even though there is a mass enhancement of the quasiparticles, there are only small changes to the Fermi surface itself, suggesting that charge order is a more likely origin, with electronic correlations that are strongly dependent on the structural parameters.

We present a methodology based on \textit{ex-situ} (post-growth) electrochemistry to control the oxygen concentration in thin films of the superconducting oxide La$_2$CuO$_{4+y}$ grown epitaxially on substrates of isostructural LaSrAlO$_4$. The superconducting transition temperature, which depends on the oxygen concentration, can be tuned by adjusting the pH level of the base solution used for the electrochemical reaction. As our main finding, we demonstrate that the dopant oxygens can either occupy the interstitial layer in an orientationally disordered state or organize into a crystalline phase via a mechanism in which dopant oxygens are inserted into the substrate, changing the lattice symmetry of both the substrate and the epitaxial film. We discuss this mechanism, and describe the resulting methodology as a platform to be explored in thin films of other transition metal oxides., Comment: 10 pages, 4 figures

We report an angle-resolved photoemission spectroscopy study of the iron-based superconductor family, Ba_{1-x}Na_{x}Fe_{2}As_{2}. This system harbors the recently discovered double-Q magnetic order appearing in a reentrant C_{4} phase deep within the underdoped regime of the phase diagram that is otherwise dominated by the coupled nematic phase and collinear antiferromagnetic order. From a detailed temperature-dependence study, we identify the electronic response to the nematic phase in an orbital-dependent band shift that strictly follows the rotational symmetry of the lattice and disappears when the system restores C_{4} symmetry in the low temperature phase. In addition, we report the observation of a distinct electronic reconstruction that cannot be explained by the known electronic orders in the system.

Author(s): He, Y; Wu, S; Song, Y; Lee, WS; Said, AH; Alatas, A; Bosak, A; Girard, A; Souliou, SM; Ruiz, A; Hepting, M; Bluschke, M; Schierle, E; Weschke, E; Lee, JS; Jang, H; Huang, H; Hashimoto, M; Lu, DH; Song, D; Yoshida, Y; Eisaki, H; Shen, ZX; Birgeneau, RJ; Yi, M; Frano, A | Abstract: We report a persistent low-energy phonon broadening around qB∼0.28 reciprocal lattice unit (r.l.u.) along the Cu-O bond direction in the high-Tc cuprate Bi2Sr2CaCu2O8+δ (Bi-2212). We show that such broadening exists both inside and outside the conventional charge-density wave (CDW) phase, via temperature-dependent measurements in both underdoped and heavily overdoped samples. Combining inelastic hard x-ray scattering, diffuse scattering, angle-resolved photoemission spectroscopy, and resonant soft x-ray scattering at the Cu L3-edge, we exclude the presence of a CDW in the heavily overdoped Bi-2212 similar to that observed in the underdoped systems. Finally, we discuss the origin of such anisotropic low-energy phonon broadening and its potential precursory role to the CDW phase in the underdoped region.

Charge-ordered ground states permeate the phenomenology of 3d-based transition metal oxides, and more generally represent a distinctive hallmark of strongly-correlated states of matter. The recent discovery of charge order in various cuprate families fueled new interest into the role played by this incipient broken symmetry within the complex phase diagram of high-Tc superconductors. Here we use resonant X-ray scattering to resolve the main characteristics of the charge-modulated state in two cuprate families: Bi2201 and YBCO. We detect no signatures of spatial modulations along the nodal direction in Bi2201, thus clarifying the inter-unit-cell momentum-structure of charge order. We also resolve the intra-unit-cell symmetry of the charge ordered state, which is revealed to be best represented by a bond-order with modulated charges on the O-2p orbitals and a prominent d-wave character. These results provide insights on the microscopic description of charge order in cuprates, and on its origin and interplay with superconductivity., Comment: A high-resolution version with supplementary material can be found at: http://www.phas.ubc.ca/~quantmat/ARPES/PUBLICATIONS/Articles/CDW_symmetry.pdf

Incommensurate charge order (CO) has been identified as the leading competitor of high-temperature superconductivity in all major families of layered copper oxides, but the perplexing variety of CO states in different cuprates has confounded investigations of its impact on the transport and thermodynamic properties. The three-dimensional (3D) CO observed in YBa2Cu3O6+x in high magnetic fields is of particular interest, because quantum transport measurements have revealed detailed information about the corresponding Fermi surface. Here we use resonant X-ray scattering to demonstrate 3D-CO in underdoped YBa2Cu3O6+x films grown epitaxially on SrTiO3 in the absence of magnetic fields. The resonance profiles indicate that Cu sites in the charge-reservoir layers participate in the CO state, and thus efficiently transmit CO correlations between adjacent CuO2 bilayer units. The results offer fresh perspectives for experiments elucidating the influence of 3D-CO on the electronic properties of cuprates without the need to apply high magnetic fields., In many cuprates the high temperature superconducting state competes with a charge ordered phase that has been difficult to investigate in detail. Here the authors show three-dimensional charge order can be stabilized in YBCO films and studied without using the high magnetic fields that are necessary in the bulk material.

We report on temperature-dependent pair distribution function measurements of Sr_{1-x}Na_{x}Fe_{2}As_{2}, an iron-based superconductor system that contains a magnetic phase with reentrant tetragonal symmetry, known as the magnetic C_{4} phase. Quantitative refinements indicate that the instantaneous local structure in the C_{4} phase comprises fluctuating orthorhombic regions with a length scale of ∼2 nm, despite the tetragonal symmetry of the average static structure. Additionally, local orthorhombic fluctuations exist on a similar length scale at temperatures well into the paramagnetic tetragonal phase. These results highlight the exceptionally large nematic susceptibility of iron-based superconductors and have significant implications for the magnetic C_{4} phase and the neighboring C_{2} and superconducting phases.

Magnetic honeycomb iridates are thought to show strongly spin-anisotropic exchange interactions which, when highly frustrated, lead to an exotic state of matter known as the Kitaev quantum spin liquid. However, in all known examples these materials magnetically order at finite temperatures, the scale of which may imply weak frustration. Here we show that the application of a relatively small magnetic field drives the three-dimensional magnet β-Li2IrO3 from its incommensurate ground state into a quantum correlated paramagnet. Interestingly, this paramagnetic state admixes a zig-zag spin mode analogous to the zig-zag order seen in other Mott-Kitaev compounds. The rapid onset of the field-induced correlated state implies the exchange interactions are delicately balanced, leading to strong frustration and a near degeneracy of different ground states., Materials with a Kitaev spin liquid ground state are sought after as models of quantum phases but candidates so far form either zig-zag or incommensurate magnetic order. Ruiz et al. find a crossover between these states in β-Li2IrO3 under weak magnetic fields, indicating strongly frustrated spin interactions.

Honeycomb iridates such as $\ensuremath{\gamma}\ensuremath{-}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ are argued to realize Kitaev spin-anisotropic magnetic exchange, along with Heisenberg and possibly other couplings. While systems with pure Kitaev interactions are candidates to realize a quantum spin-liquid ground state, in $\ensuremath{\gamma}\ensuremath{-}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ it has been shown that the presence of competing magnetic interactions leads to an incommensurate spiral spin order at ambient pressure below 38 K. We study the pressure sensitivity of this magnetically ordered state in single crystals of $\ensuremath{\gamma}\ensuremath{-}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ using resonant x-ray scattering (RXS) under applied hydrostatic pressures of up to 3 GPa. RXS is a direct probe of electronic order, and we observe the abrupt disappearance of the ${\mathbf{q}}_{\mathrm{sp}}\phantom{\rule{0.28em}{0ex}}=\phantom{\rule{0.28em}{0ex}}(0.57,\phantom{\rule{0.28em}{0ex}}0,\phantom{\rule{0.28em}{0ex}}0)$ spiral order at a critical pressure ${P}_{c}=1.4$ GPa with no accompanying change in the symmetry of the lattice.

We report on temperature-dependent pair distribution function measurements of Sr_{1-x}Na_{x}Fe_{2}As_{2}, an iron-based superconductor system that contains a magnetic phase with reentrant tetragonal symmetry, known as the magnetic C_{4} phase. Quantitative refinements indicate that the instantaneous local structure in the C_{4} phase comprises fluctuating orthorhombic regions with a length scale of ∼2 nm, despite the tetragonal symmetry of the average static structure. Additionally, local orthorhombic fluctuations exist on a similar length scale at temperatures well into the paramagnetic tetragonal phase. These results highlight the exceptionally large nematic susceptibility of iron-based superconductors and have significant implications for the magnetic C_{4} phase and the neighboring C_{2} and superconducting phases.

Resonant x-ray scattering at the Dy ${M}_{5}$ and Ni ${L}_{3}$ absorption edges was used to probe the temperature and magnetic field dependence of magnetic order in epitaxial ${\mathrm{LaNiO}}_{3}\ensuremath{-}\mathrm{DySc}{\mathrm{O}}_{3}$ superlattices. For superlattices with 2 unit cell thick ${\mathrm{LaNiO}}_{3}$ layers, a commensurate spiral state develops in the Ni spin system below 100 K. Upon cooling below ${T}_{\mathrm{ind}}=18\text{ }\text{ }\mathrm{K}$, Dy-Ni exchange interactions across the ${\mathrm{LaNiO}}_{3}\ensuremath{-}\mathrm{DySc}{\mathrm{O}}_{3}$ interfaces induce collinear magnetic order of interfacial Dy moments as well as a reorientation of the Ni spins to a direction dictated by the strong magnetocrystalline anisotropy of Dy. This transition is reversible by an external magnetic field of 3 T. Tailored exchange interactions between rare-earth and transition-metal ions thus open up new perspectives for the manipulation of spin structures in metal-oxide heterostructures and devices.

Besides superconductivity, copper-oxide high temperature superconductors are susceptible to other types of ordering. We use scanning tunneling microscopy and resonant elastic x-ray scattering measurements to establish the formation of charge ordering in the high-temperature superconductor Bi2Sr2CaCu2O8+x. Depending on the hole concentration, the charge ordering in this system occurs with the same period as those found in Y-based or La-based cuprates, and displays the analogous competition with superconductivity. These results indicate the similarity of charge organization competing with superconductivity across different families of cuprates. We observe this charge ordering to leave a distinct electron-hole asymmetric signature (and a broad resonance centered at +20 meV) in spectroscopic measurements, thereby indicating that it is likely related to the organization of holes in a doped Mott insulator., preprint version, 12 pages, 3 figures. Supplement: 8 pages, 9 figures

Physical review letters 118(2), 027401(2017). doi:10.1103/PhysRevLett.118.027401, Selective optical excitation of a substrate lattice can drive phase changes across heterointerfaces. This phenomenon is a nonequilibrium analogue of static strain control in heterostructures and may lead to new applications in optically controlled phase change devices. Here, we make use of time-resolved nonresonant and resonant x-ray diffraction to clarify the underlying physics and to separate different microscopic degrees of freedom in space and time. We measure the dynamics of the lattice and that of the charge disproportionation in $NdNiO_3$, when an insulator-metal transition is driven by coherent lattice distortions in the $LaAlO_3$ substrate. We find that charge redistribution propagates at supersonic speeds from the interface into the $NdNiO_3$ film, followed by a sonic lattice wave. When combined with measurements of magnetic disordering and of the metal-insulator transition, these results establish a hierarchy of events for ultrafast control at complex-oxide heterointerfaces., Published by APS, College Park, Md.

The competition between collective quantum phases in materials with strongly correlated electrons depends sensitively on the dimensionality of the electron system, which is difficult to control by standard solid-state chemistry. We have fabricated superlattices of the paramagnetic metal lanthanum nickelate (LaNiO(3)) and the wide-gap insulator lanthanum aluminate (LaAlO(3)) with atomically precise layer sequences. We used optical ellipsometry and low-energy muon spin rotation to show that superlattices with LaNiO(3) as thin as two unit cells undergo a sequence of collective metal-insulator and antiferromagnetic transitions as a function of decreasing temperature, whereas samples with thicker LaNiO(3) layers remain metallic and paramagnetic at all temperatures. Metal-oxide superlattices thus allow control of the dimensionality and collective phase behavior of correlated-electron systems.

The interplay between charge density waves (CDWs) and high-temperature superconductivity is currently under intense investigation. Experimental research on this issue is difficult because CDW formation in bulk copper-oxides is strongly influenced by random disorder, and a long-range-ordered CDW state in high magnetic fields is difficult to access with spectroscopic and diffraction probes. Here we use resonant x-ray scattering in zero magnetic field to show that interfaces with the metallic ferromagnet La$_{2/3}$Ca$_{1/3}$MnO$_3$ greatly enhance CDW formation in the optimally doped high-temperature superconductor YBa$_2$Cu$_3$O$_{6+\delta}$ ($\bf \delta \sim 1$), and that this effect persists over several tens of nm. The wavevector of the incommensurate CDW serves as an internal calibration standard of the charge carrier concentration, which allows us to rule out any significant influence of oxygen non-stoichiometry, and to attribute the observed phenomenon to a genuine electronic proximity effect. Long-range proximity effects induced by heterointerfaces thus offer a powerful method to stabilize the charge density wave state in the cuprates, and more generally, to manipulate the interplay between different collective phenomena in metal oxides., Comment: modified version published in Nature Materials

The understanding of the origin of superconductivity in cuprates has been hindered by the apparent diversity of intertwining electronic orders in these materials. We combined resonant x-ray scattering (REXS), scanning-tunneling microscopy (STM), and angle-resolved photoemission spectroscopy (ARPES) to observe a charge order that appears consistently in surface and bulk, and in momentum and real space within one cuprate family, Bi 2 Sr 2 − x La x CuO 6 + δ . The observed wave vectors rule out simple antinodal nesting in the single-particle limit but match well with a phenomenological model of a many-body instability of the Fermi arcs. Combined with earlier observations of electronic order in other cuprate families, these findings suggest the existence of a generic charge-ordered state in underdoped cuprates and uncover its intimate connection to the pseudogap regime.

We use femtosecond resonant soft x-ray diffraction to measure the optically stimulated ultrafast changes of charge-density wave correlations in underdoped $\mathrm{YB}{\mathrm{a}}_{2}\mathrm{C}{\mathrm{u}}_{3}{\mathrm{O}}_{6.6}$. We find that when coherent interlayer transport is enhanced by optical excitation of the apical oxygen distortions, at least 50% of the in-plane charge-density wave order is melted. These results indicate that charge ordering and superconductivity may be competing up to the charge ordering transition temperature, with the latter becoming a hidden phase that is accessible only by nonlinear phonon excitation.

Using resonant x-ray scattering, this group maps the evolution of charge density wave correlations in a series of YBa${}_{2}$Cu${}_{3}$O${}_{6+x}$ single crystals at a wide range of doping levels. Their data add important pieces to the cuprate phase diagram puzzle.

We have used polarized Raman scattering to probe lattice vibrations and charge ordering in 12 nm thick, epitaxially strained PrNiO$_3$ films, and in superlattices of PrNiO$_3$ with the band-insulator PrAlO$_3$. A carefully adjusted confocal geometry was used to eliminate the substrate contribution to the Raman spectra. In films and superlattices under tensile strain, which undergo a metal-insulator transition upon cooling, the Raman spectra reveal phonon modes characteristic of charge ordering. These anomalous phonons do not appear in compressively strained films, which remain metallic at all temperatures. For superlattices under compressive strain, the Raman spectra show no evidence of anomalous phonons indicative of charge ordering, while complementary resonant x-ray scattering experiments reveal antiferromagnetic order associated with a modest increase in resistivity upon cooling. This confirms theoretical predictions of a spin density wave phase driven by spatial confinement of the conduction electrons., PRL, in press

Nonlinear lattice excitation in YBa2Cu3O6.5 has been shown recently to transiently induce signatures of superconducting coherence up to room temperature. Here, we present ultrafast x-ray diffraction measurements used to determine the corresponding atomic structure. © 2014 OSA.

The experimental technique used throughout this thesis to investigate the ordered states of the TMO heterostructures is resonant soft X-ray scattering (RSXS).

Engineering new electronic and structural phases by combining complex materials into heterostructures is a task taken on with widespread enthusiasm around the world. Resonant X-ray diffraction was used to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO\(_{3}\).

Correlated electron systems like transition metal oxides offer coupled charge, lattice, orbit, and spin degrees of freedom, which can be combined to achieve intriguing collective phases. Many of these phases can be tuned or explored by growing the materials into heterostructures. This chapter will present a summary of the general properties of transition metal oxide compounds and the motivation for creating artifcially engineered materials via heterostructuring.

This chapter will present and discuss the evidence of incipient charge density wave order found throughout this PhD project in superconducting cuprates.

A combined analysis of x-ray absorption and resonant reflectivity data was used to obtain the orbital polarization profiles of superlattices composed of four-unit-cell-thick layers of metallic LaNiO${}_{3}$ and layers of insulating $RX$O${}_{3}$ ($R=\text{La}$, Gd, Dy and $X=\text{Al}$, Ga, Sc), grown on substrates that impose either compressive or tensile strain. This superlattice geometry allowed us to partly separate the influence of epitaxial strain from interfacial effects controlled by the chemical composition of the insulating blocking layers. Our quantitative analysis reveals orbital polarizations up to 25$%$. We further show that strain is the most effective control parameter, whereas the influence of the chemical composition of the blocking layers is comparatively small.

A combined synchrotron X-ray diffraction and transmission electron microscopy study reveals a structural phase transition controlled by the overall thickness of epitaxial nickelate-aluminate superlattices. The transition between uniform and twin-domain states is confined to the nickelate layers and leaves the aluminate layers unaffected.

We use resonant x-ray scattering to determine the momentum-dependent charge correlations in YBa(2)Cu(3) O(6.55) samples with highly ordered chain arrays of oxygen acceptors (ortho-II structure). The results reveal nearly critical, biaxial charge density wave (CDW) correlations at in-plane wave vectors (0.315, 0) and (0, 0.325). The corresponding scattering intensity exhibits a strong uniaxial anisotropy. The CDW amplitude and correlation length are enhanced as superconductivity is weakened by an external magnetic field. Analogous experiments are carried out on a YBa(2)Cu(3)O(6.6) crystal with a dilute concentration of spinless (Zn) impurities, which had earlier been shown to nucleate incommensurate magnetic order. Compared to pristine crystals with the same doping level, the CDW amplitude and correlation length are found to be strongly reduced. These results indicate a three-phase competition between spin-modulated, charge-modulated, and superconducting states in underdoped YBa(2)Cu(3)O(6+δ).

With ellipsometry, x-ray diffraction, and resistance measurements we investigated the electric-field effect on the confined electrons at the LaAlO3=SrTiO3 interface. We obtained evidence that the localization of the electrons at negative gate voltage is induced, or at least enhanced, by a polar phase transition in SrTiO3 which strongly reduces the lattice polarizability and the subsequent screening. In particular, we show that the charge localization and the polar order of SrTiO3 both develop below similar to 50 K and exhibit similar, unipolar hysteresis loops as a function of the gate voltage.

We have used resonant x-ray diffraction to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO3. We also report reference experiments on thin films of PrNiO3 and NdNiO3. The resulting data indicate a spiral state whose polarization plane can be controlled by adjusting the Ni d-orbital occupation via two independent mechanisms: epitaxial strain and quantum confinement of the valence electrons. The data are discussed in the light of recent theoretical predictions., Comment: 5 pages, 3 figures

Recently, charge density wave (CDW) order in the ${\mathrm{CuO}}_{2}$ planes of underdoped ${\mathrm{YBa}}_{2}{\mathrm{Cu}}_{3}{\mathrm{O}}_{6+\ensuremath{\delta}}$ was detected using resonant soft x-ray scattering. An important question remains: is the chain layer responsible for this charge ordering? Here, we explore the energy and polarization dependence of the resonant scattering intensity in a detwinned sample of ${\mathrm{YBa}}_{2}{\mathrm{Cu}}_{3}{\mathrm{O}}_{6.75}$ with ortho-III oxygen ordering in the chain layer. We show that the ortho-III CDW order in the chains is distinct from the CDW order in the planes. The ortho-III structure gives rise to a commensurate superlattice reflection at $Q=[0.33\text{ }0\text{ }L]$ whose energy and polarization dependence agrees with expectations for oxygen ordering and a spatial modulation of the Cu valence in the chains. Incommensurate peaks at [0.30 0 $L$] and [0 0.30 $L$] from the CDW order in the planes are shown to be distinct in $Q$ as well as their temperature, energy, and polarization dependence, and are thus unrelated to the structure of the chain layer. Moreover, the energy dependence of the CDW order in the planes is shown to result from a spatial modulation of energies of the Cu $2p$ to $3{d}_{{x}^{2}\ensuremath{-}{y}^{2}}$ transition, similar to stripe-ordered 214 cuprates.