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The nature of the magnetic order in (La2/3Sr1/3MnO3)9/(LaNiO3)3 superlattices is investigated using x-ray resonant magnetic reflectometry. We observe a new c-axis magnetic helix state in the (LaNiO3)3 layers that had never been reported in nickelates, and which mediates the ~130deg magnetic coupling between the ferromagnetic (La2/3Sr1/3MnO3)9 layers, illustrating the power of x-rays for discovering the magnetic state of complex oxide interfaces. Resonant inelastic x-ray scattering and x-ray absorption spectroscopy show that Ni-O ligand hole states from bulk LaNiO3 are mostly filled due to interfacial electron transfer from Mn, driving the Ni orbitals closer to an atomic-like 3d8 configuration. We discuss the constraints imposed by this electronic configuration to the microscopic origin of the observed magnetic structure. The presence of a magnetic helix in (La2/3Sr1/3MnO3)9/(LaNiO3)3 is crucial for modeling the potential spintronic functionality of this system and may be important for designing emergent magnetism in novel devices in general., Comment: 7 pages, 5 figures

The electronic-structural modulations of Ir$_{1-x}$Pt$_x$Te$_2$ (0 $\leqq x\leqq$ 0.12) have been examined by resonant elastic x-ray scattering (REXS) and resonant inelastic x-ray scattering (RIXS) techniques at both the Ir and Te edges. Charge-density-wave-like superstructure with wave vectors of $\mathbf{Q}$=(1/5 0 $-$1/5), (1/8 0 $-$1/8), and (1/6 0 $-$1/6) are observed on the same sample of IrTe$_2$ at the lowest temperature, the patterns of which are controlled by the cooling speeds. In contrast, superstructures around $\mathbf{Q}$=(1/5 0 $-$1/5) are observed for doped samples (0.02 $\leqq x\leqq$ 0.05). The superstructure reflections persist to higher Pt substitution than previously assumed, demonstrating that a charge density wave (CDW) can coexists with superconductivity. The analysis of the energy-dependent REXS and RIXS lineshape reveals the importance of the Te 5$p$ state rather than the Ir 5$d$ states in the formation of the spatial modulation of these systems. The phase diagram re-examined in this work suggests that the CDW incommensurability may correlate the emergence of superconducting states as-like Cu$_x$TiSe$_2$ and Li$_x$TaS$_2$., Comment: 10 pages ,9 figures

Samarium hexaboride (SmB$_6$), a Kondo insulator with mixed valence, has recently attracted much attention as a possible host for correlated topological surface states. Here, we use a combination of x-ray absorption and reflectometry techniques, backed up with a theoretical model for the resonant $M_{4,5}$ absorption edge of Sm and photoemission data, to establish laterally averaged chemical and valence depth profiles at the surface of SmB$_6$. We show that upon cleaving, the highly polar (001) surface of SmB$_6$ undergoes substantial chemical and valence reconstruction, resulting in boron termination and a Sm$^{3+}$ dominated sub-surface region. Whereas at room temperature, the reconstruction occurs on a time scale of less than two hours, it takes about 24 hours below 50 K. The boron termination is eventually established, irrespective of the initial termination. Our findings reconcile earlier depth resolved photoemission and scanning tunneling spectroscopy studies performed at different temperatures and are important for better control of polarity and, as a consequence, surface states in this system.

Polar discontinuities and redox reactions provide alternative paths to create two-dimensional electron liquids (2DELs) at oxide interfaces. Herein, we report high mobility 2DELs at interfaces involving SrTiO3 (STO) achieved using polar La7/8Sr1/8MnO3 (LSMO) buffer layers to manipulate both polarities and redox reactions from disordered overlayers grown at room temperature. Using resonant x-ray reflectometry experiments, we quantify redox reactions from oxide overlayers on STO as well as polarity induced electronic reconstruction at epitaxial LSMO/STO interfaces. The analysis reveals how these effects can be combined in a STO/LSMO/disordered film trilayer system to yield high mobility modulation doped 2DELs, where the buffer layer undergoes a partial transformation from perovskite to brownmillerite structure. This uncovered interplay between polar discontinuities and redox reactions via buffer layers provides a new approach for the design of functional oxide interfaces., Comment: Nano Letters, 2017

A nematic order in stripe-ordered cuprates was recently identified with (001) reflection at resonant energies associated with the in-plane states. However, whether this resonant reflection is ubiquitous among all 214 cuprates is still unknown. Here we report a Resonant soft X-ray Scattering (RXS) measurement on two La$_{2-x}$Sr$_x$CuO$_{4+y}$ crystals. Charge order was found in La$_2$CuO$_{4+y}$ with a total hole concentration near 0.125/Cu but no measurable (001) peak at any resonance, while in a La$_{1.94}$Sr$_{0.06}$CuO$_{4+y}$ sample near 0.16/Cu a (001) peak resonant was identified to be consistent with the presence of LTT tilting. The lack of such a (001) peak in a compound with stripe-like charge order raises questions about nematicity and the origin of the scattering feature., Comment: 5 pages, 4 figures

The electronic structure of BaFe$_2X_3$ ($X$ = S and Se) and CsFe$_2$Se$_3$ in which two-leg ladders are formed by the Fe sites are studied by means of x-ray absorption and resonant inelastic x-ray scattering spectroscopy. The x-ray absorption spectra at the Fe L edges for BaFe$_2X_3$ exhibit two components, indicating that itinerant and localized Fe 3$d$ sites coexist. Substantial x-ray linear dichroism (XLD) is observed in polarization dependent spectra, indicating the existence of orbital order or fluctuation in the Fe-ladder even above the N\'{e}el temperature $T_N$. Direct exchange interaction along the legs of the Fe-ladder stabilizes the orbital and antiferromagnetic orders in BaFe$_2$S$_3$, while the ferromagnetic molecular orbitals are realized between the rungs in CsFe$_2$Se$_3$., Comment: 7 pages,5 figures

We present a detailed synchrotron x-ray scattering study of the charge-density-wave (CDW) order in simple tetragonal HgBa$_2$CuO$_{4+\delta}$ (Hg1201). Resonant soft x-ray scattering measurements reveal that short-range order appears at a temperature that is distinctly lower than the pseudogap temperature and in excellent agreement with a prior transient reflectivity result. Despite considerable structural differences between Hg1201 and YBa$_2$Cu$_3$O$_{6+\delta}$, the CDW correlations exhibit similar doping dependencies, and we demonstrate a universal relationship between the CDW wave vector and the size of the reconstructed Fermi pocket observed in quantum oscillation experiments. The CDW correlations in Hg1201 vanish already below optimal doping, once the correlation length is comparable to the CDW modulation period, and they appear to be limited by the disorder potential from unit cells hosting two interstitial oxygen atoms. A complementary hard x-ray diffraction measurement, performed on an underdoped Hg1201 sample in magnetic fields along the crystallographic $c$ axis of up to 16 T, provides information about the form factor of the CDW order. As expected from the single-CuO$_2$-layer structure of Hg1201, the CDW correlations vanish at half-integer values of $L$ and appear to be peaked at integer $L$. We conclude that the atomic displacements associated with the short-range CDW order are mainly planar, within the CuO$_2$ layers.

Resonant X-ray scattering (RXS) has recently become an increasingly important tool for the study of ordering phenomena in correlated electron systems. Yet, the interpretation of the RXS experiments remains theoretically challenging due to the complexity of the RXS cross-section. Central to this debate is the recent proposal that impurity-induced Friedel oscillations, akin to quasiparticle interference signals observed with the scanning tunneling microscope (STM), can lead to scattering peaks in the RXS experiments. The possibility that quasiparticle properties can be probed in RXS measurements opens up a new avenue to study the bulk band structure of materials with the orbital and element selectivity provided by RXS. Here, we test these ideas by combining RXS and STM measurements of the heavy fermion compound CeMIn$_5$ (M = Co, Rh). Temperature and doping dependent RXS measurements at the Ce-M$_4$ edge show a broad scattering enhancement that correlates with the appearance of heavy f-electron bands in these compounds. The scattering enhancement is consistent with the measured quasiparticle interference signal in the STM measurements, indicating that quasiparticle interference can be probed through the momentum distribution of RXS signals. Overall, our experiments demonstrate new opportunities for studies of correlated electronic systems using the RXS technique., Comment: accepted to Science Advances

Polar catastrophe at the interface of oxide materials with strongly correlated electrons has triggered a flurry of new research activities. The expectations are that the design of such advanced interfaces will become a powerful route to engineer devices with novel functionalities. Here we investigate the initial stages of growth and the electronic structure of the spintronic Fe3O4/MgO (001) interface. Using soft x-ray absorption spectroscopy we have discovered that the so-called A-sites are completely missing in the first Fe3O4 monolayer. This allows us to develop an unexpected but elegant growth principle in which during deposition the Fe atoms are constantly on the move to solve the divergent electrostatic potential problem, thereby ensuring epitaxy and stoichiometry at the same time. This growth principle provides a new perspective for the design of interfaces., Comment: 30 pages

Understanding the interplay between charge order (CO) and other phenomena (e.g. pseudogap, antiferromagnetism, and superconductivity) is one of the central questions in the cuprate high-temperature superconductors. The discovery that similar forms of CO exist in both hole- and electron-doped cuprates opened a path to determine what subset of the CO phenomenology is universal to all the cuprates. Here, we use resonant x-ray scattering to measure the charge order correlations in electron-doped cuprates (La2-xCexCuO4 and Nd2-xCexCuO4) and their relationship to antiferromagnetism, pseudogap, and superconductivity. Detailed measurements of Nd2-xCexCuO4 show that CO is present in the x = 0.059 to 0.166 range, and that its doping dependent wavevector is consistent with the separation between straight segments of the Fermi surface. The CO onset temperature is highest between x = 0.106 and 0.166, but decreases at lower doping levels, indicating that it is not tied to the appearance of antiferromagnetic correlations or the pseudogap. Near optimal doping, where the CO wavevector is also consistent with a previously observed phonon anomaly, measurements of the CO below and above the superconducting transition temperature, or in a magnetic field, show that the CO is insensitive to superconductivity. Overall these findings indicate that, while verified in the electron-doped cuprates, material-dependent details determine whether the CO correlations acquire sufficient strength to compete for the ground state of the cuprates., Comment: Supplementary information available upon request

In underdoped cuprate superconductors, a rich competition occurs between superconductivity and charge density wave (CDW) order. Whether rotational symmetry breaking (nematicity) occurs intrinsically and generically or as a consequence of other orders is under debate. Here we employ resonant x-ray scattering in stripe-ordered (La,M)_2CuO_4 to probe the relationship between electronic nematicity of the Cu 3d orbitals, structure of the (La,M)_2O_2 layers, and CDW order. We find distinct temperature dependences for the structure of the (La,M)_2O_2 layers and the electronic nematicity of the CuO_2 planes, with only the latter being enhanced by the onset of CDW order. These results identify electronic nematicity as an order parameter that is distinct from a purely structural order parameter in underdoped striped cuprates., Comment: 23 pages including supplementary information, 3 main figures, 4 supplementary figures

Fine questions our interpretation of unidirectional-stripes over bidirectional-checkerboard, and illustrates his criticism by simulating a momentum space structure consistent with our data and corresponding to a checkerboard-looking real space density. Here we use a local rotational-symmetry analysis to demonstrate that the simulated image is in actuality composed of locally unidirectional modulations of the charge density, consistent with our original conclusions., Comment: Response to original comment: B.V. Fine, Science 351, 235 (2016) (arxiv version at http://arxiv.org/abs/1602.00888)

Bulk NdNiO_3 and thin films grown along the pseudocubic (001)_pc axis display a 1st order metal to insulator transition (MIT) together with a N\'eel transition at T=200K. Here, we show that for NdNiO3 films deposited on (111)_pc NdGaO_3 the MIT occurs at T=335K and the N\'eel transition at T=230 K. By comparing transport and magnetic properties of layers grown on substrates with different symmetries and lattice parameters, we demonstrate a particularly large tuning when the epitaxy is realized on (111)_pc surfaces. We attribute this effect to the specific lattice matching conditions imposed along this direction when using orthorhombic substrates.

The discovery of two-dimensional electron gases (2DEGs) at the interface between two insulating complex oxides, such as LaAlO3 (LAO) or gamma-Al2O3 (GAO) epitaxially grown on SrTiO3 (STO) 1,2, provides an opportunity for developing all-oxide electronic devices3,4. These 2DEGs at complex oxide interfaces involve many-body interactions and give rise to a rich set of phenomena5, for example, superconductivity6, magnetism7,8, tunable metal-insulator transitions9, and phase separation10. However, large enhancement of the interfacial electron mobility remains a major and long-standing challenge for fundamental as well as applied research of complex oxides11-15. Here, we inserted a single unit cell insulating layer of polar La1-xSrxMnO3 (x=0, 1/8, and 1/3) at the interface between disordered LaAlO3 and crystalline SrTiO3 created at room temperature. We find that the electron mobility of the interfacial 2DEG is enhanced by more than two orders of magnitude. Our in-situ and resonant x-ray spectroscopic in addition to transmission electron microscopy results indicate that the manganite layer undergoes unambiguous electronic reconstruction and leads to modulation doping of such atomically engineered complex oxide heterointerfaces. At low temperatures, the modulation-doped 2DEG exhibits clear Shubnikov-de Haas oscillations and the initial manifestation of the quantum Hall effect, demonstrating an unprecedented high-mobility and low electron density oxide 2DEG system. These findings open new avenues for oxide electronics., Comment: 29 pages, 5 figures, Accepted for publication in Nature Materials

Nickelates are known for their metal to insulator transition (MIT) and an unusual magnetic ordering, occurring at T=T_N\'eel. Here, we investigate thin films of SmNiO_3 subjected to different levels of epitaxial strain. We find that the original bulk behavior (T_N\'eel

Following the early discovery of stripe-like order in La-based copper-oxide superconductors, charge ordering instabilities were observed in all cuprate families. However, it has proven difficult to distinguish between uni- (stripes) and bi-directional (checkerboard) charge order in Y- and Bi-based materials. Here we use resonant x-ray scattering (RXS) to measure the two-dimensional structure factor in YBCO, in reciprocal space. Our data reveal the presence of charge stripe order, i.e. locally unidirectional density waves, suggesting it as the true microscopic nature of charge modulations in cuprates. At the same time, we find that the well-established competition between charge order and superconductivity is stronger for charge correlations across than along the stripes, which provides additional evidence for the intrinsic unidirectional nature of the charge order.

The analysis of x-ray reflectivity data from artificial heterostructures usually relies on the homogeneity of optical properties of the constituent materials. However, when the x-ray energy is tuned to an absorption edge, this homogeneity no longer exists. Within the same material, spatial regions containing elements at resonance will have optical properties very different from regions without resonating sites. In this situation, models assuming homogeneous optical properties throughout the material can fail to describe the reflectivity adequately. As we show here, resonant soft x-ray reflectivity is sensitive to these variations, even though the wavelength is typically large as compared to the atomic distances over which the optical properties vary. We have therefore developed a scheme for analyzing resonant soft x-ray reflectivity data, which takes the atomic structure of a material into account by "slicing" it into atomic planes with characteristic optical properties. Using LaSrMnO4 as an example, we discuss both the theoretical and experimental implications of this approach. Our analysis not only allows to determine important structural information such as interface terminations and stacking of atomic layers, but also enables to extract depth-resolved spectroscopic information with atomic resolution, thus enhancing the capability of the technique to study emergent phenomena at surfaces and interfaces., Comment: Completely overhauled with respect to the previous version due to peer review