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C. S. Fadley

Publications and source records attributed to C. S. Fadley.

At least 19 recordsLinked to original sources

Bulk Electronic Structure of Lanthanum Hexaboride (LaB6) by Hard X-ray Angle-Resolved Photoelectron Spectroscopy

In the last decade rare-earth hexaborides have been investigated for their fundamental importance in condensed matter physics, and for their applications in advanced technological fields. Among these compounds, LaB$_6$ has a special place, being a traditional d-band metal without additional f- bands. In this paper we investigate the bulk electronic structure of LaB$_6$ using hard x-ray photoemission spectroscopy, measuring both core-level and angle-resolved valence-band spectra. By comparing La 3d core level spectra to cluster model calculations, we identify well-screened peak residing at a lower binding energy compared to the main poorly-screened peak; the relative intensity between these peaks depends on how strong the hybridization is between La and B atoms. We show that the recoil effect, negligible in the soft x-ray regime, becomes prominent at higher kinetic energies for lighter elements, such as boron, but is still negligible for heavy elements, such as lanthanum. In addition, we report the bulk-like band structure of LaB$_6$ determined by hard x-ray angle-resolved photoemission spectroscopy (HARPES). We interpret HARPES experimental results by the free-electron final-state calculations and by the more precise one-step photoemission theory including matrix element and phonon excitation effects. In addition, we consider the nature and the magnitude of phonon excitations in HARPES experimental data measured at different temperatures and excitation energies. We demonstrate that one step theory of photoemission and HARPES experiments provide, at present, the only approach capable of probing true bulk-like electronic band structure of rare-earth hexaborides and strongly correlated materials.

physics.app-ph

Hard x-ray standing-wave photoemission study of the interfaces in a BiFeO$_3$/La$_{0.7}$Sr$_{0.3}$MnO$_3$ superlattice

Hybrid multiferroics such as BiFeO$_3$ (BFO) and La$_{0.7}$Sr$_{0.3}$MnO$_3$ (LSMO) heterostructures are highly interesting functional systems due to their complex electronic and magnetic properties. One of the key parameters influencing the emergent properties is the quality of interfaces, where varying interdiffusion lengths can give rise to different chemistry and distinctive electronic states. Here we report high-resolution depth resolved chemical and electronic investigation of BFO/LSMO superlattice using standing-wave hard X-ray photoemission spectroscopy in the first-order Bragg as well as near-total-reflection geometry. Our results show that the interfaces of BFO on top of LSMO are atomically abrupt, while the LSMO on top of BFO interfaces show an interdiffusion length of around 1.2 unit cells. The two interfaces also exhibit different chemical gradients, with the BFO/LSMO interface being Sr-terminated by a spectroscopically distinctive high binding energy component in Sr 2p core-level spectra, which is spatially contained within 1 unit cell from the interface. From the electronic point of view, unique valence band features were observed for bulk-BFO, bulk-LSMO and their interfaces. Our X-ray optical analysis revealed a unique electronic signature at the BFO/LSMO interface, which we attribute to the coupling between those respective layers. Valence band decomposition based on the Bragg-reflection standing-wave measurement also revealed the band alignment between BFO and LSMO layers. Our work demonstrates that standing-wave hard x-ray photoemission is a reliable non-destructive technique for probing depth-resolved electronic structure of buried layers and interfaces with sub-unit-cell resolution. Equivalent investigations can be successfully applied to a broad class of material such as perovskite complex oxides with emergent interfacial phenomena.

cond-mat.mtrl-sci

Hard x-ray standing-wave photoemission insights into the structure of an epitaxial Fe/MgO multilayer magnetic tunnel junction

The Fe/MgO magnetic tunnel junction is a classic spintronic system, with current importance technologically, and interest for future innovation. The key magnetic properties are linked directly to the structure of hard-to-access buried interfaces, and the Fe and MgO components near the surface are unstable when exposed to air, making a deeper probing, non-destructive, in-situ measurement ideal for this system. We have thus applied hard x-ray photoemission spectroscopy (HXPS) and standing-wave (SW) HXPS in the few keV energy range to probe the structure of an epitaxially-grown MgO/Fe superlattice. The superlattice consists of 9 repeats of MgO grown on Fe by magnetron sputtering on an MgO (001) substrate, with a protective Al2O3 capping layer. We determine through SW-HXPS that 8 of the 9 repeats are similar and ordered, with a period of 33 $\pm$ 4 angstrom, with minor presence of FeO at the interfaces and a significantly distorted top bilayer with ca. 3 times the oxidation of the lower layers at the top MgO/Fe interface. There is evidence of asymmetrical oxidation on the top and bottom of the Fe layers. We find agreement with dark-field scanning transmission electron microscope (STEM) and x-ray reflectivity measurements. Through the STEM measurements we confirm an overall epitaxial stack with dislocations and warping at the interfaces of ca. 5 angstrom. We also note a distinct difference in the top bilayer, especially MgO, with possible Fe inclusions. We thus demonstrate that SW-HXPS can be used to probe deep buried interfaces of novel magnetic devices with few angstrom precision.

cond-mat.mtrl-sci

Resonant photoemission with circular polarized light on magnetized LSMO

We have used resonant photoemission with circular polarized light as a new tool to obtain information about the electronic structure of half-metals. After careful sample surface preparation of La0.7Sr0.3MnO3, we have obtained a dichroic signal for the L2,3 absorption of Mn. Working with a magnetized sample and circular polarized light we observe a clear effect of the helicity of light on the position of the resonant Raman-Auger photoelectrons from the Mn 2p3p3d decay. These results allow us to achieve a rough estimate of the half-metallic spin half-gap.

cond-mat.mtrl-sci

Characterization of free standing InAs quantum membranes by standing wave hard x-ray photoemission spectroscopy

Free-standing nanoribbons of InAs quantum membranes (QMs) transferred onto a (Si/Mo) multilayer mirror substrate are characterized by hard x-ray photoemission spectroscopy (HXPS), and by standing-wave HXPS (SW-HXPS). Information on the chemical composition and on the chemical states of the elements within the nanoribbons was obtained by HXPS and on the quantitative depth profiles by SW-HXPS. By comparing the experimental SW-HXPS rocking curves to x-ray optical calculations, the chemical depth profile of the InAs(QM) and its interfaces were quantitatively derived with angstrom precision. We determined that: i) the exposure to air induced the formation of an InAsO$_4$ layer on top of the stoichiometric InAs(QM); ii) the top interface between the air-side InAsO$_4$ and the InAs(QM) is not sharp, indicating that interdiffusion occurs between these two layers; iii) the bottom interface between the InAs(QM) and the native oxide SiO$_2$ on top of the (Si/Mo) substrate is abrupt. In addition, the valence band offset (VBO) between the InAs(QM) and the SiO$_2$/(Si/Mo) substrate was determined by HXPS. The value of $VBO = 0.2 \pm 0.04$ eV is in good agreement with literature results obtained by electrical characterization, giving a clear indication of the formation of a well-defined and abrupt InAs/SiO$_2$ heterojunction. We have demonstrated that HXPS and SW-HXPS are non-destructive, powerful methods for characterizing interfaces and for providing chemical depth profiles of nanostructures, quantum membranes, and 2D layered materials.

cond-mat.mtrl-sci

Depth profiling charge accumulation from a ferroelectric into a doped Mott insulator

The electric field control of functional properties is a crucial goal in oxide-based electronics. Non-volatile switching between different resistivity or magnetic states in an oxide channel can be achieved through charge accumulation or depletion from an adjacent ferroelectric. However, the way in which charge distributes near the interface between the ferroelectric and the oxide remains poorly known, which limits our understanding of such switching effects. Here we use a first-of-a-kind combination of scanning transmission electron microscopy with electron energy loss spectroscopy, near-total-reflection hard X-ray photoemission spectroscopy, and ab-initio theory to address this issue. We achieve a direct, quantitative, atomic-scale characterization of the polarization-induced charge density changes at the interface between the ferroelectric BiFeO3 and the doped Mott insulator Ca1-xCexMnO3, thus providing insight on how interface-engineering can enhance these switching effects.

cond-mat.mtrl-sci

Superconductor to Mott insulator transition in YBa$_2$Cu$_3$O$_7$/LaCaMnO$_3$ heterostructures

The superconductor-to-insulator transition (SIT) induced by means such as external magnetic fields, disorder or spatial confinement is a vivid illustration of a quantum phase transition dramatically affecting the superconducting order parameter. In pursuit of a new realization of the SIT by interfacial charge transfer, we developed extremely thin superlattices composed of high $T_c$ superconductor YBa$_2$Cu$_3$O$_7$ (YBCO) and colossal magnetoresistance ferromagnet La$_{0.67}$Ca$_{0.33}$MnO$_3$ (LCMO). By using linearly polarized resonant X-ray absorption spectroscopy and magnetic circular dichroism, combined with hard X-ray photoelectron spectroscopy, we derived a complete picture of the interfacial carrier doping in cuprate and manganite atomic layers, leading to the transition from superconducting to an unusual Mott insulating state emerging with the increase of LCMO layer thickness. In addition, contrary to the common perception that only transition metal ions may response to the charge transfer process, we found that charge is also actively compensated by rare-earth and alkaline-earth metal ions of the interface. Such deterministic control of $T_c$ by pure electronic doping without any hindering effects of chemical substitution is another promising route to disentangle the role of disorder on the pseudo-gap and charge density wave phases of underdoped cuprates.

cond-mat.supr-con

Depth-Resolved Composition and Electronic Structure of Buried Layers and Interfaces in a LaNiO$_3$/SrTiO$_3$ Superlattice from Soft- and Hard- X-ray Standing-Wave Angle-Resolved Photoemission

LaNiO$_3$ (LNO) is an intriguing member of the rare-earth nickelates in exhibiting a metal-insulator transition for a critical film thickness of about 4 unit cells [Son et al., Appl. Phys. Lett. 96, 062114 (2010)]; however, such thin films also show a transition to a metallic state in superlattices with SrTiO$_3$ (STO) [Son et al., Appl. Phys. Lett. 97, 202109 (2010)]. In order to better understand this transition, we have studied a strained LNO/STO superlattice with 10 repeats of [4 unit-cell LNO/3 unit-cell STO] grown on an (LaAlO$_3$)$_{0.3}$(Sr$_2$AlTaO$_6$)$_{0.7}$ substrate using soft x-ray standing-wave-excited angle-resolved photoemission (SWARPES), together with soft- and hard- x-ray photoemission measurements of core levels and densities-of-states valence spectra. The experimental results are compared with state-of-the-art density functional theory (DFT) calculations of band structures and densities of states. Using core-level rocking curves and x-ray optical modeling to assess the position of the standing wave, SWARPES measurements are carried out for various incidence angles and used to determine interface-specific changes in momentum-resolved electronic structure. We further show that the momentum-resolved behavior of the Ni 3d eg and t2g states near the Fermi level, as well as those at the bottom of the valence bands, is very similar to recently published SWARPES results for a related La$_{0.7}$Sr$_{0.3}$MnO$_3$/SrTiO$_3$ superlattice that was studied using the same technique (Gray et al., Europhysics Letters 104, 17004 (2013)), which further validates this experimental approach and our conclusions. Our conclusions are also supported in several ways by comparison to DFT calculations for the parent materials and the superlattice, including layer-resolved density-of-states results.

cond-mat.str-el

Interface Engineering to Create a Strong Spin Filter Contact to Silicon

Integrating epitaxial and ferromagnetic Europium Oxide (EuO) directly on silicon is a perfect route to enrich silicon nanotechnology with spin filter functionality. To date, the inherent chemical reactivity between EuO and Si has prevented a heteroepitaxial integration without significant contaminations of the interface with Eu silicides and Si oxides. We present a solution to this long-standing problem by applying two complementary passivation techniques for the reactive EuO/Si interface: ($i$) an $in\:situ$ hydrogen-Si $(001)$ passivation and ($ii$) the application of oxygen-protective Eu monolayers --- without using any additional buffer layers. By careful chemical depth profiling of the oxide-semiconductor interface via hard x-ray photoemission spectroscopy, we show how to systematically minimize both Eu silicide and Si oxide formation to the sub-monolayer regime --- and how to ultimately interface-engineer chemically clean, heteroepitaxial and ferromagnetic EuO/Si $(001)$ in order to create a strong spin filter contact to silicon.

cond-mat.mtrl-sci

Energetic, spatial and momentum character of a buried interface: the two-dimensional electron gas between two metal oxides

The interfaces between two condensed phases often exhibit emergent physical properties that can lead to new physics and novel device applications, and are the subject of intense study in many disciplines. We here apply novel experimental and theoretical techniques to the characterization of one such interesting interface system: the two-dimensional electron gas (2DEG) formed in multilayers consisting of SrTiO$_3$ (STO) and GdTiO$_3$ (GTO). This system has been the subject of multiple studies recently and shown to exhibit very high carrier charge densities and ferromagnetic effects, among other intriguing properties. We have studied a 2DEG-forming multilayer of the form [6 unit cells STO/3 unit cells of GTO]$_{20}$ using a unique array of photoemission techniques including soft and hard x-ray excitation, soft x-ray angle-resolved photoemission, core-level spectroscopy, resonant excitation, and standing-wave effects, as well as theoretical calculations of the electronic structure at several levels and of the actual photoemission process. Standing-wave measurements below and above a strong resonance have been introduced as a powerful method for studying the 2DEG depth distribution. We have thus characterized the spatial and momentum properties of this 2DEG with unprecedented detail, determining via depth-distribution measurements that it is spread throughout the 6 u.c. layer of STO, and measuring the momentum dispersion of its states. The experimental results are supported in several ways by theory, leading to a much more complete picture of the nature of this 2DEG, and suggesting that oxygen vacancies are not the origin of it. Similar multi-technique photoemission studies of such states at buried interfaces, combined with comparable theory, will be a very fruitful future approach for exploring and modifying the fascinating world of buried-interface physics and chemistry.

cond-mat.mtrl-sci

Satellite Band Structure in Silicon Caused by Electron-Plasmon Coupling

We report the first angle-resolved photoemission measurement of the wave-vector dependent plasmon satellite structure of a three-dimensional solid, crystalline silicon. In sharp contrast to nanomaterials, which typically exhibit strongly wave-vector dependent, low-energy plasmons, the large plasmon energy of silicon facilitates the search for a plasmaron state consisting of resonantly bound holes and plasmons and its distinction from a weakly interacting plasmon-hole pair. Employing a first-principles theory, which is based on a cumulant expansion of the one-electron Green's function and contains significant electron correlation effects, we obtain good agreement with the measured photoemission spectrum for the wave-vector dependent dispersion of the satellite feature, but without observing the existence of plasmarons in the calculations.

cond-mat.mtrl-sci

Momentum-resolved electronic structure at a buried interface from soft x-ray standing-wave angle-resolved photoemission

Angle-resolved photoemission spectroscopy (ARPES) is a powerful technique for the study of electronic structure, but it lacks a direct ability to study buried interfaces between two materials. We address this limitation by combining ARPES with soft x-ray standing-wave (SW) excitation (SWARPES), in which the SW profile is scanned through the depth of the sample. We have studied the buried interface in a prototypical magnetic tunnel junction La0.7Sr0.3MnO3/SrTiO3. Depth- and momentum-resolved maps of Mn 3d eg and t2g states from the central, bulk-like and interface-like regions of La0.7Sr0.3MnO3 exhibit distinctly different behavior consistent with a change in the Mn bonding at the interface. We compare the experimental results to state-of-the-art density-functional and one-step photoemission theory, with encouraging agreement that suggests wide future applications of this technique.

cond-mat.mtrl-sci

Identifying the electronic character and role of the Mn states in the valence band of (Ga,Mn)As

We report high-resolution hard x-ray photoemission spectroscopy results on (Ga,Mn)As films as a function of Mn doping. Supported by theoretical calculations we identify, over the entire 1% to 13% Mn doping range, the electronic character of the states near the top of the valence band. Magnetization and temperature dependent core-level photoemission spectra reveal how the delocalized character of the Mn states enables the bulk ferromagnetic properties of (Ga,Mn)As.

cond-mat.str-el

Observation and resonant x-ray optical interpretation of multi-atom resonant photoemission effects in O 1s emission from NiO

We present experimental and theoretical results for the variation of the O 1s intensity from a NiO(001) surface as the excitation energy is varied through the Ni 2p1/2,3/2 absorption resonances, and as the incidence angle of the radiation is varied from grazing to larger values. For grazing incidence, a strong multi-atom resonant photoemission (MARPE) effect is seen on the O 1s intensity as the Ni 2p resonances are crossed, but its magnitude decreases rapidly as the incidence angle is increased. Resonant x-ray optical (RXRO) calculations are found to predict these effects very well, although the experimental effects are found to decrease at higher incidence angles faster than those in theory. The potential influence of photoelectron diffraction effects on such measurements are also considered, including experimental data with azimuthal-angle variation and corresponding multiple-scattering-diffraction calculations, but we conclude that they do not vary beyond what is expected on the basis of the change in photoelectron kinetic energy. Varying from linear polarization to circular polarization is found to enhance these effects in NiO considerably, although the reasons are not clear. We also discuss the relationship of these measurements to other related interatomic resonance experiments and theoretical developments, and make some suggestions for future studies in this area.

cond-mat.other

Temperature-Dependent X-Ray Absorption Spectroscopy of Colossal Magnetoresistive Perovskites

The temperature dependence of the O K-edge pre-edge structure in the x-ray absorption spectra of the perovskites La(1-x)A(x)MnO(3), (A = Ca, Sr; x = 0.3, 0.4) reveals a correlation between the disappearance of the splitting in the pre-edge region and the presence of Jahn-Teller distortions. The different magnitudes of the distortions for different compounds is proposed to explain some dissimilarity in the line shape of the spectra taken above the Curie temperature.

cond-mat.str-el

Correction of non-linearity effects in detectors for electron spectroscopy

Using photoemission intensities and a detection system employed by many groups in the electron spectroscopy community as an example, we have quantitatively characterized and corrected detector non-linearity effects over the full dynamic range of the system. Non-linearity effects are found to be important whenever measuring relative peak intensities accurately is important, even in the low-countrate regime. This includes, for example, performing quantitative analyses for surface contaminants or sample bulk stoichiometries, where the peak intensities involved can differ by one or two orders of magnitude, and thus could occupy a significant portion of the detector dynamic range. Two successful procedures for correcting non-linearity effects are presented. The first one yields directly the detector efficiency by measuring a flat-background reference intensity as a function of incident x-ray flux, while the second one determines the detector response from a least-squares analysis of broad-scan survey spectra at different incident x-ray fluxes. Although we have used one spectrometer and detection system as an example, these methodologies should be useful for many other cases.

physics.ins-det

Direct Observation of High-Temperature Polaronic Behavior In Colossal Magnetoresistive Manganites

The temperature dependence of the electronic and atomic structure of the colossal magnetoresistive oxides $La_{1-x}Sr_{x}MnO_{3}$ (x = 0.3, 0.4) has been studied using core and valence level photoemission, x-ray absorption and emission, and extended x-ray absorption fine structure spectroscopy. A dramatic and reversible change of the electronic structure is observed on crossing the Curie temperature, including charge localization and spin moment increase of Mn, together with Jahn-Teller distortions, both signatures of polaron formation. Our data are also consistent with a phase-separation scenario.

cond-mat.str-el

Differential Photoelectron Holography: A New Approach for Three-Dimensional Atomic Imaging

We propose differential holography as a method to overcome the long-standing forward-scattering problem in photoelectron holography and related techniques for the three-dimensional imaging of atoms. Atomic images reconstructed from experimental and theoretical Cu 3p holograms from Cu(001) demonstrate that this method suppresses strong forward-scattering effects so as to yield more accurate three-dimensional images of side- and back-scattering atoms.

cond-mat