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M. S. Golden

Publications and source records attributed to M. S. Golden.

At least 37 records · Page 2Linked to original sources

Defect engineering in oxide heterostructures by enhanced oxygen surface exchange

The synthesis of materials with well-controlled composition and structure improves our understanding of their intrinsic electrical transport properties. Recent developments in atomically controlled growth have been shown to be crucial in enabling the study of new physical phenomena in epitaxial oxide heterostructures. Nevertheless, these phenomena can be influenced by the presence of defects that act as extrinsic sources of both doping and impurity scattering. Control over the nature and density of such defects is therefore necessary, are we to fully understand the intrinsic materials properties and exploit them in future device technologies. Here, we show that incorporation of a strontium copper oxide nano-layer strongly reduces the impurity scattering at conducting interfaces in oxide LaAlO3-SrTiO3(001) heterostructures, opening the door to high carrier mobility materials. We propose that this remote cuprate layer facilitates enhanced suppression of oxygen defects by reducing the kinetic barrier for oxygen exchange in the hetero-interfacial film system. This design concept of controlled defect engineering can be of significant importance in applications in which enhanced oxygen surface exchange plays a crucial role.

cond-mat.mtrl-sci↗

Hard x-ray photoemission and density functional theory study of the internal electric field in SrTiO3/LaAlO3 oxide heterostructures

A combined experimental and theoretical investigation of the electronic structure of the archetypal oxide heterointerface system LaAlO3 on SrTiO3 is presented. High-resolution, hard x-ray photoemission is used to uncover the occupation of Ti 3d states and the relative energetic alignment - and hence internal electric fields - within the LaAlO3 layer. Firstly, the Ti 2p core level spectra clearly show occupation of Ti 3d states already for two unit cells of LaAlO3. Secondly, the LaAlO3 core levels were seen to shift to lower binding energy as the LaAlO3 overlayer thickness, n, was increased - agreeing with the expectations from the canonical electron transfer model for the emergence of conductivity at the interface. However, not only is the energy offset of only 300meV between n=2 (insulating interface) and n=6 (metallic interface) an order of magnitude smaller than the simple expectation, but it is also clearly not the sum of a series of unit-cell by unit-cell shifts within the LaAlO3 block. Both of these facts argue against the simple charge-transfer picture involving a cumulative shift of the LaAlO3 valence bands above the SrTiO3 conduction bands, resulting in charge transfer only for n>3. Turning to the theoretical data, our density functional simulations show that the presence of oxygen vacancies at the LaAlO3 surface at the 25% level reverses the direction of the internal field in the LaAlO3. Therefore, taking the experimental and theoretical results together, a consistent picture emerges for real-life samples in which nature does not wait until n=4 and already for n=2, mechanisms other than internal-electric-field-driven electron transfer from idealized LaAlO3 to near-interfacial states in the SrTiO3 substrate are active in heading off the incipient polarization catastrophe that drives the physics in these systems.

cond-mat.str-el↗

Anisotropic Impurity-States, Quasiparticle Scattering and Nematic Transport in Underdoped Ca(Fe1-xCox)2As2

Iron-based high temperature superconductivity develops when the `parent' antiferromagnetic/orthorhombic phase is suppressed, typically by introduction of dopant atoms. But their impact on atomic-scale electronic structure, while in theory quite complex, is unknown experimentally. What is known is that a strong transport anisotropy with its resistivity maximum along the crystal b-axis, develops with increasing concentration of dopant atoms; this `nematicity' vanishes when the `parent' phase disappears near the maximum superconducting Tc. The interplay between the electronic structure surrounding each dopant atom, quasiparticle scattering therefrom, and the transport nematicity has therefore become a pivotal focus of research into these materials. Here, by directly visualizing the atomic-scale electronic structure, we show that substituting Co for Fe atoms in underdoped Ca(Fe1-xCox)2As2 generates a dense population of identical anisotropic impurity states. Each is ~8 Fe-Fe unit cells in length, and all are distributed randomly but aligned with the antiferromagnetic a-axis. By imaging their surrounding interference patterns, we further demonstrate that these impurity states scatter quasiparticles in a highly anisotropic manner, with the maximum scattering rate concentrated along the b-axis. These data provide direct support for the recent proposals that it is primarily anisotropic scattering by dopant-induced impurity states that generates the transport nematicity; they also yield simple explanations for the enhancement of the nematicity proportional to the dopant density and for the occurrence of the highest resistivity along the b-axis.

cond-mat.supr-con↗

Surface adatom conductance filtering in scanning tunneling spectroscopy of Co-doped BaFe2As2 iron pnictide superconductors

We establish in a combination of ab initio theory and experiments that the tunneling process in scanning tunneling microscopy/spectroscopy on the A-122 iron pnictide superconductors - in this case BaFe$_{2-x}$Co$_x$As$_2$ - involve a strong adatom filtering of the differential conductance from the near-EF Fe3d states, which in turn originates from the top-most sub-surface Fe layer of the crystal. The calculations show that the dominance of surface Ba-related tunneling pathways leaves fingerprints found in the experimental differential conductance data, including large particle-hole asymmetry and an energy-dependent contrast inversion.

cond-mat.supr-con↗

Superconductivity in the doped topological insulator Cu$_x$Bi$_2$Se$_3$ under high pressure

We report a high-pressure single crystal study of the topological superconductor Cu$_x$Bi$_2$Se$_3$. Resistivity measurements under pressure show superconductivity is depressed smoothly. At the same time the metallic behavior is gradually lost. The upper critical field data $B_{c2}(T)$ under pressure collapse onto a universal curve. The absence of Pauli limiting and the comparison of $B_{c2}(T)$ to a polar state function point to spin-triplet superconductivity, but an anisotropic spin-singlet state cannot be discarded completely.

cond-mat.supr-con↗

Bilayer manganites: polarons in the midst of a metallic breakdown

The exact nature of the low temperature electronic phase of the manganite materials family, and hence the origin of their colossal magnetoresistant (CMR) effect, is still under heavy debate. By combining new photoemission and tunneling data, we show that in La{2-2x}Sr{1+2x}Mn2O7 the polaronic degrees of freedom win out across the CMR region of the phase diagram. This means that the generic ground state is that of a system in which strong electron-lattice interactions result in vanishing coherent quasi-particle spectral weight at the Fermi level for all locations in k-space. The incoherence of the charge carriers offers a unifying explanation for the anomalous charge-carrier dynamics seen in transport, optics and electron spectroscopic data. The stacking number N is the key factor for true metallic behavior, as an intergrowth-driven breakdown of the polaronic domination to give a metal possessing a traditional Fermi surface is seen in the bilayer system.

cond-mat.str-el↗

Pseudogap-less high T$_{c}$ superconductivity in BaCo$_{x}$Fe$_{2-x}$As$_{2}$

The pseudogap state is one of the peculiarities of the cuprate high temperature superconductors. Here we investigate its presence in BaCo$_{x}$Fe$_{2-x}$As$_{2}$, a member of the pnictide family, with temperature dependent scanning tunneling spectroscopy. We observe that for under, optimally and overdoped systems the gap in the tunneling spectra always closes at the bulk T$_{c}$, ruling out the presence of a pseudogap state. For the underdoped case we observe superconducting gaps over large fields of view, setting a lower limit of tens of nanometers on the length scale of possible phase separated regions.

cond-mat.supr-con↗

Dissimilarities between the electronic structure of chemically doped and chemically pressurized iron pnictides from an angle-resolved photoemission spectroscopy study

We have studied the electronic structure of EuFe2As2-xPx using high resolution angle-resolved photoemission spectroscopy. Upon substituting As with the isovalent P, which leads to a chemical pressure and to superconductivity, we observe a non-rigid-band like change of the electronic structure along the center of the Brillouin zone (BZ): an orbital and kz dependent increase or decrease in the size of the hole pockets near the Gamma - Z line. On the other hand, the diameter of the Fermi surface cylinders at the BZ corner forming electron pockets, hardly changes. This is in stark contrast to p and n-type doped iron pnictides where, on the basis of ARPES experiments, a more rigid-band like behavior has been proposed. These findings indicate that there are different ways in which the nesting conditions can be reduced causing the destabilization of the antiferromagnetic order and the appearance of the superconducting dome.

cond-mat.supr-con↗

Droplet-like Fermi surfaces in the anti-ferromagnetic phase of EuFe$_2$As$_2$, an Fe-pnictide superconductor parent compound

Using angle resolved photoemission it is shown that the low lying electronic states of the iron pnictide parent compound EuFe$_2$As$_2$ are strongly modified in the magnetically ordered, low temperature, orthorhombic state compared to the tetragonal, paramagnetic case above the spin density wave transition temperature. Back-folded bands, reflected in the orthorhombic/ anti-ferromagnetic Brillouin zone boundary hybridize strongly with the non-folded states, leading to the opening of energy gaps. As a direct consequence, the large Fermi surfaces of the tetragonal phase fragment, the low temperature Fermi surface being comprised of small droplets, built up of electron and hole-like sections. These high resolution ARPES data are therefore in keeping with quantum oscillation and optical data from other undoped pnictide parent compounds.

cond-mat.supr-con↗

Optical properties of BaFe$_{2-x}$Co$_x$As$_2$

We present detailed temperature dependent optical data on BaFe$_{2-x}$Co$_{x}$As$_{2}$ (BCFA), with x = 0.14, between 4 meV and 6.5 eV. We analyze our spectra to determine the main optical parameters and show that in this material the interband conductivity already starts around 10 meV. We determine the superfluid density to be 2.2 10^{7}$ cm^{-2}, which places optimally doped BFCA close to the Uemura line. Our experimental data shows clear signs of a superconducting gap with 2$Δ_{1}$ = 6.2 $\pm$ 0.8 meV. In addition we show that the optical spectra are consistent with the presence of an additional band of strongly scattered carriers with a larger gap, 2$Δ_{2}$ = 14 $\pm$ 2 meV.

cond-mat.supr-con↗

Orbital character variation of the Fermi surface and doping dependent changes of the dimensionality in BaFe2-xCoxAs2 from angle-resolved photoemission spectroscopy

From a combination of high resolution angle-resolved photoemission spectroscopy and density functional calculations, we show that BaFe2As2 possesses essentially two-dimensional electronic states, with a strong change of orbital character of two of the Gamma-centered Fermi surfaces as a function of kz. Upon Co doping, the electronic states in the vicinity of the Fermi level take on increasingly three-dimensional character. Both the orbital variation with kz and the more three-dimensional nature of the doped compounds have important consequences for the nesting conditions and thus possibly also for the appearance of antiferromagnetic and superconducting phases.

cond-mat.supr-con↗

The cleavage surface of the BaFe_(2-x)Co_(x)As_(2) and Fe_(y)Se_(1-x)Te_(x) superconductors: from diversity to simplicity

We elucidate the termination surface of cleaved single crystals of the BaFe_(2-x)Co_(x)As_(2) and Fe_(y)Se_(1-x)Te_(x) families of the high temperature iron based superconductors. By combining scanning tunneling microscopic data with low energy electron diffraction we prove that the termination layer of the Ba122 systems is a remnant of the Ba layer, which exhibits a complex diversity of ordered and disordered structures. The observed surface topographies and their accompanying superstructure reflections in electron diffraction depend on the cleavage temperature. In stark contrast, Fe_(y)Se_(1-x)Te_(x) possesses only a single termination structure - that of the tetragonally ordered Se_(1-x)Te_(x) layer.

cond-mat.supr-con↗

A high resolution, hard x-ray photoemission investigation of La_(2-2x)Sr_(1+2x)Mn_2O_7 (0.30<x<0.50): on microscopic phase separation and the surface electronic structure of a bilayered CMR manganite

Photoemission data taken with hard x-ray radiation on cleaved single crystals of the bilayered, colossal magnetoresistant manganite La_(2-2x)Sr_(1+2x)Mn_2O_7 (LSMO) with 0.30<x<0.50 are presented. Making use of the increased bulk-sensitivity upon hard x-ray excitation it is shown that the core level footprint of the electronic structure of the LSMO cleavage surface is identical to that of the bulk. Furthermore, by comparing the core level shift of the different elements as a function of doping level x, it is shown that microscopic phase separation is unlikely to occur for this particular manganite well above the Curie temperature.

cond-mat.str-el↗

Electronic structure studies of BaFe2As2 by angle-resolved photoemission spectroscopy

We report high resolution angle-resolved photoemission spectroscopy (ARPES) studies of the electronic structure of BaFe$_2$As$_2$, which is one of the parent compounds of the Fe-pnictide superconductors. ARPES measurements have been performed at 20 K and 300 K, corresponding to the orthorhombic antiferromagnetic phase and the tetragonal paramagnetic phase, respectively. Photon energies between 30 and 175 eV and polarizations parallel and perpendicular to the scattering plane have been used. Measurements of the Fermi surface yield two hole pockets at the $Γ$-point and an electron pocket at each of the X-points. The topology of the pockets has been concluded from the dispersion of the spectral weight as a function of binding energy. Changes in the spectral weight at the Fermi level upon variation of the polarization of the incident photons yield important information on the orbital character of the states near the Fermi level. No differences in the electronic structure between 20 and 300 K could be resolved. The results are compared with density functional theory band structure calculations for the tetragonal paramagnetic phase.

cond-mat.supr-con↗

Nanoscale superconducting gap variations, strong coupling signatures and lack of phase separation in optimally doped BaFe1.86Co0.14As2

We present tunneling data from optimally-doped, superconducting BaFe1.86Co0.14As2 and its parent compound, BaFe2As2. In the superconductor, clear coherence-like peaks are seen across the whole field of view, and their analysis reveals nanoscale variations in the superconducting gap value, Delta. The average magnitude of 2Delta is ~7.4 kBTC, which exceeds the BCS weak coupling value for either s- or d-wave superconductivity. The characteristic length scales of the deviations from the average gap value, and of an anti-correlation discovered between the gap magnitude and the zero bias conductance, match well with the average separation between the Co dopant ions in the superconducting FeAs planes. The tunneling spectra themselves possess a peak-dip-hump lineshape, suggestive of a coupling of the superconducting electronic system to a well-defined bosonic mode of energy 4.7 kBTC, such as the spin resonance observed recently in inelastic neutron scattering.

cond-mat.supr-con↗

A high resolution, hard X-ray photoemission investigation of BaFe$_2$As$_2$: moderate influence of the surface and evidence for a low degree of Fe 3d - As 4p hybridization of the near-E$_F$ electronic states

Photoemission data taken with hard X-ray radiation on cleaved single crystals of the barium parent compound of the MFe$_2$As$_2$ pnictide high temperature superconductor family are presented. Making use of the increased bulk-sensitivity upon hard X-ray excitation, and comparing the results to data taken at conventional VUV photoemission excitation energies, it is shown that the BaFe$_2$As$_2$ cleavage surface provides an electrostatic environment that is slightly different to the bulk, most likely in the form of a modified Madelung potential. However, as the data argue against a different surface doping level, and the surface-related features in the spectra are by no means as dominating as seen in systems such as YBa$_2$Cu$_3$O$_x$, we can conclude that the itinerant, near-E$_F$ electronic states are almost unaffected by the existence of the cleavage surface. Furthermore, exploiting the strong changes in photoionisation cross section between the Fe and As states across the wide photon energy range employed, it is shown that the degree of energetic overlap between the iron 3d and arsenic 4p valence bands is particularly small at the Fermi level, which can only mean a very low degree of hybridization between the Fe 3d and As 4p states near and at E$_F$. Consequently, the itinerancy of the charge carriers in this group of materials involves mainly the Fe 3d - Fe 3d overlap integrals with at best a minor role for the Fe 3d - As 4p hopping parameters, and that the states which support superconductivity upon doping are essentially of Fe 3d character.

cond-mat.supr-con↗

Non-gapped Fermi surfaces, quasiparticles and the anomalous temperature dependence of the near-$E_F$ electronic states in the CMR oxide La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ with $x=0.36$

After years of research into colossal magnetoresistant (CMR) manganites using bulk techniques, there has been a recent upsurge in experiments directly probing the electronic states at or near the surface of the bilayer CMR materials La$_{2-2x}$Sr$_{1+2x}$Mn$_2$O$_7$ using angle-resolved photoemission or scanning probe microscopy. Here we report new, temperature dependent, angle resolved photoemission data from single crystals with a doping level of $x=0.36$. The first important result is that there is no sign of a pseudogap in the charge channel of this material for temperatures below the Curie temperature $T_C$. The second important result concerns the temperature dependence of the electronic states. The temperature dependent changes in the Fermi surface spectra both at the zone face and zone diagonal regions in $k$-space indicate that the coherent quasiparticle weight disappears for temperatures significantly above $T_C$, and that the $k$-dependence of the T-induced changes in the spectra invalidate an interpretation of these data in terms of the superposition of a `universal' metallic spectrum and an insulating spectrum whose relative weight changes with temperature. In this sense, our data are not compatible with a phase separation scenario.

cond-mat.str-el↗

Antinodal quasiparticles below and above T_Curie in the CMR oxide La_(2-2x)Sr_(1+2x)Mn_(2)O_(7) with x=0.36

In light of recent conflicting angle resolved photoemission studies on the bilayered colossal magnetoresistant (CMR) manganite La_{2-2x}Sr_{1+2x}Mn_{2}O_{7} (0.36< x< 0.40), new ARPES data are presented for x=0.36 and 0.40, showing only for the former clear quasiparticle-like features at and around the (pi, 0)-point in k-space. The electronic states are clearly renormalised, both as regards their dispersion relation and lifetime due to coupling to bosonic degrees of freedom. Importantly, both the existence of quasiparticles and their renormalisation survive well into the paramagnetic state, up to 50 K above T_Curie. This argues against strong coupling to spin modes and raises questions regarding the nature of the paramagnetic insulating phase.

cond-mat.str-el↗