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R F Klie

Publications and source records attributed to R F Klie.

5 recordsLinked to original sources

Inversion of two-band superconductivity at the critical electron doping of (Mg, Al)B2.

Electron energy-loss spectroscopy (EELS) was combined with heat capacity measurements to probe changes of electronic structure and superconductivity in Mg(1-x)Al(x)B(2). A simultaneous decrease of EELS intensity from sigma-band hole states and the magnitude of the sigma gap was observed with increasing x, thus verifying that band filling results in the loss of strong superconductivity. These quantities extrapolated to zero at x approximately 0.33 as inferred from the unit cell volume. However, superconductivity was not quenched completely, but persisted with T(c) < 7 K up to about x approximately 55. Only the pi band had detectable density of states for 0.33 < or =x < or = 0.55, implying an inversion of the two-band hierarchy of MgB(2) in that regime. Since pi-band superconductivity is active in other materials such as intercalated graphite, implications for new materials with high T(c) are discussed.

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Enhanced current transport at grain boundaries in high-T(c) superconductors.

Large-scale applications of high-transition-temperature (high-T(c)) superconductors, such as their use in superconducting cables, are impeded by the fact that polycrystalline materials (the only practical option) support significantly lower current densities than single crystals. The superconducting critical current density (J(c)) across a grain boundary drops exponentially if the misorientation angle exceeds 2 degrees -7 degrees. Grain texturing reduces the average misorientation angle, but problems persist. Adding impurities (such as Ca in YBa2Cu3O7-delta; YBCO) leads to increased J(c) (refs 9, 10), which is generally attributed to excess holes introduced by Ca2+ substituting for Y3+ (ref. 11). However, a comprehensive physical model for the role of grain boundaries and Ca doping has remained elusive. Here we report calculations, imaging and spectroscopy at the atomic scale that demonstrate that in poly-crystalline YBCO, highly strained grain-boundary regions contain excess O vacancies, which reduce the local hole concentration. The Ca impurities indeed substitute for Y, but in grain-boundary regions under compression and tension they also replace Ba and Cu, relieving strain and suppressing O-vacancy formation. Our results demonstrate that the ionic radii are more important than their electronic valences for enhancing J(c).

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Atomic resolution STEM analysis of defects and interfaces in ceramic materials.

Atomic resolution scanning transmission electron microscopy (STEM) analysis, in particular the combination of Z-contrast imaging and electron energy-loss spectroscopy (EELS) has been successfully used to measure the atomic and electronic structure of materials with sub-nanometer spatial resolution. Furthermore, the combination of this incoherent imaging technique with EELS allows us to correlate certain structural features, such as defects or interfaces directly with the measured changes in the local electronic fine-structure. In this review, we will discuss the experimental procedures for achieving high-resolution Z-contrast imaging and EELS. We will describe the alignment and experimental setup for high-resolution STEM analysis and also describe some of our recent results where the combined use of atomic-resolution Z-contrast imaging and column-by-column EELS has helped solve important materials science problems.

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Observation of oxygen vacancy ordering and segregation in perovskite oxides.

Oxygen vacancies are known to dominate the overall electrical behavior of perovskite oxides, which are used in many applications. Although theories have been developed to explain the effect of these vacancies and the defect chemistry of perovskites, there has yet to be incontrovertible evidence of the fundamental origins of the structure-property relationship. However, recently developed technologies in scanning transmission electron microscopy, such as Z-contrast imaging and EELS combined with in-situ heating experiments, provide a new opportunity to address vacancy characteristics and defect chemistry on the basic atomic level. In this paper we discuss the practical aspects of these techniques and demonstrate their application to the characterization of defect chemistry and vacancies in ordered micro-domains, at domain boundaries and at grain boundaries.

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Application of atomic scale STEM techniques to the study of interfaces and defects in materials.

Incoherent imaging and analysis techniques in the scanning transmission electron microscope (STEM) provide the potential to map changes in structure, composition and bonding that occur at materials interfaces and defects on the fundamental atomic scale. Such comprehensive characterization capabilities permit a detailed analysis of the structure-property relationships of interfaces and defects to be performed. In this paper, we discuss the resolution limits of such techniques in the JEOL 2010F STEM/TEM operating both under standard conditions and at elevated temperatures. Examples of the use of such techniques to quantify the atomic scale defect chemistry at interfaces and defects in perovskite oxides, the growth and structure of II-VI and III-V quantum dots and the electronic structure of threading dislocations in GaN will also be presented.

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