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Christen, Hans M

Publications and source records attributed to Christen, Hans M.

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Smooth cubic commensurate oxides on gallium nitride

Smooth, commensurate alloys of 〈111〉-oriented Mg{sub 0.52}Ca{sub 0.48}O (MCO) thin films are demonstrated on Ga-polar, c+ [0001]-oriented GaN by surfactant-assisted molecular beam epitaxy and pulsed laser deposition. These are unique examples of coherent cubic oxide|nitride interfaces with structural and morphological perfection. Metal-insulator-semiconductor capacitor structures were fabricated on n-type GaN. A comparison of leakage current density for conventional and surfactant-assisted growth reveals a nearly 100× reduction in leakage current density for the surfactant-assisted samples. HAADF-STEM images of the MCO|GaN interface show commensurate alignment of atomic planes with minimal defects due to lattice mismatch. STEM and DFT calculations show that GaN c/2 steps create incoherent boundaries in MCO over layers which manifest as two in-plane rotations and determine consequently the density of structural defects in otherwise coherent MCO. This new understanding of interfacial steps between HCP and FCC crystals identifies the steps needed to create globally defect-free heterostructures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Focused-ion-beam induced damage in thin films of complex oxide BiFeO{sub 3}

An unexpected, strong deterioration of crystal quality is observed in epitaxial perovskite BiFeO{sub 3} films in which microscale features have been patterned by focused-ion-beam (FIB) milling. Specifically, synchrotron x-ray microdiffraction shows that the damaged region extends to tens of μm, but does not result in measureable changes to morphology or stoichiometry. Therefore, this change would go undetected with standard laboratory equipment, but can significantly influence local material properties and must be taken into account when using a FIB to manufacture nanostructures. The damage is significantly reduced when a thin metallic layer is present on top of the film during the milling process, clearly indicating that the reduced crystallinity is caused by ion beam induced charging.

36 MATERIALS SCIENCE↗
DOE OSTI2014

nomalous Interface and Surface Strontium Segregation in (La 1-y Sr y ) 2 CoO 4 /La 1-x Sr x CoO 3- Heterostructured Thin Films

Heterostructured materials have shown unusual physiochemical properties at the interfaces such as two dimensional electron gas systems, high-temperature superconductivity, and enhanced catalysis. Here we report the first atomic-scale evidence of the microscopic structure of a perovskite/Ruddlesden-Popper heterostructure (having La1-xSrxCoO3- /(La1-ySry)2CoO4 ), and anomalous strontium segregation at the interface and in the Ruddlesden-Popper structure using direct X-ray methods combined with ab initio calculations. The remarkably enhanced activity of such heterostructured surfaces relative to bulk perovskite and Ruddlesden-Popper oxides previously shown for oxygen electrocatalysis at elevated temperatures can be attributed to reduced thermodynamic penalty of oxygen vacancies in the oxide structure associated with Sr segregation observed in the heterostructure. Our findings provide insights for the design of highly active catalysts for energy conversion and storage applications.

Feng, Zhenxing↗
DOE OSTI2014

Enhanced oxygen evolution activity of IrO2 and RuO2 (100) surfaces

The activities of the oxygen evolution reaction (OER) on IrO2 and RuO2 catalysts are among the highest known to date. However, the intrinsic OER activities of surfaces with defined crystallographic orientations are not well established experimentally. Here we report that the (100) surface of IrO2 and RuO2 is more active than the (110) surface that has been traditionally explored by density functional theory studies. The relation between the OER activity and density of coordinatively undersaturated metal sites exposed on each rutile crystallographic facet is discussed. The surface-orientation dependent activities can guide the design of high-surface-area catalysts with increased activity for electrolyzers, metal-air batteries, and photoelectrochemical water splitting applications.

Electrochemisty↗
DOE OSTI2014

Structure and switching of in-plane ferroelectric nano-domains in strained PbxSr1-xTiO3 thin films

Nanoscale ferroelectrics, the active elements of a variety of nanoelectronic devices, develop denser and richer domain structures than the bulk counterparts. With shrinking device sizes understanding and controlling domain formation in nanoferroelectrics is being intensely studied. Here we show that a precise control of the epitaxy and the strain allows stabilizing a hierarchical domain architecture in PbxSr1-xTiO3 thin films, showing periodic, purely in-plane polarized, ferroelectric nano-domains that can be switched by a scanning probe.

epitaxial thin films↗
DOE OSTI2013

Antisite Defects In La0.7Sr0.3MnO3 and La0.7Sr0.3FeO3

Complex oxide thin films and superlattices with the perovskite ABO3 structure have been found to possess novel functional properties. Here, we present our discovery of antisite defects, La ions in Fe(Mn) sites (denoted as LaB), in a La0.7Sr0.3MnO3/La0.7Sr0.3FeO3 superlattice. The antisite defect was directly characterized by atomic resolution Z-contrast imaging and the composition and electronic structure was analyzed by electron energy loss spectroscopy in an aberration-corrected scanning transmission electron microscope. Density functional theory was used to calculate the formation energy, showing that the formation of the detected antisite defects is a consequence of the slightly reducing conditions during sample growth.

Gu, Meng↗
DOE OSTI2013

Nanoscale Probing of Voltage Activated Oxygen Reduction/Evolution Reactions in Nanopatterned (LaxSr1-x)CoO3- Cathodes

Bias-dependent mechanisms of reversible and irreversible electrochemical processes on a (La0.5Sr0.5)2CoO4 modified (LaxSr1-x)CoO3- surface are studied using dynamic electrochemical strain microscopy (D-ESM). The reversible oxygen reduction/evolution process is activated at voltages as low as 3 4 V and the degree of transformation increases linearly with applied bias. The irreversible processes associated with static surface deformation become apparent above 10 12 V. Post-mortem focused-ion milling combined with atomic resolution scanning transmission electron microscopy and electron energy loss spectroscopy is used to establish the mechanisms of irreversible transformations and attribute it to amorphization of the top layer of material. These studies both establish the framework for probing irreversible electrochemical processes in solids and illustrate rich spectrum of electrochemical transformations underpinning electrocatalytic activity in cobaltites.

electrochemical strain microscopy↗
DOE OSTI2013

Spatially Resolved Mapping of Oxygen Reduction/evolution Reaction on Solid-Oxide Fuel Cell Cathodes with sub-10 nm Resolution

Spatial localization of the oxygen reduction/evolution reactions (ORR/OER) on lanthanum strontium cobaltite (LSCO) surfaces with perovskite and layered perovskite structures is studied on the sub-10 nanometer level. Comparison between Electrochemical Strain Microscopy (ESM) and structural imaging by scanning transmission electron microscopy (STEM) suggest that small-angle grain boundaries act as regions with enhanced electrochemical activity. The ESM activity is compared across a family of LSCO samples, demonstrating excellent agreement with macroscopic behaviors. This study potentially paves the way for deciphering the mechanisms of electrochemical activity of solids on the level of single extended structural defects such as grain boundaries and dislocations.

Electrochemical Strain microcsopy↗
DOE OSTI2013

Room-Temperature Multiferroic Hexagonal LuFeO3

We observed the coexistence of ferroelectricity and weak ferromagnetism at room temperature in the hexagonal phase of LuFeO3 stabilized by epitaxial thin film growth. While the ferroelectricity in hexagonal LuFeO3 can be understood as arising from its polar structure, the observation of weak ferromagnetism at room temperature is remarkable considering the frustrated triangular spin structure. An explanation of the room temperature weak ferromagnetism is proposed in terms of a subtle lattice distortion revealed by the structural characterization. The combination of ferroelectricity and weak ferromagnetism in epitaxial films at room temperature offers great potential for the application of this novel multiferroic material in next generation devices.

Cheng, Xuemei↗