%0 Journal Article %J Physical Review B %D 2002 %T In Situ X-Ray Absorption Spectroscopy Study of Hydrogen Absorption by Nickel-Magnesium Thin Films %A Baker Farangis %A Ponnusamy Nachimuthu %A Thomas J. Richardson %A Jonathan L. Slack %A Rupert C.C. Perera %A Eric M. Gullikson %A Dennis W. Lindle %A Michael D. Rubin %X

Structural and electronic properties of co-sputtered Ni-Mg thin films with varying Ni to Mg ratio were studied by in situ x-ray absorption spectroscopy in the Ni L-edge and Mg K-edge regions. Codeposition of the metals led to increased disorder and decreased coordination around Ni and Mg compared to pure metal films. Exposure of the metallic films to hydrogen resulted in formation of hydrides and increased disorder. The presence of hydrogen as a near neighbor around Mg caused a drastic reduction in the intensities of multiple scattering resonances at higher energies. The optical switching behavior and changes in the x-ray spectra varied with Ni to Mg atomic ratio. Pure Mg films with Pd overlayers were converted to MgH2: The H atoms occupy regular sites as in bulk MgH2. Although optical switching was slow in the absence of Ni, the amount of H2 absorption was large. Incorporation of Ni in Mg films led to an increase in the speed of optical switching but decreased maximum transparency. Significant shifts in the Ni L3 and L2 peaks are consistent with strong interaction with hydrogen in the mixed films.

%B Physical Review B %V 67 %8 02/2003 %G eng %N 8 %1

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%2 LBNL-51067 %! Phys. Rev. B %R 10.1103/PhysRevB.67.085106 %0 Conference Paper %B Fifth International Meeting on Electrochromism %D 2002 %T Structural and Electronic Properties of Magnesium-3D Transition Metal Switchable Mirrors %A Baker Farangis %A Ponnusamy Nachimuthu %A Thomas J. Richardson %A Jonathan L. Slack %A Bruno K. Meyer %A Rupert C.C. Perera %A Michael D. Rubin %K EXAFS %K Hydrogen storage materials %K NEXAFS %K thin films %K x-ray diffraction %X

We have observed reversible mirror-to-transparent state switching in a variety of mixed metal thin films containing magnesium and first-row transition elements including Ni, Fe, Co, Mn, and Ti. The very large changes in both reflectance and transmittance on loading these films with hydrogen are accompanied by significant structural and electronic transformations. The valence states and coordination of metal atoms during hydrogen loading were followed using dynamic in situ transmissionmode X-ray absorption spectroscopy. Time-resolved Mg K-edge and Ni, Co, Mn, and Ti L-edge spectra reflect both reversible and irreversible changes in the metal environments. These spectra are compared to those of reference materials and to predictions from calculations.

%B Fifth International Meeting on Electrochromism %C Golden, CO %8 12/2002 %G eng %1

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%2 LBNL-51415 %R 10.1016/j.ssi.2003.08.041 %0 Journal Article %J Journal of Alloys and Compounds %D 2002 %T X-Ray Absorption Spectroscopy of Transition Metal-Magnesium Hydride Thin Films %A Thomas J. Richardson %A Baker Farangis %A Jonathan L. Slack %A Ponnusamy Nachimuthu %A Rupert C.C. Perera %A Nobumichi Tamura %A Michael D. Rubin %K EXAFS %K Hydrogen storage materials %K NEXAFS %K thin films %K x-ray diffraction %X

Mixed metal thin films containing magnesium and a first-row transition element exhibit very large changes in both reflectance and transmittance on exposure to hydrogen gas. Changes in electronic structure and coordination of the magnesium and transition metal atoms during hydrogen absorption were studied using dynamic in situ transmission mode X-ray absorption spectroscopy. Mg K-edge and Ni, Co, and Ti L-edge spectra reflect both reversible and irreversible changes in the metal environments. A significant shift in the nickel L absorption edge shows it to be an active participant in hydride formation. The effect on cobalt and titanium is much less dramatic, suggesting that these metals act primarily as catalysts for formation of magnesium hydride.

%B Journal of Alloys and Compounds %V 356-357 %P 204-207 %8 08/2003 %G eng %1

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%2 LBNL-50574 %& 204 %R 10.1016/S0925-8388(02)01237-9 %0 Journal Article %J Applied Physics Letters %D 2001 %T Mixed Metal Films with Switchable Optical Properties %A Thomas J. Richardson %A Jonathan L. Slack %A Baker Farangis %A Michael D. Rubin %X

Thin, Pd-capped metallic films containing magnesium and first row transition metals (Mn, Fe, Co) switch reversibly from their initial reflecting state to visually transparent states when exposed to gaseous hydrogen or following reduction cathodic polarization in an alkaline electrolyte. Reversion to the reflecting state is achieved by exposure to air or by anodic polarization. The films were prepared by co-sputtering from one magnesium target and one manganese, iron, or cobalt target. Both the dynamic optical switching range and the speed of the transition depend on the magnesium-transition metal ratio. Infrared spectra of films in the transparent, hydrided (deuterided) states support the presence of the intermetallic hydride phases Mg3MnH7, Mg2FeH6, and Mg2CoH5.

%B Applied Physics Letters %V 80 %P 1349-1351 %8 02/2002 %G eng %N 8 %1

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%2 LBNL-49043 %R 10.1063/1.1454218 %0 Journal Article %J Applied Physics Letters %D 2001 %T Switchable Mirrors Based on Nickel-Magnesium Films %A Thomas J. Richardson %A Jonathan L. Slack %A Robert D. Armitage %A Robert Kostecki %A Baker Farangis %A Michael D. Rubin %X

An electrochromic mirror electrode based on reversible uptake of hydrogen in nickel magnesium alloy films is reported. Thin, magnesium-rich Ni-Mg films prepared on glass substrates by cosputtering from Ni and Mg targets are mirror-like in appearance and have low visible transmittance. Upon exposure to hydrogen gas or on cathodic polarization in alkaline electrolyte, the films take up hydrogen and become transparent. When hydrogen is removed, the mirror properties are recovered. The transition is believed to result from reversible formation of Mg2NiH4 and MgH2. A thin overlayer of palladium was found to enhance the kinetics of hydrogen insertion and extraction, and to protect the metal surface against oxidation.

%B Applied Physics Letters %V 78 %P 3047-3049 %8 05/2001 %G eng %N 20 %1

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%2 LBNL-47180 %& 3047 %R 10.1063/1.1371959