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1.
J Phys Chem Lett ; 12(25): 5844-5849, 2021 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-34138568

RESUMEN

Oxygen atoms on transition metal surfaces are highly mobile under the demanding pressures and temperatures typically employed for heterogeneously catalyzed oxidation reactions. This mobility allows for rapid surface diffusion of oxygen atoms, as well as absorption into the subsurface and reemergence to the surface, resulting in variable reactivity. Subsurface oxygen atoms play a unique role in the chemistry of oxidized metal catalysts, yet little is known about how subsurface oxygen is formed or returns to the surface. Furthermore, if oxygen diffusion between the surface and subsurface is mediated by defects, there will be localized changes in the surface chemistry due to the elevated oxygen concentration near the emergence sites. We observed that oxygen atoms emerge preferentially along the boundary between surface phases and that subsurface oxygen is depleted before the surface oxide decomposes.

2.
Nat Commun ; 12(1): 1721, 2021 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-33741925

RESUMEN

The stacking sequence of hexagonal close-packed and related crystals typically results in steps on vicinal {0001} surfaces that have alternating A and B structures with different growth kinetics. However, because it is difficult to experimentally identify which step has the A or B structure, it has not been possible to determine which has faster adatom attachment kinetics. Here we show that in situ microbeam surface X-ray scattering can determine whether A or B steps have faster kinetics under specific growth conditions. We demonstrate this for organo-metallic vapor phase epitaxy of (0001) GaN. X-ray measurements performed during growth find that the average width of terraces above A steps increases with growth rate, indicating that attachment rate constants are higher for A steps, in contrast to most predictions. Our results have direct implications for understanding the atomic-scale mechanisms of GaN growth and can be applied to a wide variety of related crystals.

3.
J Chem Phys ; 137(5): 054708, 2012 Aug 07.
Artículo en Inglés | MEDLINE | ID: mdl-22894372

RESUMEN

Reaction pathways for complete decomposition of ammonia on the InN (0001) surface are investigated using first principles calculations. We show that while the initial NH(3) decomposition on this surface can proceed by H dissociation, its further decomposition is most favorable by H transfer. The calculated low diffusion barriers for the decomposed species on the surface imply that the metal-organic chemical vapor deposition growth of InN is a reaction-limited process rather than diffusion-limited at low adsorbate coverage.

4.
Ultramicroscopy ; 123: 74-9, 2012 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-22726263

RESUMEN

In silicon nitride structural ceramics, the overall mechanical and thermal properties are controlled by the atomic and electronic structures at the interface between the ceramic grains and the amorphous intergranular films (IGFs) formed by various sintering additives. In the last ten years the atomic arrangements of heavy elements (rare-earths) at the Si(3)N(4)/IGF interfaces have been resolved. However, the atomic position of light elements, without which it is not possible to obtain a complete description of the interfaces, has been lacking. This review article details the authors' efforts to identify the atomic arrangement of light elements such as nitrogen and oxygen at the Si(3)N(4)/SiO(2) interface and in bulk Si(3)N(4) using aberration-corrected scanning transmission electron microscopy.


Asunto(s)
Cerámica/química , Microscopía Electrónica de Transmisión de Rastreo/métodos , Compuestos de Silicona/química , Dióxido de Silicio/química , Elementos Químicos , Luz , Modelos Moleculares , Nitrógeno/química , Oxígeno/química
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