Abstract
The growth kinetics of thin (thickness <10 nm) oxide films on Zr(0001) and Zr(101−0) single-crystal surfaces were investigated by real-time in situ spectroscopic ellipsometry (RISE) and angle-resolved x-ray photoemission spectroscopy (AR-XPS). To this end, clean crystalline Zr(0001) and Zr(101−0) surfaces were prepared under UHV conditions by a cyclic treatment of alternating ion-sputtering and in vacuo annealing steps. The thus-obtained bare Zr surfaces were then exposed to dry O2(g) in the temperature range of 300 − 450 K (at a partial oxygen pressure of 10−4 Pa), while monitoring the growth kinetics by RISE. It was found that the less-densely packed Zr(101−0) surface oxidizes more readily than the densely packed Zr(0001) surface. A near-limiting thickness of the oxide film on both surfaces is attained only at oxidation temperatures T < 375 K. At T ≥ 375 K, the oxidation rate becomes controlled by the thermally activated dissolution and diffusion of oxygen in the α-Zr substrate. The higher oxidation rate of the Zr(101−0) surface for T ≥ 375 K is attributed mainly to the higher oxygen diffusivity in α-Zr along the Zr(101−0) direction than along the Zr(0001) direction.
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