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表面形态对非晶态固态水脱附D2动力学的影响。

Influence of surface morphology on D2 desorption kinetics from amorphous solid water.

作者信息

Hornekaer L, Baurichter A, Petrunin V V, Luntz A C, Kay Bruce D, Al-Halabi A

机构信息

Department of Physics, University of Southern Denmark, Campusvej 55, 5230 Odense M, Denmark.

出版信息

J Chem Phys. 2005 Mar 22;122(12):124701. doi: 10.1063/1.1874934.

Abstract

The influence of surface morphology/porosity on the desorption kinetics of weakly bound species was investigated by depositing D2 on amorphous solid water (ASW) films grown by low temperature vapor deposition under various conditions and with differing thermal histories. A broad distribution of binding energies of the D2 monolayer on nonporous and porous ASW was measured experimentally and correlated by theoretical calculations to differences in the degree of coordination of the adsorbed H2 (D2) to H2O molecules in the ASW depending on the nature of the adsorption site, i.e., surface valleys vs surface peaks in a nanoscale rough film surface. For porous films, the effect of porosity on the desorption kinetics was observed to be a reduction in the desorption rate with film thickness and a change in peak shape. This can be partly explained by fast diffusion into the ASW pore structure via a simple one-dimensional diffusion model and by a change in binding energy statistics with increasing total effective surface area. Furthermore, the D2 desorption kinetics on thermally annealed ASW films were investigated. The main effect was seen to be a reduction in porosity and in the number of highly coordinated binding sites with anneal temperature due to ASW restructuring and pore collapse. These results contribute to the understanding of desorption from porous materials and to the development of correct models for desorption from and catalytic processes on dust grain surfaces in the interstellar medium.

摘要

通过在各种条件下和具有不同热历史的低温气相沉积生长的非晶态固体水(ASW)薄膜上沉积D₂,研究了表面形态/孔隙率对弱结合物种解吸动力学的影响。通过实验测量了D₂单层在无孔和多孔ASW上的广泛结合能分布,并通过理论计算将其与取决于吸附位点性质(即纳米级粗糙薄膜表面的表面谷与表面峰)的ASW中吸附的H₂(D₂)与H₂O分子的配位程度差异相关联。对于多孔薄膜,观察到孔隙率对解吸动力学的影响是解吸速率随薄膜厚度降低以及峰形变化。这可以部分地通过简单的一维扩散模型快速扩散到ASW孔结构中以及随着总有效表面积增加结合能统计的变化来解释。此外,还研究了热退火ASW薄膜上的D₂解吸动力学。主要影响是由于ASW重构和孔塌陷,孔隙率和高配位结合位点的数量随退火温度降低。这些结果有助于理解多孔材料的解吸以及星际介质中尘埃颗粒表面解吸和催化过程的正确模型的开发。

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