Role of proton ordering in adsorption preference of polar molecule on ice surface
Role of proton ordering in adsorption preference of polar molecule on ice surface
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DOI：
10.1073/pnas.1206879109
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发表时间：
2012-07
期刊：
影响因子：
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通讯作者：
Zhaoru Sun;D. Pan;Limei Xu;E. Wang
中科院分区：
文献类型：
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作者：
Zhaoru Sun;D. Pan;Limei Xu;E. Wang
极性单体在冰面上的吸附，与冰云中的物理/化学反应以及冰的生长有关，仍然是一个悬而未决的问题，部分原因是由于冰层顶层具有不同寻常的表面特征。利用第一性原理的计算方法，利用表征悬垂原子在冰面上的不均匀性的表面质子序参数，探讨了冰表面的吸附特性。结果表明，由于悬挂的氢键和孤立的水分子不仅直接靠近冰面上吸附的极性分子，而且还远离吸附在冰面上的极性分子而产生有效电场，极性单体在冰面上的吸附能表现出很大的变化，并与冰面的质子序参数有很强的相关性。冰表面的不均匀性与吸附能之间的正相关关系表明，冰的物理/化学反应以及冰的生长可能首先发生在质子序参数较大的表面。
Adsorption of polar monomers on ice surface, relevant to the physical/chemical reaction in ice clouds as well as growth of ice, remains an open issue partially due to the unusual surface characteristics with protons at the top layer of ice. Using first-principle calculations, we explore the adsorption properties of ice surface in terms of a surface proton order parameter, which characterizes the inhomogeneity of the dangling atoms on ice surface. We show that, due to an effective electric field created by dangling OH bonds and lone pairs of water molecules not only directly neighboring but also further away from the adsorbed polar molecule on the ice surface, the adsorption energy of polar monomer on ice surface exhibits large variance and a strong correlation with the proton order parameter of ice surface. Our results about the positive correlation between the inhomogeneity of ice surface and adsorption energies suggest that the physical/chemical reactions as well as the growth of ice may prefer to occur firstly on surfaces with larger proton order parameter.