Abstract Diamond and diamond-like carbon coatings are used in many applications ranging from biomedicine to tribology. A wide range of dopants have been tested to modify the hydrophilicity of these surfaces, since this is central to their biocompatibility and tribological performance in aqueous environments. Despite the large number of experimental investigations, an atomistic understanding of the effects of different dopants on carbon film hydrophilicity is still lacking. In this study, we employ ab initio calculations to elucidate the effects of B, N, and O dopants in several mechanisms that could modify interactions with water molecules and thus hydrophilicity. These include the adsorption of intact water molecules on the surfaces, minimum energy pathways for water dissociation, and subsequent interactions of hydrogenated and hydroxylated surfaces with water molecules. We find that all of the dopants considered enhance hydrophilicity, but they do so through different means. Most notably, B dopants can spontaneously chemisorb intact water molecules and increase its interactions in H-bond networks.

中文翻译：

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硼、氮和氧掺杂金刚石表面与水分子之间相互作用机制的 Ab Initio 洞察

摘要 金刚石和类金刚石碳涂层用于从生物医学到摩擦学的许多应用中。已经测试了多种掺杂剂来改变这些表面的亲水性，因为这对于它们在水性环境中的生物相容性和摩擦学性能至关重要。尽管进行了大量的实验研究，但仍然缺乏对不同掺杂剂对碳膜亲水性影响的原子理解。在这项研究中，我们采用从头计算来阐明 B、N 和 O 掺杂剂在几种机制中的影响，这些机制可以改变与水分子的相互作用，从而改变亲水性。这些包括完整的水分子在表面上的吸附、水解离的最小能量途径、以及随后氢化和羟基化表面与水分子的相互作用。我们发现所有被考虑的掺杂剂都增强了亲水性，但它们是通过不同的方式实现的。最值得注意的是，B 掺杂剂可以自发地化学吸附完整的水分子并增加其在 H 键网络中的相互作用。