H原子在Zr(0001)表面吸附的第一性原理研究

结合蒙特卡洛（MC）模拟和第一性原理密度泛函理论（DFT）方法，从Zr-H体系微观结构、吸附概率、吸附能、Mulliken电荷布居数以及电子态密度等方面对H原子在α-Zr(0001)表面的吸附位点和吸附机理等进行计算分析。结果表明:H原子在Zr(0001)表面首先产生物理吸附，然后由物理吸附转变为化学吸附，吸附过程中电荷不断由 Zr(0001)表面原子向H原子转移，最后趋于稳定。另外，稳定吸附后的H原子直接与 Zr(0001)表面最表层原子生成化学键，且主要由H(s)、Zr(s)和Zr(d)轨道的电子态做贡献。综合分析得到H原子在Zr(0001)表面的吸附位点优先级顺序为密排六方间隙位（hcp位）＞面心立方间隙位（fcc位）＞桥位（bridge位），顶位（top位）不会产生吸附。 

First-Principle Study of H Atom Adsorption on Zr(O001) Surface

The adsorption sites and mechanism of H atom on α-Zr(0001) surface were calculated and analyzed from microstructure, adsorption probability, adsorption energy, Mulliken charge population and density of state, and etc. based on the integration of Monte Carlo (MC) simulation and first-principle density functional theory (DFT) method. The results indicated that the H atom firstly generated physical adsorption on the Zr(0001) surface and then changes to chemical adsorption. The charge continuously transferred from the surface Zr(0001) atoms to the H atom throughout the entire process, and finally stabilized. Furthermore, the H atom directly bonded with the most surface Zr(0001) atoms after stable adsorption, and the major contribution of Zr-H bond was made by partial density of state of H(s), Zr(s) and Zr(d) orbitals. Comprehensive analysis shows that the priority order of the adsorption sites of H atoms on the Zr(0001) surface is hexagonal close packed gap (hcp)> face centered cubic gap (fcc)>bridge, and the top site is the impossible adsorption site.