钨中间隙氦团簇对氢迁移行为的影响

Effect of Interstitial Helium Cluster in Tungsten on Hydrogen Migration

  • 摘要: 钨中间隙氦团簇(Hen)与氢之间具有明显的相互吸引作用,但其对氢的迁移和扩散等动力学行为的影响缺乏研究。本文采用第一性原理方法计算发现氢与Hen的结合能随氦原子数量增加先上升后下降,最高可达0.77 eV。进一步通过CI-NEB方法寻找氢在Hen附近的最佳迁移路径和迁移能垒。结果表明:氢的迁移能垒与氦原子数量密切相关,当氦原子数量≤4时,氢的迁移能垒与本征钨中相近,表明Hen对氢迁移行为影响较小;氦原子数量>4时,氢迁移能垒约为0.45 eV,是本征钨中的两倍,表现出对氢迁移明显的阻碍作用。进一步基于McNabb-Foster模型和实体动力学蒙特卡罗模拟讨论了不同温度下Hen对氢扩散和分布行为的影响。本文研究结果可为解决未来聚变堆中钨材料的氢滞留问题提供理论支持。

     

    Abstract: Tungsten (W) is widely recognized as the premier plasma-facing material (PFM) for fusion reactors. However, exposure to hydrogen (H) plasma inevitably leads to the substantial retention of H isotopes within the material, precipitating degradation issues such as blistering, swelling, and hardening. Prior studies show that material defects, such as vacancies, dislocations, and grain boundaries, can act as efficient trapping sites for H. Moreover, as a product of fusion reactions, helium (He) is heavily implanted into W via plasma irradiation. Driven by the electrophobic nature of He, these atoms aggregate at interstitial sites through a “self-trapping” mechanism, thereby forming interstitial He clusters (Hen, n indicates the number of He atoms). Although existing literature indicates that such clusters attract H, their specific impact on the kinetics of H migration and diffusion remains underexplored. In this study, the first-principles calculations were employed to investigate the dissolution of H in the vicinity of Hen in W. The climbing image nudged elastic band (CI-NEB) method was utilized to map out H migration pathways and energy barriers, while the McNabb-Foster equation was applied to quantify the influence of Hen on H diffusion. The results show that interstitial He atoms preferentially aggregate within 110 planes and form stable clusters in W. For Hen clusters with 1≤n≤7, the binding energy of H first rises and then falls with increasing He atom number, peaking at 0.77 eV (He6). CI-NEB calculations reveal that the migration energy barrier for H around these clusters is highly dependent on the number of He atoms. For clusters containing no more than four He atoms (n≤4), the migration energy barrier from a stable site to the first-nearest-neighbor (1NN) tetrahedral interstitial site (TIS) ranges from 0.11 to 0.26 eV, which is comparable to the barrier between adjacent TISs in intrinsic W (0.18-0.23 eV). As the H atom migrates further away from the cluster, the barrier stabilizes at 0.25 eV approximately, approaching that of intrinsic W. Conversely, for larger clusters (n>4), the migration barrier to the 1NN TIS rises to roughly 0.45 eV—approximately double that of intrinsic W. Outside this localized area, however, the migration energy barrier (0.12-0.19 eV) for outward diffusion reverts to levels similar to those in pure W. These findings suggest that, although smaller Hen clusters (n≤4) exert a negligible effect on H migration, larger clusters (n>4) significantly impede H migration, with the hindering effect being spatially confined to the 1NN TIS. The diffusivity ratio of H is evaluated based on the McNabb-Foster model, revealing that Hen impedes H diffusion, with the hindering effect becoming more pronounced as the number of He atoms increases. Object kinetic Monte Carlo (OKMC) simulation results indicate that using the dissociation energy as the migration barrier overestimates the trapping effect of Hen on H, leading to an excessive accumulation of H in the vicinity of Hen. Therefore, a more accurate description of the kinetic processes governing H migration and diffusion around these clusters is essential for a better understanding of H distribution in W under varying He concentrations and temperatures. These findings provide theoretical insights for mitigating H retention in W materials for future fusion reactors.

     

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