Under the continuous irradiation of high‐density and high‐energy photons from the plasma core of a fusion reactor, the plasma‐facing materials (PFMs) of tungsten (W) are in electronically excited states. How hydrogen (H) interacts with defective PFMs in an electronically excited state is an open question. The authors report the developed W‐H tight‐binding (TB) potential model and employ this model to systemically investigate the interaction between an edge dislocation in tungsten with H at different electronically excited states. With the enhancement of electronic excitation, the strong attraction of the dislocation core to H slightly fluctuates, while the attraction to H is significantly enhanced in the region outside the dislocation core. When the electronic excitation energy is ≈0.86 eV, the region of tensile stress can trap H without additional energy. Additionally, the electronic excitation simultaneously makes H migration easy. It is revealed that the transfer of partial energy of the excited electrons to the lattice leads to the nonthermal expansion of the system and affects the interaction between the edge dislocation and H. These results not only show the nonthermal effect of tuning the interaction between hydrogen and the edge dislocation in tungsten but also uncover the nature underlying these phenomena.
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