The effect of solute hydrogen on shear-coupled grain boundary (GB) migration is investigated with the dislocation-array type Σ25(430)[001] GB and a dual role of hydrogen on GB mobility is unraveled. In the low temperature and high loading rate regime, where hydrogen diffusion is substantially slower than GB motion, GB breaks away from the hydrogen atmosphere and transforms into a new stable phase with highly enhanced mobility. In the reverse regime, hydrogen atoms move along with GB, exerting a drag force on GB and decreasing its mobility. These findings provide rationale for the coexistence of hydrogen hardening and softening observed experimentally in polycrystalline materials.

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