Amorphous Thickness-Dependent Strengthening–Softening Transition in Crystalline–Amorphous Nanocomposites

Core–shell crystalline–amorphous nanocomposites, featuring nanograins surrounded by thick amorphous boundaries, are promising nanoarchitectures for achieving exceptional strength through cooperative strengthening effects. However, a comprehensive understanding of the influence of characteristic sizes, particularly the amorphous thickness, on codeformation strengthening is still lacking, limiting the attainment of the strength limit. Here, we employ molecular dynamics simulations to investigate Cu-CuTa crystalline–amorphous nanocomposites with varying grain sizes and amorphous thicknesses. Our findings demonstrate significant strengthening effects in nanocomposites, effectively suppressing the Hall–Petch breakdown observed in traditional amorphous-free nanograined Cu. Intriguingly, we observe a maximum strength followed by a strengthening–softening transition dependent on the amorphous thickness, as exemplified by a representative nanocomposite featuring a 12.5 nm grain size and a critical amorphous thickness of 4 nm. Inspired by observed shifts in atomistic mechanisms, we developed a theoretical model encompassing variations in grain size and amorphous thickness, providing valuable insights into the size–strength relationship for crystalline–amorphous nanocomposites.