This study investigates the nanomechanical response of aluminum substrates coated with crystalline or amorphous equiatomic FeNiCrCo compositionally complex alloy (CCA) layers using molecular dynamics nanoindentation. We evaluated the influence of coating microstructure and pre-relaxation via Monte Carlo/molecular dynamics (MC/MD) on deformation behavior at shallow (35 Å) and deep (65 Å) indentation depths. The relaxation process is critical for equilibrating internal stresses and homogenizing the initial stress field in amorphous phases, while preventing chaotic defect multiplication in crystalline lattices, yet it simultaneously promotes Fe and Cr surface segregation consistent with the equilibrium chemical short-range ordering of the alloy. The results reveal distinct deformation mechanisms: crystalline coatings exhibit higher peak indentation forces of about 300 ± 16 eV/Å characterized by discrete force fluctuations indicative of localized plastic events, while amorphous coatings show lower peak loads (~170–220 ± 12 eV/Å), corresponding to a reduction in load-bearing capacity of roughly 25%–40%, and smooth, continuous deformation governed by shear transformation zones. Notably, in amorphous systems, pressure-induced local crystallization occurs under load, with ordered FCC/HCP regions persisting after unloading, indicating partial irreversibility of the phase transition. Upon deep indentation into the substrate, the amorphous system exhibits a sharp increase in stiffness due to substrate compaction, whereas the crystalline system maintains high load-bearing capacity with reduced defect density in the relaxed state compared to the non-relaxed counterpart. Relaxation significantly reduces force-curve fluctuations in both systems, enhancing the stability of the mechanical response. Compared with uncoated aluminum, which exhibits extensive twin propagation and deep defect penetration, the FeNiCrCo-coated systems approximately halve the defect penetration depth and reduce the defective-atom volume fraction in the substrate by about a factor of two, thereby more effectively confining plastic deformation and preserving substrate integrity under the simulated conditions. These findings demonstrate that the synergy between coating crystallinity and rigorous relaxation protocols governs stress distribution patterns—localized hotspots in amorphous phases versus extended networks in crystalline ones—providing key insights for designing advanced protective coating–substrate systems with optimized mechanical performance.
Davletbakov et al. (Wed,) studied this question.