Understanding mono- and bi-metallic Au and Ni nanoparticle responses to fast heating.

Nanoparticle assembly, alloying and fragmentation are fundamental processes with significant implications in various fields such as catalysis, materials science, and nanotechnology. Understanding these processes under fast heating conditions is crucial for tailoring nanoparticle properties and optimizing their applications. For this, we employ molecular dynamics simulations to obtain atomic-level insights into nanoparticle behavior. The performed simulations reveal intricate details of sintering, alloying and fragmentation mechanisms shedding light on the underlying physical phenomena governing these processes. The calculation results help to visualize nanoparticle evolution upon undercritical and supercritical heating elucidating not only the role of temperature, but also of nanoparticle sizes and composition. In particular, it is shown that surface tension and surface energy play important roles not only in nanoparticle melting but also in its fragmentation. When the added energy exceeds a critical threshold, the nanoparticle begins to experience alternating compression and expansion. If the tensile stress surpasses the material's strength limit, fragmentation becomes prominent. For very small particles (with radius smaller than ∼10 nm), this occurs more rapidly, whereas sub-nano-cavitation precedes the final fragmentation in larger particles, which behave more like droplets. Interestingly, this effect depends on composition in the case of AuNi alloy nanoparticles, as expected from the phase diagrams and excess energy. The heating level required to overcome the mixing barrier is also determined and is shown to play an important role in the evolution of AuNi nanoparticles, in addition to their size. Furthermore, our findings provide insights into controlling nanoparticle synthesis for various applications in numerous nanotechnological domains, such as catalysis, sensors, material analysis, as well as deseas diagnostics and treatment. This study bridges the gap between experimental observations and theoretical predictions paving the way for designing advanced nanomaterials with enhanced functionalities.