Capturing thin-film microstructure contributions during ultrafast laser-metal interactions using atomistic simulations

Progress in the emerging fields of atomic and close-to-atomic scale manufacturing is underpinned by enhanced precision and optimization of laser-controlled nanostructuring. Understanding thin films' crystallographic orientations and microstructure effects becomes crucial for optimizing the laser-metallic thin film interactions; however, these effects remain largely unexplored at the atomic scale. Using a hybrid two-temperature model and molecular dynamics, we simulated ultrafast laser-metal interactions for gold thin films with varying crystallographic orientations and microstructure configurations. Microstructure features, namely grain size, grain topology, and local crystallographic orientation, controlled the rate and extent of lattice disorder evolution and phase transformation, particularly at lower applied fluences. Our simulations provided comprehensive insights encompassing both the nanomechanical and thermodynamic aspects of ultrafast laser-metal interactions at atomic resolution. Microstructure-aware/informed thin film fabrication and targeted defect engineering could improve the precision of nanoscale laser processing and potentially emerge as an energy-efficient optimization strategy. • Unraveling ultrafast laser-metallic thin films interactions at atomic resolution. • Crystallographic orientations and microstructure influence laser-induced deformation. • Poly-nanocrystalline thin films exhibit grain boundary mediated melting. • Comprehensive insights encompassing nanomechanics and thermodynamics.