Atomic understanding of structural deformations upon ablation of graphene

Abstract We investigate the atomic rearrangement in graphene under femtosecond pulse illumination with reactive molecular dynamics simulations and compare with ultra‐fast laser ablation experiments. To model the impact of the laser pulse irradiation, heat is locally applied to a selected area of the graphene layer and the resulting structural deformation is simulated as a function of time, providing a detailed understanding of the bond breaking process under laser illumination and subsequent re‐equilibration after the pulse is turned off. Analysis of the atomic dynamics indicates that the types of defects formed depend on the pulse energy and exposure duration. By varying the exposed area, we determine that the shape of the ablated area is not only a function of the pulse energy, but also of the beam spot size and pulse repetition. Furthermore, we apply a machine learning approach to extrapolate our simulated data to experimental length scales and reproduce the trends in ablated area as a function of temperature. Our study provides a first step towards understanding the design parameters for graphene nano‐patterning.