Defect-initiated formation mechanism of 3D carbon tracks on flexible transparent substrates by laser irradiation

Laser direct writing of 3D carbon structures onto flexible polymer substrates offers potential of rapid roll-to-roll manufacturing for a variety of key applications, including large area sensors, flexible electronics, robotics, energy storage/conversion, and other consumer applications. The specific formation mechanism of the carbon structures has been an issue of debate for many years with the prevailing notion of a simple photothermal conversion reaction that mainly depends on the total energy input. However, this view has been shown to be inconsistent with experimental observations of nonlinear changes in the resulting structures when multiple processing parameters are simultaneously changed. In this study, we propose a formation mechanism based on the nucleation and growth of laser-induced defects, which is experimentally validated by irradiating a continuous wave laser beam onto polydimethylsiloxane. The model is further validated by intentionally introducing controlled defects by femtosecond laser irradiation, and indicate the implications of a two-laser laser direct writing technique to go beyond the current processing limits. These results clarify the previously ambiguous mechanisms by which carbon structures form under laser irradiation and provide a deeper understanding of how to control photothermal processes for advanced material processing.