Pressure-Driven Laser-Induced Graphene: Transient Pressure-Enhanced Structural Ordering via Femtosecond Laser Irradiation

• • Transient pressure fields generated during femtosecond laser irradiation of polyimide films are confirmed as an intrinsic feature, with time-resolved measurements validating their presence; this pressure is harnessed to enhance graphene quality. • • MD simulations under controlled pressure conditions demonstrate that pressure promotes nucleation and stacking of graphene layers, yielding more continuous and planar graphitic networks, which directly improves structural integrity. • • XAI analysis quantitatively identifies pressure as a significant contributor to the enhanced structural ordering, providing a data-driven basis for optimizing P-LIG parameters. • • The P-LIG method offers a practical pathway to overcome limitations of photothermal (uncontrolled properties) and photochemical (narrow precursor range) approaches, enabling higher-quality graphene for flexible electronics.