This paper proposes a one-step maskless 2D nanopatterning approach named self-aligned plasmonic lithography (SPL) by line-shaped ultrafast laser ablation under atmospheric conditions for the first time. Through a theoretical calculation of electric field and experimental verification, we proved that homogeneous interference of laser-excited surface plasmon polaritons (SPPs) can be achieved and used to generate long-range ordered 2D nanostructures in a self-aligned way over a wafer-sized area within several minutes. Moreover, the self-aligned nanostructures can be freely transferred between embossed nanopillars and engraved nanoholes by modulating the excitation intensity of SPPs interference through altering the incident laser energy. The SPL technique exhibits further controllability in the shape, orientation, and period of achievable nanopatterns on a wide range of semiconductors and metals by tuning processing parameters. Nanopatterned films can further act as masks to transfer structures into other bulk materials, as demonstrated in silica.
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