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.

Flexible multidirectional strain sensors capable of simultaneously detecting strain amplitudes and directions have attracted tremendous interest. Herein, we propose a flexible multidirectional strain sensor based on a newly designed single-layer hierarchical aligned micro-/nanowire (HAMN) network. The HAMN network is efficiently fabricated using a one-step femtosecond laser patterning technology based on a modulated line-shaped beam. The anisotropic performance is attributed to the significantly different morphological changes caused by an inhomogeneous strain redistribution among the HAMN network. The fabricated strain sensor exhibits high sensitivity (gauge factor of 65 under 2.5% strain and 462 under larger strains), low response/recovery time (140 and 322 ms), and good stability (over 1000 cycles). Moreover, this single-layer strain sensor with high selectivity (gauge factor differences of ∼73 between orthogonal strains) is capable of distinguishing multidimensional strains and exhibits decoupled responses under low strains (<1%). Therefore, the strain sensors enable the precise monitoring of subtle movements, including radial pulses and wrist bending, and the rectification of pen-holding posture. Benefitting from these remarkable performances, the HAMN-based strain sensors show potential applications, including healthcare and complex human motion monitoring.

Hierarchical metal grids are proven to be a promising solution for achieving high‐performance flexible transparent electrodes (FTEs) due to their significantly enhanced conductivity without noticeably sacrificing transparency. This work develops a one‐step mask‐free line‐shaped laser lithography by separated pulse laser ablation to efficiently fabricate large‐area FTEs composed of hierarchical metal grids, namely microscale grids interconnected with aligned nanowire arrays. The linewidth of aligned wires is highly controllable from the nanometer scale far beyond the diffraction limit (<λ/10) to the micrometer scale. This work experimentally studies the overall performance of FTEs to provide a guideline for selecting the layout and feature sizes of hierarchical metal grids. Hierarchical metal grids with 50 nm nanowires aligned inside the microscale grids show outstanding optoelectronic properties and mechanical stability, with sheet resistance of 4.6 Ω sq−1, transmittance of 82.9%, and a tiny increase in sheet resistance less than 4% after 1000 cycles of bending tests. These results prove that the line‐shaped laser lithography technique is a facile, low‐cost, and high‐throughput fabrication method for high‐performance FTEs.