Ultrafast laser-induced subwavelength structures towards nanoscale: the significant role of plasmonic effects

TL;DR

This paper demonstrates that ultrafast laser ablation can spontaneously generate subwavelength plasmonic structures driven by plasmonic effects, revealing a natural mechanism for nanoscale structure formation beyond human design.

Contribution

It uncovers the intrinsic plasmonic mechanisms behind ultrafast laser-induced nanostructures and explains how physical regimes of plasmonic interaction lead to nanoscale, ultrafast ablation.

Findings

Splitting of laser-induced gratings is due to mode conversion of surface plasmons.

Scaling-down of structures results from transition from optical to electrostatic plasmonic regimes.

Multipulse ablation promotes self-generation of resonant nanostructures.

Abstract

Nowadays, via controlling surface plasmons (SPs) on elaborate man-made structures, plasmonics aiming at manipulating light beyond the diffraction limit has aroused great interest. Here, nevertheless, we demonstrate in short-pulse laser ablation ultrafast active plasmonic structures spontaneously generate in virtue of plasmonic effects rather than human ingenuity. First, the splitting of laser-induced subwavelength gratings that is experimentally evidenced on ZnO, Si, and GaAs, is confirmed to originate in the conversion of SP modes from the resonant to the nonresonant mode and further to the inphase or antiphase asymmetric mode. Further, as pulse number increases the universal scaling-down of laser-induced structures is derived from the conversion of physical regimes of plasmonic interaction from the optical to the electrostatic regime, which may arouse quasistatic SPs with interacting scales far beyond the diffraction limit and result in the ultrafast, non-thermal ablation for extraordinary electrostatic enhancement. Generally, the plasmonic mechanisms reveal the link between the deep-subwavelength space-scale and the ultra-short timescale for ultrafast laser-induced nanostructures: basically, "nanoscale" tends to eliminate electromagnetic retardation effects and bring an instant respond to the incident field, and arouse electrostatic interactions with giant local-field enhancement facilitating ultrafast ablation driven by tremendous electrostatic forces. Thus, active plasmonic structures provided with simultaneous "nanoscale" and "ultrafast" is apt to form in ultrafast ablation. In addition, the plasmonic mechanisms can act as a powerful "evolutionary force" acting in multipulse ablation and promoting the growth of resonant nanostructures-various typical plasmonic structures may be self-generated through multipulse evolution, which can be considered as a kind of natural plasmonics.