Abstract

Simple high-performance, two-stage hybrid technique was developed for fabrication of different plasmonic nanostructures, including nanorods, nanorings, as well as more complex structures on glass substrates. In this technique, a thin noble-metal film on a dielectric substrate is irradiated by a single tightly focused nanosecond laser pulse and then the modified region is slowly polished by an accelerated argon ion (Ar+) beam. As a result, each nanosecond laser pulse locally modifies the initial metal film through initiation of fast melting and subsequent hydrodynamic processes, while the following Ar+-ion polishing removes the rest of the film, revealing the hidden topography features and fabricating separate plasmonic structures on the glass substrate. We demonstrate that the shape and lateral size of the resulting functional plasmonic nanostructures depend on the laser pulse energy and metal film thickness, while subsequent Ar+-ion polishing enables to vary height of the resulting nanostructures. Plasmonic properties of the fabricated nanostructures were characterized by dark-field micro-spectroscopy, Raman and photoluminescence measurements performed on single nanofeatures, as well as by supporting numerical calculations of the related electromagnetic near-fields and Purcell factors. The developed simple two-stage technique represents a new step towards direct large-scale laser-induced fabrication of highly ordered arrays of complex plasmonic nanostructures.

Highlights

  • Functional plasmonic nanostructures (FPNs) fabricated on transparent dielectric substrates as ordered arrays of nanofeatures are the object of increasingly growing scientific interest in the last decade

  • We demonstrate for the first time that the use of direct single-shot exposure of a thin metal film by tightly focused nanosecond laser pulses, followed by slow polishing of the fabricated nanostructures by an accelerated argon-ion (Ar+) beam, in combination allows fabricating on glass substrates arrays of isolated plasmonic nanorods, separated and merged nanorings, as well as more complex nanostructures

  • The ns-laser irradiation of metal film changes its initial thickness through the initiation of fast melting and subsequent hydrodynamic processes, while the following Ar+ polishing reveals the features of its hidden topography, producing localized plasmon resonance (LPR)-supporting isolated plasmonic structures on the glass substrate

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Summary

Introduction

Functional plasmonic nanostructures (FPNs) fabricated on transparent dielectric substrates as ordered arrays of nanofeatures are the object of increasingly growing scientific interest in the last decade. Spatial scale and final topography of these processes, determining the shape of the resulting nanostructures, is controlled by the metal film irradiation conditions (pulse energy and duration, focal spot size etc.), as well as by the physical properties of the metal film and its substrate (chemical composition, thickness, optical and thermal characteristics etc.) Such approach was proved to be an efficient route for direct single-pulse fabrication of ordered arrays of resolidified nanojets (upright standing metal tips19,20), which are suitable for LPR-mediated amplification of electromagnetic fields in near-IR spectral region[21] and polarization-dependent Raman signal enhancement[22], imprinting of two-dimensional coupling elements through the excitation of intense surface plasmon-polariton (SPP) waves[23], as well as for laser-induced forward transfer (LIFT) of spherical metal and semiconductor droplets onto an acceptor substrate[24,25]. Their plasmonic properties were examined by means of dark-field (DF) micro-spectroscopy, micro-Raman and photoluminescent (PL) measurements and were modeled in the framework of finite-difference time-domain calculations of electromagnetic near-fields and related Purcell factor (PF) magnitudes

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