Abstract

In this work, we develop a Ag@Al2O3@Ag plasmonic core–shell–satellite (PCSS) to achieve highly sensitive and reproducible surface-enhanced Raman spectroscopy (SERS) detection of probe molecules. To fabricate PCSS nanostructures, we employ a simple hierarchical dewetting process of Ag films coupled with an atomic layer deposition (ALD) method for the Al2O3 shell. Compared to bare Ag nanoparticles, several advantages of fabricating PCSS nanostructures are discovered, including high surface roughness, high density of nanogaps between Ag core and Ag satellites, and nanogaps between adjacent Ag satellites. Finite-difference time-domain (FDTD) simulations of the PCSS nanostructure confirm an enhancement in the electromagnetic field intensity (hotspots) in the nanogap between the Ag core and the satellite generated by the Al2O3 shell, due to the strong core–satellite plasmonic coupling. The as-prepared PCSS-based SERS substrate demonstrates an enhancement factor (EF) of 1.7 × 107 and relative standard deviation (RSD) of ~7%, endowing our SERS platform with highly sensitive and reproducible detection of R6G molecules. We think that this method provides a simple approach for the fabrication of PCSS by a solid-state technique and a basis for developing a highly SERS-active substrate for practical applications.

Highlights

  • The collective oscillation of free electrons in the conduction band of metallic (Au and Ag) nanoparticles (NPs) occurs in interaction with light, namely localized surface plasmon resonance (LSPR) [1]

  • The evolution of Ag NPs from thin Ag films is driven by the combined effect of surface diffusion, Rayleigh instability, and minimization of the surface energy metal substrate system [31,32]

  • These widely spaced random Ag NPs were utilized as a template for the fabrication of Ag@Ag NPs and plasmonic core–shell–satellite (PCSS) nanostructures

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Summary

Introduction

The collective oscillation of free electrons in the conduction band of metallic (Au and Ag) nanoparticles (NPs) occurs in interaction with light, namely localized surface plasmon resonance (LSPR) [1]. LSPR effects strongly depend on several parameters of metallic NPs, including their size, shape, spacing, and surrounding medium [2]. Metallic NPs with various shapes, such as nanoplates, nanocages, nanotriangles, nanorods, and nanostars, have been developed to tune the LSPR wavelength in the visible to near-infrared spectrum [3,4,5,6,7]. The LSPR characteristics of metallic NPs yield strong light absorption and significant amplification of localized electromagnetic coupling at the NPs’ interfaces. Metallic NPs have been utilized as a vital component for potential plasmonic-based applications such as sensing [8], biological imaging [9], energy harvesting [10], surface-enhanced Raman spectroscopy (SERS) [11,12,13,14], and catalysis [15]

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