Abstract
Plasmon-induced polymerization can facilitate the site-selectivity and orientation of polymer growth, which enriches the toolbox of polymerization and nanofabrication. Here, we demonstrate plasmon-induced polymerization, accomplished by low-power laser excitation of gold nanoparticles (NPs). We selectively control the growth of polymers around single plasmonic NPs while monitoring the polymerization using dark field spectroscopy and subsequent scanning electron microscopy. This plasmon-induced polymerization, generated by hot electron initiation, not only precisely controls the thickness and composition of the polymer coatings but also regulates the location and orientation of the growth, which are strongly influenced by the laser polarization and near-field distribution around the plasmonic NPs. A saturation increase in the polymer thickness provides a strong support for our mechanism. This facile approach of nanoscale polymerization directed by light not only provides new opportunities in nanosynthesis and nanofabrication for functional devices, but also opens many routes for polymer physics and chemistry at the nanoscale level.
Highlights
Plasmon-induced chemistry via hot carriers has attracted great interest as it opens a new paradigm of nanochemistry for self-assembly [1], plasmonics [2], photodetection [3], photocatalysis [4, 5] and photovoltaics [6,7,8]
The laser irradiation induced a ~ 30 nm redshift of the plasmonic resonance due to the increased refractive index of the polymer coatings, which is supported by the simulations (Fig. 1(c))
The PDVB coating can be clearly visualized in the scanning electron microscopy (SEM) images (Fig. 1(d)), confirming successful polymer growth around the Au NP
Summary
Plasmon-induced chemistry via hot carriers has attracted great interest as it opens a new paradigm of nanochemistry for self-assembly [1], plasmonics [2], photodetection [3], photocatalysis [4, 5] and photovoltaics [6,7,8]. It is generally believed that plasmonexcited hot carriers trigger a series of redox chemistries at the surface of metals or semiconductors via charge transfer [9] Such injected hot electrons can be utilized to induce surface polymerization, which shifts the tuning of the plasmonic resonances with a feedback that can be self-limiting [2]. The advantage of using plasmoninduced hot electrons, compared to conventional surface-initiated radical polymerization, is the precise location and polarization dependence it gives, which strongly improves the precision for fine-tuning nanostructures. This bridges a distinct gap for the fabrication of miniaturized polymer optoelectronic devices, where excellent site-selectivity, and remote controllability and directionality are demanded
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