Carbon nanotubes for the optical far-field readout of processes that are mediated by plasmonic near-fields

TL;DR

This paper demonstrates how single-walled nanotubes can be used to optically read out near-field processes around plasmonic nanoparticles, revealing mechanisms not detectable by traditional far-field measurements, which is crucial for optimizing nanostructures.

Contribution

It introduces a method to access near-field information via far-field optical signals using nanotubes, highlighting differences between near-field and far-field responses in plasmonic systems.

Findings

Far-field detection aligns with dipolar plasmonic oscillations.

Near-field signals reveal additional mechanisms beyond far-field responses.

Spectral maxima of near-field enhancements differ from far-field bands.

Abstract

As science progresses at the nanoscopic level, it becomes more and more important to comprehend the interactions taking place at the nanoscale, where optical near-fields play a key role. Their phenomenology differs significantly from the propagative light we experience at the macroscopic level. This is particularly important in applications such as surface-enhanced spectroscopies for single-molecule detection, where often the optimization of the plasmonic structures and surfaces relies on far-field characterizations. The processes dominating in the far-field picture, though, are not the same dominating in the near-field. To highlight this, we resort to very simple metallic systems: Isolated gold nanorods in solution. We show how single-walled nanotubes can be exploited to read out processes occurring at the near-field level around metallic nanoparticles and make the information accessible in the far-field region. This is implemented by monitoring the spectral profile of the enhancement of the photoluminescence and Raman signal of the nanotubes for several excitation wavelengths. Through this excitation-resolved study, we show that the far-field optical read-out detects the transversal and longitudinal dipolar plasmonic oscillations of gold nanorods, whereas the near-field read-out through the nanotubes reveals other mechanisms to dominate. The spectral position of the maximum enhancement of the optical near-field mediated signals are located elsewhere than the far-field bands. This dichotomy between near-field and far-field response should be taken into account when optimizing plasmonic nanostructures for applications such as surface-enhanced spectroscopies.