The ability to control the position of a mesoscopic object with nanometric precision is important for the rapid progress of nanoscience. One of the most promising tools to achieve such control is optical tweezers, which trap objects near the focus of a laser beam. However, the drawbacks of conventional tweezers include a trapping volume that is diffraction-limited and significant brownian motion of trapped nanoobjects. Here, we report the first experimental realization of three-dimensional nanometric optical tweezers that are based on nanostructured substrates. Using electromagnetically coupled pairs of gold nanodots in a standard optical tweezers set-up, we create an array of subwavelength plasmonic optical traps that offer a significant increase in trapping efficiency. The nanodot optical near-fields reduce the trapping volume beyond the diffraction limit and quench brownian motion of the trapped nanoparticles by almost an order of magnitude as compared to conventional tweezers operating under the same trapping conditions. Our tweezers achieve nanoscale control of entities at significantly smaller laser powers and open new avenues for nanomanipulation of fragile biological objects.

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Nanometric optical tweezers based on nanostructured substrates

In this study, we report on ultrasensitive protein detection with lithographically prepared plasmonic nanostructures. We have engineered optical nanosensors by the combined approach of negative resist, electron beam lithography, and reactive ion etching to form highly reproducible arrays of gold dimers in which the near-field coupling in their subwavelength gap enables for scaling the sensing volume down to the single-protein scale. In good agreement with recent theoretical predictions, the dimer geometry offers enhanced sensitivity compared to isolated particles for the detection of both small organic molecules and proteins. Beyond, by exploiting size exclusion, we are capable of monitoring the number of proteins able to bind across the gap region through the precise engineering of the structures coupled to the selective binding of a surface-assembled monolayer and covalent attachment of the protein.

Plasmon near-field coupling in metal dimers as a step toward single-molecule sensing.

In this study, we report the development of a nanoparticle-enhanced biosensor by integrating both the nanoparticles and immunoassay sensing technologies into a phase interrogation surface plasmon resonance (SPR) system for detecting antigen at a concentration as low as the femtomolar range. Our work has demonstrated that the plasmonic field extension generated from the gold film to gold nanorod (GNR) has led to a drastic sensitivity enhancement. Antibody-functionalized sensing film, together with antibody-conjugated GNRs, was readily served as a plasmonic coupling partner that can be used as a powerful ultrasensitive sandwich immunoassay for cancer-related disease detection. Experimentally, it was found that the bioconjugated GNR labels enhance the tumor necrosis factor alpha (TNF-α) antigen signal with more than 40-fold increase compared to the traditional SPR biosensing technique. The underlying principle was analyzed by simulating the near-field coupling between the sensing film and the GNR. The results have shown that GNRs were readily served as promising amplification labels in SPR sensing technology.

Sensitivity Improved Surface Plasmon Resonance Biosensor for Cancer Biomarker Detection Based on Plasmonic Enhancement

We present what we believe to be the first experimental study of the optical response of collective plasmon resonances in regular arrays of nanoresonators to local environment. Recently observed collective plasmon modes arise due to diffractive coupling of localized plasmons and yield almost 1 order of magnitude improvement in resonance quality. We measure the response of these modes to tiny variations of the refractive index of both gaseous and liquid media. We show that the phase sensitivity of the collective resonances can be more than 2 orders of magnitude better than the best amplitude sensitivity of the same nanodot array as well as 1 order of magnitude better than the phase sensitivity in surface plasmon resonance sensors.

Sensitivity of collective plasmon modes of gold nanoresonators to local environment

We show that aligned gold nanotube arrays capable of supporting plasmonic resonances can be used as high performance refractive index sensors in biomolecular binding reactions. A methodology to examine the sensing ability of the inside and outside walls of the nanotube structures is presented. The sensitivity of the plasmonic nanotubes is found to increase as the nanotube walls are exposed, and the sensing characteristic of the inside and outside walls is shown to be different. Finite element simulations showed good qualitative agreement with the observed behavior. Free standing gold nanotubes displayed bulk sensitivities in the region of 250 nm per refractive index unit and a signal-to-noise ratio better than 1000 upon protein binding which is highly competitive with state-of-the-art label-free sensors.

High-Performance Biosensing Using Arrays of Plasmonic Nanotubes

A nanofabricated regular array of coupled gold nano-pillars is employed to detect local indices of refraction of different liquids using a shift of an antisymmetric plasmon resonance peak observed in the reflection spectra. The peak spectral position is found to be a unique function of the local refractive index for a wide range of indices. We discuss possible applications of the fabricated nanostructured arrays in bio and chemical sensors.

N. W. Roberts

Papers

An antisymmetric plasmon resonance in coupled gold nanoparticles as a sensitive tool for detection of local index of refraction