Reuven Gordon

Increased cut-off wavelength for a subwavelength hole in a real metal

A waveguide mode of a subwavelength rectangular hole in a real metal is analyzed. Due to coupling between surface plasmons on the long edges of the hole, the cut-off wavelength increases as the hole-width is reduced. The cut-off wavelength is found to be much larger than Rayleighs criterion for perfect metals - 2.3 times as large for a 15 nm wide hole. The analytical results are verified by finite-difference calculations. The finite difference calculations also show the influence of including material loss.

Nanoholes as nanochannels: flow-through plasmonic sensing.

We combine nanofluidics and nanoplasmonics for surface-plasmon resonance (SPR) sensing using flow-through nanohole arrays. The role of surface plasmons on resonant transmission motivates the application of nanohole arrays as surface-based biosensors. Research to date, however, has focused on dead-ended holes, and therefore failed to harness the benefits of nanoconfined transport combined with SPR sensing. The flow-through format enables rapid transport of reactants to the active surface inside the nanoholes, with potential for significantly improved time of analysis and biomarker yield through nanohole sieving. We apply the flow-through method to monitor the formation of a monolayer and the immobilization of an ovarian cancer biomarker specific antibody on the sensing surface in real-time. The flow-through method resulted in a 6-fold improvement in response time as compared to the established flow-over method.

Optical Trapping of a Single Protein

We experimentally demonstrate the optical trapping of a single bovine serum albumin (BSA) molecule that has a hydrodynamic radius of 3.4 nm, using a double-nanohole in an Au film. The strong optical force in the trap not only stably traps the protein molecule but also unfolds it. The unfolding of the BSA is confirmed by experiments with changing optical power and with changing solution pH. The detection of the trapping event has a signal-to-noise ratio of 33, which shows that the setup is extremely sensitive to detect the presence of a protein, even at the single molecule level.

Probing Dynamic Generation of Hot-Spots in Self-Assembled Chains of Gold Nanorods by Surface-Enhanced Raman Scattering

Further progress in the applications of self-assembled nanostructures critically depends on developing a fundamental understanding of the relation between the properties of nanoparticle ensembles and their time-dependent structural characteristics. Following dynamic generation of hot-spots in the self-assembled chains of gold nanorods, we established a direct correlation between ensemble-averaged surface-enhanced Raman scattering and extinction properties of the chains. Experimental results were supported with comprehensive finite-difference time-domain simulations. The established relationship between the structure of nanorod ensembles and their optical properties provides the basis for creating dynamic, solution-based, plasmonic platforms that can be utilized in applications ranging from sensing to nanoelectronics.

Attomolar Protein Detection Using in-Hole Surface Plasmon Resonance

An in-hole nanohole surface plasmon resonance sensing scheme is demonstrated. Arrays of periodic nanoholes milled through thin layers of SiO(x) and gold were used to detect the binding of organic and biological molecules inside the nanoholes, while blocking the gold surfaces outside the holes. This new approach is more efficient than the previous nanohole array method, where the response was related to binding events taking place inside of the holes and on the top gold surface. The improved sensitivity to binding events and lower detection limit are related to resonant surface plasmon enhanced transmission through the arrays of nanoholes. The sensitivity was found to be 650 nm/RIU and the detection of three attomoles of proteins was estimated from this scheme.

Hyperspectral nanoscale imaging on dielectric substrates with coaxial optical antenna scan probes

An important goal in nano science is to unlock previously inaccessible physics and dynamics within nanoscale systems by combining the efficient nanoscale field confinement/optical resolution (∼10 nm) of optical antennae and the ultrafast temporal resolution (fs) inherent in optical studies with the capabilities of modern scanning probe techniques. Here we report on a significant step toward this goal using a novel nanofabricated coaxial antenna tip capable of recording useful Raman spectra in ∼50 ms to acquire 256 by 256 pixel images on dielectric substrates with a full spectrum at each pixel.

Optical Trapping of 12 nm Dielectric Spheres Using Double-Nanoholes in a Gold Film

Optical tweezers have found many applications in biology, but for reasonable intensities, conventional traps are limited to particles >100 nm in size. We use a double-nanohole in a gold film to experimentally trap individual nanospheres, including 20 nm polystyrene spheres and 12 nm silica spheres, at a well-defined trapping point. We present statistical studies on the trapping time, showing an exponential dependence on the optical power. Trapping experiments are repeated for different particles and several nanoholes with different gap dimensions. Unusually, smaller particles can be more easily trapped than larger ones with the double-nanohole. The 12 nm silica sphere has a size and a refractive index comparable to the smallest virus particles and has a spherical shape which is the worst case scenario for trapping.

Single Molecule Directivity Enhanced Raman Scattering using Nanoantennas

Single molecule detection by directivity enhanced Raman scattering is demonstrated using nanoantennas. Bianalyte Raman scattering is used to confirm the detection of single molecules of Rhodamine 6G and Nile Blue A in aqueous solution. Calculations show that Raman enhancement factors of 10(13) can be achieved by combined optimization of the local field enhancement (hotspot with 10(11) enhancement) and antenna directionality (with 10(2) enhancement).

Enhanced second harmonic generation from nanoscale double-hole arrays in a gold film

We present enhanced second harmonic generation (SHG) from arrays with a basis of overlapping double holes. The arrays were created by focused-ion beam milling through a gold film, and the measurements were performed in the transmission geometry. By fixing the array periodicity and varying the spacing between the holes, the SHG was enhanced by an order of magnitude for the single case where the apexes of the double-hole structure were nearly touching. Numerical calculations showed a local electric field enhancement that agrees with the SHG observations. This work shows the potential of double-hole structures for nonlinear optics at the nanoscale.

Flow-Through vs Flow-Over: Analysis of Transport and Binding in Nanohole Array Plasmonic Biosensors

We quantify the efficacy of flow-through nanohole sensing, as compared to the established flow-over format, through scaling analysis and numerical simulation. Nanohole arrays represent a growing niche within surface plasmon resonance-based sensing methods, and employing the nanoholes as nanochannels can enhance transport and analytical response. The additional benefit offered by flow-through operation is, however, a complex function of operating parameters and application-specific binding chemistry. Compared here are flow-over sensors and flow-through nanohole array sensors with equivalent sensing area, where the nanohole array sensing area is taken as the inner-walls of the nanoholes. The footprints of the sensors are similar (e.g., a square 20 μm wide flow-over sensor has an equivalent sensing area as a square 30 μm wide array of 300 nm diameter nanoholes with 450 nm periodicity in a 100 nm thick gold film). Considering transport alone, an analysis here shows that given equivalent sensing area and flow rate the flow-through nanohole format enables greatly increased flux of analytes to the sensing surface (e.g., 40-fold for the case of Q = 10 nL/min). Including both transport and binding kinetics, a computational model, validated by experimental data, provides guidelines for performance as a function of binding time constant, analyte diffusivity, and running parameters. For common binding kinetics and analytes, flow-through nanohole arrays offer ∼10-fold improvement in response time, with a maximum of 20-fold improvement for small biomolecules with rapid kinetics.