Methods for tuning plasmonic and photonic optical resonances in high surface area porous electrodes.

Surface plasmons have found a wide range of applications in plasmonic and nanophotonic devices. The combination of plasmonics with three-dimensional photonic crystals has enormous potential for the efficient localization of light in high surface area photoelectrodes. However, the metals traditionally used for plasmonics are difficult to form into three-dimensional periodic structures and have limited optical penetration depth at operational frequencies, which limits their use in nanofabricated photonic crystal devices. The recent decade has seen an expansion of the plasmonic material portfolio into conducting ceramics, driven by their potential for improved stability, and their conformal growth via atomic layer deposition has been established. In this work, we have created three-dimensional photonic crystals with an ultrathin plasmonic titanium nitride coating that preserves photonic activity. Plasmonic titanium nitride enhances optical fields within the photonic electrode while maintaining sufficient light penetration. Additionally, we show that post-growth annealing can tune the plasmonic resonance of titanium nitride to overlap with the photonic resonance, potentially enabling coupled-phenomena applications for these three-dimensional nanophotonic systems. Through characterization of the tuning knobs of bead size, deposition temperature and cycle count, and annealing conditions, we can create an electrically- and plasmonically-active photonic crystal as-desired for a particular application of choice.

Visualizing the bidirectional optical transfer function for near-field enhancement in waveguide coupled plasmonic transducers.

We report visualizations of the bidirectional near-field optical transfer function for a waveguide-coupled plasmonic transducer as a metrology technique essential for successful development for mass-fabricated near-field devices. Plasmonic devices have revolutionized the observation of nanoscale phenomena, enabling optical excitation and readout from nanoscale regions of fabricated devices instead of as limited by optical diffraction. Visualizations of the plasmonic transducer modes were acquired both by local near-field excitation of the antenna on the front facet of a waveguide using the focused electron beam of a scanning electron microscope as a probe of the near-field cathodoluminescence during far-field collection from the back facet of the waveguide, and by local mapping of the optical near-field for the same antenna design using scattering scanning near-field optical microscopy as a probe of the near-field optical mode density for far-field light focused into the back facet of the waveguide. Strong agreement between both measurement types and numerical modeling was observed, indicating that the method enables crucial metrological comparisons of as fabricated device performance to as-modeled device expectations for heat-assisted magnetic recording heads, which can be extended to successful development of future near-field-on-chip devices such as optical processor interconnects.

Template-Stripped Multifunctional Wedge and Pyramid Arrays for Magnetic Nanofocusing and Optical Sensing.

We present large-scale reproducible fabrication of multifunctional ultrasharp metallic structures on planar substrates with capabilities including magnetic field nanofocusing and plasmonic sensing. Objects with sharp tips such as wedges and pyramids made with noble metals have been extensively used for enhancing local electric fields via the lightning-rod effect or plasmonic nanofocusing. However, analogous nanofocusing of magnetic fields using sharp tips made with magnetic materials has not been widely realized. Reproducible fabrication of sharp tips with magnetic as well as noble metal layers on planar substrates can enable straightforward application of their material and shape-derived functionalities. We use a template-stripping method to produce plasmonic-shell-coated nickel wedge and pyramid arrays at the wafer-scale with tip radius of curvature close to 10 nm. We further explore the magnetic nanofocusing capabilities of these ultrasharp substrates, deriving analytical formulas and comparing the results with computer simulations. These structures exhibit nanoscale spatial control over the trapping of magnetic microbeads and nanoparticles in solution. Additionally, enhanced optical sensing of analytes by these plasmonic-shell-coated substrates is demonstrated using surface-enhanced Raman spectroscopy. These methods can guide the design and fabrication of novel devices with applications including nanoparticle manipulation, biosensing, and magnetoplasmonics.

Nanopore sensing at ultra-low concentrations using single-molecule dielectrophoretic trapping.

Single-molecule techniques are being developed with the exciting prospect of revolutionizing the healthcare industry by generating vast amounts of genetic and proteomic data. One exceptionally promising route is in the use of nanopore sensors. However, a well-known complexity is that detection and capture is predominantly diffusion limited. This problem is compounded when taking into account the capture volume of a nanopore, typically 10(8)-10(10) times smaller than the sample volume. To rectify this disproportionate ratio, we demonstrate a simple, yet powerful, method based on coupling single-molecule dielectrophoretic trapping to nanopore sensing. We show that DNA can be captured from a controllable, but typically much larger, volume and concentrated at the tip of a metallic nanopore. This enables the detection of single molecules at concentrations as low as 5 fM, which is approximately a 10(3) reduction in the limit of detection compared with existing methods, while still maintaining efficient throughput.

Polarization interferometry for real-time spectroscopic plasmonic sensing.

We present quantitative, spectroscopic polarization interferometry phase measurements on plasmonic surfaces for sensing applications. By adding a liquid crystal variable wave plate in our beam path, we are able to measure phase shifts due to small refractive index changes on the sensor surface. By scanning in a quick sequence, our technique is extended to demonstrate real-time measurements. While this optical technique is applicable to different sensor geometries-e.g., nanoparticles, nanogratings, or nanoapertures-the plasmonic sensors we use here consist of an ultrasmooth gold layer with buried linear gratings. Using these devices and our phase measurement technique, we calculate a figure of merit that shows improvement over measuring only surface plasmon resonance shifts from a reflected intensity spectrum. To demonstrate the general-purpose versatility of our phase-resolved measurements, we also show numerical simulations with another common device architecture: periodic plasmonic slits. Since our technique inherently measures both the intensity and phase of the reflected or transmitted light simultaneously, quantitative sensor device characterization is possible.

Individual Template-Stripped Conductive Gold Pyramids for Tip-Enhanced Dielectrophoresis.

Gradient fields of optical, magnetic, or electrical origin are widely used for the manipulation of micro- and nanoscale objects. Among various device geometries to generate gradient forces, sharp metallic tips are one of the most effective. Surface roughness and asperities present on traditionally produced tips reduce trapping efficiencies and limit plasmonic applications. Template-stripped, noble metal surfaces and structures have sub-nm roughness and can overcome these limits. We have developed a process using a mix of conductive and dielectric epoxies to mount template-stripped gold pyramids on tungsten wires that can be integrated with a movable stage. When coupled with a transparent indium tin oxide (ITO) electrode, the conductive pyramidal tip functions as a movable three-dimensional dielectrophoretic trap which can be used to manipulate submicrometer-scale particles. We experimentally demonstrate the electrically conductive functionality of the pyramidal tip by dielectrophoretic manipulation of fluorescent beads and concentration of single-walled carbon nanotubes, detected with fluorescent microscopy and Raman spectroscopy.

Dielectrophoresis-enhanced plasmonic sensing with gold nanohole arrays.

We experimentally demonstrate dielectrophoretic concentration of biological analytes on the surface of a gold nanohole array, which concurrently acts as a nanoplasmonic sensor and gradient force generator. The combination of nanohole-enhanced dielectrophoresis, electroosmosis, and extraordinary optical transmission through the periodic gold nanohole array enables real-time label-free detection of analyte molecules in a 5 µL droplet using concentrations as low as 1 pM within a few minutes, which is more than 1000 times faster than purely diffusion-based binding. The nanohole-based optofluidic platform demonstrated here is straightforward to construct, applicable to both charged and neutral molecules, and performs a novel function that cannot be accomplished using conventional surface plasmon resonance sensors.

Ultrasmooth metallic films with buried nanostructures for backside reflection-mode plasmonic biosensing.

We present a new plasmonic device architecture based on ultrasmooth metallic surfaces with buried plasmonic nanostructures. Using template-stripping techniques, ultrathin gold films with less than 5 Å surface roughness are optically coupled to an arbitrary arrangement of buried metallic gratings, rings, and nanodots. As a prototypical example, we present linear plasmonic gratings buried under an ultrasmooth 20 nm thick gold surface for biosensing. The optical illumination and collection are completely decoupled from the microfluidic delivery of liquid samples due to the backside, reflection-mode geometry. This allows for sensing with opaque or highly scattering liquids. With the buried nanostructure design, we maintain high sensitivity and decoupled backside (reflective) optical access as with traditional prism-based surface plasmon resonance (SPR) sensors. In addition, we also gain the benefits offered by nanoplasmonic sensors such as spectral tunability and high-resolution, wide-field SPR imaging with normal-incidence epi-illumination that is simple to construct and align. Beyond sensing, our buried plasmonic nanostructures with ultrasmooth metallic surfaces can benefit nanophotonic waveguides, surface-enhanced spectroscopy, nanolithography, and optical trapping.