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We propose and demonstrate a new SERS substrate architecture that couples a dense three-dimensional (3-D) cavity nanoantenna array, through nano-gaps, with dense plasmonic nanodots; and a new nanofabrication that combines nanoimprint, guided self-assembly and self-alignment and has fabricated the architecture precisely, simply, inexpensively and over large area (4-inch wafer). We experimentally achieved not only high area-average SERS enhancement (1.2×10⁹) but also excellent uniformity (22.4% variation) at the same time over the entire large-area sample by measuring 90 points with a regular mapping distance. The best uniformity achieved is 15% variation over 1.6 mm by 1.6 mm area at slightly lower enhancement factor and is independent of the excitation laser probe size, which had an area varying from ~1 to 10,000 μm2.

Tip-enhanced Raman scattering (TERS) is a promising optical and analytical technique for chemical imaging and sensing at single molecule resolution. In particular, TERS signals generated by a gap-mode configuration where a silver tip is coupled with a gold substrate can resolve a single-stranded DNA (ssDNA) molecule with a spatial resolution below 1 nm. To demonstrate the proof of subnanometer resolution, we show direct nucleic acid sequencing using TERS of a phage ssDNA (M13mp18). M13mp18 provides a known sequence and, through our deposition strategy, can be stretched (uncoiled) and attached to the substrate by its phosphate groups, while exposing its nucleobases to the tip. After deposition, we scan the silver tip along the ssDNA and collect TERS signals with a step of 0.5 nm, comparable to the bond length between two adjacent DNA bases. By demonstrating the real-time profiling of a ssDNA configuration and furthermore, with unique TERS signals of monomeric units of other biopolymers, we anticipate that this technique can be extended to the high-resolution imaging of various nanostructures as well as the direct sequencing of other important biopolymers including RNA, polysaccharides, and polypeptides.

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We describe in detail a procedure for maximizing the bandwidth of supercontinuum generation in As(2)Se(3) chalcogenide fibers and the physics behind this procedure. First, we determine the key parameters that govern the design. Second, we find the conditions for the fiber to be endlessly single-mode; the fiber should be endlessly single-mode to maintain high nonlinearity and low coupling loss. We find that supercontinuum generation in As(2)Se(3) fibers proceeds in two stages--an initial stage that is dominated by four-wave mixing and a later stage that is dominated by the Raman-induced soliton self-frequency shift. Third, we determine the conditions to maximize the Stokes wavelength that is generated by four-wave mixing in the initial stage. Finally, we put all these pieces together to maximize the bandwidth. We show that it is possible to generate an optical bandwidth of more than 4 microm with an input pump wavelength of 2.5 microm using an As(2)Se(3) fiber with an air-hole-diameter-to-pitch ratio of 0.4 and a pitch of 3 microm. Obtaining this bandwidth requires a careful choice of the fiber's waveguide parameters and the pulse's peak power and duration, which determine respectively the fiber's dispersion and nonlinearity.