Quan Xiang

Surface enhanced Raman scattering of gold nanoparticles supported on copper foil with graphene as a nanometer gap

Gaps with single-nanometer dimensions (<10 nm) between metallic nanostructures enable giant local field enhancements for surface enhanced Raman scattering (SERS). Monolayer graphene is an ideal candidate to obtain a sub-nanometer gap between plasmonic nanostructures. In this work, we demonstrate a simple method to achieve a sub-nanometer gap by dewetting a gold film supported on monolayer graphene grown on copper foil. The Cu foil can serve as a low-loss plasmonically active metallic film that supports the imaginary charge oscillations, while the graphene can not only create a stable sub-nanometer gap for massive plasmonic field enhancements but also serve as a chemical enhancer. We obtained higher SERS enhancements in this graphene-gapped configuration compared to those in Au nanoparticles on Cu film or on graphene-SiO2-Si. Also, the Raman signals measured maintained their fine features and intensities over a long time period, indicating the stability of this Au-graphene-Cu hybrid configuration as an SERS substrate.

Optimization of the particle density to maximize the SERS enhancement factor of periodic plasmonic nanostructure array

Low-cost surface-enhanced Raman scattering (SERS) substrate with the largest possible enhancement factor is highly desirable for SERS-based sensing applications. In this work, we systematically investigated how the density of plasmonic nanostructures affects the intensity of SERS signal. By directly depositing of metallic layer on electron-beam-lithography defined dielectric nanoposts, plasmonic structures array with different densities were reliably fabricated for SERS measurements. Two main experimental phenomena were obtained: (1) the SERS intensity did not increase monotonically when increasing the density of plasmonic structures, and (2) these ultra-dense plasmonic structures resulted in the maximal SERS intensity. These results could be well explained based on finite-difference time domain (FDTD) simulations and provide robust experimental evidences to guide the design of the best possible SERS substrate.

Sensitive SERS detection at the single-particle level based on nanometer-separated mushroom-shaped plasmonic dimers

Elevated metallic nanostructures with nanogaps (<10 nm) possess advantages for surface enhanced Raman scattering (SERS) via the synergic effects of nanogaps and efficient decoupling from the substrate through an elevated three-dimensional (3D) design. In this work, we demonstrate a pattern-transfer-free process to reliably define elevated nanometer-separated mushroom-shaped dimers directly from 3D resist patterns based on the gap-narrowing effect during the metallic film deposition. By controlling the initial size of nanogaps in resist structures and the following deposited film thickness, metallic nanogaps could be tuned at the sub-10 nm scale with single-digit nanometer precision. Both experimental and simulated results revealed that gold dimer on mushroom-shaped pillars have the capability to achieve higher SERS enhancement factor comparing to those plasmonic dimers on cylindrical pillars or on a common SiO2/Si substrate, implying that the nanometer-gapped elevated dimer is an ideal platform to achieve the highest possible field enhancement for various plasmonic applications.

Polarization independent subtractive color printing based on ultrathin hexagonal nanodisk-nanohole hybrid structure arrays

Structural color printing based on plasmonic metasurfaces has been recognized as a promising alternative to the conventional dye colorants, though the color brightness and polarization tolerance are still a great challenge for practical applications. In this work, we report a novel plasmonic metasurface for subtractive color printing employing the ultrathin hexagonal nanodisk-nanohole hybrid structure arrays. Through both the experimental and numerical investigations, the subtractive color thus generated taking advantages of extraordinary low transmission (ELT) exhibits high brightness, polarization independence and wide color tunability by varying key geometrical parameters. In addition, other regular patterns including square, pentagonal and circular shapes are also surveyed, and reveal a high color brightness, wide gamut and polarization independence as well. These results indicate that the demonstrated plasmonic metasurface has various potential applications in high-definition displays, high-density optical data storage, imaging and filtering technologies.

Low-voltage-exposure-enabled hydrogen silsesquioxane bilayer-like process for three-dimensional nanofabrication.

We report a bilayer-like electron-beam lithographic process to obtain three-dimensional (3D) nanostructures by using only a single hydrogen silsesquioxane (HSQ) resist layer. The process utilizes the short penetration depth of low-energy (1.5 keV) electron irradiation to first obtain a partially cross-linked HSQ top layer and then uses a high-voltage electron beam (30 keV) to obtain self-aligned undercut (e.g. mushroom-shaped) and freestanding HSQ nanostructures. Based on the well-defined 3D resist patterns, 3D metallic nanostructures were directly fabricated with high fidelity by just depositing a metallic layer. As an example, Ag-coated mushroom-shaped nanostructures were fabricated, which showed lower plasmon resonance damping compared to their planar counterparts. In addition, the undercut 3D nanostructures also enable more reliable lift-off in comparison with the planar nanostructures, with which high-quality silver nanohole arrays were fabricated which show distinct and extraordinary optical transmission in the visible range.

Sensitive Surface-Enhanced Raman Scattering Detection Using On-Demand Postassembled Particle-on-Film Structure

Highly sensitive and low-cost surface-enhanced Raman scattering (SERS) substrates are essential for practical applications of SERS. In this work, we report an extremely simple but effective approach to achieve sensitive SERS detection of molecules (down to 10-10 M) by using a particle/molecule/film sandwich configuration. Compared to conventional SERS substrates which are preprepared to absorb analyte molecules for detection, the proposed sandwich configuration is achieved by postassembling a flexible transparent gel tape embedded with plasmonic nanoparticles onto an Au film decorated with to-be-detected analyte molecules. In such a configuration, the individual plasmonic gel tape and Au film have low or no SERS activity but the final assembled sandwich structure shows strong SERS signal due to the formation of numerous hot spots at the particle-film interface, where the analyte molecules themselves serve as both spacer and signal probes. Because of its simple configuration, we demonstrate that the proposed SERS substrate can be obtained over a large area with extremely low cost. Particularly, because of the on-demand nature and the flexibility, such a postassembly strategy provides an ideal solution to detect the pesticide residue on fruit surfaces with significantly enhanced sensitivity.

An anti-ultrasonic-stripping effect in confined micro/nanoscale cavities and its applications for efficient multiscale metallic patterning

We report a method to reliably and efficiently fabricate high-fidelity metallic structures from a ten-nanometer to a millimeter scale based on an anti-ultrasonic-stripping (AUS) effect in confined micro/nanoscale cavities. With this AUS effect, metallic structures, which are surrounded by the pre-patterned closed templates, could be defined through selectively removing the evaporated metallic layer at the top and outside of the templates by ultrasonic-cavitation-induced stripping. Because only pre-patterned templates are required for exposure in this multiscale patterning process, this AUS-based process enables much smaller and more reliable plasmonic nanogaps due to the mitigated proximity effect and allows rapid fabrication of multiscale metallic structures which require both tiny and large structures. With unprecedented efficiency and resolution down to a ten-nanometer scale, various metallic structures were fabricated using this AUS-effect-based multiscale patterning process. This AUS effect paves the way for direct writing of metallic structures with a high resolution over a large area for practical applications in plasmonics and nanogap-based electronics.