Search

Surface-enhanced Raman spectroscopy (SERS) detection of analyte molecules at ultra-low concentrations requires highly-efficient plasmonic nanostructures enabling a high hot-spot density. However, a facile and cost-effective strategy toward large-area fabrication of efficient nanostructures with significant electromagnetic field enhancement remains a great challenge. Further, SERS faces reliability issues with the molecular fingerprint at ultra-low concentrations. This work shows a one-step rapid fabrication technique utilizing glancing angle deposition for growing 3D nanopillars of Ag or Au, which is facile, scalable and cost-effective. The 3D nanopillar substrates can reliably detect analyte molecules with concentrations as low as 10-18 M with a high signal-to-noise ratio molecular fingerprint proven for Cresyl violet, p-aminothiophenol and Rhodamine 6G. The ultra-high enhancement is realized in conjunction with the formation of a high hot-spot density due to localized surface plasmons and surface plasmons at metal/air interface. A portable handheld Raman spectrometer is used to evaluate the potential application of the nanopillars for on-site diagnostics. It avoids the need for sophisticated tabletop instruments yet provides high-precision molecular specificity outside specialized laboratories. The 3D nanopillar substrates show excellent molecular detection limits at 10−15 M concentrations when tested with a handheld Raman spectrometer. The uniqueness of the 3D nanopillar features with the formation of a high density of hot-spots and one-step nanofabrication methods provide a platform to unravel on-site diagnostics with cost-effective approaches.

High-temperature stable emitters with spectral selective functionality are an absolute condition for efficient conversion of thermal radiation into electricity using thermophotovoltaic (TPV) systems. Usually, spectral selective emitters are made up of multilayered materials or geometrical structures resulting from complex fabrication processes. Here, we report a spectrally selective emitter based on a single metal layer coating of molybdenum (Mo) over a 3D dielectric pillar geometry. 3D Mo nanopillars are fabricated using large-area and cost-effective hole-mask colloidal lithography. These nanostructures show an absorptivity/emissivity of 95% below the cut-off wavelength of an InGaAsSb PV cell at 2.25 μm, and a sharp decline in absorptivity/emissivity in the near-infrared regions, approaching a low emissivity of 10%. The 3D Mo nanopillars show outstanding thermal/structural stability up to 1473 K for 24 h duration under Ar atmosphere and polarization and angle invariance up to 60° incidence angles. With a low-cost and scalable fabrication method, 3D Mo nanostructures provide tremendous opportunities in TPV and high temperature photonic/plasmonic applications. Deutsche Forschungsgemeinschaft (DFG)

Broadband absorbers, with the simultaneous advantages of thermal stability, insensitivity to light polarization and angle, robustness against harsh environmental conditions, and large area fabrication by scalable methods, are essential elements in (solar) thermophotovoltaics. Compared to the noble metal and multilayered broadband absorbers, high-temperature refractory metal-based nanostructures with low-Q resonators are reported less. In this work, 3D titanium nitride (TiN) nanopillars are investigated for ultrabroadband absorption in the visible and near-infrared spectral regions with average absorptivities of 0.94, over a wide range of oblique angles between 0° and 75°. The effect of geometrical parameters of the TiN nanopillars on broadband absorption is investigated. By combining the flexibility of nanopillar design and lossy TiN films, ultrabroadband absorption in the visible and near-infrared is obtained. A thin layer of hafnium oxide is deposited to enhance the thermal stability of TiN nanopillars. Finally, the thermal/spectral stability of the TiN nanopillars is demonstrated after annealing at 1473 K for 24 h while retaining their structural features. Thus, the TiN nanopillars can provide excellent opportunities for high-temperature applications, especially solar thermophotovoltaics. Broadband absorbers, with the simultaneous advantages of thermal stability, insensitivity to light polarization and angle, robustness against harsh environmental conditions, and large area fabrication by scalable methods, are essential elements in (solar) thermophotovoltaics. Compared to the noble metal and multilayered broadband absorbers, high-temperature refractory metal-based nanostructures with low-Q resonators are reported less. In this work, 3D titanium nitride (TiN) nanopillars are investigated for ultrabroadband absorption in the visible and near-infrared spectral regions with average absorptivities of 0.94, over a wide range of oblique angles between 0° and 75°. The effect of geometrical parameters of the TiN nanopillars on broadband absorption is investigated. By combining the flexibility of nanopillar design and lossy TiN films, ultrabroadband absorption in the visible and near-infrared is obtained. A thin layer of hafnium oxide is deposited to enhance the thermal stability of TiN nanopillars. Finally, the thermal/spectral stability of the TiN nanopillars is demonstrated after annealing at 1473 K for 24 h while retaining their structural features. Thus, the TiN nanopillars can provide excellent opportunities for high-temperature applications, especially solar thermophotovoltaics.

The detection of probe molecules at ultralow concentrations, even at the single-molecule level, can be addressed with the breakthrough concept of plasmonic hot-spot engineering. In view of that, the fabrication of nanostructures endowed with sub-10 nm gaps and extremely large near-field enhancement has gained increasing attention, becoming a key-condition for improved sensitivity. The present work demonstrates a new perspective in ultrasensitive detection by engineering every individual plasmonic nanostructure with a giant electric field confinement and superior hot-spot densities, thus eliminating the need for extremely narrow interparticle separations. The detection of probe molecules at ultralow concentrations, even at the single-molecule level, can be addressed with the breakthrough concept of plasmonic hot-spot engineering. In view of that, the fabrication of nanostructures endowed with sub-10 nm gaps and extremely large near-field enhancement has gained increasing attention, becoming a key-condition for improved sensitivity. The present work demonstrates a new perspective in ultrasensitive detection by engineering every individual plasmonic nanostructure with a giant electric field confinement and superior hot-spot densities, thus eliminating the need for extremely narrow interparticle separations.