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Register a new userSurface-enhanced Raman spectroscopy in 3D electrospun nanofiber mats coated with gold nanorods
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A. Camposeo
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Nanofibers functionalized by metal nanostructures and particles are exploited as effective flexible substrates for SERS analysis. Their complex three-dimensional structure may provide Raman signals enhanced by orders of magnitude compared to untextured surfaces. Understanding the origin of such improved performances is therefore very important for pushing nanofiber-based analytical technologies to their upper limit. Here we report on polymer nanofiber mats which can be exploited as substrates for enhancing the Raman spectra of adsorbed probe molecules. The increased surface area and the scattering of light in the nanofibrous system are individually analyzed as mechanisms to enhance Raman scattering. The deposition of gold nanorods on the fibers further amplifies Raman signals due to SERS. This study suggests that Raman signals can be finely tuned in intensity and effectively enhanced in nanofiber mats and arrays by properly tailoring the architecture, composition, and light-scattering properties of the complex networks of filaments.
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We present stacked organic lasing heterostructures made by different species of light-emitting electrospun fibers, each able to provide optical gain in a specific spectral region. A hierarchical architecture is obtained by conformable layers of fibers with disordered two-dimensional organization and three-dimensional compositional heterogeneity. Lasing polymer fibers are superimposed in layers, showing asymmetric optical behavior from the two sides of the organic heterostructure, and tailored and bichromatic stimulated emission depending on the excitation direction. A marginal role of energy acceptor molecules in determining quenching of high-energy donor species is evidenced by luminescence decay time measurements. These findings show that non-woven stacks of light-emitting electrospun fibers doped with different dyes exhibit critically-suppressed Forster resonance energy transfer, limited at joints between different fiber species. This leads to obtain hybrid materials with mostly physically-separated acceptors and donors, thus largely preventing donor quenching and making much easier to achieve simultaneous lasing from multiple spectral bands. Coherent backscattering experiments are also performed on the system, suggesting the onset of random lasing features. These new organic lasing systems might find application in microfluidic devices where flexible and bidirectional excitation sources are needed, optical sensors, and nanophotonics.
In this paper, we report our study on gold (Au) films with different thicknesses deposited on single layer graphene (SLG) as surface enhanced Raman scattering (SERS) substrates for the characterization of rhodamine (R6G) molecules. We find that an Au film with a thickness of ~7 nm deposited on SLG is an ideal substrate for SERS, giving the strongest Raman signals for the molecules and the weakest photoluminescence (PL) background. While Au films effectively enhance both the Raman and PL signals of molecules, SLG effectively quenches the PL signals from the Au film and molecules. The former is due to the electromagnetic mechanism involved while the latter is due to the strong resonance energy transfer from Au to SLG. Hence, the combination of Au films and SLG can be widely used in the characterization of low concentration molecules with relatively weak Raman signals.
Plasmonic optical tweezers are a ubiquitous tool for the precise manipulation of nanoparticles and biomolecules at low photon flux, while femtosecond-laser optical tweezers can probe the nonlinear optical properties of the trapped species with applications in biological diagnostics. In order to adopt plasmonic optical tweezers in real-world applications, it is essential to develop large-scale fabrication processes without compromising the trapping efficiency. Here, we develop a novel platform for continuous wave (CW) and femtosecond plasmonic optical tweezers, based on gold-coated black silicon. In contrast with traditional lithographic methods, the fabrication method relies on simple, single-step, maskless tabletop laser processing of silicon in water that facilitates scalability. Gold-coated black silicon supports repeatable trapping efficiencies comparable to the highest ones reported to date. From a more fundamental aspect, a plasmon-mediated efficiency enhancement is a resonant effect, and therefore, dependent on the wavelength of the trapping beam. Surprisingly, a wavelength characterization of plasmon-enhanced trapping efficiencies has evaded the literature. Here, we exploit the repeatability of the recorded trapping efficiency, offered by the gold-coated black silicon platform, and perform a wavelength-dependent characterization of the trapping process, revealing the resonant character of the trapping efficiency maxima. Gold-coated black silicon is a promising platform for large-scale parallel trapping applications that will broaden the range of optical manipulation in nanoengineering, biology, and the study of collective biophotonic effects.
Single-molecule detection with chemical specificity is a powerful and much desired tool for biology, chemistry, physics, and sensing technologies. Surface-enhanced spectroscopies enable single molecule studies, yet reliable substrates of adequate sensitivity are in short supply. We present a simple, scaleable substrate for surface-enhanced Raman spectroscopy (SERS) incorporating nanometer-scale electromigrated gaps between extended electrodes. Molecules in the nanogap active regions exhibit hallmarks of very high Raman sensitivity, including blinking and spectral diffusion. Electrodynamic simulations show plasmonic focusing, giving electromagnetic enhancements approaching those needed for single-molecule SERS.
The programmable assembly of DNA strands is a promising tool for building tailored bottom-up nanostructures. Here, we present a plasmonic nanosystem obtained by the base-pairing mediated aggregation of gold nanoparticles (NPs) which are separately functionalized with two different single-stranded DNA chains. Their controlled assembly is mediated by a complementary DNA bridge sequence. We monitor the formation of DNA assembled NP aggregates in solution, and we study their Surface Enhanced Raman Scattering (SERS) response by comparison with the single NP constituents. We interpret the revealed SERS signatures in terms of the molecular and NP organization at the nanoscale, demonstrating that the action of the DNA bridge molecule yields regular NP aggregates with controlled interparticle distance and reproducible SERS response. This demonstrates the potential of the present system as a stable, biocompatible, and recyclable SERS sensor.
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