Nicolò Maccaferri

Scanning Probe Photonic Nanojet Lithography

The use of nano/microspheres or beads for optical nanolithography is a consolidated technique for achieving subwavelength structures using a cost-effective approach; this method exploits the capability of the beads to focus electromagnetic waves into subwavelength beams called photonic nanojets, which are used to expose the photoresist on which the beads are placed. However, this technique has only been used to produce regular patterns based on the spatial arrangement of the beads on the substrate, thus considerably limiting the pool of applications. Here, we present a novel microsphere-based optical lithography technique that offers high subwavelength resolution and the possibility of generating any arbitrary pattern. The presented method consists of a single microsphere embedded in an AFM cantilever, which can be controlled using the AFM motors to write arbitrary patterns with subwavelength resolution (down to 290 nm with a 405 nm laser). The performance of the proposed technique can compete with those of commercial high-resolution standard instruments, with the advantage of a one-order-of-magnitude reduction in costs. This approach paves the way for direct integration of cost-effective, high-resolution optical lithography capabilities into several existing AFM systems.

Live Intracellular Biorthogonal Imaging by Surface Enhanced Raman Spectroscopy using Alkyne-Silver Nanoparticles Clusters

Live intracellular imaging is a valuable tool in modern diagnostics and pharmacology. Surface Enhanced Raman Spectroscopy (SERS) stands out as a non-destructive and multiplexed technique, but intracellular SERS imaging still suffers from interfering background from endogenous components. Here we show the assembly of small colloidal SERS probes with Raman signal in the cell-silent window of 1800–2900 cm−1 for biorthogonal intracellular SERS imaging of dopamine that was undistinguishable from the endogenous cell background. By linking colloidal silver nanoparticles with alkyne-dopamine adducts, clusters are formed by 2–6 nanoparticles spaced by tight interparticle gaps that exhibited high electric field enhancement and strong SERS signals of alkyne and dopamines. Due to the cell-silent signals of the alkyne, intracellular in-vitro Raman imaging shows that the dopamines on the internalized clusters remain distinguishable across the cytoplasm with good spatial resolution. Our method can be a general-purpose method for real-time imaging of biomolecules, such as proteins, peptides, DNA and drugs.

Author Correction: Live Intracellular Biorthogonal Imaging by Surface Enhanced Raman Spectroscopy using Alkyne-Silver Nanoparticles Clusters

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Plasmonic zero mode waveguide for highly confined and enhanced fluorescence emission

We fabricate a plasmonic nanoslot that is capable of performing enhanced single molecule detection at 10 μM concentrations. The nanoslot combines the tiny detection volume of a zero-mode waveguide and the field enhancement of a plasmonic nanohole. The nanoslot is fabricated on a bi-metallic film formed by the sequential deposition of gold and aluminum on a transparent substrate. Simulations of the structure yield an average near-field intensity enhancement of two orders of magnitude at its resonant frequency. Experimentally, we measure the fluorescence stemming from the nanoslot and compare it with that of a standard aluminum zero-mode waveguide. We also compare the detection volume for both structures. We observe that while both structures have a similar detection volume, the nanoslot yields a 25-fold fluorescence enhancement.

Hybrid plasmonic nanostructures based on controlled integration of MoS2 flakes on metallic nanoholes

Here, we propose an easy and robust strategy for the versatile preparation of hybrid plasmonic nanopores by means of controlled deposition of single flakes of MoS2 directly on top of metallic holes. The device is realized on silicon nitride membranes and can be further refined by TEM or FIB milling to achieve the passing of molecules or nanometric particles through a pore. Importantly, we show that the plasmonic enhancement provided by the nanohole is strongly accumulated in the 2D nanopore, thus representing an ideal system for single-molecule sensing and sequencing in a flow-through configuration. Here, we also demonstrate that the prepared 2D material can be decorated with metallic nanoparticles that can couple their resonance with the nanopore resonance to further enhance the electromagnetic field confinement at the nanoscale level. This method can be applied to any gold nanopore with a high level of reproducibility and parallelization; hence, it can pave the way to the next generation of solid-state nanopores with plasmonic functionalities. Moreover, the controlled/ordered integration of 2D materials on plasmonic nanostructures opens a pathway towards new investigation of the following: enhanced light emission; strong coupling from plasmonic hybrid structures; hot electron generation; and sensors in general based on 2D materials.

Helical light emission from plasmonic vortices via magnetic tapered tip

We investigate an architecture where a plasmonic vortex excited in a gold surface propagates on an adiabatically tapered magnetic tip and detaches to the far-field while carrying a well-defined optical angular momentum. We analyze the out-coming light and show that, despite generally high losses of flat magnetic surface, our 3D structure exhibits high energy throughput. Moreover, we show that once a magneto-optical activity is activated inside the magnetic tip a modulation of the total power transmittance is possible.

Enhanced Raman Investigation of Cell Membrane and Intracellular Compounds by 3D Plasmonic Nanoelectrode Arrays

Abstract 3D nanostructures are widely exploited in cell cultures for many purposes such as controlled drug delivery, transfection, intracellular sampling, and electrical recording. However, little is known about the interaction of the cells with these substrates, and even less about the effects of electroporation on the cellular membrane and the nuclear envelope. This work exploits 3D plasmonic nanoelectrodes to study, by surface‐enhanced Raman scattering (SERS), the cell membrane dynamics on the nanostructured substrate before, during, and after electroporation. In vitro cultured cells tightly adhere on 3D plasmonic nanoelectrodes precisely in the plasmonic hot spots, making this kind of investigation possible. After electroporation, the cell membrane dynamics are studied by recording the Raman time traces of biomolecules in contact or next to the 3D plasmonic nanoelectrode. During this process, the 3D plasmonic nanoelectrodes are intracellularly coupled, thus enabling the monitoring of different molecular species, including lipids, proteins, and nucleic acids. Scanning electron microscopy cross‐section analysis evidences the possibility of nuclear membrane poration compatible with the reported Raman spectra. These findings may open a new route toward controlled intracellular sampling and intranuclear delivery of genic materials. They also show the possibility of nuclear envelope disruption which may lead to negative side effects.

Nanoporous gold decorated with silver nanoparticles as large area efficient SERS substrate

Nanoporous gold is a very promising material platform for several plasmonic applications. Nanoporous gold can be formed by dealloying Au–Ag alloys, previously grown by means of Ag-Au co-sputtering. The optical response is completely determined by the nanostructured film features, that only depend on the initial alloy composition. It has been extensively used as SERS substrate both as thin film and nanofabricated fancy designs. Here we explore the potential application of nanoporous gold as SERS substrate as it is coupled and decorated with Ag nanoparticles. Significant enhancement has been observed in comparison with bare nanoporous film.

Magnetoplasmonic control of plasmonic vortices

We theoretically investigate the generation of far-field propagating optical beams with a desired orbital angular momentum by using an archetypical magnetoplasmonic tip surrounded by a gold spiral slit. The use of a magnetic material can lead to important implications once magneto-optical activity is activated through the application of an external magnetic field. The physical model and the numerical study presented here introduce the concept of magnetically tunable plasmonic vortex lens, namely a magnetoplasmonic vortex lens, which ensures a tunable selectivity in the polarization state of the generated nanostructured beam. The presented system provides a promising platform for a localized excitation of plasmonic vortices followed by their beaming in the far-field with an active modulation of both lights transmission and helicity.We theoretically investigate the generation of far-field propagating optical beams with a desired orbital angular momentum by using an archetypical magnetoplasmonic tip surrounded by a gold spiral slit. The use of a magnetic material can lead to important implications once magneto-optical activity is activated through the application of an external magnetic field. The physical model and the numerical study presented here introduce the concept of magnetically tunable plasmonic vortex lens, namely a magnetoplasmonic vortex lens, which ensures a tunable selectivity in the polarization state of the generated nanostructured beam. The presented system provides a promising platform for a localized excitation of plasmonic vortices followed by their beaming in the far-field with an active modulation of both lights transmission and helicity.We theoretically investigate the generation of far-field propagating optical beams with a desired orbital angular momentum by using an archetypical magnetoplasmonic tip surrounded by a gold spiral slit. The use of a magnetic material can lead to important implications once magneto-optical activity is activated through the application of an external magnetic field. The physical model and the numerical study presented here introduce the concept of magnetically tunable plasmonic vortex lens, namely a magnetoplasmonic vortex lens, which ensures a tunable selectivity in the polarization state of the generated nanostructured beam. The presented system provides a promising platform for a localized excitation of plasmonic vortices followed by their beaming in the far-field with an active modulation of both lights transmittance and helicity.