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Francesco De Angelis

Publications and source records attributed to Francesco De Angelis.

At least 37 records · Page 2Linked to original sources

How to puncture a biomembrane: elastic versus entropic rupture

A very common strategy to penetrate the cell membrane and access the internal compartment, consists of using sharp tips or nano needles. However recent experiments of cell penetration by atomic force microscopy tips show, contrary to expectations, a weak dependence of penetration force on the curvature of the tip. Using molecular dynamics simulations and analytical arguments, here we show that membrane disruption can be driven either by elastic or entropic forces depending on the membrane size. Our findings have potentially relevant implications in tissue engineering and drug delivery, as they help assessing the effectiveness of the most common membranes penetration methods.

cond-mat.soft↗

Chemically-controlled self-assembly of hybrid plasmonic nanopores on graphene

Thanks to the spontaneous interaction between noble metals and biological scaffolds, nanomaterials with unique features can be achieved following relatively straightforward and cost-efficient synthetic procedures. Here, plasmonic silver nanorings are synthesized on a ring-like Peroxiredoxin (PRX) protein and used to assemble large arrays of functional nanostructures. The PRX protein drives the seeding growth of metal silver under wet reducing conditions, yielding nanorings with outer and inner diameters down to 28 and 3 nm, respectively. The obtained hybrid nanostructures can be deposited onto a solid-state membrane in order to prepare plasmonic nanopores. In particular, the interaction between graphene and PRX allows for the simple preparation of ordered arrays of plasmonic nanorings on a 2D-material membrane. This fabrication process can be finalized by drilling a nanometer scale pore in the middle of the ring. Fluorescence spectroscopic measurements have been used to demonstrate the plasmonic enhancement induced by the metallic ring. Finally, we support the experimental findings with some numerical simulations showing that the nanorings are endowed with a remarkable plasmonic field within the cavity. Our results represent a proof of concept of a fabrication process that could be suitable for nanopore-based technologies such as next-generation sequencing and single-molecule detection.

physics.app-ph↗

Nanoporous Aluminum-Magnesium Alloy for UV enhanced spectroscopy

We report the first preparation of nanoporous Al-Mg alloy films by selective dissolution of Mg from a Mg-rich AlxMg1-x alloy. We show how to tune the stoichiometry, the porosity and the oxide contents in the final film by modulating the starting ratio between Al and Mg and the dealloying procedure. The obtained porous metal can be exploited for enhanced UV spectroscopy. In this respect, we experimentally demonstrate its efficacy in enhancing fluorescence and surface Raman scattering for excitation wavelengths of 360 nm and 257 nm respectively. Finally, we numerically show the superior performance of the nanoporous Al-Mg alloy in the UV range when compared to equivalent porous gold structures. The large area to surface ratio provided by this material make it a promising platform for a wide range of applications in UV/deep-UV plasmonics.

physics.app-ph↗

Single-molecule DNA Bases Discrimination in Oligonucleotides by Controllable Trapping in Plasmonic Nanoholes

Surface-enhanced Raman spectroscopy (SERS) sensing of DNA sequences by plasmonic nanopores could pave a way to new generation single-molecule sequencing platforms. The SERS discrimination of single DNA bases depends critically on the time that a DNA strand resides within the plasmonic hot spot. However, DNA molecules flow through the nanopores so rapidly that the SERS signals collected are not sufficient for single-molecule analysis. In this work, we report an approach to control the time that molecules reside in the hot spot by physically adsorbing them onto a gold nanoparticle and then trapping the single nanoparticle in a plasmonic nanohole. By trapping the nanoparticle for up to minutes, we demonstrate single-molecule SERS detection of all 4 DNA bases as well as discrimination of single nucleobases in a single oligonucleotide. Our method can be extended easily to label-free sensing of single-molecule amino acids and proteins.

physics.optics↗

Plasmon-Assisted Suppression of Surface Trap States and Enhanced Band-Edge Emission in a Bare CdTe Quantum Dot

Colloidal quantum dots have emerged as a versatile photoluminescent and optoelectronic material. Limitations like fluorescence intermittency, non-radiative Auger recombination and surface traps are commonly addressed by growing a wide-bandgap shell. However, the shell isolates the excitonic wave function and reduces its interaction with the external environment necessary for different applications. Furthermore, their long emission lifetime hinders their use in high-speed optoelectronics. Here, we demonstrate a high degree of control on the photophysics of a bare core CdTe quantum dot solely by plasmon-coupling, showing that more than 99% of the surface defect-state emission from a trap-rich quantum dot can be quenched. Moreover, the band-edge state excitonic and biexcitonic emission rates are Purcell enhanced by 1460 and 613-fold, respectively. Our findings show how plasmon-coupling on bare quantum dots could make chemical approaches developed for improving their optical properties unnecessary, with implications for nanoscale lasers, light emitting devices, solar cells, and ultrafast single-photon sources.

cond-mat.mes-hall↗

Switchable two-state plasmonic tweezers for dynamic manipulation of nano-objects

In this work we present a plasmonic platform capable of trapping nano-objects as small as 100 nm in two different spatial configurations. The switch between the two trapping states, localized on the tip and on the outer wall of a vertical gold nanochannel, can be activated by a variation in the focusing position of the excitation laser along the main axis of the nanotube. We show that the trapping mechanism is facilitated by both an electromagnetic and thermal action. The inner and outer trapping states are respectively characterized by a static and a dynamic behavior and their stiffness was measured by analyzing the position of the trapped specimens as a function of time. In addition, it was demonstrated that the stiffness of the static state is high enough to trap of particles as small as 40nm. These results show a simple, controllable way to generate a switchable two-state trapping regime, which could find applications as a model for the study of dynamic trapping or as mechanism for the development of nanofluidic devices.

physics.app-ph↗

Cooperative energy transfer controls the spontaneous emission rate beyond field enhancement limits

Quantum emitters located in proximity to a metal nanostructure individually transfer their energy via near-field excitation of surface plasmons. The energy transfer process increases the spontaneous emission (SE) rate due to plasmon-enhanced local field. Here, we demonstrate significant acceleration of quantum emitter SE rate in a plasmonic nano-cavity due to cooperative energy transfer (CET) from plasmon-correlated emitters. Using an integrated plasmonic nano-cavity, we realize up to six-fold enhancement in the emission rate of emitters coupled to the same nano-cavity on top of the plasmonic enhancement of the local density of states. The radiated power spectrum retains the plasmon resonance central frequency and lineshape, with the peak amplitude proportional to the number of excited emitters indicating that the observed cooperative SE is distinct from super-radiance. Plasmon-assisted CET offers unprecedented control over the SE rate and allows to dynamically control the spontaneous emission rate at room temperature enabling an SE rate based optical modulator.

cond-mat.mes-hall↗

Surface Thermal Gradients Activated by Enhanced Molecular Absorption in Mid-infrared Vertical Antenna Arrays

We investigate local heat generation by molecules at the apex of polymer-embedded vertical antennas excited at resonant mid-infrared wavelengths, exploiting the surface enhanced infrared absorption (SEIRA) effect. The embedding of vertical nanoantennas in a non-absorbing polymer creates thermal isolation between the apical hotspot, the locus of heat generation, and the heat sink represented by the substrate. Vibrational mid-infrared absorption by strongly absorbing molecules located at the antenna apex then generates nanoscale temperature gradients at the surface. We imaged the thermal gradients by using a nano-photothermal expansion microscope, and we found values up to 10 K/microm in conditions where the radiation wavelength resonates with both the molecule vibrations and the plasmonic mode of the antennas. Values up to 1000 K/microm can be foreseen at maximum quantum cascade laser power. The presented system provides a promising thermoplasmonic platform for antenna-assisted thermophoresis and resonant mid-infrared photocatalysis.

physics.app-ph↗

Site-selective functionalization of plasmonic nanopores for enhanced fluorescence and Förster Resonance Energy Transfer

In this work, we use a site-selective functionalization strategy to decorate plasmonic nanopores with one or more fluorescent dyes. Using an easy and robust fabrication method, we manage to build single plasmonic rings on top of dielectric nanotubes with different inner diameters. The modulation of the dimension of the nanopores allows us to both tailor their field confinement and their Purcell Factor in the visible spectral range. In order to investigate how the changes in geometry influence the fluorescence emission efficiency, thiol-conjugated dyes are anchored on the plasmonic ring, thus forming a functional nanopore. We study the lifetime of ATTO 520 and ATTO 590 attached in two different configurations: single dye, and FRET pair. For the single dye configuration, we observe that the lifetime of both single dyes decreases as the size of the nanopore is reduced. The smallest nanopores yield an experimental Purcell Factor of 6. For the FRET pair configuration, we measure two regimes. For large nanopore sizes, the FRET efficiency remains constant. Whereas for smaller sizes, the FRET efficiency increases from 30 up to 45% with a decrease of the nanopore size. These findings, which have been also supported by numerical simulations, may open new pathways to engineer the energy transfer in plasmonic nanopores with potential applications in photonics and biosensing, in particular in single-molecule detection towards sequencing.

physics.optics↗

Selective intracellular delivery and intracellular recordings combined on MEA biosensors

Biological studies on in vitro cell cultures are of fundamental importance to investigate cells response to external stimuli, such as new drugs for treatment of specific pathologies, or to study communication between electrogenic cells. Although three-dimensional (3D) nanostructures brought tremendous improvements on biosensors used for various biological in vitro studies, including drug delivery and electrical recording, there is still a lack of multifunctional capabilities that could help gaining deeper insights in several bio-related research fields. In this work, the electrical recording of large cell ensembles and the intracellular delivery of few selected cells are combined on the same device by integrating microfluidics channels on the bottom of a multi-electrode array decorated with 3D hollow nanostructures. The novel platform allows to record intracellular-like action potentials from large ensembles of cardiomyocytes derived from human Induced Pluripotent Stem Cells (hiPSC) and from the HL-1 line, while different molecules are selectively delivered into single/few targeted cells. The proposed approach shows high potential for enabling new comprehensive studies that can relate drug effects to network level cell communication processes.

physics.app-ph↗

Controlled integration of MoS2 flakes on nanopores by means of electrophoretic deposition

We propose an easy and robust strategy for the versatile integration of 2D material flakes on plasmonic nanoholes by means of controlled deposition of MoS2 via electrophoretic process. The method can be applied both to simple metallic flat nanostructures and to complex 3D metallic structures both comprising nanoholes. The deposition method allows the decoration of large ordered arrays of plasmonic structures with single or few layers of MoS2. We show that the plasmonic field generated by the nanohole can interact significantly with the 2D layer, thus representing an ideal system for hybrid 2D-Material/Plasmonic investigation. The controlled and ordered integration of 2D materials on plasmonic nanostructures opens a pathway towards, for instance, enhanced light emission; strong coupling from plasmonic hybrid structures; hot electron generation; and sensors based on 2D materials.

physics.app-ph↗

Controlled Intracellular Delivery of Single Particles in Single Cells by 3D Hollow Nanoelectrodes

We present an electrophoretic platform based on 3D hollow nanoelectrodes capable of controlling and quantifying the intracellular delivery of single nanoparticles in single selected cells by surface-enhanced Raman spectroscopy (SERS). The gold-coated hollow nanoelectrode has a sub-femtoliter inner volume that allows the confinement and enhancement of electromagnetic fields upon laser illumination to distinguish the SERS signals of a single nanoparticle flowing through the nanoelectrode. The tight wrapping of cell membranes around the nanoelectrodes enables effective membrane electroporation such that single gold nanorods are delivered into a living cell with a delivery rate subject to the applied bias voltage. The capability of the 3D hollow nanoelectrodes to porate cells and reveal single emitters from the background under live flow is promising for the analysis of both intracellular delivery and sampling.

physics.app-ph↗

Nanostructured Hyperbolic Meta-Antennas Enable Arbitrary Control of Scattering vs Absorption

We show that meta-antennas made of a composite material displaying type II hyperbolic dispersion enable precise and controlled spectral separation of absorption and scattering processes in the visible/near-infrared frequency range. The experimental evidence is supported by a comprehensive theoretical study. We demonstrate that the physical mechanism responsible for the aforementioned effect lies in the different natures of the plasmonic modes excited within the hyperbolic meta-antennas. We prove that it is possible to have a pure scattering channel if an electric dipolar mode is induced, while a pure absorption process can be obtained if a magnetic dipole is excited. Also, by varying the geometry of the system, the relative weight of scattering and absorption can be tuned, thus enabling an arbitrary control of the decay channels. Importantly, both modes can be efficiently excited by direct coupling with the far-field radiation, even when the radiative channel (scattering) is almost totally suppressed, hence making the proposed architecture suitable for practical applications.

physics.app-ph↗

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 commercial 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. Nanopore

physics.app-ph↗

Tangramob: an agent-based simulation framework for validating urban smart mobility solutions

Estimating the effects of introducing a range of smart mobility solutions within an urban area is a crucial concern in urban planning. The lack of a Decision Support System (DSS) for the assessment of mobility initiatives, forces local public authorities and mobility service providers to base their decisions on guidelines derived from common heuristics and best practices. These approaches can help planners in shaping mobility solutions, but given the high number of variables to consider the effects are not guaranteed. Therefore, a solution conceived respecting the available guidelines can result in a failure in a different context. In particular, difficult aspects to consider are the interactions between different mobility services available in a given urban area, and the acceptance of a given mobility initiative by the inhabitants of the area. In order to fill this gap, we introduce Tangramob, an agent-based simulation framework capable of assessing the impacts of a Smart Mobility Initiative (SMI) within an urban area of interest. Tangramob simulates how urban traffic is expected to evolve as citizens start experiencing the newly offered traveling solutions. This allows decision makers to evaluate the efficacy of their initiatives taking into account the current urban system. In this paper we provide an overview of the simulation framework along with its design. To show the potential of Tangramob, 3 mobility initiatives are simulated and compared on the same scenario. This shows how it is possible to perform comparative experiments so as to align mobility initiatives to the user goals.

cs.MA↗

Cell membrane disruption by vertical nanopillars: the role of membrane bending and traction forces

Gaining access to the cell interior is fundamental for many applications, such as electrical recording, drug and biomolecular delivery. A very promising technique consists of culturing cells on nano/micro pillars. The tight adhesion and high local deformation of cells in contact with nanostructures can promote the permeabilization of lipids at the plasma membrane, providing access to the internal compartment. However, there is still much experimental controversy regarding when and how the intracellular environment is targeted and the role of the geometry and interactions with surfaces. Consequently, we investigated, by coarse-grained molecular dynamics simulations of the cell membrane, the mechanical properties of the lipid bilayer under high strain and bending conditions. We found out that a high curvature of the lipid bilayer dramatically lowers the traction force necessary to achieve membrane rupture. Afterwards, we experimentally studied the permeabilization rate of cell membrane by pillars with comparable aspect ratios but different sharpness values at the edges. The experimental data support the simulation results: even pillars with diameters in the micron range may cause local membrane disruption when their edges are sufficiently sharp. Therefore, the permeabilization likelihood is connected to the local geometric features of the pillars rather than diameter or aspect ratio. The present study can also provide significant contributions to the design of 3D biointerfaces for tissue engineering and cellular growth.

physics.bio-ph↗

Multiband Plasmonic Sierpinski Carpet Fractal Antennas

Deterministic fractal antennas are employed to realize multimodal plasmonic devices. Such structures show strongly enhanced localized electromagnetic fields typically in the infrared range with a hierarchical spatial distribution. Realization of engineered fractal antennas operating in the optical regime would enable nanoplasmonic platforms for applications, such as energy harvesting, light sensing, and bio/chemical detection. Here, we introduce a novel plasmonic multiband metamaterial based on the Sierpinski carpet (SC) space-filling fractal, having a tunable and polarization-independent optical response, which exhibits multiple resonances from the visible to mid-infrared range. We investigate gold SCs fabricated by electron-beam lithography on CaF$_{2}$ and Si/SiO$_{2}$ substrates. Furthermore, we demonstrate that such resonances originate from diffraction-mediated localized surface plasmons, which can be tailored in deterministic fashion by tuning the shape, size, and position of the fractal elements. Moreover, our findings illustrate that SCs with high order of complexity present a strong and hierarchically distributed electromagnetic near-field of the plasmonic modes. Therefore, engineered plasmonic SCs provide an efficient strategy for the realization of compact active devices with a strong and broadband spectral response in the visible/mid-infrared range. We take advantage of such a technology by carrying out surface enhanced Raman spectroscopy (SERS) on Brilliant Cresyl Blue molecules deposited onto plasmonic SCs. We achieve a broadband SERS enhancement factor up to $10^{4}$, thereby providing a proof-of-concept application for chemical diagnostics.

physics.optics↗

MIM Structure for optical vortex beam generator at nanoscale level

Optical beams carrying orbital angular momentum (OAM) can find tremendous applications in several fields. In order to apply these particular beams in photonic integrated devices innovative optical elements have been proposed. Here we are interested in the generation of OAM-carrying beams at the nanoscale level. We design and experimentally demonstrate a plasmonic optical vortex emitter, based on a metal-insulator-metal holey plasmonic vortex lens. Our plasmonic element is shown to convert impinging circularly polarized light to an orbital angular momentum state capable of propagating to the far-field. Moreover, the emerging OAM can be externally adjusted by switching the handedness of the incident light polarization. The device has a radius of few micrometers and the OAM beam is generated from subwavelength aperture. The fabrication of integrated arrays of PVLs and the possible simultaneous emission of multiple optical vortices provide an easy way to the large-scale integration of optical vortex emitters for wide-ranging applications.

physics.optics↗