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90 result(s) for "Garoli, Denis"
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SERS discrimination of single DNA bases in single oligonucleotides by electro-plasmonic trapping
Surface-enhanced Raman spectroscopy (SERS) sensing of DNA bases by plasmonic nanopores could pave a way to novel methods for DNA analyses and 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. In fact, DNA molecules flow through the nanopores so rapidly that the SERS signals collected are not sufficient for single-molecule analysis. Here, we report an approach to control the residence time of molecules in the hot spot by an electro-plasmonic trapping effect. By directly adsorbing molecules onto a gold nanoparticle and then trapping the single nanoparticle in a plasmonic nanohole up to several minutes, we demonstrate single-molecule SERS detection of all four 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. Sensing DNA bases by surface-enhanced Raman spectroscopy (SERS) in plasmonic nanopores has suffered from rapid flow through of molecules. Here, the authors attach DNA molecules to gold nanoparticles which, due to electro-plasmonic trapping, allow for controlled residence times and discrimination of single nucleotides.
Transmembrane voltage-gated nanopores controlled by electrically tunable in-pore chemistry
Gating is a fundamental process in ion channels configured to open and close in response to specific stimuli such as voltage across cell membranes thereby enabling the excitability of neurons. Here we report on voltage-gated solid-state nanopores by electrically tunable chemical reactions. We demonstrate repetitive precipitation and dissolution of metal phosphates in a pore through manipulations of cation flow by transmembrane voltage. Under negative voltages, precipitates grow to reduce ionic current by occluding the nanopore, while inverting the voltage polarity dissolves the phosphate compounds reopening the pore to ionic flux. Reversible actuation of these physicochemical processes creates a nanofluidic diode of rectification ratio exceeding 40000. The dynamic nature of the in-pore reactions also facilitates a memristor of sub-nanowatt power consumption. Leveraging chemical degrees of freedom, the present method may be useful for creating iontronic circuits of tunable characteristics toward neuromorphic systems. Ion channels in cell membranes open and close in response to electrical stimuli, playing a critical role in cellular signaling and homeostasis. Here, the authors show a similar gating functionality in solid-state nanopores, achieved through transmembrane voltage control of in-pore chemistry.
Ultrafast all-optical switching enabled by epsilon-near-zero-tailored absorption in metal-insulator nanocavities
Ultrafast control of light−matter interactions is fundamental in view of new technological frontiers of information processing. However, conventional optical elements are either static or feature switching speeds that are extremely low with respect to the time scales at which it is possible to control light. Here, we exploit the artificial epsilon-near-zero (ENZ) modes of a metal-insulator-metal nanocavity to tailor the linear photon absorption of our system and realize a nondegenerate all-optical ultrafast modulation of the reflectance at a specific wavelength. Optical pumping of the system at its high energy ENZ mode leads to a strong redshift of the low energy mode because of the transient increase of the local dielectric function, which leads to a sub-3-ps control of the reflectance at a specific wavelength with a relative modulation depth approaching 120%. All-optical switching allows control of one optical signal using another, holding potential to overcome the limitations of electrical switches via ultrafast manipulation of light. In this work, sub-3 ps all-optical switching is achieved in an epsilon-near-zero nanocavity, exhibiting a relative modulation depth of 120% at a specific wavelength.
Chemistry-driven autonomous nanopore membranes
Fabrication of pores at the atomic scale remains a significant challenge in modern nanotechnology, hindering the study of ion transport and molecular dynamics in confined spaces. Here, we introduce a chemically controllable break-membrane approach that enables the repeated formation and closure of nanoscale pores in SiN x membranes through manipulating the in-pore electrochemical reaction conditions by transmembrane voltage. Ionic current measurements reveal distinct conductance features that are consistent with ion dehydration and transport through highly confined channels approaching sub-nanometer dimensions. The scalable nature of this platform, which allows multiple pores to be actuated simultaneously, offers a powerful tool for probing ion transport and fluid dynamics in extreme confinement. Beyond advancing fundamental understanding of ion transport and fluid dynamics, this chemically driven membrane system holds promise for applications in single-molecule sensing, neuromorphic computing, and nanoreactor design. This study shows how a simple voltage can repeatedly open and close nanoscale pores in a solid membrane, revealing new ways to control ion flow at the atomic scale for advanced nanofluidic technologies.
Dependence of the damage in optical metal/dielectric coatings on the energy of ions in irradiation experiments for space qualification
Terrestrial accelerator facilities can generate ion beams which enable the testing of the resistance of materials and thin film coatings to be used in the space environment. In this work, a TiO 2 /Al bi-layer coating has been irradiated with a He + beam at three different energies. The same flux and dose have been used in order to investigate the damage dependence on the energy. The energies were selected to be in the range 4–100 keV, in order to consider those associated to the quiet solar wind and to the particles present in the near-Earth space environment. The optical, morphological and structural modifications have been investigated by using various techniques. Surprisingly, the most damaged sample is the one irradiated at the intermediate energy, which, on the other hand, corresponds to the case in which the interface between the two layers is more stressed. Results demonstrate that ion energies for irradiation tests must be carefully selected to properly qualify space components.
Metal-Modified Montmorillonite as Plasmonic Microstructure for Direct Protein Detection
Thanks to its negative surface charge and high swelling behavior, montmorillonite (MMT) has been widely used to design hybrid materials for applications in metal ion adsorption, drug delivery, or antibacterial substrates. The changes in photophysical and photochemical properties observed when fluorophores interact with MMT make these hybrid materials attractive for designing novel optical sensors. Sensor technology is making huge strides forward, achieving high sensitivity and selectivity, but the fabrication of the sensing platform is often time-consuming and requires expensive chemicals and facilities. Here, we synthesized metal-modified MMT particles suitable for the bio-sensing of self-fluorescent biomolecules. The fluorescent enhancement achieved by combining clay minerals and plasmonic effect was exploited to improve the sensitivity of the fluorescence-based detection mechanism. As proof of concept, we showed that the signal of fluorescein isothiocyanate can be harvested by a factor of 60 using silver-modified MMT, while bovine serum albumin was successfully detected at 1.9 µg/mL. Furthermore, we demonstrated the versatility of the proposed hybrid materials by exploiting their plasmonic properties to develop liquid label-free detection systems. Our results on the signal enhancement achieved using metal-modified MMT will allow the development of highly sensitive, easily fabricated, and cost-efficient fluorescent- and plasmonic-based detection methods for biomolecules.
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.
Adaptive nanopores: A bioinspired label-free approach for protein sequencing and identification
Single molecule protein sequencing would tremendously impact in proteomics and human biology and it would promote the development of novel diagnostic and therapeutic approaches. However, its technological realization can only be envisioned, and huge challenges need to be overcome. Major difficulties are inherent to the structure of proteins, which are composed by several different amino-acids. Despite long standing efforts, only few complex techniques, such as Edman degradation, liquid chromatography and mass spectroscopy, make protein sequencing possible. Unfortunately, these techniques present significant limitations in terms of amount of sample required and dynamic range of measurement. It is known that proteins can distinguish closely similar molecules. Moreover, several proteins can work as biological nanopores in order to perform single molecule detection and sequencing. Unfortunately, while DNA sequencing by means of nanopores is demonstrated, very few examples of nanopores able to perform reliable protein-sequencing have been reported so far. Here, we investigate, by means of molecular dynamics simulations, how a re-engineered protein, acting as biological nanopore, can be used to recognize the sequence of a translocating peptide by sensing the “shape” of individual amino-acids. In our simulations we demonstrate that it is possible to discriminate with high fidelity, 9 different amino-acids in a short peptide translocating through the engineered construct. The method, here shown for fluorescence-based sequencing, does not require any labelling of the peptidic analyte. These results can pave the way for a new and highly sensitive method of sequencing.
Gated MoS2/SiN nanochannel for tunable ion transport and protein translocation
Ionic transport in nanofluidic channels holds great promise for applications such as single-molecule analysis, molecular manipulation, and energy harvesting. However, achieving precise control over ion transport remains a major challenge. In this work, we introduce a MoS 2 /SiN hybrid nanochannel architecture that enables electrical tuning of ionic transport via external gating, and we examine its potential for osmotic power generation and single-molecule detection. To fabricate the channels, we employed a combined focused ion beam (FIB) milling and dry transfer method, producing sub-10 nm thick structures while preserving the structural integrity and electronic properties of MoS 2 —essential for reliable surface charge modulation. We first investigated how the gate voltage influences ionic conductance, finding evidence of gate-dependent modulation of ion selectivity under different bias polarities, with a rectification ratio of up to 10 in 1 M KCl. Next, by applying a salt concentration gradient across the nanochannels, we demonstrated the feasibility of this platform for osmotic energy generation, achieving a maximum power output of ~ 18 pW from a single channel and ~ 144 pW and ~ 337 pW from 10-channels and 20-channels array, corresponding to a high power density of ~ 18 kW/m². Finally, we tested the system for single-molecule sensing, showing that linearized bovine serum albumin (BSA) produced translocation signals with notably long dwell times exceeding previous reports. Together, these results highlight gated MoS 2 /SiN nanochannels as a promising platform for tunable nanofluidics, with potential applications in controlled molecular transport and energy generation from osmotic gradients. Graphical Abstract
Morphology-modified contributions of electronic transitions to the optical response of plasmonic nanoporous gold metamaterial
Nanoporous metals have emerged as promising functional architectures with tunable optical and electronic properties, high surface areas, and applicability in sensing, catalysis, and biomedicine. While their linear optical behavior and morphological properties have been extensively studied, the electronic properties, and in particular how they are affected by morphology, remain not fully understood. Here we combine experimental and theoretical studies of electronic excitation and relaxation in a nanoporous gold metamaterial. Optical pump–probe experiments show slower electron relaxation dynamics compared to the continuous film, consistent with a higher transient electronic temperature and stronger smearing of the Fermi–Dirac distribution, well reproduced by an extended two-temperature model. Furthermore, cathodoluminescence measurements reveal broadband localized plasmon resonances, and atomistic simulations disentangle intra- and interband effects, demonstrating that nanoscale porosity fundamentally reshapes the electronic response. These findings support nanoporosity as a key design parameter for controlling steady-state and ultrafast optical behavior in plasmonic materials. Nanoporous metals offer the potential for tunability of electronic and optical properties. Here, the authors combine experimental studies and theoretical modeling to explore how nanoporous morphology shapes the intraband and interband contributions to the optical response of gold.