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1.
Nanoscale ; 12(2): 851-863, 2020 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-31830198

RESUMO

A detailed structural investigation of the semiconductor-to-metal transition (SMT) in vanadium dioxide thin films deposited on sapphire substrates by pulsed laser deposition was performed by in situ temperature-dependent X-ray diffraction (XRD) measurements. The structural results are correlated with those of infrared radiometry measurements in the SWIR (2.5-5 µm) and LWIR (8-10.6 µm) spectral ranges. The main results indicate a good agreement between XRD and optical analysis, therefore demonstrating that the structural transition from monoclinic to tetragonal phases is the dominating mechanism for controlling the global properties of the SMT transition. The picture that emerges is a SMT transition in which the two phases (monoclinic and tetragonal) coexist during the transition. Finally, the thermal hysteresis, measured for thin films with different thickness, showed a clear dependence of the transition temperature and the width of the hysteresis loop on the film thickness and on the size of the crystallites.

2.
Opt Express ; 27(17): 24260-24273, 2019 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-31510318

RESUMO

Active, ultra-fast external control of the emission properties at the nanoscale is of great interest for chip-scale, tunable and efficient nanophotonics. Here we investigated the emission control of dipolar emitters coupled to a nanostructure made of an Au nanoantenna, and a thin vanadium dioxide (VO2) layer that changes from semiconductor to metallic state. If the emitters are sandwiched between the nanoantenna and the VO2 layer, the enhancement and/or suppression of the nanostructure's magnetic dipole resonance enabled by the phase change behavior of the VO2 layer can provide a high contrast ratio of the emission efficiency. We show that a single nanoantenna can provide high magnetic field in the emission layer when VO2 is metallic, leading to high emission of the magnetic dipoles; this emission is then lowered when VO2 switches back to semiconductor. We finally optimized the contrast ratio by considering different orientation, distribution and nature of the dipoles, as well as the influence of a periodic Au nanoantenna pattern. As an example of a possible application, the design is optimized for the active control of an Er3+ doped SiO2 emission layer. The combination of the emission efficiency increase due to the plasmonic nanoantenna resonances and the ultra-fast contrast control due to the phase-changing medium can have important applications in tunable efficient light sources and their nanoscale integration.

3.
ACS Appl Mater Interfaces ; 10(46): 39512-39523, 2018 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-30359523

RESUMO

Implantable devices need specific tailored surface morphologies and chemistries to interact with the living systems or to actively induce a biological response also by the release of drugs or proteins. These customized requirements foster technologies that can be implemented in additive manufacturing systems. Here, we present a novel approach based on spraying processes that allow to control separately topographic features in the submicron range (∼60 nm to 2 µm), ammine or carboxylic chemistry, and fluorophore release even on temperature-sensitive biodegradable polymers such as polycaprolactone (PCL). We developed a two-steps process with a first deposition of 220 nm silica and poly(lactic- co-glycolide) (PLGA) fluorescent nanoparticles by aerosol followed by the deposition of a fixing layer by an atmospheric pressure plasma jet (APPJ). The nanoparticles can be used to create the nanoroughness and to include active molecule release, while the capping layer ensures stability and the chemical functionalities. The process is enabled by a novel APPJ which allows deposition rates of 10-20 nm·s-1 at temperatures lower than 50 °C using argon as the process gas. This approach was assessed on titanium alloys for dental implants and on PCL films. The surfaces were characterized by Fourier transform infrared, atomic force microscopy, and scanning electron microscopy (SEM). Titanium alloys were tested with the preosteoblast murine cells line, while the PCL film was tested with fibroblasts. Cell behavior was evaluated by viability and adhesion assays, protein adsorption, cell proliferation, focal adhesion formation, and SEM. The release of a fluorophore molecule was assessed in the cell growing media, simulating a drug release. Osteoblast adhesion on the plasma-treated materials increased by 20% with respect to commercial titanium alloy implants. Fibroblast adhesion increased by a 100% compared to smooth PCL substrates. The release of the fluorophore by the dissolution of the PLGA nanoparticles was verified, and the integrity of the encapsulated drug model was confirmed.


Assuntos
Liberação Controlada de Fármacos , Poliésteres/química , Copolímero de Ácido Poliláctico e Ácido Poliglicólico/química , Próteses e Implantes , Dióxido de Silício/química , Células 3T3 , Aerossóis/química , Ligas/química , Animais , Argônio , Materiais Biocompatíveis/química , Adesão Celular , Linhagem Celular , Sistemas de Liberação de Medicamentos , Fibroblastos/citologia , Humanos , Camundongos , Microscopia de Força Atômica , Microscopia Eletrônica de Varredura , Nanopartículas , Osteoblastos/citologia , Gases em Plasma , Espectroscopia de Infravermelho com Transformada de Fourier , Propriedades de Superfície , Temperatura , Titânio/química
4.
Sci Rep ; 8(1): 13811, 2018 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-30218048

RESUMO

The laser-induced plasmon heating of an ordered array of silver nanoparticles, under continuous illumination with an Ar laser, was probed by rare-earth fluorescence thermometry. The rise in temperature in the samples was monitored by measuring the temperature-sensitive photoluminescent emission of a europium complex (EuTTA) embedded in PMMA thin-films, deposited onto the nanoparticles array. A maximum temperature increase of 19 °C was determined upon resonant illumination with the surface plasmon resonance of the nanoarray at the highest pump Ar laser power (173 mW). The experimental results were supported by finite elements method electrodynamic simulations, which provided also information on the temporal dynamics of the heating process. This method proved to be a facile and accurate approach to probe the actual temperature increase due to photo-induced plasmon heating in plasmonic nanosystems.

5.
Nanoscale ; 10(11): 5182-5190, 2018 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-29492500

RESUMO

In this work we present the study of the ultra-fast dynamics of the nonlinear optical response of a honeycomb array of silver triangular nanoprisms, performed using a femtosecond pulsed laser tuned with the dipolar surface plasmon resonance of the nanoarray. Nonlinear absorption and refraction, and their time-dependence, were explored using the z-scan and time-resolved excite-probe techniques. Nonlinear absorption is shown to change sign with the input irradiance and the behavior was explained on the basis of a three-level model. The response time was determined to be in the picosecond regime. A technique based on a variable frequency chopper was also used in order to discriminate the thermal and electronic contributions to the nonlinearity, which were found to have opposite signs. All these findings propel the investigated nanoprism arrays as good candidates for applications in advanced ultra-fast nonlinear nanophotonic devices.

6.
Materials (Basel) ; 10(7)2017 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-28773075

RESUMO

One fundamental requirement in the search for novel magnetic materials is the possibility of predicting and controlling their magnetic anisotropy and hence the overall hysteretic behavior. We have studied the magnetism of Au:Co films (~30 nm thick) with concentration ratios of 2:1, 1:1, and 1:2, grown by magnetron sputtering co-deposition on natively oxidized Si substrates. They consist of a AuCo ferromagnetic alloy in which segregated ultrafine Co particles are dispersed (the fractions of Co in the AuCo alloy and of segregated Co increase with decreasing the Au:Co ratio). We have observed an unexpected hysteretic behavior characterized by in-plane anisotropy and crossed branches in the loops measured along the hard magnetization direction. To elucidate this phenomenon, micromagnetic calculations have been performed for a simplified system composed of two exchange-coupled phases: a AuCo matrix surrounding a Co cluster, which represents an aggregate of particles. The hysteretic features are qualitatively well reproduced provided that the two phases have almost orthogonal anisotropy axes. This requirement can be plausibly fulfilled assuming a dominant magnetoelastic character of the anisotropy in both phases. The achieved conclusions expand the fundamental knowledge on nanocomposite magnetic materials, offering general guidelines for tuning the hysteretic properties of future engineered systems.

7.
Nanoscale ; 9(28): 10117-10125, 2017 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-28695942

RESUMO

Nanosphere lithography coupled with reactive ion etching has been used to synthesize hexagonal ordered arrays of Au-Ag bimetallic semi-nanoshells to be used as plasmonic biosensors. The degree of lateral interaction between adjacent semi-nanoshells can be controlled by tailoring the reactive ion etching time in order to boost the global plasmonic properties through the formation of near-field hot-spots, which in turn can improve the sensitivity of the biosensors. To test the efficiency of the proposed system as a biosensor, we used an established protocol for the detection of biomolecules (local sensitivity), based on the receptor-ligand approach and using the biotin-streptavidin model system. We also tested the sensitivity to a homogeneous change in the refractive index of the buffer over the sensor (bulk sensitivity). Comparing the obtained results to those of an array of nanoprisms, chosen as a benchmark, significantly higher performances both in local and bulk sensitivities have been found, in agreement with electrodynamics simulations based on finite-element methods.


Assuntos
Técnicas Biossensoriais , Ouro/química , Nanoconchas/química , Prata/química , Ressonância de Plasmônio de Superfície , Ligas
8.
Sci Rep ; 7(1): 5307, 2017 07 13.
Artigo em Inglês | MEDLINE | ID: mdl-28706203

RESUMO

Ordered metallic nanoprism arrays have been proposed as novel and versatile systems for the observation of nonlinear effects such as nonlinear absorption. The study of the effect of the local field reinforcement on the fast optical third order nonlinear response around the Surface Plasmon Resonance is of great interest for many plasmonic applications. In this work, silver nanoprism arrays have been synthesized by the nanosphere lithography method. A low repetition rate tunable picosecond laser source was used to study the irradiance and wavelength dependence of the nonlinear absorption properties around the dipolar and quadrupolar resonances of the nanoarray with the use of the z-scan technique. The irradiance dependence of the on-resonance nonlinearity was studied, and a spectral region where nonlinear absorption is negligible was identified. This is important for the possible application of these materials in optical information processing devices.

9.
Nanoscale ; 7(29): 12411-8, 2015 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-26129696

RESUMO

The nonlinear absorption properties of bidimensional arrays of Au-Ag bilayered nanoprisms have been investigated by z-scan measurements as a function of the bimetallic nanoprism composition. A tunable ps laser system was used to excite the ultrafast, electronic nonlinear response matching the laser wavelength with the quadrupolar surface plasmon resonances, in the visible range, of each nanoprism array. Due to the strong electromagnetic field confinement effects at the nanoprism tips, demonstrated by finite element method simulations, these nanosystems proved to have enhanced nonlinear optical properties. Moreover, a tunable changeover from reverse saturable absorption (RSA) to saturable absorption (SA) can be obtained by properly controlling the bimetallic composition of the nanoprisms, without modifying the overall morphology of the nanosystems. This capability makes these nanosystems extremely interesting for the realization of solid-state nanophotonic devices with enhanced ultrafast nonlinear optical properties.

10.
Nanoscale ; 7(19): 8968-77, 2015 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-25921415

RESUMO

The very early steps of Au metal cluster formation in Er-doped silica have been investigated by high-energy resolution fluorescence-detected X-ray absorption spectroscopy (HERFD-XAS). A combined analysis of the near-edge and extended part of the experimental spectra shows that Au cluster nucleation starts from a few Au and O atoms covalently interconnected, likely in the presence of embryonic Au-Au correlation. The first Au clusters, characterized by a well defined Au-Au coordination distance, form upon 400 °C inert annealing. The estimated upper limit of the Gibbs free energy for the associated heterogeneous nucleation is 0.06 eV per atom, suggesting that the Au nucleation is assisted by matrix defects, most likely non-bridging oxygen atoms. The experimental results indicate that the formed subnanometer Au clusters can be applied as effective core-shell systems in which the Au atoms of the 'core' develop a metallic character, whereas the Au atoms in the 'shell' can retain a partially covalent bond with O atoms of the silica matrix. High structural disorder at the Au site is found upon neutral annealing at a moderate temperature (600 °C), likely driven by the configurational disorder of the defective silica matrix. A suitable choice of the Au concentration and annealing temperature allows tailoring of the Au cluster size in the sub-nanometer range. The interaction of the Au cluster surface with the surrounding silica matrix is likely responsible for the infrared luminescence previously reported on the same systems.

11.
Phys Chem Chem Phys ; 17(42): 28262-9, 2015 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-25921085

RESUMO

The occurrence of a very efficient non-resonant energy transfer process forming ultrasmall Au-Ag nanoalloy clusters and Er(3+) ions is investigated in silica. The enhancement of the room temperature Er(3+) emission efficiency by an order of magnitude is achieved by coupling rare-earth ions to molecule-like (Au(x)Ag(1-x))N alloy nanoclusters with N = 10-15 atoms and x = 0.6 obtained by optimized sequential ion implantation on Er-implanted silica. For comparison, AuN nanoclusters obtained by the same approach and with the same size and numerical density showed an enhancement by only a factor of 2 with respect to pure Er emission, demonstrating the beneficial effect of using nanoalloyed clusters. The temperature evolution of the energy transfer process is investigated by photoluminescence and exhibits a maximum efficiency at about 600 °C, where the clusters reach the optimal size and the silica matrix completely recovers the implantation damage. The nanoalloy cluster composition and size have been studied by EXAFS analysis, which indicated a stronger Ag-O interaction with respect to the Au-O one and a preferential location of the Ag atoms at the nanoalloy cluster surface.


Assuntos
Ligas , Érbio/química , Ouro/química , Nanoestruturas , Teoria Quântica , Dióxido de Silício/química , Prata/química
12.
Biosens Bioelectron ; 65: 346-53, 2015 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-25461180

RESUMO

Plasmonic sensors based on ordered arrays of nanoprisms are optimized in terms of their geometric parameters like size, height, aspect ratio for Au, Ag or Au0.5-Ag0.5 alloy to be used in the visible or near IR spectral range. The two figures of merit used for the optimization are the bulk and the surface sensitivity: the first is important for optimizing the sensing to large volume analytes whereas the latter is more important when dealing with small bio-molecules immobilized in close proximity to the nanoparticle surface. A comparison is made between experimentally obtained nanoprisms arrays and simulated ones by using Finite Elements Methods (FEM) techniques.


Assuntos
Ligas/química , Ouro/química , Nanopartículas Metálicas/química , Prata/química , Ressonância de Plasmônio de Superfície/métodos , Análise de Elementos Finitos , Nanopartículas Metálicas/ultraestrutura , Refratometria
13.
Phys Chem Chem Phys ; 16(29): 15158-63, 2014 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-24935519

RESUMO

Sub-nanometric Au nanoclusters are known to act as very efficient sensitizers for the luminescent emission of Er(3+) ions in silica through a non-resonant broad-band energy-transfer mechanism. In the present work the energy-transfer process is investigated in detail by room temperature photoluminescence characterization of Er and Au co-implanted silica systems in which a different degree of coupling between Er(3+) ions and Au nanoclusters is obtained. The results allow us to definitely demonstrate the short-range nature of the interaction in agreement with non-radiative energy-transfer mechanisms. Moreover, an upper limit to the interaction length is also set by the Au-Au intercluster semi-distance which is smaller than 2.4 nm in the present case.

14.
ACS Appl Mater Interfaces ; 6(10): 7773-81, 2014 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-24750118

RESUMO

We report the achievement of sensitive gas detection using periodic silver nanoprisms fabricated by a simple and low-cost lithographic technique. The presence of sharp tips combined with the periodic arrangement of the nanoprisms allowed the excitement of isolated and interacting localized surface plasmon resonances. Specific sensing capabilities with respect to aromatic hydrocarbons were achieved when the metal nanoprism arrays were coupled in the near field with functional hybrid films, providing a real-time, label-free, and reversible methodology. Ultra-high-vacuum temperature-programmed desorption measurements demonstrated an interaction energy between the sensitive film and analytes in the range of 55-71 kJ/mol. The far-field optical properties and the detection sensitivity of the sensors, modeled using a finite element method, were correlated to experimental data from gas sensing tests. An absorbance variation of 1.2% could be observed and associated with a theoretical increase in the functional film refractive index of ∼0.001, as a consequence to the interaction with 30 ppm xylene. The possibility of detecting such a small variation in the refractive index suggests the highly promising sensing capabilities of the presented technique.

15.
Nanoscale ; 6(3): 1560-6, 2014.
Artigo em Inglês | MEDLINE | ID: mdl-24322302

RESUMO

The preparation of palladium alloy nanoparticles is of great interest for many applications, especially in catalysis. Starting from presynthesized nanoparticles of a less noble metal, a transmetallation reaction involving a redox process at the nanoparticle surface can be exploited to modify the nanoparticle composition and crystalline phase. As an example, monodispersed ε-cobalt and face-centered cubic copper nanoparticles were synthesized in organic solvents at high temperature and the as-formed nanoparticles were reacted with palladium(ii) hexafluoroacetylacetonate resulting in the formation of alloyed nanoparticles whose composition closely follows the reactant ratio. The oxidative state of the nanoparticle surface greatly affects the success of the transmetallation reaction and a reduction treatment was necessary to achieve the desired final product. Electron microscopy and X-ray diffraction showed that for cobalt a limiting palladium content for the ε-phase alloy is found, above which an fcc alloy nucleates, while for copper the fcc crystalline phase is preserved throughout the whole composition range.

16.
Nanoscale ; 6(3): 1716-24, 2014.
Artigo em Inglês | MEDLINE | ID: mdl-24343160

RESUMO

Ultra-small molecule-like AuN nanoclusters made by a number of atoms N less than 30 were produced by ion implantation in silica substrates. Their room temperature photoluminescence properties in the visible and near-infrared range have been investigated and correlated with the Er sensitization effects observed in Er-Au co-implanted samples. The intense photoluminescence emission under 488 nm laser excitation occurs in three different spectral regions around 750 nm (band A), 980 nm (band B) and 1150 nm (band C) as a consequence of the formation of discrete energy levels in the electronic structure of the molecule-like AuN nanoclusters. Indeed, energy maxima of bands A and C scale with N(-1/3) as expected for quantum confined systems. Conversely, the energy maximum of band B appears to be almost independent of size, suggesting a contribution of electronic surface states. A clear correlation between the formation of band B in the samples and Er-related photoemission is demonstrated: the band at 980 nm related to AuN nanoclusters resonant with the corresponding Er(3+) absorption level, is suggested as an effective de-excitation channel through which the Au-related photon energy may be transferred from Au nanoclusters to Er ions (either directly or mediated by photon absorption), eventually producing the Er-related infrared emission at 1540 nm.

17.
Nano Lett ; 13(10): 4785-9, 2013 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-24050533

RESUMO

The quest for efficient ways of modulating localized surface plasmon resonance is one of the frontiers in current research in plasmonics; the use of a magnetic field as a source of modulation is among the most promising candidates for active plasmonics. Here we report the observation of magnetoplasmonic modes on colloidal gold nanoparticles detected by means of magnetic circular dichroism (MCD) spectroscopy and provide a model that is able to rationalize and reproduce the experiment with unprecedented qualitative and quantitative accuracy. We believe that the steep slope observed at the plasmon resonance in the MCD spectrum can be very efficient in detecting changes in the refractive index of the surrounding medium, and we give a simple proof of principle of its possible implementation for magnetoplasmonic refractometric sensing.


Assuntos
Técnicas Biossensoriais , Dicroísmo Circular , Nanopartículas Metálicas/química , Coloides/química , Ouro/química , Campos Magnéticos , Refratometria
18.
Nanoscale ; 4(19): 5972-9, 2012 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-22907103

RESUMO

Metal (Au, Pt, Au@Pt) and metal oxide (TiO(2)) nanoparticles are synthesized with colloidal techniques and subsequently used as nanocrystal inks for thin films deposition. The optical properties of Au colloids are strongly influenced by both Pt and TiO(2) interfaces: while platinum causes a damping and a blue-shift of the Au Surface Plasmon Resonance (SPR) peak as a consequence of the metal-metal interaction, the anatase matrix is responsible for the red shift of the plasmon frequency due to the increased refractive index. By a careful tailoring of the nanoparticles synthesis, high quality, scattering-free films composed of an anatase matrix embedding Au, Pt and Au@Pt colloids are deposited at room temperature and stabilized at 200 °C. Room temperature exposure of these films to hydrogen leads to optical changes. In the case of Au, there is a slow blue shift of the surface plasmon band, resulting in a wavelength dependent optical response. Much faster but smaller optical changes occur for titania films containing Pt. When both metals are present, the optical response of the gold is much faster. This is attributed to spillover of hydrogen atoms from platinum to gold. This synergy enables enhanced optical sensing of hydrogen at room temperature by combining the low temperature dissociation of H(2) on Pt with the intensive surface plasmon response of the gold nanocrystals.


Assuntos
Ouro/química , Hidrogênio/análise , Platina/química , Ressonância de Plasmônio de Superfície , Titânio/química , Nanopartículas Metálicas/química , Nanopartículas Metálicas/ultraestrutura , Temperatura
19.
Opt Lett ; 36(7): 1203-5, 2011 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-21479030

RESUMO

We have developed an Ir/Si multilayer for extreme ultraviolet (EUV) applications. Normal incidence reflectance measurements of a prototype film tuned to 30 nm wavelength show superior performance relative to a conventional Mo/Si multilayer structure; we also find good stability over time. Transmission electron microscopy and electron dispersive x-ray spectroscopy have been used to examine the microstructure and interface properties of this system: we find amorphous Si layers and polycrystalline Ir layers, with asymmetric interlayer regions of mixed composition. Potential applications of Ir/Si multilayers include instrumentation for solar physics and laboratory EUV beam manipulation.

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