Tesi di Dottorato
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Item Plasmon phenomena in graphene-related and beyond-graphene materials: a time-dependent density functional theory approach.Plasmon phenomena in graphene-related and beyond-graphene materials: a time-dependent density functional theory approach.(2017-02-24) Vacacela Gomez, Cristian Isaac; Pantano, Pietro; Sindona, AntonioItem Integration of mercury atmospheric models in a framework for interoperable workflow execution(2017-01-16) Boldrini, Enrico; Carbone, Vincenzo; Pirrone, Nicola; Nativi, StefanoItem Viaggio nel mondo dei quanti. Le avventure di Alice nel paese delle meraviglie(2014-11-12) Santopaolo, Valentina; Pantano, Pietro; Piperno, FrancescoL’era digitale, internet e la multimedialità hanno notevolmente modificato il modo in cui ragazzi e adolescenti fruiscono le informazioni, rispetto alla precedente generazione. Abbiamo di fronte degli individui, i nativi digitali, che hanno accesso giornaliero ai social network, agli smartphone, alle app, tutti ricchi di contenuti multimediali che implicano una propensione verso le immagini, la lettura veloce e il multitasking. Sono cresciuti con una minore capacità di attenzione verso il testo scritto e un’attenzione più spiccata verso l’immagine. Tutto ciò deve far riflettere sulla necessità di creare nuovi modelli e contenuti per la divulgazione scientifica, che siano più appropriati e si adeguino al nuovo modo di approcciarsi e fruire le informazioni. Il presente progetto propone un prodotto multimediale che comprende il fumetto, il libro illustrato e il CD interattivo come mezzo alternativo di comunicazione e insegnamento della fisica quantistica agli adolescenti, essendo questi contenuti molto prossimi ai modelli comunicativi che risultano familiari agli adolescenti. Contenuto del progetto è una storia, con un personaggio molto noto, Alice del celebre romanzo di Lewis Carroll, Alice's Adventures in Wonderland, protagonista di un viaggio “alternativo” rispetto a quello che ‘storicamente’ ha fatto. Un viaggio in un mondo popolato da elettroni, fotoni e scienziati impegnati a spiegare gli strani principi della fisica quantistica, che sembrano curiosi almeno quanto quelli del paese delle meraviglie.Item Optical trapping and manipulation exploiting liquid crystalline systems(2012-11-30) Hernandez, Raul Josue; Versace, Carlo; Cipparrone, GabriellaThis thesis and all the research contained within, pretends to develop new ideas and concepts on liquid crystals (LC) and optical trapping and manipulation. The combination between optical tweezers and LC systems promises unique and exciting results. The content on the thesis is presented for those with some experience in the elds of liquid crystal and optical manipulation, and for those who are interested in begin to learn about these matters, proposing an overview of much existing work and a correlation between di erent science branches like soft matter, photonics and optical control. Two main research lines has been developed involving liquid crystalline systems and polarized optical tweezers. In the rst part, nematic LC droplets in water have been adopted to study the mechanical properties of light elds with a polarization gradient, i.e. optical tweez- ers based on polarization holographic techniques with non conventional trapping in an extended interferometric optical trap. For this purpose, LC emulsions in wa- ter were prepared, obtaining droplets with radial or bipolar director con guration, which result in optically isotropic or anisotropic particles. Exploiting the vecto- rial nature of the light and its interaction with LC droplets, an unconventional opto-hydrodynamical control and trapping has been demonstrated. The planned experiments shown that a hydrodynamic force, known as Magnus force, never con- sidered in optical micromanipulation experiments, can play an important role in the optical micromanipulation and should be considered whenever particles are forced to spin and dragged in a uid. In the second part, the study was mainly focused into developing an innovative and versatile soft matter object, namely chiral-solid microspheres. They were created by combining very simple self-assembling and photoinduced processes of the soft mat- ter, i.e. photopolymerizing cholesteric LC droplets in water emulsion. The ability to control the internal helical geometry using chemical agents in the precursor LC emulsion enables to obtain solid microspheres with radial, conical, or cylindrical con gurations of the helical structures that exhibit unique optical properties. Their exclusive capabilities were demonstrated by optical manipulation experiments in- volving optical tweezers. A unique and dichotomous behavior has been revealed by polarized circularly polarized tweezers: an attractive or repulsive optical force is ex- erted by varying the light polarization. Moreover, the application of the chiral-solid microspheres as optical microresonators for creating microlasers was also demon- strated. The high performance as well as the novel and exclusive properties make these chiral microparticles good candidates for developing new concepts in colloidal materials science, microphotonics, microlasers, optical trapping and manipulation, micro- and opto uidics and microsensors.Item Electronic Excitations ofGraphene, Graphene Nickel interfaces, and Carbon Nanotubes(2012-11-30) Pisarra, Michele; Riccardi, Pierfrancesco; Fiore, RobertoItem A Lévy Walk approach to the propagation of solar energetic particles(2013-11-26) Trotta, Enrico Maria; Bertolini, Roberto; Zimbardo, GaetanoThis thesis is dedicated to the problem of energetic particle propagation in the solar wind, with special emphasis on the propagation of solar energetic particles (SEPs). Those particles are accelerated either in the low corona by flares, usually giving rise to so-called impulsive SEP events, or in the higher corona by the shock driven by coronal mass ejections, giving rise to the so-called gradual SEP events. In either case, energetic particles propagate in the solar wind along the spiral magnetic field, and then reach the Earth’s environment, where they can intensify the auroral emission and downgrade or even damage spacecraft operations. Indeed, SEPs represent one of the major hazards of the research programme known as space weather, which aims at reducing the risks associated with the solar and space activities. The fluxes of energetic particles measured in the Earth’s environment depend both on the source strength and on the propagation properties. Traditionally, two limiting transport regimes are considered, that is, di usive transport and scatter-free, i.e., ballistic, transport. However, in the last two decades, anomalous transport regimes in which the mean square displacement grows nonlinearly with time have become more and more common. An anomalous transport regime, either subdi usive or superdi usive, would influence in a fundamental way the flux of solar energetic particles reaching the Earth. To study this problem we have developed two approaches, one based on the analysis of SEP fluxes measured by spacecraft in the solar wind, and the other on the numerical simulation of SEPs in the case of superdi usive transport. In the first approach, we considered SEPs measurements by ACE, Wind and other spacecraft for the case o mpulsive SEP events, and compared the time profile of the energetic particles with that corresponding to the di erent forms which the propagator assumes in the case of superdi usive transport. The comparison gives direct information on the transport regime, showing that electrons propagate in a superdi usive way with anomalous di usion exponent alpha running from 1.2 to 1.75. For protons, quasi-ballistic transport regimes are also found. In the second approach, the statistical mechanism giving rise to superdi usion, namely the Lévy random walk, is investigated numerically. We developed a new numerical code which simulates the Lévy walk while changing the parameters which determine the pace of transport, that is the exponent of the power law tails of the jump probability distribution. This code reproduces well the anomalous transport predictions for the mean square displacement and for the propagator of Lévy walks, while allowing a clear and simple identification of the parameters determining the transport regime. Therefore this code represents a powerful tool to compare the simulation results to spacecraft data. Comparison with the data has been considered both for impulsive and gradual SEP events. In this thesis, we show that the numerical code reproduces well the observations o mpulsive events for the various transport regimes. Additional work is required to apply the code to the propagation of gradual SEP events, as modeling of the shock source is required. While this will be implemented in the near future, the e ectivitiy of the numerical code will allow an important improvement in the understanding of SEP propagation and in the prediction of space weather perturbationsItem Air quality and pollutant modelling in the mediterranean regionDocumenti elettronici(2013-11-11) Gengarelli, Christian Natale; Bertolini, Roberto; Pirrone, Nicola; Carbone, Vincenzo; Hedgecock, MichaelL'inquinamento atmosferico viene de nito come la presenza di sostanze che possono avere e etti dannosi sulla salute umana o sull'intero sistema ambientale (EC, 2008), causando e etti misurabili sugli animali, sulla vegetazione e sui diversi materiali. Queste sostanze, dette inquinanti, usualmente non sono presenti nella normale composizione atmosferica o lo sono ma a concentrazioni estremamente basse. Tra i pi u pericolosi inquinanti presenti in atmosfera c' e il mercurio (Hg), un inquinante globale sotto controllo soprattutto negli ultimi anni (UNEP, 2013b; Mason et al., 2012; Driscoll et al., 2013) in quanto provoca gravi e etti nocivi sulla salute umana. Elevate concentrazioni di mercurio negli ecosistemi sono causate dalle emissioni dirette, ma anche da reazioni chimiche che avvengono in atmosfera e dalle condizioni meteorologiche che, governate dalla sica dell'atmosfera, regolano la distribuzione, il trasporto e la deposizione del mercurio. Per individuare le cause delle elevate concentrazioni di inquinanti in atmosfera e necessaria un adeguata rete di monitoraggio, ma e molto complicato coprire vaste aree geogra che con stazioni di misura. Diviene dunque necessario ricorrere a modelli matematici che simulano le condizioni atmosferiche dal punto di vista sia meteorologico che chimico, in modo da ottenere i fattori sui quali e possibile intervenire per migliorare la qualit a dell'aria. Questo lavoro di tesi mostra lo sviluppo di un modello regionale online che simula il ciclo atmosferico del mercurio, in modo da valutare ed identi care le relazioni tra sorgenti e recettori a scala regionale e gli andamenti temporali degli scenari di emissione di mercurio attuali e futuri. Il risultato e una versione ampliata del modello numerico per la chimica ed il trasporto atmosferico WRF/Chem (modello Weather Research and Forecasting per la meteorologia integrato con la chimica atmosferica, Grell et al. (2005)), che pu o simulare il ciclo atmosferico del mercurio online. Questa versione del modello e in grado di riprodurre i campi di concentrazione ed i ussi di deposizione del mercurio a scala regionale, includendo le emissioni da sorgenti sia antropogeniche che naturali e simulando le interazioni e le reazioni chimiche che avvengono in atmosfera, nonch e i processi di deposizione. Per lo sviluppo di questo modello e stato necessario indagare i diversi aspetti della chimica del mercurio, analizzando ed implementando le interazioni con gli altri gas presenti in atmosfera, con la radiazione solare, con il vapore acqueo e con la pioggia; queste interazioni regolano i processi di ossidazione, riduzione e deposizione del mercurio. Inoltre sono stati implementati nel modello i processi di emissione da parte di sorgenti antropiche e naturali, parametrizzando le emissioni di mercurio dovute agli incendi boschivi e l'evasione di mercurio nell'interfaccia atmosfera - super ce del mare. Oltre alle deposizioni di mercurio da parte delle piogge (deposizione wet) sono stati implementati i meccanismi per deposizione al suolo dovuta alla forza gravitazionale ed ai moti atmosferici (deposizione dry). Il modello e in grado di riprodurre la variazione stagionale delle concentrazioni di mercurio, rappresentando adeguatamente anche gli andamenti di HgII e HgP nello strato atmosferico al limite con la super ce del Mar Mediterraneo (Mediterranean MBL). La medie annuali delle deposizioni di mercurio wet e dry modellate sono simili, ma con di erente distribuzione spaziale: la deposizione wet domina nelle zone umide mentre la deposizione dry e maggiore vicino alle sorgenti di emissione. Comparando le deposizioni con l'evasione di mercurio dalla super ce del mare risulta che il Mar Mediterraneo e una sorgente di mercurio per tutta l'area, con circa 70Mg di mercurio emessi in un anno. I risultati suggeriscono inoltre che nel MBL Mediterraneo il Bromo e un importante ossidante del mercurio. Il modello WRF/Chem e stato inizialmente usato per investigare la produzione fotochimica di un importante costituente atmosferico che in uenza il ciclo del mercurio nell'area del Mar Mediterraneo, l'ozono troposferico (O3). Oltre ad in uenzare il ciclo del mercurio, l'ozono e anche un pericoloso inquinante: elevate concentrazioni di ozono in prossimit a del suolo sono infatti dannose sia per la salute umana che per la produzione agricola. L'analisi modellistica dell'inquinamento da ozono troposferico mostra una forte in- uenza delle emissioni prodotte dalle navi che transitano nel Mar Mediterraneo, stimando il loro contributo in circa il 10{20% delle concentrazioni di ozono nelle aree continentali.Item Active plasmonics in soft matter doped with gold nanoparticles plasmonica attiva in materia soffice drogata con nanoparticelle d'oro(2013-11-29) Cataldi, Ugo; Bartolino, Roberto; Caputo, Roberto; Versace, Carlo C.The main objective of this study is active plasmonics. The work has been focussed on the design, characterization and theoretical interpretation of novel systems. Top-down and bottom-up, self-assembling, approaches have been utilized to realize devices where spherical gold nanoparticles have been periodically and randomly arranged. Two main paths have been followed to achieve this goal. In the first one, by utilizing a rigid periodic structure as a host platform for soft-matter (cholesteric liquid crystals) mixed with plasmonic nano-entities, was possible to obtain a chirally-organized tuneable plasmonic system. The tunability of the obtained device has been induced by applying temperature changes or external electric fields. In the second one, the surface of an elastomeric platform has been randomly covered by gold-nanoparticles. Controlled nano-chemistry processes have been successively applied to the nanoparticles (immobilized on the surface) to locally increase their size. The elastic properties of the template together with the increased size of particles have allowed a systematic study of the coupling between near-fields of the spherical nanostructures. Colloidal nano-chemistry technics have been utilized both to synthetize spherical gold nano-particles and to increase their sizes. Spectroscopic analysis has been used to analyse the response of obtained structures under electrical, thermodynamical and mechanical stimuli. SEM and TEM imaging have been exploited to study the morphology of devices, the shape of nano-structures and to measure their sizes. Moreover, from SEM images, through the use of a MatLab code written to the purpose, it has been possible to extract fundamental parameters used to perform a theoretical analysis of experimental resultsItem Synthesis and characterization of enstatite and talc doped with zinc and manganese(2013-11-11) Catalano, Manuela; Bartolino, Roberto; Cazzanelli, Enzo; Versace, Carlo C.; Bloise, AndreaIn recent years, particular interest has been addressed by researchers in the synthesis and study of silicates such as enstatite MgSiO3 and talc Mg3Si4O10(OH)2. The first one is useful for several technological applications such as substrates in electronics, high frequency insulators, thermal insulators in high temperatures applications, and as luminescent materials in laser technology. The latter, because of the low cost and good properties (i.e. resistant to heat and acids, hydrophobic, electrical insulating) is widely used in many different products such as ceramics, papers, cosmetics, foods, polymers and filler in composites. The usual presence of foreign ions (e.g., Mn, Ti, Ni, etc.) and their inconstant amounts in natural enstatite and talc hinder the use of these minerals as high-performance materials. For these reasons, in recent years pure and doped enstatite and talc have been grown and characterized in several different ways. Nevertheless, there are still various problems to be solved in order to obtain very high quality crystals and the desired changes in the physical and chemical properties of them when they are doped with metal elements. In this work, Zn-doped enstatite, Mn-doped enstatite, Zn-doped talc and Mn-doped talc have been grown and characterized with different techniques. The starting materials and the final products were characterized and studied by binocular microscope, powder crystal X-ray diffraction (XRPD), scanning electron microscopy with energy-dispersive spectrometry (SEM/EDS), single-crystal X-ray diffraction (XRD), micro-Raman (μ-R), cathodoluminescence (CL), differential scanning calorimetry, thermogravimetric analysis (DSC-TG) and Fourier transform infrared spectroscopy (FT-IR). Zn- and Mn-doped enstatite was successfully produced by slow-cooling flux growth method, using MoO3, V2O5, Li2CO3 as melting agent. Several starting mixtures, with different MnO or ZnO concentrations, were first held at 1350 °C, 1250 °C 1050 °C and 950 °C and then slowly cooled down to 700 °C or 600 °C with different cooling rate (3.75 °C/h, 2.1 °C/h, 1.8 °C/h 1.7 °C/h). Enstatite crystallizes in the orthorhombic and monoclinic systems as revealed by XRD and Raman spectra. Transparent Zn-doped enstatite ( max length of 3.5 mm) and reddish Mn-doped enstatite (max length of 8 mm) single crystals are euhedral in form, not homogeneous in width and inclusion free. Maximum content of Mn-dopant is 14.52 wt %, while the maximum amount of Zn-dopant is 10.49 wt%. Crystals grow under equilibrium conditions only when the dopant content is maintained at low value. When either Zn or Mn is totally substituted for Mg in the starting material, no enstatite is produced. The presence of the dopant in the enstatite structure causes a decrease in unit cell volume respect to the pure one and strongly affects the CL-signal and micro-Raman spectra. CL spectrum of Mn-doped enstatite contains a broad emission located at 677 nm and attributed to the 4T1g(G)→6A1g(S) transition of octahedral Mn2+ centres. The presence of Zn in enstatite induces very remarkable peak broadening by the mode at 133 cm-1 and 343 cm-1 in the Raman spectra; for these modes a strong component of metal ion displacement must be postulated. Raman spectra of Mn-enstatite show: i) a general decrease of Raman intensity due to the increase in surface reflection when the MnO dopant concentration increases; ii) a widening and a down shifting of the peak positions indicating changes in vibrational modes because of the increasing presence of MnO. Zn- and Mn-doped talc was successfully synthesized in hydrothermal conditions at temperatures of 300, 500 and 650 °C, under constant pressure of 2 kbar and reaction time of 160 hours. Talc morphology and content of dopant within the crystals show strong dependence on crystallization temperature. Talc exhibits a cabbage-like morphology, its classical hexagonal tabular morphology and fibrous morphology. The best temperature to obtain the highest abundance of Zn- and Mn-doped talc is 650 °C. A decrease in temperature from 650 to 300 °C: i) worsens the reactions and poorly crystallized Zn- and Mn-doped talc is obtained; ii) increases the content of zinc or manganese dopant. Talc only grows when Mg is not totally substituted by either zinc or manganese in the starting mixture. Zn-doped talc formation is increased by treating the starting mixture with H2O + HCl; conversely, the reactant H2O + CaCl2 inhibits the growth of talc. In order to increase doped talc yield, large amounts of aqueous solution is as crucial as high temperatures. The presence of varying amounts of metal elements replacing Mg in talc influences its temperature decomposition. Indeed, the thermal stability of Zn- and Mn-doped talc decreases with respect to pure one. Zn-dopant in talc mainly affected the hydroxyl stretching fundamental peak (3674 cm-1), splitting itself into as many as four peaks with respect to non-doped talc, which displayed only a sharp band. The splitting appears to be dependent on the degree of substitution of the magnesium in the octahedral layer and related to the electronegativity difference between Zn and Mg. Future studies will be carried out on these materials to have a better knowledge of other physical properties, useful in novel applications.Item Periodic and aperiodic structures realized by innovative soft-metter based techniques(2014-05-19) Infusino, Melissa; Umeton, Cesare; Agostino, Raffaele; Falcone, GiovanniIl presente lavoro di tesi `e basato sullo studio e l’utilizzo di tecniche sperimentali per la realizzazione di strutture periodiche ed a-periodiche su diverse scale di grandezza. La prima tecnica oggetto di studio rappresenta un nuovo approccio rispetto alle usuali tecniche olografiche e prevede l’utilizzo delle pi`u recenti tecnologie realizzate nell’ambito dell’olografia diffrattiva, quali i modulatori di fase spaziale. I modulatori di fase spaziale consentono la produzione di distribuzioni di intensit`a sia periodiche che a-periodiche ed in generale rendendo possibili geometrie difficilmente realizzabili con le classiche tecniche di interferenza a multi-fascio. Il sistema fotosensibile di partenza `e costituito da una miscela di pre-polimeri e cristalli liquidi nematici: la separazione di fase tra le due componenti `e indotta dalla fotopolimerizzazione. L’impiego dei cristalli liquidi consente la realizzazione di strutture dinamiche le cui propriet`a ottiche sono modificabili attraverso l’applicazione di stimoli esterni, quali campi elettrici ed ottici. Le strutture relizzate hanno una periodicit`a micrometrica che le rende applicabili nel campo dell’ottica. La seconda tecnica studiata si basa su fenomeni di auto-assemblaggio nei polimeri a blocchi e consente il raggiungimento di scale di grandezza inferiori: la periodicit`a delle strutture realizzate raggiunge infatti poche decine di nanometri. Nella tecnica di autoassemblaggio la separazione di fase tra le componenti `e regolata semplicemente dalla temperatura del sistema e le strutture risultanti hanno delle caratteristiche fortemente dipendenti dalle dimensioni dei costituenti. 3