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This thesis presents the design of multifunctional structures through the optimal placement of nanomaterial additives. Varying the concentration of Carbon Nanotubes (CNTs) in a polymer matrix affects its local effective properties, including mechanical stiffness, electrical conductivity, and piezoresistivity. These local properties in turn drive global multifunctional performance objectives. A topology optimization algorithm determines the optimal distribution of CNTs within an epoxy matrix in an effort to design a set of structures that are capable of performing some combination of mechanical, electrical, or peizoresistive functions. A Pareto-Based Restart Method is introduced and may be used within a multi-start gradient based optimization to obtain well defined multiobjective Pareto Fronts. A linear design variable filter is used to limit the influence of checkerboarding. The algorithm is presented and applied to the design of beam cross-sections and 2D plane stress structures. It is shown that tailoring the location of even a small amount of CNT (as low as 2 percent and as high as 10 percent, by volume) can have significant impact on stiffness, electrical conductivity, and strain-sensing performance. Stiffness is maximized by placing high concentrations of CNT in locations that either maximize the bending rigidity or minimize stress concentrations. Electrical conductivity is maximized by the formation of highly conductive paths between electrodes. Strain-sensing is maximized via location of percolation volume fractions of CNTs in high strain areas, manipulation of the strain field to increase the strain magnitude in these areas, and by avoiding negative contributions of piezoresistivity from areas with differing net signed strains. It is shown that the location of the electrodes can affect sensing performance. A surrogate model for simultaneous optimization of electrode and topology is introduced and used to optimize a 2D plane stress structure. This results in a significant increase in sensing performance when compared to the fixed-electrode topology optimization. / Ph. D. / This dissertation presents a method that allows for the best placement of a limited amount of filler material within a base matrix material to form an optimal composite structure. Adding filler material, in this case Carbon Nanotubes, can change the effective behavior of the composite structure, enhancing the capabilities of the base matrix material by adding structural stiffness, electrical conductivity, and even the ability for the structure to measure its own strains. The degree to which these changes occur is dependent on the amount of filler material present in any given subsection of the structure. The method then is focused on determining how much of the filler to place in different subsections of the structure to maximize several measures of performance. These measures pertain to structural performance, electrical conductivity, and the structure’s ability to sense strains. Steps are taken within the method to remove non-physical designs and also to find the overall best design, called the global minima. The method is applied to several test structures of varying complexity, and it is shown that the optimization method can heavily influence performance by tailoring the filler material distribution. Further electrical and sensing performance gains can be obtained by properly selecting where the electrodes are located on the structure. This is demonstrated by including electrode placement in the design method along with the filler distribution.

Chemically and physically patterned surfaces can be used as templates to guide nano- and micro- scale particle assembly, but the design is often limited by an inability to sufficiently characterize how pattern features influence local particle-surface interactions on the order of thermal energy, kT. The research outlined in this dissertation describes comprehensive optical microscopy (i.e. evanescent wave, video) measurements and analyses of many-body and multi-dimensional interactions, dynamics and structure in inhomogeneous colloidal fluid systems. In particular, I demonstrate how non-intrusive observation of an ensemble of particles diffusing past each other and over a physically patterned surface topography can be used to obtain sensitive images of energy landscape features. I also link diffusing colloidal probe dynamics to energy landscape features, which is important for understanding the temporal imaging process and self-assembly kinetics. A complementary effort in this dissertation investigated the use of external AC electric fields to reversibly tune colloidal interactions to produce metastable ordered configurations. In addition, the electrical impedance spectra associated with colloidal assemblies formed between interfacial microelectrode gaps was measured and consistently modelled using representative equivalent circuits. Significant results from this dissertation include the synergistic use of the very same colloids as both imaging probes and building blocks in feedback controlled selfassembly on patterns. Cycling the AC field frequencies was found to be an effective way to anneal equilibrium colloidal configurations. Quantitative predictions of dominant transport mechanisms as a function of AC electric field amplitude and frequency were able to consistently explain the steady-state colloidal microstructures formed within electrode gaps observed using video microscopy. A functional electrical switch using gold nanoparticles was realized by reversibly forming and breaking colloidal wires between electrode gaps. Extension of the concepts developed in this dissertation suggest a general strategy to engineer the assembly of colloidal particles into ordered materials and controllable devices that provide the basis for numerous emerging technologies (e.g. photonic crystals, nanowires, reconfigurable antennas, biomimetic materials).

L’ingénierie tissulaire vise à régénérer des organes ou des tissus lésés. Ainsi, les gels de fibrine sont largement utilisés pour la reconstruction de différents tissus. Cependant, à concentration physiologique, ils ne peuvent pas être manipulés. Pour améliorer leurs propriétés mécaniques, ils peuvent être combinés dans une architecture de Réseaux Interpénétrés de Polymères (RIP) à un réseau de polymère synthétique (PVA ou POE). Ces RIPs peuvent être rendus biodégradables en copolymérisant d’albumine bovine de sérum modifiée par des groupements méthacrylate (BSAm) avec le partenaire synthétique.Selon leurs compositions, ces matériaux peuvent être complètement dégradés ou fragmentés après quelques jours en présence de thermolysine, une enzyme protéolytique. Ces cinétiques de dégradation de ces RIPs ont été étudiées en suivant le relargage des fragments protéiques hors du matériau, d’une part, et la diminution de leurs propriétés viscoélastiques, d’autre part. Leur biocompatibilité a été vérifiée : des fibroblastes cultivés à leur surface présentent une viabilité supérieure à 90% après 5 semaines de culture et leur prolifération est suivie de la synthèse de macromolécules de la Matrice Extracellulaire.Afin de leur ajouter une action bactéricide et d’augmenter encore leur résistance mécanique, des sels d’ammonium ont également été incorporés à certains de ces RIPs. Enfin, la synthèse de tels RIP a été mise au point à partir de plasma sanguin. Les éventuels phénomènes de rejet lors de leur intégration au sein du corps devraient ainsi être limités. De plus, le plasma sanguin contenant un grand nombre de facteurs de croissance et de molécules bioactives, la réparation tissulaire devrait ainsi être améliorée. / Tissue engineering aims to regenerate deficient tissues and organs. Fibrin gels are widely used for the reconstruction of various tissues. However, at physiological concentration, they can’t be handled. To improve their mechanical properties, they can be combined with a synthetic polymeric network (PVA or PEO) in an Interpenetrating Polymer Network (IPN) architecture. These IPN can be made biodegradable by crosslinking the Bovine Serum Albumin modified by methacrylate groups (BSAm) with the synthetic partner.Depending on the composition, these materials can be fully degraded or fragmented after several days of incubation with thermolysin, a proteolytic enzyme. The degradation kinetics of these hydrogels were studied by following the release of proteic fragments from the material and by the loss of viscoelastic properties. The biocompatibility was also verified: fibroblasts cultivated on the surface show a viability of over 90% after 5 weeks of culture and the proliferation is followed by the synthesis of Extracellular Matrix macromolecules.To add a bactericide property, and to increase their mechanical resistance, ammonium salts were incorporated in those IPN. Lastly, the synthesis of these IPN were adapted, starting from whole blood plasma. Rejection phenomena upon implantation should thus be hindered. Moreover, blood plasma contains a wide variety of growth factors and bioactive molecules, which should improve tissue regeneration.

abstract: Single-layer pentagonal materials have received limited attention compared with their counterparts with hexagonal structures. They are two-dimensional (2D) materials with pentagonal structures, that exhibit novel electronic, optical, or magnetic properties. There are 15 types of pentagonal tessellations which allow plenty of options for constructing 2D pentagonal lattices. Few of them have been explored theoretically or experimentally. Studying this new type of 2D materials with density functional theory (DFT) will inspire the discovery of new 2D materials and open up applications of these materials in electronic and magnetic devices.In this dissertation, DFT is applied to discover novel 2D materials with pentagonal structures. Firstly, I examine the possibility of forming a 2D nanosheet with the vertices of type 15 pentagons occupied by boron, silicon, phosphorous, sulfur, gallium, germanium or tin atoms. I obtain different rearranged structures such as a single-layer gallium sheet with triangular patterns. Then the exploration expands to other 14 types of pentagons, leading to the discoveries of carbon nanosheets with Cairo tessellation (type 2/4 pentagons) and other patterns. The resulting 2D structures exhibit diverse electrical properties. Then I reveal the hidden Cairo tessellations in the pyrite structures and discover a family of planar 2D materials (such as PtP2), with a chemical formula of AB2 and space group pa ̄3. The combination of DFT and geometries opens up a novel route for the discovery of new 2D materials. Following this path, a series of 2D pentagonal materials such as 2D CoS2 are revealed with promising electronic and magnetic applications. Specifically, the DFT calculations show that CoS2 is an antiferromagnetic semiconductor with a band gap of 2.24 eV, and a N ́eel temperature of about 20 K. In order to enhance the superexchange interactions between the ions in this binary compound, I explore the ternary 2D pentagonal material CoAsS, that lacks the inversion symmetry. I find out CoAsS exhibits a higher Curie temperature of 95 K and a sizable piezoelectricity (d11=-3.52 pm/V). In addition to CoAsS, 34 ternary 2D pentagonal materials are discovered, among which I focus on FeAsS, that is a semiconductor showing strong magnetocrystalline anisotropy and sizable Berry curvature. Its magnetocrystalline anisotropy energy is 440 μeV/Fe ion, higher than many other 2D magnets that have been found. Overall, this work not only provides insights into the structure-property relationship of 2D pentagonal materials and opens up a new route of studying 2D materials by combining geometry and computational materials science, but also shows the potential applications of 2D pentagonal materials in electronic and magnetic devices. / Dissertation/Thesis / Doctoral Dissertation Materials Science and Engineering 2020

Παρατηρείται ότι, το ΙΑΜ έχει ήδη εδρεώσει τη θέση του ανάμεσα στα δομικά υλικά. Όμως για να μπορεί να χαρακτηριστεί ως πολυλειτουργικό υλικό, θα πρέπει να παρέχει και άλλες λειτουργίες μη δομικής φύσεως. Η διατριβή αυτή, επικεντρώθηκε στην ανίχνευση βλάβης σε στοιχεία ΙΑΜ μέσω διηλεκτρικών μετρήσεων και πιο συγκεκριμένα μέσω της μεταβολής της ηλεκτρικής αντίστασης στα στοιχεία αυτά. Τα αποτελέσματα των πειραματικών δοκιμών θα χρησιμοποιηθούν ώστε να θέσουν τις βάσεις για κατάλληλους συντελεστές συσχέτισης μεταξύ της εξέλιξης της βλάβης και της πιεζοαντίστασης σε στοιχεία ΙΑΜ. / This thesis presents the preliminary results of an ongoing experimental program aiming at assessing the piezoresistivity of carbon textile reinforced concrete dumbbell specimens under monotonic tensile loading, along the direction of loading. During testing both longitudinal strain and longitudinal electrical resistivity were recorded; electrical resistivity measurements were realized using a high-precision multimeter. The results of this experimental campaign may be used for setting the ground for establishing appropriate correlation factors between damage progression and piezoresistivity properties for TRC elements.

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The use of Fibre Reinforced Polymer (FRP) composite materials in structural applications has increased in the past decades in high­performance sectors, such as in the automotive and aeronautic industries, for weight reduction purposes. However, FRP composite materials can offer more significant innovation potential. The application of CNTs in conjunction with composite material can allow the creation of multifunctional materials, relying on FRP for the structural side and CNT for the sensing ability. In this master thesis, the embedment of a Vertical Aligned Carbon Nanotube (VACNT) layer into the interlaminar region of Carbon Fibre (CF) laminates to provide polyvalent sensing ability to the material was investigated. In order to obtain accurate results, the sensor had to be isolated from the rest of the laminate. For this reason, the main problem to be solved in this project was the electrical isolation on the CNT layer and its contacts from the layers of CF laminate. This study aims to find a suitable isolation technique in order to apply the CNT sensor technology, developed in previous studies, into CF laminate. Although thought for aerospace applications, these sensors could be applied to different structural components in various fields. / Användningen av fiberförstärkta polymerer (FRP)-­kompositmaterial i strukturella applikationer har ökat under de senaste decennierna i högpresterande sektorer, såsom i fordons­ och flygindustrin, för viktminskningsändamål. FRP-­kompositmaterial kan dock erbjuda mer betydande innovationspotential. Användningen av CNTs i kombination med kompositmaterial kan möjliggöra skapandet av multifunktionella material, beroende på FRP för den strukturella sidan och CNT för avkänningsförmågan. I denna masteruppsats undersöktes inbäddningen av ett Vertical Aligned Carbon Nanotube (VACNT) lager i den interlaminära regionen av Carbon Fiber (CF) laminat för att ge polyvalent avkänningsförmåga till materialet. För att få exakta resultat måste sensorn isoleras från resten av laminatet. Av denna anledning var huvudproblemet som skulle lösas i detta projekt den elektriska isoleringen på CNT-­lagret och dess kontakter från lagren av CF­-laminat. Denna studie syftar till att hitta en lämplig isoleringsteknik för att tillämpa CNT­sensorteknologin, utvecklad i tidigare studier, i CF-­laminat. Även om de är tänkta för flygtillämpningar, kan dessa sensorer appliceras på olika strukturella komponenter inom olika områden.

<p dir="ltr">Piezoelectric polymers and ceramics have applications throughout many fields, including their use as pressure sensors and transducers. Of the polymers, poly(vinylidene fluoride – trifluoroethylene) (P(VDF-TrFE)), has been the go-to for its high piezoelectric performance. With the addition of aluminum nanopowders (nAl), P(VDF-TrFE) acts as a binder and oxidizer, creating an energetic composite, a so-called piezoenergetic. However, this typically results in lower d₃₃ coefficients and can have lower reactivity since ideal mixtures may short when poled. Here, we develop and demonstrate single-layer and multilayer polymer composite films with high piezoelectric and energetic content. We prepared single-layer thin film piezoelectric energetic composites of nAl and P(VDF-TrFE) and a combination of thermal annealing and poling at elevated temperatures enabled full poling of 9 wt.% nAl/P(VDF-TrFE) films with d₃₃ of 22.7 pC/N that is comparable to P(VDF-TrFE) films. We also investigated the addition of barium titanate (BaTiO₃) particles as a piezoelectric ceramic to enhance the d₃₃ coefficient. In the neat polymer, BaTiO₃ had differing effects depending on the particle size, with 200 nm particles improving the d₃₃ coefficient more than the 1 μm particles. However, neither size of BaTiO₃ particle had a substantial effect on the piezoelectricity in the 9 wt.% nAl/P(VDF-TrFE) films. We also prepared hot-pressed, three-layer “sandwich” P(VDF-TrFE) – 30 wt.% nAl/P(VDF-TrFE) – P(VDF-TrFE) composites, which had marginally lower d₃₃ coefficients than the single-layer 9 wt.% nAl/P(VDF-TrFE) films. However, the 30 wt.% nAl/P(VDF-TrFE) sandwich films were far more energetic than the 9 wt.% nAl/P(VDF-TrFE) films, as confirmed by simultaneous differential scanning calorimetry and thermogravimetric analysis (DSC/TGA) and deflagration studies. The single films will often fail to fully sustain a deflagration, while the sandwich films burn completely. In addition, we can ignite the sandwich samples with an electrical discharge making these films also useful in ignition applications. To demonstrate the use of piezoenergetic films, 9 wt.% nAl/P(VDF-TrFE) single layer and 30 wt.% nAl/P(VDF-TrFE) sandwich films were calibrated as pressure gauges using a mini drop weight setup, and then demonstrated as a pressure gage. The improvements in the piezoelectric coefficient of the 9 wt.% nAl/P(VDF-TrFE) single layer films, as well as the energetic performance in the form of the 30 wt.% nAl/P(VDF-TrFE) sandwich films strongly amplify the existing potential of these multifunctional composites in energetic and pressure sensing applications.</p>