Cette thèse s'inscrit dans la thématique de la nano-optomécanique et de l'emploi de nanorésonateurs mécaniques comme sonde de force ultrasensible pour étudier leur interaction avec la lumière. Pour cela, un nanofil de carbure de silicium est positionné dans un faisceau laser fortement focalisé. Cela permet, en mesurant les fluctuations de l'intensité transmise, d'observer avec grande dynamique et une sensibilité proche de la limite quantique standard le mouvement Brownien du nanorésonateur. La grande sensibilité en force des nanofils, inhérente à leur très faible masse, permet d'étudier l'action en retour de la mesure, c'est-à-dire la force exercée par le laser focalisé sur le nanofil. L'exploitation de la légère levée de dégénérescence observée entre les deux polarisations mécaniques transverses permet de réaliser une cartographie vectorielle bidimensionnelle du champ de force optique, avec une sonde de diamètre sub-longueur d'onde. Cette mesure permet également de mettre en évidence le caractère non-conservatif de l'interaction lumière-matière, dont la signature emblématique est l'existence de vorticité dans le champ de force mesuré. Ce dernier présente de très fortes variations spatiales, qui modifient profondément la dynamique du nanofil. Cette action en retour de la mesure est responsable d'un fort couplage entre les deux polarisations mécaniques du mode fondamental du nanofil. Le caractère bidimensionnel du couplage ainsi que la topologie non-conservative du champ de force conduisent à une bifurcation et à une instabilité dynamique du nanofil. Cette nouvelle instabilité optomécanique est observée avec des forces optiques instantanées, qui suivent instantanément les variations d'intensités vues par le nanofil. En présence d'absorption, le cas plus général d'un champ de force partiellement retardé par les constantes de temps thermiques est également étudié, conduisant à un refroidissement, spécifique et accordable en position, des deux polarisations mécaniques. Enfin l'interaction lumière-matière entre le laser et le nanofil et la grande variété des propriétés optomécaniques accessibles à cette approche sont développés. Ces développements démontrent la possibilité d'observer et de contrôler optiquement des nanorésonateurs mécaniques de très grande sensibilité, proche de l'attonewton, pour des mesures vectorielles ultrasensibles de champ de force. / This thesis is related to the field of nano-optomechanics and the use of nanomechanical resonators as ultrasensitive force sensor to study their interaction with light. A silicon carbide nanowire is positioned in a tightly focused laser beam. This enables, by measuring the transmitted intensity fluctuations, to observe with great dynamics and with a sensitivity close to the standard quantum limit the Brownian motion of the nanoresonator. The huge force sensitivity of the nanowires, due to their ultra low mass, permits to study the measurement backaction, which is induced by the force exerted on the nanowire by the focused laser beam. The exploitation of the slight degeneracy observed between the two transverse mechanical polarizations enables to realize a vectorial bidimensional cartography of the optical force field, with a probe of sub-wavelength diameter. This measurement highlights the non-conservative feature of the light-matter interaction, a symbolic signature being the existence of vorticity in the measured force field. The latter shows strong spatial variations, which modify deeply the nanowire dynamics. This measurement backaction is responsible of a strong coupling between the two mechanical polarizations of the nanowire fundamental mode. The bidimensional feature of the coupling and the force field non-conservative topology lead to a bifurcation and to a dynamical instability of the nanowire. This new optomechanical instability is observed with instantaneous optical forces, which follows instantaneously the intensity variations seen by the nanowire. In presence of absorption, a more general case of a force field partially delayed by the thermal time constants is studied, leading to a cooling, specific and tunable with the position, of the two mechanical polarizations. Then, the light-matter interaction between a laser and the nanowire and the great variety of optomechanical properties accessible with this approach are developed. These developments demonstrate the ability to observe and control optically nanomechanical resonators with a huge sensitivity, close to the attonewton, for ultrasensitive measurements of vectorial force fields.

Living organisms are made up of a multitude of individual cells that are surrounded by biomolecules and fluids. It is well known that cells are highly regulated by biochemical signals; however it is now becoming clear that cells are also influenced by the mechanical forces and mechanical properties of the local microenvironment. Extracellular forces causing cellular deformation can originate from many sources, such as fluid shear stresses arising from interstitial or blood flow, mechanical stretching during breathing or compression during muscle contraction. Cells are able to sense variations in the mechanical properties (elasticity) of their microenvironment by actively probing their surroundings by utilizing specialized proteins that are involved in sensing and transmitting mechanical information. The actin cytoskeleton and myosin-II motor proteins form a contractile (actomyosin) network inside the cell that is connected to the extracellular microenvironment through focal adhesion and integrin sites. The transmission of internal actomyosin strain to the microenvironment via focal adhesion sites generates mechanical traction forces. Importantly, cells generate traction forces in response to extracellular forces and also to actively probe the elasticity of the microenvironment. Many studies have demonstrated that extracellular forces can lead to rapid cytoskeletal remodeling, focal adhesion regulation, and intracellular signalling which can alter traction force dynamics. As well, cell migration, proliferation and stem cell fate are regulated by the ability of cells to sense the elasticity of their microenvironment through the generation of traction forces. In vitro studies have largely explored the influence of substrate elasticity and extracellular forces in isolation, however, in vivo cells are exposed to both mechanical cues simultaneously and their combined effect remains largely unexplored. Therefore, a series of experiments were performed in which cells were subjected to controlled extracellular forces as on substrates of increasing elasticity. The cellular response was quantified by measuring the resulting traction force magnitude dynamics. Two cell types were shown to increase their traction forces in response to extracellular forces only on substrates of specific elasticities. Therefore, cellular traction forces are regulated by an ability to sense and integrate at least two pieces of mechanical information - elasticity and deformation. Finally, this ability is shown to be dependent on the microtubule network and regulators of myosin-II activity.

No description available.

<p> Brønsted acid zeolites can be synthesized in a wide range of topologies, each characterized by diverse void sizes, shapes, and micropore connectivity. The location of Brønsted acid sites (H+-sites) within microporous voids of different size and shape, and the relative proximity of H+-sites influences their reactivity. Additionally, the diffusion of reactant and product molecules through a given zeolite topology depends on micropore size, tortuosity, and connectivity. The coupled influences of reaction kinetics and intrazeolite reactant and product diffusion govern rates and selectivity for a plethora of zeolite-catalyzed reactions and underlie the well-established effects of “shape-selectivity”. The independent effects of reaction and diffusion on rates and selectivity for a given reaction are often obfuscated by concomitant changes in the zeolite properties governing diffusion (e.g., crystallite size) and reactivity (e.g., H+-site density or proximity) in zeolite materials synthesized with conventional methods. Herein, we develop synthetic methods to decouple H+-site density, proximity and crystallite size in medium-pore, 10-membered ring (10-MR) zeolites, and evaluate the independent effects of these material properties on the kinetic and transport phenomena that govern propene oligomerization catalysis. </p> <p>Among synthetic methods to influence H+-site proximity in zeolites, varying the charge-density and ratio of structure directing agent (SDA) cations that compensate anionic charges in frameworks at Al centers has been reported to influence H+-site proximity in MFI and CHA zeolites of fixed H+-site density. Changes in H+-site proximity can be evaluated using Co2+ cations to selectively titrate and quantify subsets of proximal H+-sites (H+-site pairs); conditions to perform such titrations were identified for MEL zeolites. The fraction of paired H+-sites changed concurrently with changes in framework Al content in MEL zeolites synthesized using a single organic SDA (OSDA), tetrabutylammonium hydroxide (TBA+). Synthesis of MEL with mixtures of TBA+ and Na+ as an inorganic SDA (ISDA), at fixed total SDA and Al content, allowed the fraction of paired H+-sites to be systematically varied in MEL zeolites of fixed H+-site density, reflecting changes in the location and quantity of charge-balancing SDAs with Na+/TBA+ ratio. The energetic favorability of SDA occlusion in MEL was also evaluated with density functional theory (DFT). In contrast to MEL, occluded SDA content in TON zeolites crystallized with varied OSDA (1,6-diaminohexane, or 1,8-diamooctane) and K+ content, at fixed total SDA content, was invariant with K+/OSDA ratio, reflecting a different mechanism of SDA occlusion in TON. These findings provide an approach to influence H+-site pairs in 10-MR zeolites of fixed H+-site density and demonstrate the dependence of SDA occlusion on zeolite topology.</p> <p>The independent influences of H+-site and crystallite properties on rates and selectivity of propene oligomerization to heavier alkenes in a representative medium-pore zeolite topology (MFI) were explored by interrogating suites of samples crystallized with independently varied H+-site density (0.3–5.7 H+/u.c.), proximity, and crystallite size (0.03–2.65 μm) over a wide range of reaction conditions (483–523 K, 7–615 kPa C3H6). Dimerization rates (per H+) decreased with increasing crystallite size among MFI materials synthesized with fixed H+-site density (0.3 or 1.3 H+/u.c.), revealing the strong and ubiquitous influence of intrazeolite diffusion limitations on measured dimerization rates. Weisz-Prater criterion analyses, in conjunction with dimerization rate transients upon step-changes in reaction conditions, indicate that these intrazeolite diffusion limitations arise from a product-derived organic phase occluded within zeolitic micropores during propene oligomerization catalysis, which restricts intrazeolite diffusion by lowering the effective diffusivities of propene and product alkenes. This occluded organic phase becomes heavier in composition at higher propene pressures and lower reaction temperatures, which favor chain growth over β-scission, resulting in more severe intrazeolite diffusional constraints. The composition of the occluded organic phase was also found to depend on H+-site density in MFI zeolites. Rate constants (per H+) of dimerization and trimerization were higher on MFI samples of dilute H+-site density, resulting in faster growth of heavier oligomer products and consequently lower effective diffusivities compared to MFI samples of higher H+-site density. The convoluted influences of reaction and diffusion on measured propene oligomerization rates result in apparent reaction orders that deviate from the first-order dependence of rates on propene pressure expected in the limit of strict kinetic control. Accounting for the coupled influences of reaction and diffusion on propene oligomerization rates and the influence of H+-site density on intrazeolite diffusion, rationalizes contradictory conclusions among prior reports about the dependence of oligomerization rates on H+-site density, proximity, and crystallite size, which did not identify or consider the influences of intrazeolite diffusion in their interpretations of rate data. </p> <p>Finally, we explore the consequences of zeolite pore size and connectivity for reactivity and intrazeolite diffusion during propene oligomerization by interrogating H-zeolites of different topologies. Intrazeolite diffusional constraints are imposed by an occluded organic phase and influence dimerization rates among medium-pore zeolite topologies (MFI, MEL, TON), but such constraints are alleviated on large-pore zeolite topologies (FAU, MOR, *BEA), reflecting the slower growth and faster diffusion of heavy oligomer products in large-pore zeolites. Among medium-pore zeolites, the composition of the occluded organic phase, and consequently the effective diffusivities of propene and product alkenes, is influenced by void size. Analysis of product selectivity on zeolites of different pore size and connectivity (TON, MOR, MFI) reveals that TON restricts the growth of heavier oligomer products, resulting in effective diffusivities that are higher on TON compared to MFI, and are relatively invariant with propene pressure and H+-site density. Together, the findings herein demonstrate the ability of slow-diffusing products to impose intrazeolite diffusional constraints on other products during alkene oligomerization catalysis, and reveal the critical influence of reaction conditions, H+-site density, and micropore size on the composition of this occluded organic phase, and consequently intrazeolite diffusional constraints. Ultimately, this work demonstrates how kinetic studies performed on well-defined zeolite materials can reveal important changes in reaction and diffusion phenomena, which are otherwise inextricably convoluted, and provides a framework through which such effects can be assessed for other zeolite-catalyzed molecular chain-growth reactions. </p>

<p>Nuclear fission energy has developed for more than five decades and become one of the most important low-carbon energy forms. The extreme environment in the advanced reactors, including high operating temperature and high neutron radiation dose, raises new challenges for structural materials. To date, no materials are immune to radiation damage. Bombardment by energetic particles displaces atoms from their original sites, leaves various forms of defect aggregates after cascade, and degrades the properties of the irradiated materials. FeCrAl alloys, known for their excellent high-temperature oxidation resistance, were developed under the accident tolerant fuel program in hope to replace the Zr cladding alloys in future reactors. The radiation response and mechanical properties of FeCrAl alloy have attracted great attention. The objective of this thesis is two-fold. First, investigate the high temperature mechanical behavior of coarse-grained FeCrAl alloys with and without irradiation from the perspective of small-scale testing. Second, develop a fine-grained FeCrAl alloy variant and evaluate its mechanical properties and radiation tolerance.</p> <p>Critical resolved shear stress of pristine and proton irradiated CG FeCrAl alloy was quantified at elevated temperatures. {112}<111> slip system exhibited higher irradiation induced hardening compared with the {110}<111> slip system. Gradient FeCrAl alloy was fabricated through surface mechanical grinding treatment. In situ pillar compression tests revealed an excellent combination of strength and deformability of ultra-fine-grained (UFG) FeCrAl alloys. The activation energy for plastic deformation of a nanolaminate (NL) FeCrAl alloy was determined through strain rate jump tests. Ex situ Fe-ion irradiation showed the interplay between dislocation loops and grain coarsening and their contributions to the mechanical properties of the irradiated UFG FeCrAl alloys. In situ Kr ion irradiation studies on the helium pre-injected NL FeCrAl and CG FeCrAl show that the helium induced swelling was effectively reduced in NL alloy due to their abundant grain boundaries serving as defect sinks. The findings in this thesis may provide innovative perspectives on the design and manufacture of novel FeCrAl alloys with outstanding mechanical properties and radiation tolerance.</p> <p><br></p>

The enhancement of strength of nanoscale materials such as face-centered cubic metal nanowires is well known and arises largely from processes mediated by high energy surface atoms. This leads to strong size effects in nanoscale plasticity; ,smaller is stronger. Yet, other factors, such as crystalline defects also contribute greatly to the mechanical properties. In particular, twin boundaries, which are pervasive and energetically favorable defects in face-centered cubic metal nanowires, have been shown to greatly enhance the strength, furthermore this increase in strength has been shown to be directly influenced by the twin density. However, attempts to control the introduction of beneficial defects remains challenging. Additionally, even minor local variations in the crystalline structure or size of metal nanowires may have drastic effects on the yielding of metal nanowires, which are difficult to measure through tensile and bending tests. In this study, atomic force microscopy based nanoindentation techniques are used to measure the local plasticity of Ni-Au bimetallic as well as Cu and Ag metallic nanowires. In the first part of the thesis the hardness of bimetallic nanowires synthesized through template-assisted electrodeposition is measured and found to show significant size-effects. It was found that the nanoindentation hardness was governed by materials properties, the observed indentation size effects were dependent on geometrical factors. The second part of this thesis presents a methodology to control the crystal structure of Ag and Cu nanowires through direct electrodeposition techniques, which were tested directly as grown on the substrate to limit effects of pre-straining. Ag nanowires showed marked size-effects as well as two distinct modes of deformation which we attribute to the defects that arise during crystalline growth. We also show control of the surface microstructure in Cu nanowires which leads to strengths that are more than doubled compared to single crystalline Cu nanowires. Finally, we present support from classic crystal growth theory to justify that the observed plasticity in Ag and Cu nanowires is largely dependent on defects that are nucleated through changes in the growth environment.

We study the plasticity mechanisms of diffusionless martensite phase transformation in Nickel-Titanium, one of the most widely used shape memory alloys. The research here involves four thrusts focusing on different length and time scales: (I) Molecular statics and dynamics simulations are applied to study the nanotwin structures and temperature-driven B2 → B19′ phase transitions. (II) Molecular dynamics simulations are performed to explore the stress-driven martensitic phase transformation governing the pseudoelasticity and shape memory effects in NiTi nanopillars. (III) Monte Carlo simulations are conducted to characterize the temperature- driven B2 → B19 phase transition and the patterning of martensitic nanotwins in NiTi thin films. (IV) Phase field simulations are performed to predict the formation and evolution of complex martensitic microstructures, including the detailed analysis of twin compatibility under complex loading conditions. We also study the nucleation-controlled plasticity mechanisms in different metals of Cu, Al and Ni. Our work focuses on understanding how dislocations nucleate in single crystals. Interatomic potential finite element method is applied to determine when, where and how dislocations nucleate during nanoindentation in metals such as Cu, Al and Ni.

<p>This study is focused on designing and characterizing protein-based building blocks in order to construct self-assembled nano-structured biomaterials. In detail, this research aims to: (1) investigate a new class of proteins that possess nanospring behaviors at a single-molecule level, and utilize these proteins along with currently characterized elastomeric proteins as building blocks for nano-structured biomaterials; (2) develop a new method to accurately measure intermolecular interactions of self-assembling two or more arbitrary (poly)peptides, and select some of them which have appropriate tensile strength for crosslinking the proteins to construct elastomeric biomaterials; (3) construct well-defined protein building blocks which are composed of elastomeric proteins terminated with self-oligomerizing crosslinkers, and characterize self-assembled structures created by the building blocks to determine whether the elasticity of proteins at single-molecule level can be maintained.</p><p>Primary experimental methods of this research are (1) atomic force microscope (AFM) based single-molecule force spectroscopy (SMFS) that allows us to manipulate single molecules and to obtain their mechanical properties such as elasticity, unfolding and refolding properties, and force-induced conformational changes, (2) AFM imaging that permits us to identify topology of single molecules and supramolecular structures, and (3) protein engineering that allows us to genetically connect elastomeric proteins and self-assembling linkers together to construct well-defined protein building blocks.</p><p>Nanospring behavior of á-helical repeat proteins: We revealed that á-helical repeat proteins, composed of tightly packed á-helical repeats that form spiral-shaped protein structures, unfold and refold in near equilibrium, while they are stretched and relaxed during AFM based SMFS measurements. In addition to minimal energy dissipation by the equilibrium process, we also found that these proteins can yield high stretch ratios (>10 times) due to their packed initial forms. Therefore, we, for the first time, recognized a new class of polypeptides with nanospring behaviors. </p><p>Protein-based force probes for gauging molecular interactions: We developed protein-based force probes for simple, robust and general AFM assays to accurately measure intermolecular forces between self-oligomerization of two or more arbitrary polypeptides that potentially can serve as molecular crosslinkers. For demonstration, we genetically connected the force probe to the Strep-tag II and mixed it with its molecular self-assembling partner, the Strep-Tactin. Clearly characterized force fingerprints by the force probe allowed identification of molecular interactions of the single Strep-tag II and Strep-Tactin complex when the complex is stretched by AFM. We found a single energy barrier exists between Strep-tag II and Strep-Tactin in our given loading rates. Based upon our demonstration, the use of the force probe can be expanded to investigate the strength of interactions within many protein complexes composed of homo- and hetero-dimers, and even higher oligomeric forms. Obtained information can be used to choose potential self-assembling crosslinkers which can connect elastomeric proteins with appropriate strength in higher-order structures. </p><p>Self-assembled nano-structured biomaterials with well-defined protein-based building blocks: We constructed well-defined protein building blocks with tailored mechanical properties for self-assembled nano-structured materials. We engineered protein constructs composed of tandem repeats of either a I27-SNase dimer or a I27 domain alone and terminated them with a monomeric streptavidin which is known to form extremely stable tetramers naturally. By using molecular biology and AFM imaging techniques, we found that these protein building blocks transformed into stable tetrameric complexes. By using AFM based SMFS, we measured, to our knowledge for the first time, the mechanical strength of the streptavidin tetramer at a single-molecule level and captured its mechanical anisotropy. Using streptavidin tetramers as crosslinkers offers a unique opportunity to create well-defined protein based self-assembled materials that preserve the molecular properties of their building blocks.</p> / Dissertation

L'étude du couplage hybride entre les vibrations d'un résonateur mécanique et un degré de liberté quantique requiert une très grande sensibilité en force. Ceci a motivé le développement récent de nano-oscillateurs ultra-légers, qui constituent des sondes de force ultra-sensibles opérant désormais au niveau de l'attoNewton.Le premier volet de ce travail traite de l'habillage mécanique d'un nanofil suspendu de carbure de silicium, oscillant dans deux directions transverses. Son évolution Brownienne ou excitée dans un champ de force externe perturbe ses propriétés : fréquences et directions propres de vibration. Une technique de mesure optique des vibrations du nanofil en deux dimensions a été développée. Elle a permis, dans un premier temps, de cartographier un champ de force électrostatique, révélant une phénoménologie de l'habillage spécifique aux dimensions supérieures à un. En particulier, les composantes cisaillantes du champ induisent une rotation des directions propres de vibration. Dans un deuxième temps, la technique de mesure a été testée dans un champ de force optique, produit par un laser focalisé sur le nanofil, et qui contient une composante rotationnelle, non conservative. On rapporte l'observation d'une brisure de l'orthogonalité des modes propres, d'une distorsion et d'une amplification des spectres de mouvement Brownien, toutes en accord avec le modèle décrivant l'habillage mécanique du nanofil par ce champ de force externe non potentiel. A partir d'un protocole adapté à la multi-dimensionnalité du système, une déviation à la relation fluctuation-dissipation a également été mesurée : il s'agit d'une conséquence de la sortie de l'équilibre induite par la force optique non-conservative. L'étude des propriétés thermodynamiques du système suggère des corrections à la relation fluctuation-dissipation et prédit enfin un phénomène de compression du bruit thermique de l'oscillateur en champ de force rotationnel.Le deuxième volet de la thèse concerne le système hybride constitué d'un nanofil et d'un qubit de spin, un centre coloré NV du diamant attaché à son extrémité. Les propriétés optiques de cette source de photons uniques oscillante sont caractérisées à partir de la mesure de corrélations spatio-temporelles de la fluorescence du centre NV sur lesquelles les vibrations de l'oscillateur se retrouvent encodées. Nous avons ainsi développé un système de mesure du mouvement compatible avec de très faibles flux de photons, inférieurs en particulier au taux de décohérence mécanique. La dernière partie de ce manuscrit présente une étude préliminaire du couplage du spin-mécanique. Après l'observation d'un triplet de Mollow phononique, les développements expérimentaux de la première partie de la thèse ont été intégrés à une expérience hybride de seconde génération stabilisée amenant la mesure de force ultra-sensible à la portée du système hybride. / The study of the hybrid coupling between the vibrations of a mechanical resonator and a quantum degree of freedom requires extremely high force sensitivities. This was one of the motivations for the recent development of ultra-light nano-oscillators which are ultra-sensitive force probes now routinely operating at the attoNewton level.The first part of this work deals with the mechanical dressing of a silicon carbide suspended nanowire oscillating in two transverse directions. Its Brownian or driven evolution in an external force field modifies its mechanical properties: eigen-frequencies and eigen-directions of oscillation. An optical technique to measure the nanowire vibrations in two dimensions was developed. First, this technique enabled to map out an electrostatic force field, which revealed a dressing phenomenology specific to dimensions greater than one. In particular, shearing components of the force field are responsible for a rotation of the eigen-directions of vibration. Second, the measurement technique was tested in an optical force field applied by a laser focused on the nanowire. This field contains a rotational, non-conservative component. The reported experimental observations: eigenmodes orthogonality breaking, distorsion and amplification of Brownian motion spectra, are all in good agreement with the model of the mechanical dressing. Using a protocol adapted to the multidimensionality of the system, a deviation to the fluctuation-dissipation relation has also been measured, as a consequence of the non-conservative force bringing the system out of equilibrium. The study of this system's thermodynamic properties suggests corrections to the fluctuation-dissipation relation and predicts a squeezing of the oscillator's thermal noise in rotational force fields.The second part of the thesis concerns the hybrid system composed of a nanowire and a spin qubit: a colored NV center in diamond bound to its extremity. The optical properties of this oscillating single photon source are characterized through the measurement of space-time fluorescence correlations on which the oscillator's vibrations are encoded. We then developed a motion measurement technique compatible with very low photon fluxes, in particular inferior to the mechanical decoherence rate. The last part of the manuscript presents a preliminary study of the spin-mechanical coupling. After the observation of a phononic Mollow triplet, the experimental developments of the first part of the thesis were integrated in a second-generation stabilized hybrid experiment bringing the ultrasensitive force measurement within the reach of the hybrid system.

Une analyse détaillée des propriétés physico-chimiques des nanoparticules (NP) anthropogéniques est nécessaire pour comprendre à un niveau mécanistique leurs interactions/toxicité potentielle avec/envers les composants biotiques des systèmes aquatiques naturels. Une telle analyse est également requise pour réaliser une évaluation complète et une optimisation de la performance des méthodes d’(ultra)filtration développées pour circonscrire le relargage des NPs dans les milieux aquatiques. Dans ce contexte, l'objectif de cette thèse de doctorat était de déchiffrer les processus physico-chimiques fondamentaux régissant la capture de nanodendrimères carboxylés (PAMAM-COOH) - utilisés fréquemment dans des applications biomédicales – par des films multicouches du type (poly(diallyldiméthylammonium)chlorure-poly(acide acrylique))n ((PDADMAC-PAA)n) assemblés par déposition séquentielle des composantes polymériques cationique et anionique. À cette fin, une étude systématique des propriétés électrohydrodynamiques des NPs PAMAM-COOH a d'abord été effectuée en fonction du pH et de la concentration en sel monovalent du milieu. Sur la base de la théorie électrocinétique de particules molles ayant une fonctionnalité zwitterionique, il est démontré que les caractéristiques électriques interfaciales des NPs considérées sont déterminées à la fois par des contributions électrostatiques de surface et volumique des nanoparticules, lesquelles dependent de l’extension intraparticulaire de la double couche électrique. L’existence de ces deux types de contributions conduit à un changement remarquable de signe de la mobilité des NPs en modifiant la concentration du sel monovalent en solution et à une dépendance prononcé du point de zéro mobilité des NPs avec la concentration de l’électrolyte. En outre, une confrontation quantitative entre résultats expérimentaux et théorie souligne comment les modifications structurales des NPs induites par des changements de pH et de salinité affectent les caractéristiques électrocinétiques des dendrimères. Dans une deuxième partie, la structure, la morphologie et les propriétés mécaniques des films PDADMAC-PAA et leur évolution temporelle dans des conditions de vieillissement naturel ou après traitement thermique ont été déterminées par microscopie à force atomique (AFM) et analyses microspectroscopie Raman. Les résultats démontrent que les films multicouches PDADMAC-PAA de type exponentiel présentent des caractéristiques mécaniques et structurelles typiques de films polyélectrolytes multicouches à croissance linéaire. En particulier, leur relaxation lente vers un état d’équilibre est accélérée après traitement thermique à 60°C et se révèle être intimement liée à l'instabilité de domaines de films riches en PDADMAC, épuisés en eau (faits confirmés par la théorie de la fonctionnelle de la densité) et marqués par la présence de structures caractéristiques en forme de ‘donuts’. Dans une dernière partie, des résultats préliminaires sont donnés pour la dépendance de l'élasticité des films multicouches PDADMAC-PAA avec la concentration en solution de nanodendrimères. Les résultats suggèrent que ces films multicouches complexes constituent une option prometteuse pour la capture et l'élimination de nanodendrimères carboxylés présents en milieux aqueux / A detailed analysis of the physicochemical properties of engineered nanoparticles (NPs) is required to understand on a mechanistic level their interactions/potential toxicity with/towards biotic components of fresh water systems. Such an analysis is further mandatory to achieve a comprehensive evaluation and optimisation of the performance of (ultra)filtration methods developed to prevent NPs release into aquatic media. Within this context, the aim of this PhD thesis was to decipher the basic physico-chemical processes governing the loading of carboxylated-poly(amidoamine) (PAMAM-COOH) nanodendrimers -commonly employed in biomedical applications- into layer-by-layer assembled (poly(diallyl dimethyl ammonium) chloride-poly(acrylic acid))n ((PDADMAC-PAA)n) multilayer films. For that purpose, a systematic investigation of the electrohydrodynamic properties of PAMAM-COOH NPs was first performed as a function of pH and monovalent salt concentration in solution. On the basis of advanced electrokinetic theory for soft particles with zwitterionic functionality, it is demonstrated that the interfacial electrostatic features of the considered NPs are determined both by surface and bulk particle contributions to an extent that depends on electrolyte concentration. This leads to a remarkable NPs mobility reversal with changing monovalent salt concentration and to a marked dependence of the point of zero NPs mobility on electrolyte content. In addition, confrontation between experiments and theory further highlights how pH- and salt-mediated modifications of the NP particle structure affect dendrimer electrokinetic features at large pH and/or low salt concentrations. In a second part, the structure, morphology and mechanical properties of PDADMAC-PAA films, and their evolution over time under natural aging conditions or after thermal treatment, were addressed from atomic force microscopy (AFM) and Raman microspectroscopy analyses. Results evidence that PDADMAC-PAA multilayer films of exponential type exhibit mechanical and structural features that are typical for polyelectrolyte multilayer films with linear growth. In particular, their slow relaxation to equilibrium is accelerated after heating treatment at 60°C and, in line with density functional theory computation, this relaxation dynamics is shown to be intimately connected to instability of film domains rich in PDADMAC, depleted in water and marked by the presence of characteristic donut-like structures. In a final part, the reported dependence of PDADMAC-PAA multilayer films elasticity on concentration of nanodendrimers in bulk solution suggests that these complex multilayer films constitute a promising option to be further investigated for the loading and removal of carboxylated nanodendrimers from aqueous environments