Amorphous Placement and Informed Diffusion for Timely Monitoring by Autonomous, Resource-Constrained, Mobile Sensors

Personal communication devices are increasingly equipped with sensors for passive monitoring of encounters and surroundings. We envision the emergence of services that enable a community of mobile users carrying such resource-limited devices to query such information at remote locations in the field in which they collectively roam. One approach to implement such a service is directed placement and retrieval (DPR), whereby readings/queries about a specific location are routed to a node responsible for that location. In a mobile, potentially sparse setting, where end-to-end paths are unavailable, DPR is not an attractive solution as it would require the use of delay-tolerant (flooding-based store-carry-forward) routing of both readings and queries, which is inappropriate for applications with data freshness constraints, and which is incompatible with stringent device power/memory constraints. Alternatively, we propose the use of amorphous placement and retrieval (APR), in which routing and field monitoring are integrated through the use of a cache management scheme coupled with an informed exchange of cached samples to diffuse sensory data throughout the network, in such a way that a query answer is likely to be found close to the query origin. We argue that knowledge of the distribution of query targets could be used effectively by an informed cache management policy to maximize the utility of collective storage of all devices. Using a simple analytical model, we show that the use of informed cache management is particularly important when the mobility model results in a non-uniform distribution of users over the field. We present results from extensive simulations which show that in sparsely-connected networks, APR is more cost-effective than DPR, that it provides extra resilience to node failure and packet losses, and that its use of informed cache management yields superior performance.

Improved delineation of short cortical association fibers and gray/white matter boundary using whole-brain three-dimensional diffusion tensor imaging at submillimeter spatial resolution.

Recent emergence of human connectome imaging has led to a high demand on angular and spatial resolutions for diffusion magnetic resonance imaging (MRI). While there have been significant growths in high angular resolution diffusion imaging, the improvement in spatial resolution is still limited due to a number of technical challenges, such as the low signal-to-noise ratio and high motion artifacts. As a result, the benefit of a high spatial resolution in the whole-brain connectome imaging has not been fully evaluated in vivo. In this brief report, the impact of spatial resolution was assessed in a newly acquired whole-brain three-dimensional diffusion tensor imaging data set with an isotropic spatial resolution of 0.85 mm. It was found that the delineation of short cortical association fibers is drastically improved as well as the definition of fiber pathway endings into the gray/white matter boundary-both of which will help construct a more accurate structural map of the human brain connectome.

A Diffusion MRI Tractography Connectome of the Mouse Brain and Comparison with Neuronal Tracer Data.

Interest in structural brain connectivity has grown with the understanding that abnormal neural connections may play a role in neurologic and psychiatric diseases. Small animal connectivity mapping techniques are particularly important for identifying aberrant connectivity in disease models. Diffusion magnetic resonance imaging tractography can provide nondestructive, 3D, brain-wide connectivity maps, but has historically been limited by low spatial resolution, low signal-to-noise ratio, and the difficulty in estimating multiple fiber orientations within a single image voxel. Small animal diffusion tractography can be substantially improved through the combination of ex vivo MRI with exogenous contrast agents, advanced diffusion acquisition and reconstruction techniques, and probabilistic fiber tracking. Here, we present a comprehensive, probabilistic tractography connectome of the mouse brain at microscopic resolution, and a comparison of these data with a neuronal tracer-based connectivity data from the Allen Brain Atlas. This work serves as a reference database for future tractography studies in the mouse brain, and demonstrates the fundamental differences between tractography and neuronal tracer data.

The Diffusion of Risks in Public Private Partnership Contracts

Purpose The UK government argues that the benefits of public private partnership (PPP) in delivering public infrastructure stem from: transferring risks to the private sector within a structure in which financiers put their own capital at risk; and, the performance based payment mechanism, reinforced by the due diligence requirements imposed by the lenders financing the projects (HM Treasury, 2010). Prior studies of risk in PPPs have investigated ‘what’ risks are allocated and to ‘whom’, that is to the public or the private sector. The purpose of this study is to examine ‘how’ and ‘why’ PPP risks are diffused by their financiers. Design/methodology/approach This study focuses on the financial structure of PPPs and on their financiers. Empirical evidence comes from interviews conducted with equity and debt financiers. Findings The findings show that the financial structure of the deals generates risk aversion in both debt and equity financiers and that the need to attract affordable finance leads to risk diffusion through a network of companies using various means that include contractual mitigation through insurance, performance support guarantees, interest rate swaps and inflation hedges. Because of the complexity this process generates, both procurers and suppliers need expensive expert advice. The risk aversion and diffusion and the consequent need for advice add cost to the projects impacting on the government’s economic argument for risk transfer. Limitations and implications The empirical work covers the private finance initiative (PFI) type of PPP arrangements and therefore the risk diffusion mechanisms may not be generalisable to other forms of PPP, especially those that do not involve the use of high leverage or private finance. Moreover, the scope of this research is limited to exploring the diffusion of risk in the private sector. Further research is needed on how risk is diffused in other settings and on the value for money implication of risk diffusion in PPP contracts. Originality/value The expectation inherent in PPP is that the private sector will better manage those risks allocated to it and because private capital is at risk, financiers will perform due diligence with the ultimate outcome that only viable projects will proceed. This paper presents empirical evidence that raises questions about these expectations. Key words: public private partnership, risk management, diffusion, private finance initiative, financiers

Beyond the ideal free distribution: More general models of predator distribution

The ideal free distribution model which relates the spatial distribution of mobile consumers to that of their resource is shown to be a limiting case of a more general model which we develop using simple concepts of diffusion. We show how the ideal free distribution model can be derived from a more general model and extended by incorporating simple models of social influences on predator spacing. First, a free distribution model based on patch switching rules, with a power-law interference term, which represents instantaneous biased diffusion is derived. A social bias term is then introduced to represent the effect of predator aggregation on predator fitness, separate from any effects which act through intake rate. The social bias term is expanded to express an optimum spacing for predators and example solutions of the resulting biased diffusion models are shown. The model demonstrates how an empirical interference coefficient, derived from measurements of predator and prey densities, may include factors expressing the impact of social spacing behaviour on fitness. We conclude that empirical values of log predator/log prey ratio may contain information about more than the relationship between consumer and resource densities. Unlike many previous models, the model shown here applies to conditions without continual input. (C) 1997 Academic Press Limited.</p>

Diffusion coefficients in dense and supercritical fluids

Os coeficientes de difusão (D 12) são propriedades fundamentais na investigação e na indústria, mas a falta de dados experimentais e a inexistência de equações que os estimem com precisão e confiança em fases comprimidas ou condensadas constituem limitações importantes. Os objetivos principais deste trabalho compreendem: i) a compilação de uma grande base de dados para valores de D 12 de sistemas gasosos, líquidos e supercríticos; ii) o desenvolvimento e validação de novos modelos de coeficientes de difusão a diluição infinita, aplicáveis em amplas gamas de temperatura e densidade, para sistemas contendo componentes muito distintos em termos de polaridade, tamanho e simetria; iii) a montagem e teste de uma instalação experimental para medir coeficientes de difusão em líquidos e fluidos supercríticos. Relativamente à modelação, uma nova expressão para coeficientes de difusão a diluição infinita de esferas rígidas foi desenvolvida e validada usando dados de dinâmica molecular (desvio relativo absoluto médio, AARD = 4.44%) Foram também estudados os coeficientes de difusão binários de sistemas reais. Para tal, foi compilada uma extensa base de dados de difusividades de sistemas reais em gases e solventes densos (622 sistemas binários num total de 9407 pontos experimentais e 358 moléculas) e a mesma foi usada na validação dos novos modelos desenvolvidos nesta tese. Um conjunto de novos modelos foi proposto para o cálculo de coeficientes de difusão a diluição infinita usando diferentes abordagens: i) dois modelos de base molecular com um parâmetro específico para cada sistema, aplicáveis em sistemas gasosos, líquidos e supercríticos, em que natureza do solvente se encontra limitada a apolar ou fracamente polar (AARDs globais na gama 4.26-4.40%); ii) dois modelos de base molecular biparamétricos, aplicáveis em todos os estados físicos, para qualquer tipo de soluto diluído em qualquer solvente (apolar, fracamente polar e polar). Ambos os modelos dão origem a erros globais entre 2.74% e 3.65%; iii) uma correlação com um parâmetro, específica para coeficientes de difusão em dióxido de carbono supercrítico (SC-CO2) e água líquida (AARD = 3.56%); iv) nove correlações empíricas e semi-empíricas que envolvem dois parâmetros, dependentes apenas da temperatura e/ou densidade do solvente e/ou viscosidade do solvente. Estes últimos modelos são muito simples e exibem excelentes resultados (AARDs entre 2.78% e 4.44%) em sistemas líquidos e supercríticos; e v) duas equações preditivas para difusividades de solutos em SC-CO2, em que os erros globais de ambas são inferiores a 6.80%. No global, deve realçar-se o facto de os novos modelos abrangerem a grande variedade de sistemas e moléculas geralmente encontrados. Os resultados obtidos são consistentemente melhores do que os obtidos com os modelos e abordagens encontrados na literatura. No caso das correlações com um ou dois parâmetros, mostrou-se que estes mesmos parâmetros podem ser ajustados usando um conjunto muito pequeno de dados, e posteriormente serem utilizados na previsão de valores de D 12 longe do conjunto original de pontos. Uma nova instalação experimental para medir coeficientes de difusão binários por técnicas cromatográficas foi montada e testada. O equipamento, o procedimento experimental e os cálculos analíticos necessários à obtenção dos valores de D 12 pelo método de abertura do pico cromatográfico, foram avaliados através da medição de difusividades de tolueno e acetona em SC-CO2. Seguidamente, foram medidos coeficientes de difusão de eucaliptol em SC-CO2 nas gamas de 202 – 252 bar e 313.15 – 333.15 K. Os resultados experimentais foram analisados através de correlações e modelos preditivos para D12.

New stimuli-responsive block random copolymers and their aggregation

Les polymères sensibles à des stimuli ont été largement étudiés ces dernières années notamment en vue d’applications biomédicales. Ceux-ci ont la capacité de changer leurs propriétés de solubilité face à des variations de pH ou de température. Le but de cette thèse concerne la synthèse et l’étude de nouveaux diblocs composés de deux copolymères aléatoires. Les polymères ont été obtenus par polymérisation radicalaire contrôlée du type RAFT (reversible addition-fragmentation chain-transfer). Les polymères à bloc sont formés de monomères de méthacrylates et/ou d’acrylamides dont les polymères sont reconnus comme thermosensibles et sensible au pH. Premièrement, les copolymères à bloc aléatoires du type AnBm-b-ApBq ont été synthétisés à partir de N-n-propylacrylamide (nPA) et de N-ethylacrylamide (EA), respectivement A et B, par polymérisation RAFT. La cinétique de copolymérisation des poly(nPAx-co-EA1-x)-block-poly(nPAy-co-EA1-y) et leur composition ont été étudiées afin de caractériser et évaluer les propriétés physico-chimiques des copolymères à bloc aléatoires avec un faible indice de polydispersité . Leurs caractères thermosensibles ont été étudiés en solution aqueuse par spectroscopie UV-Vis, turbidimétrie et analyse de la diffusion dynamique de la lumière (DLS). Les points de trouble (CP) observés des blocs individuels et des copolymères formés démontrent des phases de transitions bien définies lors de la chauffe. Un grand nombre de macromolécules naturels démontrent des réponses aux stimuli externes tels que le pH et la température. Aussi, un troisième monomère, 2-diethylaminoethyl methacrylate (DEAEMA), a été ajouté à la synthèse pour former des copolymères à bloc , sous la forme AnBm-b-ApCq , et qui offre une double réponse (pH et température), modulable en solution. Ce type de polymère, aux multiples stimuli, de la forme poly(nPAx-co-DEAEMA1-x)-block-poly(nPAy-co-EA1-y), a lui aussi été synthétisé par polymérisation RAFT. Les résultats indiquent des copolymères à bloc aléatoires aux propriétés physico-chimiques différentes des premiers diblocs, notamment leur solubilité face aux variations de pH et de température. Enfin, le changement d’hydrophobie des copolymères a été étudié en faisant varier la longueur des séquences des blocs. Il est reconnu que la longueur relative des blocs affecte les mécanismes d’agrégation d’un copolymère amphiphile. Ainsi avec différents stimuli de pH et/ou de température, les expériences effectuées sur des copolymères à blocaléatoires de différentes longueurs montrent des comportements d’agrégation intéressants, évoluant sous différentes formes micellaires, d’agrégats et de vésicules.

Nanostructure des particules polymériques : aspects physiques, chimiques et biologiques

Les nanotechnologies appliquées aux sciences pharmaceutiques ont pour but d’améliorer l’administration de molécules actives par l’intermédiaire de transporteurs nanométriques. Parmi les différents types de véhicules proposés pour atteindre ce but, on retrouve les nanoparticules polymériques (NP) constituées de copolymères “en bloc”. Ces copolymères permettent à la fois l’encapsulation de molécules actives et confèrent à la particule certaines propriétés de surface (dont l’hydrophilicité) nécessaires à ses interactions avec les milieux biologiques. L’architecture retenue pour ces copolymères est une structure constituée le plus fréquemment de blocs hydrophiles de poly(éthylène glycol) (PEG) associés de façon linéaire à des blocs hydrophobes de type polyesters. Le PEG est le polymère de choix pour conférer une couronne hydrophile aux NPs et son l’efficacité est directement liée à son organisation et sa densité de surface. Néanmoins, malgré les succès limités en clinique de ces copolymères linéaires, peu de travaux se sont attardés à explorer les effets sur la structure des NPs d’architectures alternatives, tels que les copolymères en peigne ou en brosse. Durant ce travail, plusieurs stratégies ont été mises au point pour la synthèse de copolymères en peigne, possédant un squelette polymérique polyesters-co-éther et des chaines de PEG liées sur les groupes pendants disponibles (groupement hydroxyle ou alcyne). Dans la première partie de ce travail, des réactions d’estérification par acylation et de couplage sur des groupes pendants alcool ont permis le greffage de chaîne de PEG. Cette méthode génère des copolymères en peigne (PEG-g-PLA) possédant de 5 à 50% en poids de PEG, en faisant varier le nombre de chaînes branchées sur un squelette de poly(lactique) (PLA). Les propriétés structurales des NPs produites ont été étudiées par DLS, mesure de charge et MET. Une transition critique se situant autour de 15% de PEG (poids/poids) est observée avec un changement de morphologie, d’une particule solide à une particule molle (“nanoagrégat polymére”). La méthode de greffage ainsi que l’addition probable de chaine de PEG en bout de chaîne principale semblent également avoir un rôle dans les changements observés. L’organisation des chaînes de PEG-g-PLA à la surface a été étudiée par RMN et XPS, méthodes permettant de quantifier la densité de surface en chaînes de PEG. Ainsi deux propriétés clés que sont la résistance à l’agrégation en conditions saline ainsi que la résistance à la liaison aux protéines (étudiée par isothermes d’adsorption et microcalorimétrie) ont été reliées à la densité de surface de PEG et à l’architecture des polymères. Dans une seconde partie de ce travail, le greffage des chaînes de PEG a été réalisé de façon directe par cyclo-adition catalysée par le cuivre de mPEG-N3 sur les groupes pendants alcyne. Cette nouvelle stratégie a été pensée dans le but de comprendre la contribution possible des chaines de PEG greffées à l’extrémité de la chaine de PLA. Cette librairie de PEG-g-PLA, en plus d’être composée de PEG-g-PLA avec différentes densités de greffage, comporte des PEG-g-PLA avec des PEG de différent poids moléculaire (750, 2000 et 5000). Les chaines de PEG sont seulement greffées sur les groupes pendants. Les NPs ont été produites par différentes méthodes de nanoprécipitation, incluant la nanoprécipitation « flash » et une méthode en microfluidique. Plusieurs variables de formulation telles que la concentration du polymère et la vitesse de mélange ont été étudiées afin d’observer leur effet sur les caractéristiques structurales et de surface des NPs. Les tailles et les potentiels de charges sont peu affectés par le contenu en PEG (% poids/poids) et la longueur des chaînes de PEG. Les images de MET montrent des objets sphériques solides et l'on n’observe pas d’objets de type agrégat polymériques, malgré des contenus en PEG comparable à la première bibliothèque de polymère. Une explication possible est l’absence sur ces copolymères en peigne de chaine de PEG greffée en bout de la chaîne principale. Comme attendu, les tailles diminuent avec la concentration du polymère dans la phase organique et avec la diminution du temps de mélange des deux phases, pour les différentes méthodes de préparation. Finalement, la densité de surface des chaînes de PEG a été quantifiée par RMN du proton et XPS et ne dépendent pas de la méthode de préparation. Dans la troisième partie de ce travail, nous avons étudié le rôle de l’architecture du polymère sur les propriétés d’encapsulation et de libération de la curcumine. La curcumine a été choisie comme modèle dans le but de développer une plateforme de livraison de molécules actives pour traiter les maladies du système nerveux central impliquant le stress oxydatif. Les NPs chargées en curcumine, montrent la même transition de taille et de morphologie lorsque le contenu en PEG dépasse 15% (poids/poids). Le taux de chargement en molécule active, l’efficacité de changement et les cinétiques de libérations ainsi que les coefficients de diffusion de la curcumine montrent une dépendance à l’architecture des polymères. Les NPs ne présentent pas de toxicité et n’induisent pas de stress oxydatif lorsque testés in vitro sur une lignée cellulaire neuronale. En revanche, les NPs chargées en curcumine préviennent le stress oxydatif induit dans ces cellules neuronales. La magnitude de cet effet est reliée à l’architecture du polymère et à l’organisation de la NP. En résumé, ce travail a permis de mettre en évidence quelques propriétés intéressantes des copolymères en peigne et la relation intime entre l’architecture des polymères et les propriétés physico-chimiques des NPs. De plus les résultats obtenus permettent de proposer de nouvelles approches pour le design des nanotransporteurs polymériques de molécules actives.

Lean construction: Arenas of enactment, models of diffusion and the meaning of 'leanness'

The existing literature on lean construction is overwhelmingly prescriptive with little recognition of the social and politicised nature of the diffusion process. The prevailing production-engineering perspective too often assumes that organizations are unitary entities where all parties strive for the common goal of 'improved performance'. An alternative perspective is developed that considers the diffusion of lean construction across contested pluralistic arenas. Different actors mobilize different storylines to suit their own localized political agendas. Multiple storylines of lean construction continuously compete for attention with other management fashions. The conceptualization and enactment of lean construction therefore differs across contexts, often taking on different manifestations from those envisaged. However, such localized enactments of lean construction are patterned and conditioned by pre-existing social and economic structures over which individual managers have limited influence. Taking a broader view, 'leanness' can be conceptualized in terms of a quest for structural flexibility involving restructuring, downsizing and outsourcing. From this perspective, the UK construction industry can be seen to have embarked upon leaner ways of working in the mid-1970s, long before the terminology of lean thinking came into vogue. Semi-structured interviews with construction sector policy-makers provide empirical support for the view that lean construction is a multifaceted concept that defies universal definition.

Determination of the gas diffusion coefficient of a peat grassland soil

Peatland habitats are important carbon stocks that also have the potential to be significant sources of greenhouse gases, particularly when subject to changes such as artificial drainage and application of fertilizer. Models aiming to estimate greenhouse gas release from peatlands require an accurate estimate of the diffusion coefficient of gas transport through soil (Ds). The availability of specific measurements for peatland soils is currently limited. This study measured Ds for a peat soil with an overlying clay horizon and compared values with those from widely available models. The Ds value of a sandy loam reference soil was measured for comparison. Using the Currie (1960) method, Ds was measured between an air-filled porosity (ϵ) range of 0 and 0.5 cm3 cm−3. Values of Ds for the peat cores ranged between 3.2 × 10−4 and 4.4 × 10−3 m2 hour−1, for loamy clay cores between 0 and 4.7 × 10−3 m2 hour−1 and for the sandy reference soil they were between 5.4 × 10−4 and 3.4 × 10−3 m2 hour−1. The agreement of measured and modelled values of relative diffusivity (Ds/D0, with D0 the diffusion coefficient through free air) varied with soil type; however, the Campbell (1985) model provided the best replication of measured values for all soils. This research therefore suggests that the use of the Campbell model in the absence of accurately measured Ds and porosity values for a study soil would be appropriate. Future research into methods to reduce shrinkage of peat during measurement and therefore allow measurement of Ds for a greater range of ϵ would be beneficial.

Diffusion analysis of one photosensitizer in bovine teeth using fluorescence optical imaging

Some photosensitizers (PSs) used for PACT (Antimicrobial Photodynamic Therapy) show an affinity for bacterial walls and can be photo-activated to cause the desired damage. However, on dentine bacterias may be less susceptible to PACT as a result of limited penetration of the PS. The aim of this study was to evaluate the diffusion of one PS based on hematoporphyrin on dentine structures. Twelve bovine incisors were used. Class III cavities (3 x 3 x 1 mm) were prepared on the mesial or distal surfaces using a diamond bur. Photogem (R) solution at 1 mg/mL (10 uL for each cavity) was used. The experimental Groups were divided according to thickness of dentine remaining and etched or no-etched before the PS application. The fluorescence excitation source was a VelScope (R) system. For image capture a scientific CCD color camera PixelFly (R) was coupled to VelScope. For image acquisition and processing, a computational routine was developed at Matlab (R). Fick's Law was used to obtain the average diffusion coefficient of PS. Differences were found between all Groups. The longitudinal temporal diffusion was influenced by the different times, thickness and acid etching.

Comparison of teicoplanin disk diffusion and broth microdilution methods against clinical isolates of Staphylococcus aureus and S. epidermidis

The CLSI M100-S19 document has recommended the disuse of vancomycin disks for staphylococci and informed that studies on the action of teicoplanin in disk-diffusion testing should be performed. We describe the comparison of two methods, disk diffusion and broth microdilution, for determining teicoplanin susceptibility in clinical isolates of staphylococci. Overall results showed an aggregation rate of 96.8%; Staphylococcus aureus showed total agreement while S. epidermidis showed 93.8% of agreement. According to these local results, disk diffusion can still be employed to teicoplanin susceptibility determination for staphylococci in our institution.

The aggregation process in tetraethoxysilane-derived sonogels as an analogy to the critical phenomenon

The structural evolution in silica sols prepared from tetraethoxysilane (TEOS) sonohydrolysis was studied 'in situ' using small-angle x-ray scattering (SAXS). The structure of the gelling system can be reasonably well described by a correlation function given by gamma(r) similar to (1/R(2))(1/r) exp(- r/xi), where xi is the structure correlation length and R is a chain persistence length, as an analogy to the Ornstein-Zernike theory in describing critical phenomenon. This approach is also expected for the scattering from some linear and branched molecules as polydisperse coils of linear chains and random f-functional branched polycondensates. The characteristic length. grows following an approximate power law with time t as xi similar to t(1) (with the exponent quite close to 1) while R remains undetermined but with a constant value, except at the beginning of the process in which the growth of. is slower and R increases by only about 15% with respect to the value of the initial sol. The structural evolution with time is compatible with an aggregation process by a phase separation by coarsening. The mechanism of growth seems to be faster than those typically observed for pure diffusion controlled cluster-cluster aggregation. This suggests that physical forces (hydrothermal forces) could be actuating together with diffusion in the gelling process of this system. The data apparently do not support a spinodal decomposition mechanism, at least when starting from the initial stable acid sol studied here.

Structure and aggregation kinetics of vinyltriethoxysilane-derived organic/silica hybrids

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

A SAXS study of kinetics of aggregation of TEOS-derived sonogels at different temperatures

The kinetics of aggregation of tetraethoxysilane (TEOS)-derived silica sols, produced by acid-catalyzed and ultrasound-stimulated hydrolysis, were studied by 'in situ' measurements of small-angle X-ray scattering (SAXS) at the temperatures 40 degreesC, 60 degreesC and 70 degreesC. The results were analyzed in terms of the evolution with time (t) of the SAXS intensity probing the mass fractal characteristics of the system, the average radius of gyration (Rc,) of the clusters and the number of primary particles per cluster. The aggregation process yields mass fractal structures which exhibit a scattering exponent (alpha) practically equal to 2, in the probed length scale range (5.3 nm < 1/q < 0.22 nm), beneath and even far beyond the gel point. This suggests that a is a direct measure of the real mass fractal dimension (D) of the structure. The precursor sol (pH = 2) exhibits I nm mean sized clusters with mass fractal dimension D similar to 1.9. Increasing the pH to 4.5, the cluster mean size and the number of primary particles per cluster increase but the system keeps a more opened structure (D similar to 1.4). In the first aggregation stages, D increases up to similar to2 by incorporating primary particles to the clusters without changing their mean size. From this stage, the aggregation progresses following a thermally activated scaling law well described by R-G similar tot(1/D) in all cases. This is indicative of a diffusion-controlled cluster-cluster aggregation process. The activation energy of the process was found to be 91.7 kJ/mol. (C) 2001 Elsevier B.V. B.V. All rights reserved.