Surface and bulk stresses drive morphological changes in fibrous microtissues

Nikolaos Bouklas, Erik Mailand, Mahmut Selman Sakar
2019
Journal paper

Abstract

Engineered fibrous tissues consisting of cells encapsulated within collagen gels are widely used three-dimensional (3D) in vitro models of morphogenesis and wound healing. While cell-mediated matrix remodeling that occurs within these scaffolds has been extensively studied, less is known about the mesoscale physical principles governing the dynamics of tissue shape. Here we show, both experimentally and by using computer simulations, how surface contraction through the development of surface stresses (analogous to surface tension in fluids) coordinates with bulk contraction to drive shape evolution in constrained 3D microtissues. We used microelectromechanical systems (MEMS) technology to generate arrays of fibrous microtissues and robot-assisted microsurgery to perform local incisions and implantation. We introduce a technique based on phototoxic activation of a small molecule to selectively kill cells in a spatially controlled manner. The model simulations, which reproduced the experimentally observed shape changes after surgical and photochemical operations, indicate that fitting of only bulk and surface contractile moduli is sufficient for the prediction of the equilibrium shape of the microtissues. The computational and experimental methods we have developed provide a general framework to study and predict the morphogenic states of contractile fibrous tissues under external loading at multiple length scales.

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Fractal surfaces in adhesive wear processes.

Ramin Aghababaei, Tobias Brink, Enrico Milanese, Jean-François Molinari

Wear of materials plays a key role in the durability of manifactured objects and it has thus an economical importance in our society. In spite of the efforts, a unified picture of the underlying physics of the phenomenon is still far from being reached, because of the numerous mechanisms and processes that constitute the complexity of wear. Moving one step closer to the understanding of the physics of wear would mean enhancing our understanding of all the related fields that it affects, like friction and contact mechanics. The evolution of the surfaces morphology upon sliding is one of the aspects that need further investigations. In fact, while it is known that newly created surfaces by means of crack propagation are self-affine, what happens to existing surfaces rubbed against one another is still unclear. What is known from experimental studies is that self-affinity is preserved for highly abrasive wear and that in other cases the worn surface undergoes asymmetric changes with respect of its original mean plane. Surface roughness is also linked to the wear rate, as rough surfaces are found to deteriorate more in the running-in, up to the point that they have been smoothed enough and the wear rate becomes smaller and constant (the opposite happening for surface that are initially too smooth). As atomistic simulations have been proved to be an effective means of investigation for the understanding of the physics of wear, we adopt a recently developed approach to investigate the surface roughness evolution under adhesive wear processes (i.e, when the material loss is mainly due to transfer of particles from one body to another). The simulated system is two-dimensional, with periodic boundary conditions along the horizontal direction to allow for continuous sliding at constant velocity of the top surface over the bottom one. In the early stages of contact, the two surfaces form a debris particle that continuously rolls between them, interacting with them by removing material and deforming them. The peculiarity of the performed simulations is that they are long enough to allow for an investigation of the surfaces geometry evolution over time. The simulations display the two-regime evolution of the surfaces, characterized by high wear rate at running- in and lower wear rate in later stages of the process. Once the running-in is over, the morphology of the sliding surfaces and of the rolling debris particle are analyzed by means of their PSD. All the analyzed surfaces appear self-affine, and their heights are positively correlated. This type of roughness is consistent with the ones found in faults and, by analogy with gradient percolation models, hints that short range interactions prevail on long range elasticity. In some cases it is also observed that, after the running-in, the debris particle can heavily perturb the process increasing again the roughness of the mating surfaces, similarly to the running-in conditions. Despite the fact that this is not the picture commonly expected, it can be explained analyzing the debris particle geometry and the stress state at the contact interface. In particular, roughness enhancement happens by removal of material from the opposing surfaces when the particle is approximately round, while an irregular shape favours the presence of stress singularities in the particle itself and thus the deposit of material from the particle on the opposing surfaces. In this presentation we analyze different initial setups (i.e. different morphologies, system size, materials), seeing how the final self-affine morphology is independent of the initial state and how the shape of the rolling particle can alter the wear process.

2018

This thesis deals with a laboratory study of heterogeneous reactions involving bromine and chlorine containing reservoir species on alkali salt substrates which are relevant to the marine boundary layer, and on ice substrates which are relevant to the lower stratosphere. The aim is to obtain reliable data on uptake coefficients γ and reaction mechanisms for the sake of extrapolation of results obtained in the laboratory to atmospheric conditions. The experiments have been performed in a Teflon coated Knudsen flow reactor equipped with a quadrupole mass spectrometer. The reactions of BrONO2 with solid alkali halides have been studied at ambient temperature. The initial uptake coefficients γ0 of BrONO2 on NaCl and KBr substrates are γ0 = 0.31 ± 0.10 and γ0 = 0.32 ± 0.09, respectively. For NaCl substrates BrCl, Br2 and HCl and for KBr both Br2 and HBr are observed as products. HCl and HBr result from the interaction of NaCl and KBr, respectively, with HNO3 generated in the hydrolysis of BrONO2 with H2O condensed on the salt sample. Using NaCl we observed Br2 which is formed from heterogeneous BrONO2 decomposition occurring on solid KBr samples. Halogen exchange reactions are competing with hydrolysis and decomposition which also take place on non-reactive salts (NaNO3, Na2SO4). A high rate of initial uptake (0.2 ≤ γ0 ≤ 0.4) and a Br2 yield on the order of 50 % are observed on non-reactive salts with a closed mass balance for Br2. The ClONO2-salt system has been reinvestigated. Experiments on NaCl, KBr (reactive salts) and on NaNO3 and Na2SO4 (non-reactive salts) have been performed. The hydrolysis of ClONO2 was not observable in contrast to heterogeneous decomposition which occurred on non-reactive salts with a Cl2 yield of (25 ± 5) %. Calculations have been performed using a 0-D box model in order to observe the effects of heterogeneous chemistry on sea salt in the marine boundary layer. Chlorine and bromine chemistry is activated by heterogeneous reactions occurring on NaCl and KBr which are the sole sources of chlorine and bromine in the model. Simulations performed with chlorine heterogeneous chemistry and gas phase chemistry indicate: 1) Denitrification of the troposphere (NOy converted to solid nitrates). 2) Increase of the oxidative capacity of the troposphere by the release of Cl atoms. When bromine chemistry is added to the model, the recombination reaction of NO2 with BrO leads to an increase of tropospheric denitrification through formation of BrONO2. Calculations show that at high [NOx], the most important bromine reservoir is BrONO2, while at low [NOx] HOBr is the most important bromine reservoir. The uptake of HNO3 on ice, solid sulfuric acid solutions and solid ternary solutions (STS) has been investigated at 180 to 211 K. The uptake coefficient γ decreases from 0.30 at 180 K to 0.06 at 211 K. The Arrhenius representation shows two distinct regimes. The first at low temperatures (180-190 K) shows a constant value γ of 0.3, whereas the second regime at T > 195 K corresponds to an activation energy of Ea = -7 ± 1 kcal/mol. At a fixed temperature, γ is independent of [HNO3] thus confirming a rate law first order in [HNO3]. The γ values of HNO3 on H2SO4/H2O solid solutions linearly decreases from 0.20 (0.10) at 10 wt % H2SO4 to 0.05 (0.03) at 98 wt % H2SO4 at 180 K (200K). The γ values of HNO3 with STS of H2SO4/HNO3/H2O is equal to 0.10 ± 0.03 in the temperature range 185-195 K at conditions where the composition of the interface was held constant at the given temperature by adding an external flow of H2O. Br2O hydrolysis on ice surfaces occurs rapidly in the chosen temperature range of 180 to 210 K. At a fixed temperature the uptake kinetics follow an apparent first order rate law in [Br2O]. The observed negative temperature dependence leads to an activation energy Ea for heterogeneous hydrolysis of -2.3 ± 0.6 kcal/mol. These facts point towards a complex reaction mechanism implying that the interaction of Br2O with ice is not an elementary reaction. BrONO2 hydrolysis has been measured on bulk (B), condensed (C) and single crystal (SC) ice in the temperature range 180-210 K. On all types of ice, HOBr and Br2O are observed as products. At a fixed temperature the rate law is first order in [BrONO2] with γ ≈ 0.3 at 180 K. The observed negative temperature dependence leads to an activation energy Ea for the hydrolysis of BrONO2 on pure ice of -2.0 ± 0.2, -2.1 ± 0.2 and -6.6 ± 0.3 kcal/mol on (C), (B) and (SC) ice, respectively, pointing towards different kinetics of BrONO2 on these different types of ice. Doping the ice samples with HBr leads to the formation of Br2, preceded by BrONO2 hydrolysis. The Arrhenius representation corresponds to an activation energy of Ea = -1.2 ± 0.2 kcal/mol. We investigated the structural properties of the near-surface region of various types of HX (X = Cl or Br) doped ice. Basically, we studied the time dependent [HX] in the interface region using the fast reaction titration XONO2 + HX → X2 + HNO3. These experiments reveal that HX is located near the surface of the substrate in a well defined region of thickness I. The HX molecules composing the interface are immediately available for the titration reaction, whatever the flow of XONO2. In the temperature range 190-200 K, we measured a value of IHCl = 43 ± 16, 250 ± 50 and 444 ± 120 nm for (SC), (C) and (B) ices, respectively and IHBr = 110 ± 15 nm on (C) ice at 205K. Finally, we assessed the bulk diffusion coefficient for HX, DHX by modeling our results according to Fick's laws of diffusion. We obtained values of DHCl = 4.5·10-15 - 1.0·10-12 cm2/s at 190 K and DHBr = (6.5 ± 3.0)·10-15 cm2/s at 205 K.

EPFL2001

The focus of this thesis was on the mechanisms of release of volatile molecules from smectite clay minerals. The weight loss was monitored by thermogravimetry, differential calorimetry, and mass spectrometry under isothermal conditions and under ramp temperature conditions. Modeling of the clay-volatile release systems was performed with the help of finite element method calculations at the macroscopic level and ab initio calculations at the molecular level. A first comparison between finite element method simulations and experimental data for the evaporation of bulk volatile liquids under a convective gas flow showed the calculations to be in good agreement with experiments. Results of the simulations were used to develop a semi-analytical model explaining the dependence of the evaporation on the total pressure, the carrier gas flow, the temperature, and material constants. In particular, its temperature dependence could be approximated to good accuracy by an Arrhenius-type equation derived from the semi-analytical model. Differential calorimetry measurements of the heats of vaporization showed equilibrium conditions at the surface of the liquids to be satisfied. The same approach was extended to the release of model volatiles (water, ethanol, ethyl acetate and toluene) from smectite clays. At high coverage, the release was found to be close to that for the bulk liquids. Its decrease with time followed the behaviour observed in the respective curves of the gas/condensed phase partition coefficients, the equilibrium desorption isotherms. Equilibrium condition at the surface of the sample was evidenced by a comparison between the measured heats of vaporization and the equilibrium desorption isotherms. The differences observed in the measured equilibrium desorption isotherms of the volatile on the smectite clays could be rationalized by the use of ab initio calculations of the binding of the volatiles on the surface of a sodium smectite clay. At low coverage, the differences could be attributed to their differences in binding energies with the clay counter ions, which could be explained in terms of the chemical nature of the interacting species. At high coverage, the differences could be related to the properties of the bulk liquids, because high coverage corresponds to high activities of the volatiles on the clay samples. The differences observed in the measured rates of release of the volatiles from the smectite clays could be rationalized by the use of finite element calculations and the semi-analytical model developed for the bulk liquids, taking as input parameters the measured equilibrium desorption isotherms, that determines the volatile gas phase concentration at the surface of the sample. The slower rates of release of ethanol and ethyl acetate from the smectite clay, compared to water, could be explained from their differences in their equilibrium desorption isotherms from the clay, though diffusion effects also played a minor role. However, the slower rate of release of toluene, compared to water, could only be explained by its slow diffusion in the smectite clay. Diffusion effects were found to be enhanced with an increase in the size of the aggregate, such that, in addition to the binding strength of the counter ions, the swelling capacity of the clay, allowing the clay to clump, was also found to be an important factor for the controlled release of volatiles from the clay. Ion-exchange of the clay with lithium cations was found to be optimal in terms of ionic strength of the cation and swelling capacity, as compared to other metallic cations and small organic cations. This clay modification was tested on the release of malodorous compounds determined in cat urine by mass spectrometry and sniffing experiments. The smectite clay modified by ion-exchange with lithium cations showed improved controlled release of volatile organic compounds found in cat urine, compared to the sodium smectite, and improved clumping capacity compared to the calcium smectite. The calcium smectite clay used by Nestlé Purina could be modified by column exchange with lithium cations in high quantities. However the potential toxicity of the lithium is unknown. Additional information was obtained by ab initio calculations on the interaction of water with the smectite. The calculations of the binding of one to six water molecules on the surface of a sodium clay showed the water molecules bind to the cation and form hydrogen bonds between each other and with the clay oxygens, leading to the formation of different configurations for the same number of water molecules on the clay surface. With an increase in the number of water molecules on the surface of the clay, intermolecular interaction between the water molecules became gradually more important than sodium-water interactions. The binding energy was also found to be dependent on the location of the charge substitution in the clay (tetrahedral or octahedral) and to the formation of hydrogen bonds between the water molecule and a basal oxygen linked to a tetrahedral replacement. With an increase in the number of water molecules bound to one counter ion, the sodium counter ion was found to move away from the clay surface. The dynamic calculations of water molecules in the clay interlayer showed both the water molecules and the cations to be mobile. The average diffusion coefficient of the water molecules was reduced compared to that of bulk water, due to restrictions imposed by both the clay platelets and the counter ions. The structure of the water molecules showed to be similar to that of bulk water with a preferential orientation of their hydroxyl group almost perpendicular to the clay surface. The difference in the state of order of the water molecules around the sodium cation was interpreted as a symptom of hysteresis as observed in the measured equilibrium sorption isotherm.

EPFL2009

EPFL2001

Fractal surfaces in adhesive wear processes.

Ramin Aghababaei, Tobias Brink, Enrico Milanese, Jean-François Molinari

2018

EPFL2009