22 research outputs found
Evolution of entanglements during the response to a uniaxial deformation of lamellar triblock copolymers and polymer glasses
Using coarse-grained molecular-dynamics simulations, a generic
styrene-(block)-butadiene-(block)-styrene (SBS) triblock copolymer under
lamellar conformation is used in order to investigate the mutual entanglement
evolution when a structure of alternating glassy (S)/rubbery (B) layers is
submitted to an imposed deformation. By varying the amount of loop chains
between each phase, i.e. noncrossing chains, it is possible to generate
different types of S/B interface definitions. A specific boundary driven
tensile strain protocol has been developed in order to mimic "real" experiments
and measure the stress-strain curve. The same protocol is also applied to a
reference state consisting in a directed glassy homopolymers, as well as to an
isotropic glassy polymer. The evolution of initial mutual entanglements from
the undeformed samples during the whole deformation process is monitored. It is
shown for all considered systems that initial entanglements mostly participate
to the preyield regime of the stress-strain curve and that this network is
debonded during the strain-hardening regime. For triblocks with a non-null
amount of crossing chains, the lower the amount is, the longer the memory
effect of the initial entanglement network in the postyield regime is. On the
fly distributions of entanglements, which depart from the postyield regime,
depict memory effects and long time correlations during the strain-hardening
regime. For triblocks, loop chains reinforce these effects.Comment: 10 pages, 11 figure
Inhomogeneous elastic response of silica glass
Using large scale molecular dynamics simulations we investigate the
properties of the {\em non-affine} displacement field induced by macroscopic
uniaxial deformation of amorphous silica,a strong glass according to Angell's
classification. We demonstrate the existence of a length scale
characterizing the correlations of this field (corresponding to a volume of
about 1000 atoms), and compare its structure to the one observed in a standard
fragile model glass. The "Boson-peak'' anomaly of the density of states can be
traced back in both cases to elastic inhomogeneities on wavelengths smaller
than , where classical continuum elasticity becomes simply unapplicable
Statics of polymer droplets on deformable surfaces
The equilibrium properties of polymer droplets on a soft deformable surface
are investigated by molecular dynamics simulations of a bead-spring model. The
surface consists of a polymer brush with irreversibly end-tethered linear
homopolymer chains onto a flat solid substrate. We tune the softness of the
surface by varying the grafting density. Droplets are comprised of bead-spring
polymers of various chain lengths. First, both systems, brush and polymer
liquid, are studied independently in order to determine their static and
dynamic properties. In particular, using a numerical implementation of an AFM
experiment, we measure the shear modulus of the brush surface and compare the
results to theoretical predictions. Then, we study the wetting behavior of
polymer droplets with different contact angles and on substrates that differ in
softness. Density profiles reveal, under certain conditions, the formation of a
wetting ridge beneath the three-phase contact line. Cap-shaped droplets and
cylindrical droplets are also compared to estimate the effect of the line
tension with respect to the droplet size. Finally, the results of the
simulations are compared to a phenomenological free-energy calculation that
accounts for the surface tensions and the compliance of the soft substrate.
Depending on the surface/drop compatibility, surface softness and drop size, a
transition between two regimes is observed: from one where the drop surface
energy balances the adhesion with the surface, which is the classical
Young-Dupr\'e wetting regime, to another one where a coupling occurs between
adhesion, droplet and surface elastic energies.Comment: 13 pages, 11 figure
Molecular transport and flow past hard and soft surfaces: Computer simulation of model systems
The properties of polymer liquids on hard and soft substrates are
investigated by molecular dynamics simulation of a coarse-grained bead-spring
model and dynamic single-chain-in-mean-field (SCMF) simulations of a soft,
coarse-grained polymer model. Hard, corrugated substrates are modelled by an
FCC Lennard-Jones solid while polymer brushes are investigated as a
prototypical example of a soft, deformable surface. From the molecular
simulation we extract the coarse-grained parameters that characterise the
equilibrium and flow properties of the liquid in contact with the substrate:
the surface and interface tensions, and the parameters of the hydrodynamic
boundary condition. The so-determined parameters enter a continuum description
like the Stokes equation or the lubrication approximation.Comment: 41 pages, 13 figure
Dynamic and elastic heterogeneities in a 2D model glass
A generic soft-glass prototype is considered, as the glass transition is approached. Using standard methods, and by means of Molecular Dynamics simulation, a growing critical length scale (DH) is extracted upon cooling. On the other hand, this glass is also well characterized in the low-temperature limit, from which it has been shown that its elastic response under applied deformation involves some correlated particle displacements called elastic heterogeneities (EH). We then first aim to address the connection between both lengths. As EH appear to involve some structural rearrangements, this problem then also address either the structural nature of DH or the suitability of DH to capture EH's formation. It is shown that standard methods upon cooling fail to capture the birth of EH, but mainly capture, for the lowest temperatures, fluctuations around an effective theory of elasticity for amorphous materials, in which the medium can be considered as continuous above a length scale of the order of DH. We then test a recently proposed theory of the critical slowing-down of supercooled liquids, which predicts some scaling laws for DH. Such scalings are recovered for our soft model glass