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Register a new userForce-induced desorption of uniform block copolymers
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Esaias J Janse van Rensburg
Publication date
2020
fields
Physics
and research's language is
English
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We investigate self-avoiding walk models of linear block copolymers adsorbed at a surface and desorbed by the action of a force. We rigorously establish the dependence of the free energy on the adsorption and force parameters, and the form of the phase diagram for several cases, including $AB$-diblock copolymers and $ABA$-triblock copolymers, pulled from an end vertex and from the central vertex. Our interest in block copolymers is partly motivated by the occurrence of a novel mixed phase in a directed walk model of diblock copolymers cite{Iliev} and we believe that this paper is the first rigorous treatment of a self-avoiding walk model of the situation.
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We analyze the phase diagrams of self-avoiding walk models of uniform branched polymers adsorbed at a surface and subject to an externally applied vertical pulling force which, at critical values, desorbs the polymer. In particular, models of adsorbed branched polymers with homeomorphism types stars, tadpoles, dumbbells and combs are examined. These models generalize earlier results on linear, ring and $3$-star polymers. In the case of star polymers we confirm a phase diagram with four phases (a free, an adsorbed, a ballistic, and a mixed phase) first seen in the paper by Janse van Rensburg EJ and Whittington SG 2018 J. Phys. A: Math. Theor. 51 204001 for $3$-star polymers. The phase diagram of tadpoles may include four phases (including a mixed phase) if the tadpole is pulled from the adsorbing surface by the end vertex of its tail. If it is instead pulled from the middle vertex of its head, then there are only three phases (the mixed phase is absent). For a dumbbell pulled from the middle vertex of a ring, there are only three phases. For combs with $t$ teeth there are four phases, independent of the value of $t$ for all $t ge 1$.
We investigate the phase diagram of a self-avoiding walk model of a 3-star polymer in two dimensions, adsorbing at a surface and being desorbed by the action of a force. We show rigorously that there are four phases: a free phase, a ballistic phase, an adsorbed phase and a mixed phase where part of the 3-star is adsorbed and part is ballistic. We use both rigorous arguments and Monte Carlo methods to map out the phase diagram, and investigate the location and nature of the phase transition boundaries. In two dimensions, only two of the arms can be fully adsorbed in the surface and this alters the phase diagram when compared to 3-stars in three dimensions.
We consider a simple cubic lattice self-avoiding walk model of 3-star polymers adsorbed at a surface and then desorbed by pulling with an externally applied force. We determine rigorously the free energy of the model in terms of properties of a self-avoiding walk, and show that the phase diagram includes 4 phases, namely a ballistic phase where the extension normal to the surface is linear in the length, an adsorbed phase and a mixed phase, in addition to the free phase where the model is neither adsorbed nor ballistic. In the adsorbed phase all three branches or arms of the star are adsorbed at the surface. In the ballistic phase two arms of the star are pulled into a ballistic phase, while the remaining arm is in a free phase. In the mixed phase two arms in the star are adsorbed while the third arm is ballistic. The phase boundaries separating the ballistic and mixed phases, and the adsorbed and mixed phases, are both first order phase transitions. The presence of the mixed phase is interesting because it doesnt occur for pulled, adsorbed self-avoiding walks. In an atomic force microscopy experiment it would appear as an additional phase transition as a function of force.
The critical Casimir force (CCF) arises from confining fluctuations in a critical fluid and thus it is a fluctuating quantity itself. While the mean CCF is universal, its (static) variance has previously been found to depend on the microscopic details of the system which effectively set a large-momentum cutoff in the underlying field theory, rendering it potentially large. This raises the question how the properties of the force variance are reflected in experimentally observable quantities, such as the thickness of a wetting film or the position of a suspended colloidal particle. Here, based on a rigorous definition of the instantaneous force, we analyze static and dynamic correlations of the CCF for a conserved fluid in film geometry for various boundary conditions within the Gaussian approximation. We find that the dynamic correlation function of the CCF is independent of the momentum cutoff and decays algebraically in time. Within the Gaussian approximation, the associated exponent depends only on the dynamic universality class but not on the boundary conditions. We furthermore consider a fluid film, the thickness of which can fluctuate under the influence of the time-dependent CCF. The latter gives rise to an effective non-Markovian noise in the equation of motion of the film boundary and induces a distinct contribution to the position variance. Within the approximations used here, at short times, this contribution grows algebraically in time whereas, at long times, it saturates and contributes to the steady-state variance of the film thickness.
The equilibrium properties of a system of passive diffusing particles in an external magnetic field are unaffected by the Lorentz force. In contrast, active Brownian particles exhibit steady-state phenomena that depend on both the strength and the polarity of the applied magnetic field. The intriguing effects of the Lorentz force, however, can only be observed when out-of-equilibrium density gradients are maintained in the system. To this end, we use the method of stochastic resetting on active Brownian particles in two dimensions by resetting them to the line $x=0$ at a constant rate and periodicity in the $y$ direction. Under stochastic resetting, an active system settles into a nontrivial stationary state which is characterized by an inhomogeneous density distribution, polarization and bulk fluxes perpendicular to the density gradients. We show that whereas for a uniform magnetic field the properties of the stationary state of the active system can be obtained from its passive counterpart, novel features emerge in the case of an inhomogeneous magnetic field which have no counterpart in passive systems. In particular, there exists an activity-dependent threshold rate such that for smaller resetting rates, the density distribution of active particles becomes non-monotonic. We also study the mean first-passage time to the $x$ axis and find a surprising result: it takes an active particle more time to reach the target from any given point for the case when the magnetic field increases away from the axis. The theoretical predictions are validated using Brownian dynamics simulations.
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