The influence of time-dependent hydrodynamics on polymer centre-of-mass motionC. P. Lowe1, A. F. Bakker2 and M. W. Dreischor1
1 van 't Hoff Institute for Molecular Science, The University of Amsterdam Nieuwe Achtergracht 166, 1018 WV Amsterdam, The Netherlands
2 Faculty of Applied Science, Delft University of Technology Lorentzweg 1, 2628 CJ Delft, The Netherlands
(Received 11 March 2003; accepted in final form 1 June 2004)
We describe simulations of isolated ideal polymer chains consisting of N monomers. The solvent is simulated using a dissipative ideal gas maintained at a set temperature by a Lowe-Andersen thermostat. By choosing a particular ratio of the Kuhn length to the monomer hydrodynamic radius, long-polymer scaling of the diffusion coefficient holds even for chains composed of a few beads. However, this requires that the model capture the hydrodynamics correctly on length scales equivalent to a typical solvent particle separation. It does. The decay of the centre-of-mass velocity autocorrelation function, C(t), for short chains scales rapidly to a function independent of N, so we can determine the long-polymer limit of the function. At long times it decays with an algebraic long-time tail of the form . This is consistent with the predictions of theories that take into account the time dependence of the intra-polymer hydrodynamic interactions. We argue that the scaling of the decay implies that the intra-polymer hydrodynamic interactions propagate on a surprisingly rapid time scale.
47.50.+d - Non-Newtonian fluid flows.
05.40.-a - Fluctuation phenomena, random processes, noise, and Brownian motion.
02.70.Ns - Molecular dynamics and particle methods.
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