Coarsening in the electrohydrodynamic patterning of thin polymer films

Abstract

Periodic pillarlike microstructures can be created from initially flat polymer films via the electrohydrodynamic instabilities. Those patterns, however, are metastable. Our experimental observations show that the average pillar size increases slowly after linear growth. Major coarsening events then take place over times several orders of magnitude longer than the linear growth time. For all fill ratios, a logarithmic time dependence of the average pillar size can be identified, i.e., <S> proportional to ln t. Thicker films, however, have faster coarsening rates than thinner films. Linear stability analysis of the pseudosteady states reveals two major coarsening mechanisms, collision and Ostwald ripening, which can also be identified from experimental images. We then reduce the original partial differential equation (PDE) into a pair of ODEs, which govern the interaction between pillars due to the above two coarsening mechanisms. From this, a logarithm scaling law is obtained for both low and high fill ratios and the coarsening rate is slower for lower fill ratios, consistent with experimental observations. We also find that arrays with more uniform sizes tend to start coarsening later, but they coarsen faster than more "disperse" arrays, which could be possibly utilized in experiments for controlling the onset and speed of coarsening. The logarithm scaling in the electrohydrodynamic coarsening phenomenon, which differs from coarsening in spinodal decomposition and dewetting of thin liquid films, is due to the significant nonlinear effect of Maxwell stresses and geometric confinement on the disjoining pressure at both top and bottom electrodes.