Evolution of self-organized two-dimensional patterns of nanoclusters through demixing

A mixture of dodecanethiol-capped Au nanoparticles (AuNPs) and the amphiphilic fatty acid, stearic acid, spread as a monomolecular layer on water surface, is observed with Brewster angle microscopy (BAM) to form a two-dimensional network of AuNP clusters through demixing, at concentration of AuNPs by weight ((rho) over bar) > 10% and the surface pressure (pi) >= 10 mNm(-1). For pi = 15 mNm(-1), the number of nodes (n) remains unchanged till similar to 2 hours and then changes over to a lower n state, where the pattern consists of almost perfect circles with greater in-plane thickness of the AuNP lamellae. For the higher n state the mean-square fluctuation of BAM intensity remains flat and then decays as f(xi) = xi(2 alpha) with alpha similar to 0.6 (correlated fluctuations) over the length scales of 400 mu m-6 mu m and below 6 mu m, respectively. For the lower n state the fluctuation decays almost over the entire length scale with alpha = 0.3, indicating emergence of aperiodicity from quasiperiodicity and a changeover to anticorrelated fluctuations. These patterns can be looked at as two distinct chaotic trajectories in the I-I' phase space of the system (I being the scattered light intensity at any position of the pattern and I' its gradient) with characteristic Lyapunov exponents.