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General Non-equilibrium Theory of Colloid Dynamics

A non-equilibrium extension of Onsager's canonical theory of thermal fluctuations is employed to derive a self-consistent theory for the description of the statistical properties of the instantaneous local concentration profile n(r,t) of a colloidal liquid in terms of the coupled time evolution equations of its mean value n(r,t) and of the covariance σ(r,r';t) \equiv <δn(r,t)δn(r',t)> of its fluctuations δn(r, t) = n(r, t) - n(r, t). These two coarse-grained equations involve a local mobility function b(r, t) which, in its turn, is written in terms of the memory function of the two-time correlation function C(r, r' ; t, t') \equiv <δn(r, t)δn(r',t')>. For given effective interactions between colloidal particles and applied external fields, the resulting self-consistent theory is aimed at describing the evolution of a strongly correlated colloidal liquid from an initial state with arbitrary mean and covariance n^0(r) and σ^0(r,r') towards its equilibrium state characterized by the equilibrium local concentration profile n^(eq)(r) and equilibrium covariance σ^(eq)(r,r'). This theory also provides a general theoretical framework to describe irreversible processes associated with dynamic arrest transitions, such as aging, and the effects of spatial heterogeneities.