Understanding thermodynamic properties, including also the phase behavior of poly mer solutions, polymer melts, and blends, has been a long-standing challenge [1][2][3][4][5][6][7]. Initially, the theoretical description was based on the lattice model introduced by Flory and Huggins [1][2][3][4][5][6][7]. In this model, a flexible macromolecule is represented by a (self-avoiding) random walk on a (typically simple cubic) lattice, such that each bead of the polymer takes one node of the lattice, and a bond between neighboring beads of the chain molecule takes a link of the lattice. For a binary polymer blend (A,B), two types of chains occur on the lattice (and possibly also free volume or vacant sites, which we denote as ). The model (normally) does not take into account any disparity in size and shape of the (effective) monomeric units of the two partners of a polymer mixture. Between (nearest neighbor) pairs AA, AB, and BB of effective monomers, pairwise interaction energies, e AA , e AB and e BB , are assumed. Thus, this model dis regards all chemical detail (as would be embodied in the atomistic modeling [8-10], where different torsional potentials and bond-angle potentials of the two constituents can describe different chain stiffness).Despite the simplicity of this lattice model, it is still a formidable problem of statistical mechanics, and its numerically exact treatment already requires largescale Monte Carlo simulations [11][12][13]. Consequently, the standard approach has been [1-7] to treat this Flory-Huggins lattice model in mean-field approximation, which leads to the following expression for the excess free energy density of mixing [4]:1:1Here w A , w B and w V 1 w B are the volume fractions of monomers of type A, B and of vacant sites, respectively. Every lattice site has to be taken by either w A Edited by Avraam I. Isayev