Exclusion statistics for structured particles on topologically correlated states. II. Multicomponent lattice gases.

Abstract

Statistical thermodynamics of particles having a spectrum of topological correlated states and observing statistical exclusion is developed to describe mixtures of species of arbitrary size and shape. A generalized statistical distribution is obtained through a configuration space ansatz recently introduced for single species accounting for the multiple exclusion statistical phenomena, where spatially correlated particle states can be simultaneously excluded by more than one particle. Statistical exclusion on a correlated states spectrum is characterized by exclusion statistical parameters β_{cij} which are self-consistently determined within the multiple exclusion from thermodynamic boundary conditions. Self-exclusion and cross-exclusion frequency functions e_{ij}(n) and average cumulative exclusion functions G_{ij}(n) are introduced to characterize the state exclusion spectrum as density varies. Haldane's statistics and Wu's distribution for statistically independent excluding species are recovered in the limit of uncorrelated states for single species as well as for mixtures of self- and cross-excluding species with constant mutual statistical exclusion. The multiple exclusion statistics formalism is applied to the k-mer problem on a square lattice rationalized as a mixture of two differently oriented self-excluding and cross-excluding pseudospecies. An isotropic-nematic and a high-density nematic-isotropic (disordered) phase transitions is predicted only for k≥7. The isotropic-nematic transition is continuum as expected, but the high-density transition results in a first-order one. The formalism provides phase coexistence lines and the chemical potential dependence of the low- and high-density branches in the nematic regime. The theoretical approach to lattice gases presented in this work offers a unique general framework applicable to mixtures of entropy-complex lattice gases. From this framework, k-mer phase transitions can be reproduced, and significant configuration features can be derived from the state exclusion spectrum functions.