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We examine the ordering of the Lower Consolute Solution Temperatures (LCSTs) for a set of dimethylpyridines. Density functional theory (DFT) is used. The equilibrium geometries and binding energies of dimers, each comprised of a pair of dimethylpyridines in a sandwich conformation and one H2O molecule at a pivotal site between the nitrogens (the 21 dimer), are calculated. It was shown previously that dimer formation in the water-rich zone of the phase diagram has a crucial role in dimethylpyridine demixing. In the resulting dimer diffu
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