Liquid polymorphism, order-disorder transitions and anomalous behavior: A Monte Carlo study of the Bell–Lavis model for water

Abstract

Monte Carlo simulation strategies for computing the wetting properties of fluids at geometrically rough surfaces J. Chem. Phys. 135, 184702 (2011) Semi-bottom-up coarse graining of water based on microscopic simulations J. Chem. Phys. 135, 184101 (2011) Hydrophobic interactions in presence of osmolytes urea and trimethylamine-N-oxide J. Chem. Phys. 135, 174501 (2011) Potential of mean force between identical charged nanoparticles immersed in a size-asymmetric monovalent electrolyte J. Chem. Phys. 135, 164705 (2011) Additional information on J. Chem. Phys. The Bell-Lavis model for liquid water is investigated through numerical simulations. The lattice-gas model on a triangular lattice presents orientational states and is known to present a highly bonded low density phase and a loosely bonded high density phase. We show that the model liquid-liquid transition is continuous, in contradiction with mean-field results on the Husimi cactus and from the cluster variational method. We define an order parameter which allows interpretation of the transition as an order-disorder transition of the bond network. Our results indicate that the order-disorder transition is in the Ising universality class. Previous proposal of an Ehrenfest second order transition is discarded. A detailed investigation of anomalous properties has also been undertaken. The line of density maxima in the HDL phase is stabilized by fluctuations, absent in the mean-field solution.

Phase transition properties of the Bell-Lavis model

“…The spin-1 variables and mapping scheme to the BEG model were suggested by Young and Lavis 33 . This scheme was later employed by Barbosa et al 30 who used convenient lattice-gas variables to separately describe occupational and orientational ordering (see, also 31 ). In Ref.…”

“…30,34 the BL model was solved by the cluster variation method and a weak first-order phase transition was again obtained. Later Fiore et al 31 performed Monte Carlo (MC) calculations and attributed the transition to the Ising universality class, claiming that the first order phase transition obtained in previous papers was the artifact arising due to the Bethe-like (cluster) methods used for calculation.…”

Hydration and anomalous solubility of the Bell-Lavis model as solvent

“…AtT = 0, coexistence between a gas and a structured liquid of low density (SL) and coexistence between the structured low-density liquid and the nonstructured high-density liquid are present [32]. However, for finite temperatures, the transition between the two liquids becomes critical, as shown from detailed systematic analysis of simulational data [25]. The two liquid phases do not coexist and the density varies continuously at the phase transition as shown by susceptibility measurements on sublattice density fluctuations [27].…”

“…Both models present several of the anomalous features of water [14][15][16][17][18][19][20][21][22][23][24][25][26][27]. However, the second kind of model does not involve specific orientation of low-energy pairs of particles: pair energy is controlled by distance, not by orientation.…”

“…Our approach is that of a minimal statistical model. We consider a two-dimensional lattice model proposed originally by Bell and Lavis [7] and shown by us [25,27] to exhibit many anomalous properties despite the absence of liquid polymorphism. In this study we add noninteracting solute particles which occupy a single lattice site in order to investigate the effect of solute on solvent properties as well as the effect of solute solubility.…”