Lattice model for water-solute mixtures

Furlan, Alexandre Penteado; Almarza, N. G.; Barbosa, Márcia C.

doi:10.1063/1.4964396

Cited by 6 publications

(4 citation statements)

References 66 publications

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“…This isotropic phase corresponds to the gas phase in the general model. As noted in the Introduction, continuous gas-HDL phase transitions have already been observed in simulations of the nonsymmetric two-dimensional 10 and three-dimensional 12,13,16 ALG models, while a discontinuous transition was found in the mean-field approach for the symmetric model considered here 17 . In the 2D case 10,17 , the transition is observed for reduced chemical potentials μ ≡ µ/γ 1.…”

Section: Modelmentioning

confidence: 54%

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Order-disorder transition in a two-dimensional associating lattice gas

2019

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We study an associating lattice gas (ALG) using Monte Carlo simulation on the triangular lattice and semianalytical solutions on Husimi lattices. In this model, the molecules have an orientational degree of freedom and the interactions depend on the relative orientations of nearest-neighbor molecules, mimicking the formation of hydrogen bonds. We focus on the transition between the high-density liquid (HDL) phase and the isotropic gas phase in the limit of full occupancy, corresponding to chemical potential µ → ∞, which has not yet been studied systematically. Simulation results show a continuous phase transition at τ c = k B T c /γ = 0.4763(1) (where −γ is the bond energy) between the low-temperature HDL phase, with a non-vanishing mean orientation of the molecules, and the high-temperature isotropic phase. Results for critical exponents and the Binder cumulant indicate that the transition belongs to the three-state Potts model universality class, even though the ALG Hamiltonian does not have the full permutation symmetry of the Potts model. In contrast with simulation, the Husimi lattice results furnish a discontinuous phase transition, characterized by a discontinuity of the nematic order parameter. The transition temperatures (τ c = 0.51403 and 0.51207 for trees built with triangles and hexagons, respectively) are slightly higher than the one found via simulation. Since the Husimi lattice studies show that the ALG phase diagram features a discontinuous gas-HDL line for finite µ, three possible scenarios arise. The first is that in the limit µ → ∞ the first-order line ends in a critical point; the second is a change in the nature of the transition at some finite chemical potential; the third is that the entire line is one of continuous phase transitions. Results from other ALG models and the fact that mean-field approximations show a discontinuous phase transition for the three-state Potts model (known to possess a continuous transition) lends some weight to the third alternative.Following the ideas of Bell and Lavis, Henriques and Barbosa introduced a two-dimensional (2D) associating arXiv:1903.08306v1 [cond-mat.stat-mech]

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Section: Modelmentioning

confidence: 54%

“…Variants of the ALG model have been investigated, among them, three-dimensional (3D) [11][12][13] and symmetric versions 14,15 . The 3D model 11,12 is defined on a bodycentered cubic lattice in which each molecule possesses four bonding, and four inert arms.…”

Section: Introductionmentioning

confidence: 99%

Order-disorder transition in a two-dimensional associating lattice gas

2019

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“…Several modifications of the H&B model have been proposed 22,35,40 . Of particular interest here is the symmetric version introduced by Balladares et al 22 , in which no distinction is made between donor and acceptor arms.…”

Section: Introductionmentioning

confidence: 99%

Phase diagram and critical properties of a two-dimensional associating lattice gas

Ibagon,

Furlan,

Oliveira

et al. 2021

Preprint

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We revisit the associating lattice gas (ALG) introduced by Henriques et al. [PRE 71, 031504 (2005)] in its symmetric version. In this model, defined on the triangular lattice, interaction between molecules occupying nearest-neighbor sites depends on their relative orientation, mimicking the formation of hydrogen bonds in network-forming fluids. Although all previous studies of this model agree that it has a disordered fluid (DF), a low-density liquid (LDL) and a high-density liquid (HDL) phase, quite different forms have been reported for its phase diagram. Here, we present a thorough investigation of its phase behavior using both transfer matrix calculations and Monte Carlo (MC) simulations, along with finite-size scaling extrapolations. Results in striking agreement are found using these methods. The critical point associated with the DF-HDL transition at full occupancy, identified by Furlan and coworkers [Phys. Rev. E 100, 022109 (2019)] is shown to be one terminus of a critical line separating these phases. In opposition to previous simulation studies, we find that the transition between the DF and LDL phases is always discontinuous, similar to the LDL-HDL transition. The associated coexistence lines meet at the point where the DF-HDL critical line ends, making it critical-end-point. Overall, the form of the phase diagram observed in our simulations is very similar to that found in the exact solution of the model on a Husimi lattice. Our results confirm that, despite the existence of some waterlike anomalies in this model, it is unable to reproduce key features of the phase behavior of liquid water.

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“…Yet in comparison to pure water, the topology of the hydrogen bond network of these aqueous alcohols—which underpin their fundamenal physical properties—remains elusive. Depending upon the concentration, significant heterogeneity of the overall mixture may be observed, a feature that complicates experimental study and analysis of molecular simulations . Although the ensemble of hydrogen bonded environments may be complex, one specific experimental technique that can be used to probe the local geometric structure of hydrogen bonding molecules is X‐ray absorption spectroscopy (XAS) .…”

Section: Introductionmentioning

confidence: 99%

X‐ray absorption signatures of hydrogen‐bond structure in water–alcohol solutions

Stetina

Clark

2018

Int J of Quantum Chemistry

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Despite fundamental importance, the experimental characterization of the hydrogen bond network, particularly in multicomponent protic solutions, remains a challenge. Although recent work has experimentally validated that the oxygen K-edge X-ray absorption spectra is sensitive to local hydrogen bond patterns in pure water and aqueous alcohol solutions, the generality of this observation is unknown-as is the sensitivity to the electronic structure of the alcohol cosolvent. In this work, we investigate the electronic structure of water solvated alcohol model geometries using energy specific time-dependent density functional theory to calculate oxygen K-edge X-ray excitations. We find that the geometry of dangling hydrogen bonds in pure water is the main contributor to the pre-edge feature seen in the X-ray absorption spectra, agreeing with previous experimental and theoretical work. We then extend this result to solvated alcohol systems and observe a similar phenomenon, yet importantly, the increase of electron donation from alkyl chains to the alcohol OH group directly correlates to the strength of the core excitation on the dangling hydrogen bond model geometry. This trend arises from a stronger transition dipole moment due to electron localization on the OH group. K E Y W O R D S co-solvent, hydrogen bond, TDDFT, XAS

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Lattice model for water-solute mixtures

Cited by 6 publications

References 66 publications

Order-disorder transition in a two-dimensional associating lattice gas

Order-disorder transition in a two-dimensional associating lattice gas

Phase diagram and critical properties of a two-dimensional associating lattice gas

X‐ray absorption signatures of hydrogen‐bond structure in water–alcohol solutions

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