Toward In Silico Prediction of CO2 Diffusion in Champagne Wines.

Carbon dioxide diffusion is the main physical process behind the formation and growth of bubbles in sparkling wines, especially champagne wines. By approximating brut-labeled champagnes as carbonated hydroalcoholic solutions, molecular dynamics (MD) simulations are carried out with six rigid water models and three CO2 models to evaluate CO2 diffusion coefficients. MD simulations are little sensitive to the CO2 model but proper water modeling is essential to reproduce experimental measurements. A satisfactory agreement with nuclear magnetic resonance (NMR) data is only reached at all temperatures for simulations based on the OPC and TIP4P/2005 water models; the similar efficiency of these two models is attributed to their common properties such as low mixture enthalpy, same number of hydrogen bonds, alike water tetrahedrality, and multipole values. Correcting CO2 diffusion coefficients to take into account their system-size dependence does not significantly alter the quality of the results. Estimates of viscosities deduced from the Stokes-Einstein formula are found in excellent agreement with viscometry on brut-labeled champagnes, while theoretical densities tend to underestimate experimental values. OPC and TIP4P/2005 water models appear to be choice water models to investigate CO2 solvation and transport properties in carbonated hydroalcoholic mixtures and should be the best candidates for any MD simulations concerning wines, spirits, or multicomponent mixtures with alike chemical composition.