New article on DFT and interfacial properties of hydrogen

Our new paper entitled Classical density functional theory for interfacial properties of hydrogen, helium, deuterium, neon, and their mixtures has been published in The Journal of Chemical Physics.

In the article, we present a classical density functional theory (DFT) for fluid mixtures that is based on a third-order thermodynamic perturbation theory of Feynman-Hibbs-corrected Mie potentials. The DFT is developed to study the interfacial properties of hydrogen, helium, neon, deuterium, and their mixtures, i.e., fluids that are strongly influenced by quantum effects at low temperatures. White Bear fundamental measure theory is used for the hard-sphere contribution of the Helmholtz energy functional, and a weighted density approximation is used for the dispersion contribution. For mixtures, a contribution is included to account for non-additivity in the Lorentz–Berthelot combination rule. Predictions of the radial distribution function from DFT are in excellent agreement with results from molecular simulations, both for pure components and mixtures. Above the normal boiling point and 5% below the critical temperature, the DFT yields surface tensions of neon, hydrogen, and deuterium with average deviations from experiments of 7.5%, 4.4%, and 1.8%, respectively. The surface tensions of hydrogen/deuterium, para-hydrogen/helium, deuterium/helium, and hydrogen/neon mixtures are reproduced with a mean absolute error of 5.4%, 8.1%, 1.3%, and 7.5%, respectively. The surface tensions are predicted with an excellent accuracy at temperatures above 20 K. The poor accuracy below 20 K is due to the inability of Feynman–Hibbs-corrected Mie potentials to represent the real fluid behavior at these conditions, motivating the development of new intermolecular potentials. This DFT can be leveraged in the future to study confined fluids and assess the performance of porous materials for hydrogen storage and transport.

This is an article together with my colleague at Porelab, Morten Hammer, and our collaborators at the University of Stuttgart, Gernot Bauer, Rolf Stierle, and Joachim Gross. We were so fortunate that the article ended up as a Featured article at the front page of Volume 158, Issue 10 of the Journal of Chemical Physics (see below).