Water is of the utmost importance for life and technology. However, a genuinely predictive ab initio model of water has eluded scientists. We demonstrate that a fully ab initio approach, relying on the strongly constrained and appropriately normed (SCAN) density functional, provides such a description of water. SCAN accurately describes the balance among covalent bonds, hydrogen bonds, and van der Waals interactions that dictates the structure and dynamics of liquid water. Notably, SCAN captures the density difference between water and ice Ih at ambient conditions, as well as many important structural, electronic, and dynamic properties of liquid water. These successful predictions of the versatile SCAN functional open the gates to study complex processes in aqueous phase chemistry and the interactions of water with other materials in an efficient, accurate, and predictive, ab initio manner. Significance Water is vital to our everyday life, but its structure at a molecular level is still not fully understood from either experiment or theory. The latter is hampered by our inability to construct a purely predictive, first principles model. The difficulty in modeling water lies in capturing the delicate interplay among the many strong and weak forces that govern its behavior and phase diagram. Herein, molecular simulations with a recently proposed nonempirical quantum mechanical approach (the SCAN density functional) yield an excellent description of the structural, electronic, and dynamic properties of liquid water. SCAN (strongly constrained and appropriately normed)-based approaches, which describe diverse types of bonds in materials on an equal, accurate footing, will likely enable efficient and reliable modeling of aqueous phase chemistry.

Magic-angle twisted bilayer graphene (TBG) has attracted significant interest recently due to the discoveries of diverse correlated and topological states. In this work, we study the phonon properties in magic-angle TBG based on many-body classical potential and interatomic forces generated by a deep neural network trained with data from ab initio calculations. We have discovered a number of soft modes which can exhibit dipolar, quadrupolar, and octupolar vibrational patterns in real space, as well as some time-reversal breaking chiral phonon modes. We have further studied the phonon effects on the electronic structures by freezing certain soft phonon modes. We find that if a soft quadrupolar phonon mode is assumed to be frozen, the system would exhibit a charge order which is perfectly consistent with recent experiments. Moreover, once some low-frequency C_2z-breaking modes get frozen, the Dirac points at the charge neutrality point would be gapped out, which provides an alternative perspective to the origin of correlated insulator state at charge neutrality point.

Hydration in Mg²⁺ solutions is critical in the chemical and biological industries. Researchers have identified a rigid first hydration shell, but the effects of ion-water and hydrogen bonding (HB) interactions beyond the first shell of Mg²⁺, especially when ion pairs form at high concentrations, remain controversial. On the basis of density functional theory, machine learning molecular dynamics was performed to study the second shell of Mg²⁺ in MgCl₂ solutions at various concentrations. At low concentrations, while both SCAN and PBE+TS-vdW predict a rigid first shell, SCAN affords a more softened structure due to its weakened HB interaction. The weakened HB interaction reveals the retarding effect of Mg²⁺ on the water reorientation of the second shell. With an increasing concentration, SCAN reproduces the decreasing trend of the hydration number, which originates from Cl^- entering the second shell of Mg²⁺. Our results highlight the importance of accurately described ion-water interaction and HB interaction in the intermediate range.

Adsorption of polar monomers on ice surface, relevant to the physical/chemical reaction in ice clouds as well as growth of ice, remains an open issue partially due to the unusual surface characteristics with protons at the top layer of ice. Using first-principle calculations, we explore the adsorption properties of ice surface in terms of a surface proton order parameter, which characterizes the inhomogeneity of the dangling atoms on ice surface. We show that, due to an effective electric field created by dangling OH bonds and lone pairs of water molecules not only directly neighboring but also further away from the adsorbed polar molecule on the ice surface, the adsorption energy of polar monomer on ice surface exhibits large variance and a strong correlation with the proton order parameter of ice surface. Our results about the positive correlation between the inhomogeneity of ice surface and adsorption energies suggest that the physical/chemical reactions as well as the growth of ice may prefer to occur firstly on surfaces with larger proton order parameter.