Using Neural Networks force fields to ascertain the quality of ab initio simulations of liquid water

Alberto Torres, Luana S. Pedroza, Marivi Fernandez-Serra,and Alexandre R.Rocha,  submitted to J. Phys. Chem. C (2021)

Using an end-to-end differentiable implementation of the Kohn-Sham self-consistent field equations, we obtain an accurate neural network-based exchange and correlation (XC) functional of the electronic density. The functional is optimized using information on both energy and density while exact constraints are enforced through an appropriate neural network architecture. We evaluate our model against different families of XC approximations and show that, for non-empirical functionals, there is a strong linear correlation between energy and density errors. We use this correlation to define a novel XC functional quality metric that includes both energy and density errors, leading to a new, improved way to rank different approximations. Judged by this metric, our machine-learned functional significantly outperforms those within the same rung of approximations.