Machine Learning the Physical Nonlocal Exchange–Correlation Functional of Density-Functional Theory

We train a neural network as the universal exchange-correlation functional of density-functional theory that simultaneously reproduces both the exact exchange-correlation energy and the potential. This functional is extremely nonlocal but retains the computational scaling of traditional local or semilocal approximations. It therefore holds the promise of solving some of the delocalization problems that plague density-functional theory, while maintaining the computational efficiency that characterizes the Kohn-Sham equations. Furthermore, by using automatic differentiation, a capability present in modern machine-learning frameworks, we impose the exact mathematical relation between the exchange-correlation energy and the potential, leading to a fully consistent method. We demonstrate the feasibility of our approach by looking at one-dimensional systems with two strongly correlated electrons, where density-functional methods are known to fail, and investigate the behavior and performance of our functional by varying the degree of nonlocality.