Discontinuous projection method for large, accurate electronic structure calculations in real space*

For decades, the planewave (PW) pseudopotential method has been the method of choice for large, accurate Kohn-Sham calculations of condensed matter systems, in ab initio molecular dynamics simulations in particular. However, due to its reliance on a Fourier basis, the method has proven notoriously difficult to parallelize at scale, thus limiting the length and time scales accessible. In this talk, we discuss new developments aimed at increasing the scales accessible substantially, while retaining the fundamental simplicity, systematic convergence, and generality instrumental to the PW method's success in practice. The key idea is to release the constraint of continuity in the basis set, and with the freedom so obtained, employ a basis of local Kohn-Sham eigenfunctions to solve the global Kohn-Sham problem. In so doing, the basis obtained is highly efficient, requiring just a few tens of basis functions per atom to attain chemical accuracy, while simultaneously strictly local, orthonormal, and systematically improvable. We show how this basis can be employed to accelerate current state-of-the-art real-space methods substantially by reducing the dimension of the real-space Hamiltonian by up to three orders of magnitude. Results for metallic and insulating systems of up to 27,000 atoms using up to 38,000 processors demonstrate the scalability of the methodology in a discontinuous Galerkin formulation. Proceeding via projection of the real-space Hamiltonian instead promises to reach larger scales still.