Stochastic Density Functional Theory Through the Lens of the Multilevel Monte Carlo Method

Abstract. The stochastic density functional theory (sDFT) has exhibited advantages over the standard Kohn–Sham DFT method and has become an attractive approach for large-scale electronic structure calculations. The sDFT method avoids the expensive matrix diagonalization by introducing a set of random orbitals and approximating the density matrix via Chebyshev expansion of a matrix-valued function. In this work, we study the sDFT with a plane-wave discretization and discuss variance reduction algorithms in the framework of multilevel Monte Carlo methods. In particular, we show that the density matrix evaluation in sDFT can be decomposed into many levels by increasing the plane-wave cutoffs or the Chebyshev polynomial orders. This decomposition renders the computational cost independent of the discretization size or temperature. To demonstrate the efficiency of the algorithm, we provide a rigorous analysis of the statistical errors and present numerical experiments on some material systems.