Accelerating Optical Absorption Spectra and Exciton Energy Computation for Nanosystems via Interpolative Separable Density Fitting

Abstract: We present an efficient way to solve the Bethe-Salpeter equation (BSE), a model for the computation of absorption spectra in molecules and solids that includes electron-hole excitations. Standard approaches to construct and diagonalize the Bethe-Salpeter Hamiltonian require at least $\O(N_e^5)$ operations, where $N_e$ is proportional to the number of electrons in the system, limiting its application to small systems. Our approach is based on the interpolative separable density fitting (ISDF) technique to construct low rank approximations to the bare and screened exchange operators associated with the BSE Hamiltonian. This approach reduces the complexity of the Hamiltonian construction to $\O(N_e^3)$ with a much smaller pre-constant. Here, we implement the ISDF method for the BSE calculations within the Tamm-Dancoff approximation (TDA) in the BerkeleyGW software package. We show that ISDF-based BSE calculations in molecules and solids reproduce accurate exciton energies and optical absorption spectra with significantly reduced computational cost.