Bethe Salpeter Equation Spectra for Very Large Systems

TL;DR

This paper introduces an efficient stochastic method for calculating optical spectra of large molecules using the Bethe-Salpeter equation, significantly reducing computational cost and enabling analysis of systems with over 500 electrons.

Contribution

The paper presents a novel stochastic approach to compute the Coulomb interaction in Bethe-Salpeter spectra, achieving cubic scaling and enabling large system analysis.

Findings

Successfully computed spectra for a 520-electron fullerene system

Reduced computational time to less than 4000 core hours

Achieved cubic scaling with system size

Abstract

We present a highly efficient method for the extraction of optical properties of very large molecules via the Bethe-Salpeter equation. The crutch of this approach is the calculation of the action of the effective Coulombic interaction, $W$, through a stochastic TD Hartree propagation, which uses only 10 stochastic orbitals rather than propagating the full sea of occupied states. This leads to a scaling that is at most cubic in system size, with trivial MPI parallelization. We apply this new method to calculate the spectra and electronic density of the dominant excitons of a carbon-nanohoop bound fullerene system with 520 electrons, using less than 4000 core hours.