Optical absorption spectra from the $GW$-Bethe-Salpeter framework for thousands of atoms

Abstract

The frequency-dependent absorption and emission of light determine the colors of matter and underpin today's technologies, from solar cells to light-emitting diodes. Predicting optical properties from first principles remains a computational challenge, especially for large and disordered systems. The $GW$ plus Bethe-Salpeter equation ($GW$-BSE) approach provides predictive accuracy for optical properties, but conventional implementations become costly as system size grows. Here, we present a $GW$-BSE framework combining real-time propagation, atom-centered basis sets, and a locally optimized real-space resolution of the identity. The cost of each propagation step scales quadratically with system size and roughly equals the cost of one self-consistent-field iteration in a density-functional calculation with a semilocal functional. This computational efficiency allows us to calculate the absorption spectrum of a nanographene containing 4616 atoms and opens a path toward routine calculations of optical properties for large disordered systems.