A Multilayer Approach to the Equation of Motion Coupled-Cluster Method for the Electron Affinity

Abstract

We have presented a multilayer implementation of the equation of motion coupled-cluster method for the electron affinity, based on local and pair natural orbitals. The method gives consistent accuracy for both localized and delocalized anionic states and results in many-fold speed-up as compared to the canonical and DLPNO-based implementation of the EA-EOM-CCSD method. We have also developed an explicit fragment-based approach which can lead to even higher speed-up with little loss in accuracy. The multilayer method can be used to treat the environmental effect of both bonded and nonbonded nature on the electron attachment process in large molecules.