Optical excitation from anti-causally corrected real-time dynamics in a minimal basis

Abstract

Here we demonstrate workably accurate estimation of optical excitation threshold for large systems comprising of hundreds of atoms through an anti-causally corrected(ACC) real-time dynamics(RTD) approach implemented in a minimal tight-binding basis constituted by the directed hybrid atomic Wannier orbitals. A correction to the Hamiltonian is applied anti-causally at all time steps to account for electron-hole interaction using the density-density response function. Minimality of basis and ease of transferability of parameters to large systems arises from the directed nature of the Wannierized hybrid basis orbitals used.With self-energy corrected TB parameters evaluated at the DFT + G 0 W 0 level, the proposed ACC-RTD scheme can be systematically parametrized to render optical excitation threshold for systems of experimentally realizable length-scales through inexpensive computation.