Toward GW Calculations on Thousands of Atoms

We provide the input files needed to reproduce the results of the article Toward GW Calculations on Thousands of Atoms J. Wilhelm, D. Golze, L. Talirz, J. Hutter, C. A. Pignedoli J. Phys. Chem. Lett. 9, 306–312 (2018) DOI:10.1021/acs.jpclett.7b02740 The GW approximation of many-body perturbation theory is an accurate method for computing electron addition and removal energies of molecules and solids. In a canonical implementation, however, its computational cost is in the system size N, which prohibits its application to many systems of interest. We present a full-frequency GW algorithm in a Gaussian-type basis, whose computational cost scales with N2 to N3. The implementation is optimized for massively parallel execution on state-of-the-art supercomputers and is suitable for nanostructures and molecules in the gas, liquid or condensed phase, using either pseudopotentials or all electrons. We validate the accuracy of the algorithm on the GW100 molecular test set, finding mean absolute deviations of 35 meV for ionization potentials and 27 meV for electron affinities. Furthermore, we study the length-dependence of quasiparticle energies in armchair graphene nanoribbons of up to 1734 atoms in size, and compute the local density of states across a nanoscale heterojunction.