Version 2 2016-07-13, 18:06Version 2 2016-07-13, 18:06
Version 1 2016-07-13, 17:42Version 1 2016-07-13, 17:42
dataset
posted on 2016-06-22, 00:00authored byPeter Scherpelz, Marco Govoni, Ikutaro Hamada, Giulia Galli
We
present an implementation of G0W0 calculations including spin–orbit coupling
(SOC) enabling investigations of large systems, with thousands of
electrons, and we discuss results for molecules, solids, and nanocrystals.
Using a newly developed set of molecules with heavy elements (called
GW-SOC81), we find that, when based upon hybrid density functional
calculations, fully relativistic (FR) and scalar-relativistic (SR) G0W0 calculations
of vertical ionization potentials both yield excellent performance
compared to experiment, with errors below 1.9%. We demonstrate that
while SR calculations have higher random errors, FR calculations systematically
underestimate the VIP by 0.1 to 0.2 eV. We further verify that SOC
effects may be well approximated at the FR density functional level
and then added to SR G0W0 results for a broad class of systems. We also address
the use of different root-finding algorithms for the G0W0 quasiparticle equation
and the significant influence of including d electrons in the valence
partition of the pseudopotential for G0W0 calculations. Finally, we present
statistical analyses of our data, highlighting the importance of separating
definitive improvements from those that may occur by chance due to
a limited number of samples. We suggest the statistical analyses used
here will be useful in the assessment of the accuracy of a large variety
of electronic structure methods.