Accelerating the Fermi-Löwdin Orbital Descriptor Optimizations for Self-Interaction Free Density Functional Theory Calculations.

The Fermi-Löwdin Self Interaction Correction (FLO-SIC) method was introduced to address the shortcomings of standard density functional approximation calculations by removing the spurious electron self-interaction [1-4]. Within this method, a set of Fermi orbital descriptors (FODs) need to be optimized to minimize the energy. Current FOD optimization algorithms require large numbers of steps and the number of steps grows with systems size, that is, as the number of FODs increases. Moreover, every step in this optimization process requires the time-consuming evaluation of single-particle potential energy functions. Here we propose a strategy to reduce the number of single particle potential evaluations, making the FOD optimization step in FLO-SIC calculations more efficient. We will present proof-of-concept results for small molecules and compare with existing optimization schemes.

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[3] M R Pederson 2015 J. Chem. Phys. 142 064112
[4] Z H Yang, M R Pederson and J P Perdew 2017 Phys. Rev. A 95(5) 052505