Robust and Efficient Auxiliary Density Perturbation Theory Calculations.

Abstract

A new iterative solver for the recently developed time-dependent auxiliary density perturbation theory is presented. It is based on the Eirola-Nevanlinna algorithm for large nonsymmetric linear equation systems. The new methodology is validated by static and dynamic polarizability calculations of small molecules. Comparison between the analytic and iterative solutions of the response equation system shows excellent agreement for the calculated static and dynamic polarizabilities. The new iterative solver reduces the formal scaling from [Symbol: see text](N(4)) to [Symbol: see text](N(3)). Furthermore, the observed computational scaling for linear alkane chains is N(1.6). This subquadratic behavior is possible in systems with a few hundred atoms because of the very small prefactors of the [Symbol: see text](N(3)) and [Symbol: see text](N(2)) steps remaining in the iterative solver. To demonstrate the potential of this new methodology, static polarizabilities of giant fullerenes up to C960, with more than 14,000 basis functions, are calculated.