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Flaig, Denis; Ochsenfeld, Christian (2013): An extrapolation method for the efficient calculation of molecular response properties within Born-Oppenheimer molecular dynamics. In: Physical Chemistry Chemical Physics, Vol. 15, No. 23: pp. 9392-9396


The calculation of molecular response properties in dynamic molecular systems is a major challenge that requires sampling over many steps of, e. g., Born-Oppenheimer molecular dynamics (BO-MD) simulations. We present an extrapolation scheme to accelerate such calculations for multiple steps within BO-MD trajectories or equivalently within other sampling methods of conformational space. The extrapolation scheme is related to the one introduced by Pulay and Fogarasi Chem. Phys. Lett., 2004, 386, 272] for self-consistent field (SCF) energy calculations. We extend the extrapolation to the quantities within our density matrix-based Laplace-transformed coupled perturbed SCF (DL-CPSCF) method that allows for linear-scaling calculations of response properties for large molecular systems. Here, we focus on the example of calculating NMR chemical shifts for which the number of required DL-CPSCF iterations reduces by roughly 40-70%.