Polarization Energies from Efficient Representation of the Linear Density-Density Response Function

摘要

The authors present a proof-of-concept study for the calculation of atomic forces on a solvated molecule by means of the linear density-density response function in its moment expanded representation. The density-density response function represents an efficient way to compute molecular forces for arbitrary external potentials via an ab initio scheme, without the need to perform an explicit self-consistent quantum chemical calculation for each configuration of the chemical environment. Here, the authors show that it is indeed possible to determine the atomic forces of interacting bulk-like molecular complexes due to polarization effects of the surrounding molecules with good accuracy. This study represents a significant step the practical applicability of the approach, which is still in a development phase. The potential application of the computational scheme in terms of molecular dynamics simulations is illustrated by considering a variety of cluster conformations, as they would be found within a molecular dynamics trajectory.