Efficient Calculation of the Energy of a Molecule in an Arbitrary Electric Field

by Pulay, P.; Janowski, T.

In thermodynamic (e.g., Monte Carlo) simulations with electronic embedding, the energy of the active site or solute must be calculated for millions of configurations of the environment (solvent or protein matrix) to obtain reliable statistics. This precludes the use of accurate but expensive ab initio and density functional techniques. Except for the immediate neighbors, the effect of the environment is electrostatic. We show that the energy of a molecule in the irregular field of the environment can be determined very efficiently by expanding the electric potential in known functions, and precalculating the first and second order response of the molecule to the components of the potential. These generalized multipole moments and polarizabilities allow the calculation of the energy of the system without further ab initio calculations. Several expansion functions were explored: polynomials, distributed inverse powers, and sine functions. The latter provide the numerically most stable fit but require new types of integrals. Distributed inverse powers can be simulated using dummy atoms, and energies calculated this way provide a very good approximation to the actual energies in the field of the environment.

Journal
International Journal of Quantum Chemistry
Volume
109
Issue
10
Year
2009
Start Page
2113-2120
URL
https://dx.doi.org/10.1002/qua.22064
ISBN/ISSN
1097-461X; 0020-7608
DOI
10.1002/qua.22064