Efficient Calculation of Electrostatic Energies for Large-Scale Nonadiabatic Molecular Dynamics in a Site Basis
Samuele Giannini, Ljiljana Stojanovic, Matthew Ellis, Guido Falk von Rudorff, Jochen Blumberger
TL;DR
This paper introduces a more efficient method to calculate electrostatic energies in large-scale molecular simulations, improving accuracy and agreement with experimental results.
Contribution
A new computational scheme for efficiently calculating electrostatic energies in nonadiabatic molecular dynamics simulations.
Findings
Including electrostatic site energy fluctuations reduces hole delocalization and mobility in crystalline anthracene.
Electrostatics improve agreement with experimental mobilities and anisotropy without changing the transport mechanism.
Omitting electrostatic site energy disorder is reasonable for acenes but not sufficient for near-quantitative agreement with experiments.
Abstract
Nonadiabatic molecular dynamics simulation of charge and exciton transport in molecular materials and biological systems are often carried out in a (quasi-)diabatic or site basis. Such simulations require the calculation of the electrostatic site energy of all possible charge or excited states of the system at each molecular dynamics step, which quickly becomes computationally prohibitive when Ewald summation is used. By combining the damped shifted force real space electrostatic summation method with a suitable addition-subtraction scheme, we show that the calculation of electrostatic energy and forces for N mol site energies can be carried out at a small and system size independent overhead compared to the calculation for a single site energy. This advance enables us to include full electrostatic interactions in nonadiabatic molecular dynamics simulations for charge and exciton…
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Taxonomy
TopicsOrganic Electronics and Photovoltaics · Molecular Junctions and Nanostructures · Spectroscopy and Quantum Chemical Studies