Double-charge model for classical force-field simulations

In a traditional classical force-field model, the atomic point charge that generates the electrostatic potential, and the Born charge induced by atomic movement, are represented by the same charge parameter. But their actual values can be very different, and correct values for both of them are needed in order to yield the correct atomic structure (electrostatic charge) and phonon spectrum (Born charge). This is particularly true for nanostructure calculations. Here, we introduce a double-charge model (DCM) to reconcile the difference between the electrostatic charge and Born charge. The DCM allows us to reproduce the accurate ab initio phonon spectrum not only in bulk systems, but also for nanostructures (slabs and nanowires). This enables the use of classical force fields to study phonon spectra of large nanostructures, which are important for many phenomena from carrier dynamics to thermo conductivities.