Density Functional Tight-Binding Model for Lithium-Silicon Alloys

OVIEDO, MA. BELÉN; FERNANDEZ, FRANCISCO; OTERO, MANUEL; LEIVA, EZEQUIEL P. M.; PAZ, S. ALEXIS; PAZ, S. ALEXIS

JOURNAL OF PHYSICAL CHEMISTRY A

AMERICAN CHEMICAL SOCIETY

Lugar: Washington; Año: 2023 vol. 127 p. 2637 - 2637

1089-5639

he predictive power of molecular dynamic simulations is mainly restricted by the time scale and model accuracy. Many systems of current relevance are of such complexity that requires addressing both issues simultaneously. This is the case of silicon electrodes in Li-ion batteries, where different Li$_x$Si alloys are formed during charge/discharge cycles. While first-principles treatments for this system are seriously limited by the computational cost of exploring its large conformational space, classical force-fields are not transferable enough to represent it accurately. Density Functional Tight-Binding (DFTB) is an intermediate complexity approach capable of capturing the electronic nature of different environments with a relatively low computational cost. In this work, we present a new set of DFTB parameters suited to model amorphous Li$_x$Si alloys. The latter is the usual finding upon cycling the Si electrodes in the presence of Li-ions. The model parameters are constructed with