RT Journal Article
T1 Transferable Classical Force Field for Pure and Mixed Metal Halide Perovskites Parameterized from First-Principles
A1 Seijas-Bellido, Juan Antonio
A1 Samanta, Bipasa
A1 Valadez-Villalobos, Karen
A1 Gallardo, Juan Jesús
A1 Navas, Javier
A1 Balestra, Salvador R. G.
A1 Madero Castro, Rafael María
A1 Vicent-Luna, Jose Manuel
A1 Tao, Shuxia
A1 Caspary Toroker, Maytal
A1 Anta, Juan
K1 Classical Molecular Dynamics
K1 Metal-halide perovskites
AB Many key features in photovoltaic perovskites occurin relatively long time scales and involve mixed compositions. Thisrequires realistic but also numerically simple models. In this workwe present a transferable classical force field to describe the mixedhybrid perovskite MAxFA1¿xPb(BryI1¿y)3 for variable composition(¿x, y ¿ [0, 1]). The model includes Lennard-Jones andBuckingham potentials to describe the interactions between theatoms of the inorganic lattice and the organic molecule, and theAMBER model to describe intramolecular atomic interactions.Most of the parameters of the force field have been obtained bymeans of a genetic algorithm previously developed to parametrizethe CsPb(BrxI1¿x)3 perovskite (Balestra et al. J. Mater. Chem. A.2020, DOI: 10.1039/d0ta03200j). The algorithm finds the best parameter set that simultaneously fits the DFT energies obtained forseveral crystalline structures with moderate degrees of distortion with respect to the equilibrium configuration. The resulting modelreproduces correctly the XRD patterns, the expansion of the lattice upon I/Br substitution, and the thermal expansion coefficients.We use the model to run classical molecular dynamics simulations with up to 8600 atoms and simulation times of up to 40 ns. Fromthe simulations we have extracted the ion diffusion coefficient of the pure and mixed perovskites, presenting for the first time thesevalues obtained by a fully dynamical method using a transferable model fitted to first-principles calculations. The values herereported can be considered as the theoretical upper limit, that is, without grain boundaries or other defects, for ion migrationdynamics induced by halide vacancies in photovoltaic perovskite devices under operational conditions.
PB American Chemical Society
SN 1549-9596
YR 2022
FD 2022-05-01
LK http://hdl.handle.net/10433/13900
UL http://hdl.handle.net/10433/13900
LA en
NO Journal of Chemical Education and Modelling
NO Identificador de proyecto: PCI2019-111839-2 (SCALEUP)
NO TU/e
DS RIO
RD May 9, 2026