Using molecular dynamics for multislice TEM simulation of thermal diffuse scattering in AlGaN

•Molecular dynamics simulations used to determine thermal displacements.•Used for frozen phonon simulations of CTEM and STEM.•Stillinger–Weber type potential derived for the thermal dynamics of AlGaN.•Displacement calculations in alloys including correlation.•Comparison to quantum mechanical calculated results shows very good agreement. For simulation of transmission electron microscopic images and diffraction patterns, the accurate inclusion of thermal diffuse scattering by phonons is important. In the frozen phonon multislice algorithm, this is possible, if thermal displacements according to the realistic, quantum mechanical distribution can be generated. For pure crystals, quantum mechanical calculations based on DFT yield those displacements. But for alloys one is usually restricted to the Einstein approximation, where correlations between atoms are neglected. In this article, molecular dynamics simulations are discussed and used as an alternative method for displacement calculation. Employing an empirical Stillinger–Weber type potential, classical motion is used as an approximation for the quantum mechanical dynamics. Thereby, correlations and possible static atomic displacements are inherently included. An appropriate potential is devised for AlGaN by fitting to force constant matrices determined from DFT and elastic constants of AlN and GaN. A comparison shows that the empiric potential reproduces phonon dispersions and displacement expectations from DFT references. The validity for alloys is successfully demonstrated by comparison to DFT calculations in special quasirandom structures. Subsequently, molecular dynamics were used in multislice simulations of both conventional and scanning TEM images. The resulting images are in very good agreement with DFT based calculations, while a slight yet significant deviation from Einstein approximation results can be seen, which can be attributed to the neglect of correlations in the latter. The presented potential hence proves to be a useful tool for accurate TEM simulations of AlGaN alloys.