Inelastic Neutron Scattering and Density Functional Theory–Molecular Dynamics Study of Si Dynamics inTi3SiC2

Abstract

Observed differences between measured and calculated elastic constants forTi3SiC2are investigated using Density Functional Theory and Inelastic Neutron Scattering. The agreement between the calculated lattice dynamics and the dynamics measured by inelastic neutron scattering is considered good except at energies below ~20 meV where discrepancies suggest anharmonic potentials. This suggestion is confirmed by Density Functional Theory—Molecular Dynamics simulation which shows multiple site occupancy of the Si atoms within the basal plane at finite temperature and produces a calculated inelastic spectrum in better agreement with the measured spectrum in the low‐energy region. The highly anharmonic potential energy surface of theSiatoms offers an explanation for the failure of elastic constants, calculated based on the harmonic approximation, to agree with initial experimental measurements.