Molecular-dynamics computer-simulation of an ionic molecular solid LiKSO₄ has been carried out at 300 and 1000 K using the atom-atom potentials obtained from lattice dynamical studies. We observe hopping of lithium ions to interstitial positions which is related to reorientations of sulphate tetrahedra.

Coherent inelastic neutron scattering measurements have been carried out on the high temperature superconductors Tl₂CaBa₂Cu₂O₈ (Tl-2122,T_c=107 K) and YBa₂Cu₃O₇ (Y-123,T_c=92 K), at the Dhruva reactor at Trombay. The density of phonon states in Tl-2122 is enhanced at 6–17 meV and reduced at 40–70meV compared to that in Y-123.

Rigid-ion model calculations of phonon dispersion relations, densities of states and partial densities of states of the highT_c superconductor La₂CuO₄ and its isostructural compound La₂NiO₄ have been carried out both in the tetragonal and orthorhombic phases of La₂CuO₄ and the tetragonal phase of La₂NiO₄. The calculations are in fair agreement with reported experiments. The computed phonon dispersion in the tetragonal phase of La₂CuO₄ reproduces the soft mode behaviour for the lowest Σ₄ TO branch which is found to harden in the orthorhombic phase, consistent with experimental data.

An empirical interatomic potential for YBa₂Cu₃O_7−δ is determined for different oxygen contents (δ=0 to 1), consisting of Coulomb and short-range interactions. The calculated structure and phonon spectrum, and the results of molecular-dynamics computer simulation on the orthorhombic-to-tetragonal phase transition are in fair agreement with reported experiments.

In this article we briefly review the lattice dynamics and molecular dynamics simulation techniques, as used for complex ionic and molecular solids, and demonstrate a number of applications through examples of our work. These computational studies, along with experiments, have provided microscopic insight into the structure and dynamics, phase transitions and thermodynamical properties of a variety of materials including fullerene, high temperature superconducting oxides and geological minerals as a function of pressure and temperature. The computational techniques also allow the study of the structures and dynamics associated with disorder, defects, surfaces, interfaces etc.

Molecular dynamics simulations, in combination with lattice dynamics studies, based on semiempirical interatomic potentials, have been very useful in the study of properties of complex novel materials at high temperature and pressure. Various properties such as the equation of state, elastic and thermodynamic properties, phase transitions and melting have been studied. These studies help in understanding the synthesis of important new and novel materials, especially the amorphous materials, compounds with unusually coordinated atoms, (e.g. with five-coordinated silicon atoms), materials with controlled thermal expansion, etc. A few examples will be discussed from our recent studies.