Computer Simulations of Simple Liquids with Tetrahedral Local Order : the Supercooled Liquid, Solids and Phase Transitions

The understanding of complex condensed matter systems is an area of intense study. In this thesis, some properties of simple liquids with strong preference for tetrahedral local ordering are explored. These liquids are amenable to supercooling, and give complex crystalline structures on eventual crystallisation. All liquids studied are simple, monatomic and are similar to real metallic liquids. The vibrational density of states of a glass created in simulation is calculated. We show a correspondence between the vibrational properties of the crystal and the glass, indicating that the vibrational spectra of crystals can be used to understand the more complex vibrational spectra of the glass of the same substance. The dynamics of supercooled liquids is investigated using a previously not implemented comprehensive measure of structural relaxation. This new measure decays more slowly in the deeply supercooled domain than the commonly used measure. A new atomic model for octagonal quasicrystals is presented. The model is based on findings from a molecular dynamics simulation that resulted in 45˚ twinned β-Mn. A decoration is derived from the β-Mn unit cell and the unit cell of the intermediate structure found at the twinning interface. Extensive simulations are used to explore the phase diagram of a liquid at low densities. The resulting phase diagram shows a spinodal line and a phase coexistence region between a liquid and a crystalline phase ending in a critical point. This contradicts the old conclusion of the Landau theory -- that continuous transitions between liquids and crystals cannot exist The same liquid is explored at higher densities. Upon cooling the liquid performs a first order liquid-liquid phase transition. The low temperature liquid is shown to be strong and to have very good glass forming abilities. This result offers new insights into fragile to strong transitions and suggests the possibility of a good metallic glass former.
At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 2: Submitted. Paper 3: In progress.