Phase Transformations in Computer Simulated Icosahedrally Ordered Phases

Abstract: Computer simulations play a profound and fundamental role inmodern theoretical physics, chemistry and materials science. Tounderstand the complex physics of metally liquids, metals,quasicrystals and metally glasses a working model imposing thelocal and global order is needed. Experiments and theory havepredicted the local order in liquid metals to beicosahedral.The current work has been done using molecular dynamicscomputer simulations of a monatomic system using a simplepair-potential for the interactions. Two new pair-potentialshas been developed, the Zetterling-1(Z1) and Zetterling-2(Z2)potentials. They are specifically modeled to impose icosahedralorder. The basis for the development of the potentials was theold Dzugutov potential which is known to freeze into adodecagonal quasicrystal. The new Zetterling potentials have alonger interaction range and a narrower first minimum. The morenarrow first minimum will enhance the local icosahedralordering and the longer interaction range was introduced toincorporate a second maximum in the potential mimicing theFriedel oscillations found in metallic systems. These Friedeloscillations are due to the singularity which arises at theFermi surface due to the screening of the positive charge bythe electron gas.Five papers are included in the study. The first two papersare studies of icosahedral clustering in the liquid andsupercooled liquid. The simulations in Paper I was done usingthe old Dzugutov potential while the new potentials were usedin Paper II using both molecular dynamics and the Basin Hoppingalgorithm presented in Chapter 5. Paper III considers theconcept of dynamical ergodicity in the context of thesuper-cooled liquid behaviour. The simulations were made usingthe old Dzugutov potential. Paper IVr eports a moleculardynamics simulation using the Dzugutov potential undersuper-cooling. A formation of icosahedrally structured domainswith distinctly slow diffusion which grows with cooling in alow-dimensional manner and percolate around Tc, the criticaltemperature of the mode-coupling theory. A sharp slowing downof the structural relaxation relative to diffusion is observed.It is concluded that this effect cannot be accounted for by thespatial variation in atomic mobility. The low-dimensionalclustering is discussed as a possible mechanism of fragility.Paper Vin vestigates the crystallization of a simple monatomicliquid model which utilizes the Zetterling-1 potential. Thesystem forms a thermodynamically stable solid phase exhibitingcubic symmetry. Its diffraction pattern is identified as thatof ?-brass, a tetrahedrally packed crystalline structurewith 52 atoms in the unit cell.Keywords:simple liquids, molecular dynamics, pairpotential, icosahedral cluster.