Phonons, quantized lattice vibrations, govern most of the thermophysical properties of solid-state materials such that understanding the temperature dependent lattice dynamics is of great technological importance. I performed inelastic neutron scattering measurements at the Spallation Neutron Source on ARCS, a wide-angular chopper spectrometer, to measure phonon dispersions and density of states over a wide range of temperatures. Large phonon anharmonicities manifested by phonon energy shifts and broadenings were observed in both measured phonon dispersions and phonon density of states. The sources of deviations from the simple harmonic model with temperature were elucidated using experimentally assessed lattice dynamics coupled with ab initio methods. Pure anharmonicity dominates the changes in lattice dynamics with temperature and therefore drive the entropy and thermophysical properties of thermal expansion and thermal conductivity. Crystal structure, anharmonicity, and nuclear quantum effects all play important roles in the thermal expansion of silicon, and a simple mechanical explanation is inappropriate. The quantum effect of nuclear vibrations is also expected to be important for thermal expansion of many materials. My experimental techniques capture the linewidth broadenings from phonon anharmonicity needed to calculate thermal conductivity. The methods developed for data reduction on single crystal inelastic neutron scattering data and predicting macroscopic quantities should also be useful for understanding microscopic mechanisms behind thermophysical properties for materials
