Paper detail

Wave theory of lattice dynamics

I present the mathematical structure of classical phonon theory in a general form, which emphasizes the wave natures of phonons, and which can serve as a robust foundation for further development of the theory of strongly interacting phonons. I also show that the Fourier transform (FT) of the mass-weighted velocity-velocity correlation function (mVVCF) is exactly the distribution of the classical kinetic energy among frequencies and wavevectors. Because this result is classically exact, it is general: It is as valid, theoretically, for a liquid or a molecule in a non-thermal non-stationary state as it is for a crystal at thermal equilibrium at a low temperature. Therefore, as well as being of fundamental importance to physical theory, this result implies that calculating the FT of the mVVCF from atomistic simulations is a much more powerful computational tool than it is believed to be. Existing theory shows only that the FT of the mVVCF is proportional to the vibrational density of states at thermal equilibrium, and under the simplifying assumption that the number of available vibrational states is equal to the number of degrees of freedom.