Date of Award

Fall 9-2016

Embargo Period


Degree Type


Degree Name

Doctor of Philosophy (PhD)


Mechanical Engineering


Alan McGaughey


Thermal transport across three-dimensional Lennard-Jones superlattices, two-dimensional heterostructures of graphene and hexagonal boron nitride (hBN), and in C60 molecular crystals is studied atomistically. The first two systems are studied as finite junctions placed between bulk leads, while the molecular crystal is studied as a bulk. Two computational methods are used: molecular dynamics (MD) simulations and harmonic lattice dynamics calculations in conjunction with the scattering boundary method (SBM). In Lennard-Jones superlattice junctions with a superlattice period of four atomic monolayers at low temperatures, those with mass-mismatched leads have a greater thermal conductance than those with mass-matched leads. We attribute this lead effect to interference between and the ballistic transport of emergent junction vibrational modes. The lead effect diminishes when the temperature is increased, when the superlattice period is increased, and when interfacial disorder is introduced, and is reversed in the harmonic limit. In graphene-hBN heterostructure junctions, the thermal conductance is dominated by acoustic phonon modes near the Brillouin zone center that have high group velocity, population, and transmission coefficient. Out-of-plane modes make their most significant contributions at low frequencies, whereas in-plane modes contribute across the frequency spectrum. Finite-length superlattice junctions between graphene and hBN leads have a lower thermal conductance than comparable junctions between two graphene leads due to lack of transmission in the hBN phonon band gap. The thermal conductances of bilayer systems differ by less that 10% from their single-layer counterparts on a per area basis, in contrast to the strong thermal conductivity reduction when moving to from single- to multi-layer graphene. We model C60 molecules using the polymer consistent force-field and compute the single molecule vibrational spectrum and heat capacity. In the face-center cubic C60 molecular crystal at a temperature of 300 K, we find three frequency peaks in the center-of-mass translations at 20, 30 and 38 cm􀀀1, agreeing with the average frequencies of the three acoustic branches of the frozen phonon model of the same system and suggesting that a phonon description of center-of-mass translations. We use both direct method and Green- Kubo MD simulations to predict the thermal conductivity of the molecular crystals at a temperature of 300 K. We find that the thermal conductivity of the molecular crystal is 20 to 50% lower than that of a reduced order model where only molecular center-ofmass translations are present, suggesting that molecular vibrations and rotations act as significant scattering sources for the center-of-mass phonons.