Ab initio thermal transport properties of nanostructures from density functional perturbation theory
We present a comprehensive first-principles study of the thermal transport properties of low-dimensional nanostructures such as polymers and nanowires. An approach is introduced where the phonon quantum conductance is computed from the combination of accurate plane-wave density functional theory electronic structure calculations, the evaluation of the interatomic force constants through density functional perturbation theory for lattice dynamics, and the calculation of transport properties by a real-space Green’s function method based on the Landauer formalism. This approach is computationally very efficient, can be straightforwardly implemented as a post-processing step in a standard electronic structure calculation (Quantum ESPRESSO and WanT in the present implementation), and allows us to directly link the thermal transport properties of a device to the coupling, dimensionality, and atomistic structure of the system. It provides invaluable insight into the mechanisms that govern heat flow at the nanoscale and paves the way to the fundamental understanding of phonon engineering in nanostructures.