High-Throughput Calculations of Thermal Conductivity in Nanoporous Materials: The Case of Half-Heusler Compounds

Abstract: Achieving low thermal conductivity and good electrical properties is a crucial condition for thermal energy harvesting materials. Nanostructuring offers a very powerful tool to address both requirements: in nanostructured materials, boundaries preferentially scatter phonons compared to electrons. The search for low-thermal-conductivity nanostructures is typically limited to materials with simple crystal structures, such as silicon, because of the complexity arising from modeling branch- and wave vector- dependent nanoscale heat transport. Using the phonon mean-free-path (MFP) dependent Boltzmann transport equation, a model that overcomes this limitation, we compute thermal transport in 75 nanoporous half-Heusler compounds for different pore sizes. We demonstrate that the optimization of thermal transport in nanostructures should take into account both bulk thermal properties and geometry-dependent phonon suppression, two aspects that are typically engineered separately. In fact, our work predicts that, given a set of bulk materials and a system geometry, the ordering of the thermal conductivity of the nanostructure does not necessarily align with that of the bulk: We show that what dictates thermal transport is the interplay between the bulk MFP distribution and the nanostructuring length scale of the material. Finally, we derive a thermal transport model that enables fast systems screening within large bulk material repositories and a given geometry. Our study motivates the need for a holistic approach to engineering thermal transport and provides a method for high-throughput materials discovery.