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Introducing hierarchical disorder from multiple defects into materialsthrough nanostructuring is one of the most promising directions to achieveextremely low thermal conductivities and thus improve thermoelectricperformance. The success of nanostructuring relies on charge carriers havingshorter mean-free-paths than phonons so that the latter can be selectivelyscattered. Nevertheless, introducing disorder into a material often comes atthe expense of scattering charge carriers as well as phonons. In order todetermine the tradeoff between the degradation of the lattice thermalconductivity and of the power factor due to this, we perform a theoreticalinvestigation of both phonon and electron transport in nanocrystalline,nanoporous Si geometries. We use molecular dynamics for phonon transportcalculations and the non-equilibrium Green's function method for electronictransport. We report on the engineering tradeoff that the porosity (number ofpores and their in-between distance) has on the overall thermoelectricperformance for the material optimization. We indeed find that the reduction inthermal conductivity is stronger compared to the reduction in the power factor,for the low porosities considered in this study (up to 5 %), and that the ZTfigure of merit can experience a large increase, especially when grainboundaries are included, compared to just nanoporosity.

Modelling thermoelectric performance in nanoporous nanocrystalline silicon