Prediction of Giant Thermoelectric Efficiency in Crystals with Interlaced Nanostructure

We present a theoretical study of the thermoelectric efficiency of "interlaced crystals", recently discovered in hexagonal-CuInS2 nanoparticles. Interlaced crystals are I-III-VI2 or II-IV-V2 tetrahedrally bonded compounds. They have a perfect Bravais lattice in which the two cations have an infinite set of possible ordering patterns within the cation sublattice. The material comprises nanoscale interlaced domains and phases with corresponding boundaries. Here we employ density functional theory and large-scale molecular dynamics calculations based on model classical potentials to demonstrate that the phase and domain boundaries are effective phonon scatterers and greatly suppress thermal conductivity. However, the absence of both structural defects and strain in the interlaced material results in a minimal effect on electronic properties. We predict an increase of thermal resistivity of up to 2 orders of magnitude, which makes interlaced crystals an exceptional candidate for thermoelectric applications.