Creating Zipper-Like van der Waals Gap Discontinuity in Low-Temperature-Processed Nanostructured PbBi2n Te1+3n : Enhanced Phonon Scattering and Improved Thermoelectric Performance.

Nanoengineered materials can embody distinct atomic structures which deviate from that of the bulk-grain counterpart and induce significantly modified electronic structures and physical/chemical properties. The phonon structure and thermal properties, which can also be potentially modulated by the modified atomic structure in nanostructured materials, however, are seldom investigated. Employed here is a mild approach to fabricate nanostructured PbBi2n Te1+3n using a solution-synthesized PbTe-Bi2 Te3 nano-heterostructure as a precursor. The as-obtained monoliths have unprecedented atomic structure, differing from that of the bulk counterpart, especially the zipper-like van der Waals gap discontinuity and the random arrangement of septuple-quintuple layers. These structural motifs break the lattice periodicity and coherence of phonon transport, leading to ultralow thermal conductivity and excellent thermoelectric z T.