We describe an innovative interfacial design concept and nanostructuring of novel BiSbTe (BST) nanoassembled films comprising unique air-solid interfaces from micro-scaled open gaps to isolated sealed mesopores, and high-quality solid-solid ones including the coherent grain boundaries and specific twins, utilizing pulsed laser deposition (PLD), for potentially activating multiple thermoelectric enhancing mechanisms. The unusual mesopore embedded BST films exhibit the highest power factor of ∼33 μW cm K, which is comparable to or higher than the previously reported values for BST, and the corresponding relatively low thermal diffusivity in contrast to that for dense pore-less BST films evidently reveals the crucial role of the three-dimensionally and densely arranged air-solid interfaces in significantly arising the phonon scattering.

According to the innovative design concept of omnidirectional quasi-order hetero-nanocomposites proposed for potentially realizing high thermoelectric performance, a series of superarchitectures consisting of longitudinally periodic diamond-like carbon (DLC) interlayers in latitudinally well-aligned Bi–Sb–Te (BST)-based nanostructures were successfully demonstrated for the first time using dual-beam pulsed laser deposition. This work confirmed that the periodic appearance of DLC is a practical approach to instantly resetting the BST deposition into another new crystal growth cycle. The optimized Seebeck coefficient of ∼500 μV K–1 and the corresponding power factor of ∼40 μW cm–1 K–2 achieved are comparable to or higher than the reported values for BST or BST-based nanocomposites, which evidently originated from the periodically added DLC, as clarified in the Pisarenko plot. In addition, the DLC additives effectively reduce the thermal transport as qualitatively evidenced by micro-Raman characterizations.