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Boundary-engineering in nanostructures has the potential to dramaticallyimpact the development of materials for high-efficiency conversion of thermalenergy directly into electricity. In particular, nanostructuring ofsemiconductors can lead to strong suppression of heat transport with littledegradation of electrical conductivity. Although this combination of materialproperties is promising for thermoelectric materials, it remains largelyunexplored. In this work, we introduce a novel concept, the directional phononsuppression function, to unravel boundary-dominated heat transport inunprecedented detail. Using a combination of density functional theory and theBoltzmann transport equation, we compute this quantity for nanoporous siliconmaterials. We first compute the thermal conductivity for the case with alignedcircular pores, confirming a significant thermal transport degradation withrespect to the bulk. Then, by analyzing the information on the directionalityof phonon suppression in this system, we identify a new structure ofrectangular pores with the same porosity that enables a four-fold decrease inthermal transport with respect to the circular pores. Our results illustratethe utility of the directional phonon suppression function, enabling newavenues for systematic thermal conductivity minimization and potentiallyaccelerating the engineering of next-generation thermoelectric devices.

Directional Phonon Suppression Function as a Tool for the Identification of Ultralow Thermal Conductivity Materials