Lattice-to-Total Thermal Conductivity Ratio: A Phonon-Glass Electron-Crystal Descriptor for Data-Driven Thermoelectric Design

Abstract

Thermoelectrics (TEs) are promising candidates for energy harvesting with performance quantified by figure of merit, $ZT$. To accelerate the discovery of high-$ZT$ materials, efforts have focused on identifying compounds with low thermal conductivity $κ$. Using a curated dataset of 71,913 entries, we show that high-$ZT$ materials reside not only in the low-$κ$ regime but also cluster near a lattice-to-total thermal conductivity ratio ($κ_\mathrm{L}/κ$) of approximately 0.5. This optimal ratio provides a quantitative descriptor for the well-known phonon-glass electron-crystal (PGEC) design concept. Building on this insight, we construct a framework consisting of two machine learning models for the lattice and electronic components of thermal conductivity that jointly provide both $κ$ and $κ_\mathrm{L}/κ$ for screening and guiding the optimization of TE materials. By applying this framework to 104,567 inorganic compounds, we identify 2,522 ultralow-$κ$ candidates while simultaneously evaluating their proximity to the optimal PGEC regime. A follow-up case study on chemical doping demonstrates how the framework can qualitatively provide optimization strategies that shift pristine materials toward the ideal $κ_\mathrm{L}/κ$ $\approx$ 0.5 target. Ultimately, by integrating rapid screening with PGEC-guided optimization, our data-driven framework takes a critical step towards closing the gap between materials discovery and performance enhancement.