Abstract
The development of efficient thermal energy management devices such as thermoelectrics and barrier coatings often relies on compounds having low lattice thermal conductivity (κl). Here, we present the computational discovery of a large family of 628 thermodynamically stable quaternary chalcogenides, AMM′Q3 (A = alkali/alkaline earth/post-transition metals; M/M′ = transition metals, lanthanides; Q = chalcogens) using high-throughput density functional theory (DFT) calculations. We validate the presence of low κl in these materials by calculating κl of several predicted stable compounds using the Peierls–Boltzmann transport equation. Our analysis reveals that the low κl originates from the presence of either a strong lattice anharmonicity that enhances the phonon-scatterings or rattler cations that lead to multiple scattering channels in their crystal structures. Our thermoelectric calculations indicate that some of the predicted semiconductors may possess high energy conversion efficiency with their figure-of-merits exceeding 1 near 600 K. Our predictions suggest experimental research opportunities in the synthesis and characterization of these stable, low κl compounds.
Highlights
An important focus in materials science research has been to discover hitherto unknown materials with properties that might hold the keys to solving the most pressing problems in renewable energy, energy harvesting, or semiconductor power electronics.The augmentation of new materials discovery and the prediction of their properties have been accelerated by the advent of advanced computer algorithms coupled with high-throughput (HT) screening methods[1,2,3,4,5,6,7,8,9,10] using accurate quantum mechanical calculations based on density functional theory (DFT)
We present the computational discovery of a large number of stable (628) and low-energy metastable (852) quaternary chalcogenides AMM′Q3 (A = alkali, alkaline earth, posttransition metals; M/M′ = transition metals, lanthanides; Q = chalcogens) that span a huge chemical space across the periodic table
Our analysis reveals that the underlying physical principles governing the low κl in Type-II
Summary
An important focus in materials science research has been to discover hitherto unknown materials with properties that might hold the keys to solving the most pressing problems in renewable energy, energy harvesting, or semiconductor power electronics. Rather than generating the input crystal structures in a brute-force manner by substituting every element of the periodic table at all atomic sites in the prototype structures, in this work we restricted ourselves by the following screening criteria which are derived by examining the experimentally known AMM′Q3 compounds: (1) we substitute alkali, alkaline earth, or post-transition metal elements at the A-site. (4) We exclude any radioactive elements during the prototype decorations some of the known AMM′Q3 compounds contain them Adhering to these preconditions helps us narrow down our search space of compound exploration, reduces the computational cost, and most importantly it increases the success rates of stable compound prediction through HT-DFT transport properties of some of the predicted stable compounds using the Peierls–Boltzmann transport equation (PBTE) show that these compounds exhibit innate low κl due to the presence of strong lattice anharmonicity or rattler cations
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