Li Ruoxi, Li Xin, Xi Lili, Yang Jiong, Singh David J, Zhang Wenqing
Materials Genome Institute , Shanghai University , 99 Shangda Road , Shanghai 200444 , China.
Department of Physics and Astronomy , University of Missouri , Columbia , Missouri 65211 , United States.
ACS Appl Mater Interfaces. 2019 Jul 17;11(28):24859-24866. doi: 10.1021/acsami.9b01196. Epub 2019 Apr 26.
High-throughput (HTP) calculations are a highly promising direction for the discovery of novel functional materials. Here we use an HTP framework to investigate the electronic structures and p-type thermoelectric properties of the ABX compounds with diamond-like structures. We show application of HTP both to identify compounds and also to identify underlying trends. A total of 65 entries out of 84 908 in the Materials Informatics Platform are selected for this study. The electronic structures and chemical-bonding analyses reveal that there exists a general conductive network consisting of the anion X sublattice, which dominates the electrical transport properties of the compounds. Electrical and thermal transport properties of the 41 pnictide and chalcogenide compounds with sufficient band gaps are studied. Pnictide compounds have relatively smaller Seebeck coefficients than the chalcogenide compounds. This is due to the smaller effective masses around the valence band maxima. The electrical conductivities and power factors, however, are better in pnictide compounds. This is because pnictide compounds have high electronic group velocities and electronic relaxation times. Combined with the predictions of lattice thermal conductivities based on the Slack model, 12 novel p-type and n-type ABX materials with high ZT values are predicted.
高通量（HTP）计算是发现新型功能材料的一个极具前景的方向。在此，我们使用一个HTP框架来研究具有类金刚石结构的ABX化合物的电子结构和p型热电性能。我们展示了HTP在识别化合物以及识别潜在趋势方面的应用。本研究从材料信息学平台的84908个条目中总共选取了65个条目。电子结构和化学键分析表明，存在一个由阴离子X亚晶格构成的通用导电网络，它主导着化合物的电输运性质。对41种具有足够带隙的磷化物和硫族化物化合物的电输运和热输运性质进行了研究。磷化物化合物的塞贝克系数比硫族化物化合物相对更小。这是由于价带最大值附近的有效质量较小。然而，磷化物化合物的电导率和功率因子更好。这是因为磷化物化合物具有较高的电子群速度和电子弛豫时间。结合基于斯莱克模型对晶格热导率的预测，预测出了12种具有高ZT值的新型p型和n型ABX材料。
