Density functional theory study of bulk properties of transition metal nitrides
Density functional theory study of bulk properties of transition metal nitrides
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过渡金属氮化物体性能的密度泛函理论研究
DOI：
10.1039/d2cp06082e
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发表时间：
2023
影响因子：
3.3
通讯作者：
Kattel, Shyam
中科院分区：
文献类型：
--
作者：
Lynn, Michael O.;Ologunagba, Damilola;Dangi, Beni B.;Kattel, Shyam
采用密度泛函理论（DFT）方法计算了过渡金属氮化物（TMN）的晶格常数、形成能和空位形成能。用6种不同的DFT交换势和关联势（LDA、AM 05、BLYP、PBE、rPBE和PBEsol）得到的结果表明，用rPBE得到的实验晶格常数最好，而用AM 05、PBE、rPBE和PBEsol得到的值介于LDA和BLYP计算值之间.观察到的晶格常数和形成能之间的线性关系与TM的平均半径和在TMN中TM和N的电负性的差异，分别。我们计算的空位形成能，在一般情况下，表明N-空位比TM-空位在大多数TMN更有利。我们观察到，N-空位形成能与计算的体形成能线性相关，这表明具有大的负形成能的TMN不太容易形成N-空位。因此，我们的结果，从这个广泛的DFT研究不仅提供了一个系统的比较各种DFT泛函在计算TMN的性能，但也作为参考数据的计算驱动的实验设计的材料。
Density functional theory (DFT) calculations are performed to compute the lattice constants, formation energies and vacancy formation energies of transition metal nitrides (TMNs) for transition metals (TM) ranging from 3d–5d series. The results obtained using six different DFT exchange and correlation potentials (LDA, AM05, BLYP, PBE, rPBE, and PBEsol) show that the experimental lattice constants are best predicted by rPBE, while the values obtained using AM05, PBE, rPBE and PBEsol lie between the LDA and BLYP calculated values. A linear relationship is observed between the lattice constants and formation energies with the mean radii of TM and the difference in the electronegativity of TM and N in TMNs, respectively. Our calculated vacancy formation energies, in general, show that N-vacancies are more favorable than TM-vacancies in most TMNs. We observe that N-vacancy formation energies are linearly correlated with the calculated bulk formation energies indicating that TMNs with large negative formation energies are less susceptible to the formation of N-vacancies. Thus, our results from this extensive DFT study not only provide a systematic comparison of various DFT functionals in calculating the properties of TMNs but also serve as reference data for the computation-driven experimental design of materials.