Establishing the Accuracy of Broadly Used Density Functionals in Describing Bulk Properties of Transition Metals
Establishing the Accuracy of Broadly Used Density Functionals in Describing Bulk Properties of Transition Metals
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DOI：
10.1021/ct3010326
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发表时间：
2013-03-01
影响因子：
5.5
通讯作者：
Illas, Francesc
中科院分区：
文献类型：
--
作者：
Janthon, Patanachai;Kozlov, Sergey M.;Illas, Francesc
各种常用的密度泛函的性能建立通过比较计算值的原子结构数据，结合能，和体积模量的所有过渡金属可用的实验数据。探索的泛函是局部密度近似（LDA）的Ceperley-Alder（CA），Vosko-Wilk-Nussair（VWN）实现;广义梯度近似（GGA）的Perdew-Wang（PW 91）和Perdew-Burke-Ernzerhof（PBE）形式，以及PBE的RPBE和PBESol修改，旨在更好地描述吸附能和散装固体晶格性质。本系统的研究表明，PW 91和PBE始终提供最小的计算值和实验值之间的差异。对几种面心立方（fcc）过渡金属（111）表面能的额外计算表明，LDA产生最准确的结果，而所有其他泛函显着低估了实验值。RPBE严重低估了表面能，这可能是表面化学活性降低和RPBE描述吸附能的更好性能的起源。
The performance of various commonly used density functionals is established by comparing calculated values of atomic structure data, cohesive energies, and bulk moduli of all transition metals to available experimental data. The functionals explored are the Ceperley-Alder (CA), Vosko-Wilk-Nussair (VWN) implementation of the Local Density Approximation (LDA); the Perdew-Wang (PW91) and Perdew-Burke-Ernzerhof (PBE) forms of the Generalized Gradient Approximation (GGA), and the RPBE and PBEsol modifications of PBE, aimed at better describing adsorption energies and bulk solid lattice properties, respectively. The present systematic study shows that PW91 and PBE consistently provide the smallest differences between the calculated and experimental values. Additional calculations of the (111) surface energy of several face centered cubic (fcc) transition metals reveal that LDA produces the most accurate results, while all other functionals significantly underestimate the experimental values. RPBE severely underestimates surface energy, which may be the origin for the reduced surface chemical activity and the better performance of RPBE describing adsorption energies.