Assessing the performance of exchange-correlation functionals on lattice constants of binary solids at room temperature within the quasiharmonic approximation

doi:10.1103/PhysRevB.108.024306

IMR OpenIR

	Assessing the performance of exchange-correlation functionals on lattice constants of binary solids at room temperature within the quasiharmonic approximation
	Shao, Xiaofei 1; Liu, Peitao 2; Franchini, Cesare 3,4,5; Xia, Yi 6; He, Jiangang 1
通讯作者	He, Jiangang(jghe2021@ustb.edu.cn)
	2023-07-20
发表期刊	PHYSICAL REVIEW B
ISSN	2469-9950
卷号	108 期号:2 页码:9
摘要	The exchange-correlation functional is at the core of density functional theory (DFT) and determines the accuracy of DFT in describing the interactions among electrons/ions in solids and molecules. The strongly constrained and appropriately normed functional (SCAN) and its derivatives, regularized SCAN (rSCAN) and regularized-restored SCAN (r2SCAN), are particularly promising due to their remarkable overall accuracy in the description of various properties while retaining a high computational efficiency as compared to hybrid functionals. However, an exhaustive assessment on the performance of these functionals in predicting the finite-temperature lattice constant of solids is still lacking. Here, we systematically study the room-temperature lattice constants of 60 cubic binary compounds within the quasiharmonic approximation using SCAN, rSCAN, r2SCAN, local density approximation (LDA), and two common generalized gradient approximation (GGA) functionals, Perdew-Burke-Ernzerhof (PBE) and revised PBE for solid and surface (PBEsol). We found that SCAN exhibits numerical instabilities in free energy calculations, manifested by the presence of spurious imaginary frequencies in phonon dispersion relationships and poor fitting in Murnaghan's equation of state of Helmholtz free energy for 30 compounds. The revised SCAN functionals show much better numerical stabilities and reduce the number of the compounds with numerical issues to 22 and 9 for rSCAN and r2SCAN, respectively. The mean relative absolute errors (MRAE) of the calculated lattice constants at room temperature for the remaining 30 binary compounds are 0.92%, 1.10%, 0.32%, 0.51%, 0.58%, and 0.67% for LDA, PBE, PBEsol, SCAN, rSCAN, and r2SCAN, respectively. Furthermore, we found that the SCAN functional incorrectly predicts unstable phonon modes for a few compounds at their equilibrium volumes, which indicates the existence of a new ground state structure with lower energy than the cubic structure at 0 K, disagreeing with experiments. Our results provide a useful guide in choosing suitable functionals in describing anharmonic phonons and shed light on second-order force constant calculations that may help to develop more accurate exchange-correlation functionals for solids.
资助者	Fundamental Research Funds for the Central Universities China (USTB) ; Shenyang National Research Center for Materials Science ; Portland State University's laboratory setup fund ; USTB MatCom of Beijing Advanced Innovation Center for Materials Genome Engineering
DOI	10.1103/PhysRevB.108.024306
收录类别	SCI
语种	英语
资助项目	Fundamental Research Funds for the Central Universities China (USTB) ; Shenyang National Research Center for Materials Science[E21SLA07] ; Portland State University's laboratory setup fund ; USTB MatCom of Beijing Advanced Innovation Center for Materials Genome Engineering
WOS研究方向	Materials Science ; Physics
WOS类目	Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:001059715200004
出版者	AMER PHYSICAL SOC
引用统计	被引频次：9[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/179115
专题	中国科学院金属研究所
通讯作者	He, Jiangang
作者单位	1.Univ Sci & Technol Beijing, Sch Math & Phys, Beijing 100083, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Univ Vienna, Fac Phys, A-1090 Vienna, Austria 4.Ctr Computat Mat Sci, A-1090 Vienna, Austria 5.Alma Mater Studiorum Univ Bologna, Dept Phys & Astron Augusto Righi, I-40127 Bologna, Italy 6.Portland State Univ, Dept Mech & Mat Engn, Portland, OR 97201 USA
推荐引用方式 GB/T 7714	Shao, Xiaofei,Liu, Peitao,Franchini, Cesare,et al. Assessing the performance of exchange-correlation functionals on lattice constants of binary solids at room temperature within the quasiharmonic approximation[J]. PHYSICAL REVIEW B,2023,108(2):9.
APA	Shao, Xiaofei,Liu, Peitao,Franchini, Cesare,Xia, Yi,&He, Jiangang.(2023).Assessing the performance of exchange-correlation functionals on lattice constants of binary solids at room temperature within the quasiharmonic approximation.PHYSICAL REVIEW B,108(2),9.
MLA	Shao, Xiaofei,et al."Assessing the performance of exchange-correlation functionals on lattice constants of binary solids at room temperature within the quasiharmonic approximation".PHYSICAL REVIEW B 108.2(2023):9.