Vacancy formation enthalpy of filled d-band noble metals by hybrid functionals

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	Vacancy formation enthalpy of filled d-band noble metals by hybrid functionals
	W. W. Xing; P. T. Liu; X. Y. Cheng; H. Y. Niu; H. Ma; D. Z. Li; Y. Y. Li; X. Q. Chen
	2014
发表期刊	Physical Review B
ISSN	1098-0121
卷号	90 期号:14
摘要	First-principles determination of the vacancy formation enthalpies has been long-term believed to be highly successful for metals. However, a widely known fact is that the various conventional density functional theory (DFT) calculations with the typical semilocal approximations show apparent failures to yield accurate enthalpies of Ag and Au. Recently, the previously commonly assumed linear Arrhenius extrapolation to determine the vacancy formation enthalpies at T = 0 K from the high-temperature measured concentration of thermally created vacancies has been demonstrated to have to be replaced by the non-Arrhenius local Gruneisen theory (LGT) [A. Glensk, B. Grabowski, T. Hickel, and J. Neugebauer, Phys. Rev. X 4, 011018 (2014)]. The large discrepancies between the conventional DFT-PBE data and the unrevised experimental vacancy formation enthalpies disappear for Cu and Al. Even by following the same LGT revisions for Ag, the large discrepancies still remain substantial at T = 0 K. Here, we show that the hybrid functional (HSE), by including nonlocal exchange interactions to extend the conventional DFT method, can further correct these substantial failures. Upon a comparison of the experimental valence-band spectra for Cu, Ag, and Au, we have determined the HSE exchange-correlated mixing parameters a of 0.1, 0.25, and 0.4, and further derived the HSE enthalpies of vacancy formation of 1.09, 0.94, and 0.72 eV, respectively; in nice agreement with available LGT-revised experimental data. Our HSE results shed light on how to improve the theoretical predictions to accurately determine the defect formation energies and related thermodynamical properties.
部门归属	[xing, weiwei ; liu, peitao ; cheng, xiyue ; niu, haiyang ; ma, hui ; li, dianzhong ; li, yiyi ; chen, xing-qiu] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china. ; chen, xq (reprint author), chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china. ; xingqiu.chen@imr.ac.cn
关键词	Thermal-equilibrium Vacancies 1st-principles Calculations Positron-annihilation Transition Alloys Photoemission Platinum Energy Copper States
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语种	英语
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/73452
专题	中国科学院金属研究所
推荐引用方式 GB/T 7714	W. W. Xing,P. T. Liu,X. Y. Cheng,et al. Vacancy formation enthalpy of filled d-band noble metals by hybrid functionals[J]. Physical Review B,2014,90(14).
APA	W. W. Xing.,P. T. Liu.,X. Y. Cheng.,H. Y. Niu.,H. Ma.,...&X. Q. Chen.(2014).Vacancy formation enthalpy of filled d-band noble metals by hybrid functionals.Physical Review B,90(14).
MLA	W. W. Xing,et al."Vacancy formation enthalpy of filled d-band noble metals by hybrid functionals".Physical Review B 90.14(2014).