Relative stability of FeS2 polymorphs with the random phase approximation approach

doi:10.1039/c8ta00759d

CORC > 化学研究所 > 中国科学院化学研究所

	Relative stability of FeS2 polymorphs with the random phase approximation approach
	Zhang, Min-Ye; Cui, Zhi-Hao; Jiang, Hong
刊名	JOURNAL OF MATERIALS CHEMISTRY A
	2018-04-21
卷号	6 期号:15 页码:6606-6616
ISSN号	2050-7488
DOI	10.1039/c8ta00759d
英文摘要	Iron disulfide (FeS2) has attracted a lot of interest for photovoltaic and photoelectrochemical applications due to its favorable electronic and optical properties. The theoretical description of FeS2 has been confronted with the problem of common density functional approximations failing to correctly account for the relative stability of pyrite and marcasite polymorphs of FeS2. We address this issue by using the adiabatic-connection fluctuation-dissipation theorem (ACFDT) in the random phase approximation (RPA). The relative stability of the two polymorphs is correctly predicted, and a significantly improved agreement with experiment compared to that from local, semi-local and hybrid functionals is obtained in terms of the enthalpy of transformation, regardless of the density functional approximations used in producing the input wave functions for RPA calculations. We attribute the stability of the pyrite phase to the electron correlation related to the low energy excitation from Fe d states to the S-S sigma(*)(p) state. Equilibrium volumes very close to the experimental values are predicted for both phases as well. The contributions of zero-point energy corrections and finite temperature effects are considered and found to be insignificant compared to dynamical correlation included in the ACFDT-RPA approach. This study highlights the importance of considering the difference in high-order dynamical correlation as described by ACFDT-RPA due to the distinction in the Kohn-Sham band structure for a correct description of the relative stability of competing phases that are energetically very close to each other.
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000430368900049
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/42895]
专题	中国科学院化学研究所
通讯作者	Jiang, Hong
作者单位	Peking Univ, State Key Lab Rare Earth Mat Chem & Applicat, Inst Theoret & Computat Chem, Beijing Natl Lab Mol Sci,Coll Chem & Mol Engn, Beijing 100871, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Min-Ye,Cui, Zhi-Hao,Jiang, Hong. Relative stability of FeS2 polymorphs with the random phase approximation approach[J]. JOURNAL OF MATERIALS CHEMISTRY A,2018,6(15):6606-6616.
APA	Zhang, Min-Ye,Cui, Zhi-Hao,&Jiang, Hong.(2018).Relative stability of FeS2 polymorphs with the random phase approximation approach.JOURNAL OF MATERIALS CHEMISTRY A,6(15),6606-6616.
MLA	Zhang, Min-Ye,et al."Relative stability of FeS2 polymorphs with the random phase approximation approach".JOURNAL OF MATERIALS CHEMISTRY A 6.15(2018):6606-6616.