First-principles study of H, Cl and F passivation for Cu2ZnSnS4(112) surface states

doi:10.7498/aps.67.20180626

	First-principles study of H, Cl and F passivation for Cu2ZnSnS4(112) surface states
	Wang Xiao-Ka 1; Tang Fu-Ling1,2 ; Xue Hong-Tao1 ; Si Feng-Juan 1; Qi Rong-Fei 1; Liu Jing-Bo 2
	2018-08-20
发表期刊	Wuli Xuebao/Acta Physica Sinica
ISSN	10003290
卷号	67 期号:16
摘要	The first-principles calculation method is used to systematically investigate the lattice structure, energy band, density of states of the bulk Cu2ZnSnS4, surface reconstruction, and mechanism of adsorption and passivation of F, Cl and H atoms on Cu2ZnSnS4 (112) surface. We find that the surface reconstruction occurs on the Cu-Zn-Sn-terminated Cu2ZnSnS4 (112) surface and this reconstruction introduces surface self-passivation. By analyzing the partial density of states of the atoms on the S-terminated Cu2ZnSnS4 (112) surface, it can be seen that surface states near the Fermi level are mainly contributed by 3d orbitals of Cu atoms and 3p orbits of S atoms at the top of the valence band. When a single F, Cl or H atom is adsorbed on the S-terminated Cu2ZnSnS4 (112) surface, all three kinds of atoms exhibit an optimal stability at a specific top adsorption site in comparison with at the bridge, hcp and fcc sites. And this top position is also the position of the S atom that has the greatest influence on the surface states. When two atoms of the same kind are adsorbed on the surface, H, Cl or F atoms occupy the top sites of two S atoms that cause surface states on the Cu2ZnSnS4 (112) surface, which have the lowest adsorption energy. And the surface states near the Fermi level are partially reduced. Therefore, two S atoms that cause the surface states are the main targets of S-terminated Cu2ZnSnS4 (112) surface passivation. It has also been found that the passivation effect of H atom for surface states is the most significant and the effect of Cl atom is better than that of F atom. Comparing the partial density of states, the Bader charge and the differential charge of the atoms before and after adsorption, we find that the main reason for the decrease of the surface states is that the adsorption atoms obtain electrons from the S atoms, and the state density peaks of the Cu and S atoms at the Fermi level almost disappear completely. In the surface model, the F atom obtains the same number of electrons from the two S atoms, while the two S atoms have different effects on the surface states. And the H and Cl atoms obtain fewer electrons from the S atoms, that have less influence on the surface states. It may be the reason why the passivation effect of F atom is slightly less than that of H and Cl atoms. © 2018 Chinese Physical Society.
关键词	Adsorption Atoms Calculations Chlorine Copper Copper compounds Fermi level Passivation Surface reconstruction Surface states Tin compounds Zinc compounds Adsorption energies Cu2ZnSnS4 First-principles calculation First-principles study Number of electrons Partial density of state Passivation effect Surface passivation
DOI	10.7498/aps.67.20180626
收录类别	EI ; SCIE
语种	中文
WOS研究方向	Physics
WOS类目	Physics, Multidisciplinary
WOS记录号	WOS:000443384900022
出版者	Institute of Physics, Chinese Academy of Sciences
EI入藏号	20184806161690
EI主题词	Fluorine compounds
EI分类号	539.2.1 Protection Methods ; 544.1 Copper ; 802.3 Chemical Operations ; 804 Chemical Products Generally ; 921 Mathematics ; 931 Classical Physics ; Quantum Theory ; Relativity ; 931.3 Atomic and Molecular Physics ; 932 High Energy Physics ; Nuclear Physics ; Plasma Physics
引用统计	被引频次[WOS]：0 [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	https://ir.lut.edu.cn/handle/2XXMBERH/150561
专题	材料科学与工程学院省部共建有色金属先进加工与再利用国家重点实验室
通讯作者	Tang Fu-Ling
作者单位	1.Lanzhou Univ Technol, Dept Mat Sci & Engn, State Key Lab Adv Proc & Recycling Nonferrous Met, Lanzhou 730050, Gansu, Peoples R China; 2.Texas A&M Univ, Dept Chem, 700 Univ Blvd, Kingsville, TX 78363 USA
第一作者单位	兰州理工大学
通讯作者单位	兰州理工大学
第一作者的第一单位	兰州理工大学
推荐引用方式 GB/T 7714	Wang Xiao-Ka,Tang Fu-Ling,Xue Hong-Tao,et al. First-principles study of H, Cl and F passivation for Cu2ZnSnS4(112) surface states[J]. Wuli Xuebao/Acta Physica Sinica,2018,67(16).
APA	Wang Xiao-Ka,Tang Fu-Ling,Xue Hong-Tao,Si Feng-Juan,Qi Rong-Fei,&Liu Jing-Bo.(2018).First-principles study of H, Cl and F passivation for Cu2ZnSnS4(112) surface states.Wuli Xuebao/Acta Physica Sinica,67(16).
MLA	Wang Xiao-Ka,et al."First-principles study of H, Cl and F passivation for Cu2ZnSnS4(112) surface states".Wuli Xuebao/Acta Physica Sinica 67.16(2018).