拉伸形变及电场作用对黑磷烯吸附Si原子电学特性影响的密度泛函理论研究

卫琳; 刘贵立; 王家鑫; 穆光耀; 张国英

doi:10.7498/aps.70.20210812

摘要

构建了覆盖度为2.778%的黑磷烯吸附硅原子模型, 基于密度泛函理论计算了模型的电子特性, 并通过应力及电场对其电子特性进行调控. 研究表明: 当前研究的覆盖度下, Si原子的吸附导致黑磷烯几何对称性被破坏, 加剧了体系内的电荷转移, 完成轨道再杂化. 使黑磷烯带隙消失, 实现了其由半导体向准金属的转变. 其稳定的吸附位是位于P原子环中间的H位. 拉伸和电场均降低了黑磷烯体系稳定性. 拉伸形变使黑磷烯吸附Si原子结构打开带隙, 且带隙与形变量成正比, 实现对其带隙的调控. 电场与拉伸共作用下, 电场的引入使黑磷烯吸附Si原子带隙变窄且完成体系由直接带隙向间接带隙的转变. 带隙依旧随形变量增加而增加. 吸附Si原子的黑磷烯体系带隙可调性高于未吸附体系, 且易于实现带隙的稳定调控.

关键词:

Abstract

In this paper, a model of Si atom adsorbed on black phosphorene with a coverage of 2.778% is constructed and the electronic properties of the model are calculated based on density functional theory. Moreover, the electronic properties are regulated by stress and electric field. Under the coverage of the current research, the results show that the adsorption of Si atoms results in the destruction of the black phosphorene’s geometric symmetry, which intensifies the charge transfer in the system and completes the orbital re-hybrid. The band gap of black phosphorene thus disappears and the transition from semiconductor to quasi metal is completed. The stable adsorption is at the H site in the middle of the P atomic ring. Both tensile field and electric field reduce the stability of the system. Owing to the tensile deformation, the band gap is opened by the structure of Si atom adsorbed on black phosphorene. And since the band gap is proportional to the deformation variable, it can be regulated and controlled. Under the combined action of electric field and tensile, the introduction of the electric field leads the band gap of Si adsorbed on black phosphorene system to be narrowed and the transition from the direct band gap to an indirect one to be completed. The band gap still goes up in proportion to the increase of deformation. The band gap of Si atom adsorbed on black phosphorene system is more adjustable than that of the Si atom that is not adsorbed on black phosphorene system, and the stable adjustment of the band gap is more likely to be realized.

Keywords:

作者及机构信息

1.
沈阳工业大学建筑与土木工程学院, 沈阳　110870

2.
沈阳师范大学物理学院, 沈阳　110034

通信作者: 刘贵立, garylll@sina.com

基金项目: 国家自然科学基金(批准号: 51371049)、辽宁省自然科学基金(批准号: 20102173)和辽宁省教育厅计划(批准号: LZGD2019003)资助的课题

Authors and contacts

1.
College of Architecture and Civil Engineering, Shenyang University of Technology, Shenyang 110870, China

2.
College of Physics, Shenyang Normal University, Shenyang 110034, China

Corresponding author: Liu Gui-Li, garylll@sina.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51371049), the Natural Science Foundation of Liaoning Province, China (Grant No. 20102173), and the Liaoning Provincial Department of Education Planned Project of China (Grant No. LZGD2019003).

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施引文献

图 1 本征黑磷烯模型　(a)黑磷烯的主视图、俯视图、侧视图; (b)黑磷烯结构示意图

Fig. 1. Intrinsic black phosphorene model: (a) Front view, top view, and side view of black phosphorene; (b) schematic diagram of the structure of black phosphorene.

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图 2 黑磷烯能带结构和DOS

Fig. 2. Band structure and DOS of black phosphorene.

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图 3 黑磷烯吸附Si原子模型　(a)主视图; (b)示意图; (c) P原子编号示意图

Fig. 3. Si adsorbed on black phosphorene model: (a) Main view; (b) diagrammatic sketch; (c) numbering diagram of P atom.

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图 4 黑磷烯吸附Si原子模型几何优化结构　(a) T位; (b) B位; (c) H位

Fig. 4. Geometry optimization of Si adsorbed on black phosphorene model: (a) T site; (b) B site; (c) H site.

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图 5 黑磷体系能带结构　(a)本征黑磷烯; (b) T位吸附; (c) B位吸附; (d) H位吸附

Fig. 5. Band structure of black phosphorene system: (a) Intrinsic black phosphorene; (b) T site adsorption; (c) B site adsorption; (d) H site adsorption.

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图 6 黑磷烯吸附体系DOS　(a) T位; (b) B位; (c) H位

Fig. 6. The DOS of Si adsorbed on black phosphorene system: (a) T site; (b) B site; (c) H site.

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图 7 (a)单个P原子DOS图; (b) P原子得失电子示意图; 红色球体代表得到电子的P原子, 蓝色球体代表失去电子的P原子

Fig. 7. (a) DOS diagram of single P atom; (b) schematic diagram of gain and loss of electrons of P atom. The red sphere represents the P atom that gets electrons, and the blue sphere represents the P atom that loses electrons.

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图 8 黑磷烯电荷差分密度图　(a)本征黑磷烯; (b)黑磷烯吸附Si原子

Fig. 8. Differential charge density of the black phosphorene: (a) Intrinsic black phosphorene; (b) Si adsorbed on black phosphorene system.

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图 9 本征黑磷烯与黑磷烯吸附体系电荷密度图　(a)主视图; (b)俯视图; (c)侧视图

Fig. 9. Charge density diagram of the adsorption system of intrinsic black phosphorene and black phosphorene: (a) Main view; (b) top view; (c) side view.

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图 10 考虑泊松比前后、拉伸形变量为2%的黑磷烯能带结构　(a)纯黑磷烯; (b)黑磷烯吸附Si原子; (c)电场与形变共作用的纯黑磷烯; (d) 电场与形变共作用的黑磷烯吸附Si原子

Fig. 10. Band structure of black phosphorene with 2% tensile deformation before and after considering Poisson’s ratio (a) Pure BP, (b) Si absorbed on BP, (c) pure BP with co-action of electric field and deformation, (d) Si absorbed on BP with co-action of electric field and deformation.

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图 11 (a)—(e)拉伸形变量为2%—10%的黑磷烯能带结构; (f)—(j)拉伸形变量为2%—10%的黑磷烯吸附Si原子体系能带结构

Fig. 11. (a)−(e) Band structure of black phosphorene with 2%−10% tensile deformation; (f)−(j) band structure of Si adsorbed on black phosphorene with 2%−10% tensile deformation.

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图 12 (a)形变为8%的黑磷烯结构俯视图; (b)形变为8%的黑磷烯电荷差分密度

Fig. 12. (a) Top view of the structure of 8% tensile deformation black phosphorene; (b) differential charge density of 8% tensile deformation phosphorene.

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图 13 (a)—(e)拉伸形变量为2%—10%的纯黑磷烯(BP)以及黑磷烯吸附Si原子体系(BP-Si)态密度结构; (f)黑磷烯带隙变化曲线

Fig. 13. (a)−(e) The DOS of black phosphorene (BP) and Si adsorbed on black phosphorene (BP-Si) with 2%−10% tensile deformation; (f) band gap curves of black phosphorene.

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图 14 电场作用下纯黑磷烯与黑磷烯吸附Si原子体系　(a), (b)能带结构, 其中蓝色虚线代表黑磷及黑磷烯吸附体系的能带结构, 黑色实现代表电场作用下黑磷烯及其吸附体系的能带结构; (c) DOS结构

Fig. 14. Si adsorbed on black phosphorene system and pure black phosphorene under electric field: (a), (b) Band structure, the blue dotted line represents the energy band structure of black phosphorus and black phosphorene adsorption system, and the black realization represents the energy band structure of black phosphorus and its adsorption system under the action of electric field; (c) DOS.

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图 15 (a)—(e)电场作用下拉伸形变量为2%—10%的黑磷烯能带结构; (f)—(j)电场作用下拉伸形变量为2%—10%的黑磷烯吸附Si原子体系能带结构

Fig. 15. (a)−(e) Band structure of black phosphorene with 2%−10% tensile deformation under electric field; (f)−(j) band structure of Si adsorbed on black phosphorene system with 2%−10% tensile deformation under electric field.

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图 16 (a)—(e)电场作用下拉伸形变量为2%—10%的黑磷烯吸附Si原子体系能带结构; (f)黑磷烯带隙变化曲线

Fig. 16. (a)−(e) Band structure of Si adsorbed on black phosphorene system with 2%−10% tensile deformation under the action of electric field; (f) band gap curves of black phosphorene.

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表 1 吸附原子所在原子环的P—P键键长与Si原子吸附高度

Table 1. Relationship between P—P bond length and Si adsorption height.

吸附位	P—Si/	P—P(1)/Å	P—P(2)/Å	P—P(3)/Å	P—P(4)/Å	d₀/Å
T	2.283	2.214	2.206	2.206	2.207	1.138
B	2.236	2.256	2.186	2.236	2.212	1.880
H	2.312	2.221	2.200	2.204	2.230	1.160

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表 2 P原子间键长及键级

Table 2. Bond length and bond order between P atoms.

	P₄—P₁₀, P₃₄—P₄	P₁₀—P₁₆, P₂₈—P₃₄	P₁₆—P₂₂, P₂₂—P₂₈	本征P—P	P_{16, 28}—Si	P₂₀—Si
键长/Å	2.162	2.497	2.210	2.210	2.331	2.312
键级	0.48	1.00	0.45	0.47	0.42	0.33

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表 3 P原子的Mulliken电荷布居数

Table 3. Mulliken charge population of P atom.

原子编号	P_{10, 34}	P_{16, 28}	P_{11, 35}	P_{8, 12, 13, 25, 32, 36}	P_{1, 7, 9, 17, 24, 29, 31, 33}	P_{2, 15, 18, 19, 23, 27, 30}	P_{3, 4, 14, 26}	P_{5, 22}	P₆	P₂₀	P₂₁	Si
Total/e	5.10	5.06	5.04	5.02	5.01	4.99	4.98	4.97	4.96	4.94	4.93	3.78
Charge/e	–0.10	–0.06	–0.04	–0.02	–0.01	0.01	0.02	0.03	0.04	0.06	0.07	0.22

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表 4 拉伸形变作用下纯黑磷烯单原子结合能和黑磷烯吸附Si原子吸附能

Table 4. Monoatomic binding energy of black phosphorene and adsorption energy of Si adsorbed on black phosphorene under tensile deformation.

形变量/%	0	2	4	6	8	10
结合能/eV	–5.774	–5.755	–5.719	–5.703	–5.701	–5.688
吸附能/eV	3.970	3.914	3.864	3.683	3.652	3.657

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表 5 电场与拉伸共作用下纯黑磷烯单原子结合能和黑磷烯吸附Si原子吸附能

Table 5. Single atom binding energy of black phosphorene and adsorption energy of Si adsorbed on black phosphorene system under the action of electric field and tensile.

形变量/%	0	2	4	6	8	10
结合能/eV	–2.507	–2.485	–2.457	–2.439	–2.433	–2.421
吸附能/eV	3.461	3.420	3.366	3.254	3.214	3.210

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