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二维磁性材料的研究是一大热点, 其中单层CrSi2表现出优良的磁性, 有望应用于自旋电子学等领域, 但金属性限制了其部分层面的应用与发展. 采用基于密度泛函理论的第一性原理赝势平面波方法研究了不同元素(Ti, V, Co, Ni)、不同掺杂浓度(原子百分比为3.70%, 7.41%, 11.1%)对二维CrSi2电子结构、磁学及光学性质的影响, 期望改善二维CrSi2材料的相关性质, 也为开发基于二维CrSi2的电子器件提供有效的理论基础. 研究表明: 二维CrSi2在远红外以及紫外范围内的吸收系数与反射系数都很强, 表现出优异的光学性质. 在原子百分比为3.70%的浓度下掺杂Ti, V, Ni后, 成功打开了二维CrSi2的带隙, 导致其分别向间接半导体、稀磁半导体和半金属铁磁体转变, 同时, 掺杂能对单分子层CrSi2的磁性进行有效的调控. 掺杂后的二维CrSi2拥有良好的光学性质, 多数掺杂体系的光学性质峰值增大并发生蓝移, 但在原子百分比为11.1%的掺杂浓度下, 吸收峰红移. 二维CrSi2有望成为高稳定性的新型自旋电子器件的制备材料.
Two-dimensional materials have shown excellent optical, mechanical, thermal or magnetic properties, and have promising applications in the high performance electronic, optical, spintronic devices and energy transfer, energy storage, etc. Monolayer transition metal silicide CrSi2 has shown ferromagnetism and metal properties in previous studies, and it is expected to become a new two-dimensional material. The Ti, V, Co, Ni doped two-dimensional CrSi2 are studied with different doping concentrations by using the first-principal pseudopotential plane wave method based on density functional theory, and electronic structure, magnetic and optical properties are calculated and analyzed. The results show that the density of states in the two-dimensional CrSi2 system is asymmetric, and the crystal cells have obvious ferromagnetism with a magnetic moment of 3.55 μB. Two-dimensional CrSi2 has strong absorptivity and reflectivity in the far infrared and ultraviolet range, showing excellent optical properties. The electronic structures and magnetic properties of Ti, V, Co or Ni doped CrSi2 with different concentrations are calculated and analyzed, and the results show that the magnetic moment of the two-dimensional CrSi2 varies after doping different elements at a doping concentration of 3.70 at%. After doping Ti, the magnetic moment of the system changes to 0 μB at a doping concentration of 3.70 at%, showing that it is an indirect semiconductor. After doping V, the magnetic moment becomes smaller at a doping concentration of 3.70 at%, and the system has two degrees of freedom: electron charge and spin, showing the properties of diluted magnetic semiconductors. After doping Ni, the band gap Eg=0.09 eV appears in the spin-up band of the system at a doping concentration of 3.70 at%, while the spin-down band is metallic, and the system shows semi-metallic properties. The magnetic moment changes to 3.71 μB after doping Ti at a doping concentration of 7.41 at%. After doping Co and Ni, the magnetic moment of the system becomes smaller at the doping concentration of 7.41 at%, and the spin-down 3d orbital electrons of ferromagnetic elements take the dominant position. After doping Ni, the magnetic moment becomes 0.37 μB at the doping concentration of 7.41 at%. After doping Ti, the magnetic moment becomes 2.79 μB at a doping concentration of 33.3 at at%, after doping V, the magnetic moment becomes 2.27 μB, and the degree of spin becomes weaker at a doping concentration of 11.1 at%. After doping Co, the magnetic moment becomes 1.81 μB at the doping concentration of 11.1 at%. The magnetic moment becomes 1.5 μB after doping Ni at the doping concentration of 11.1 at%, which proves that the spin-up d orbital has less electronic contribution to the magnetic moment. The energy band range of each system is enlarged, and the interaction between atoms is enlarged, and the energy level splitting energy is enlarged at the doping concentration of 11.1 at%, which indicates that the effective mass of the system becomes smaller, the mobility of carriers turns stronger, and the metallization of materials grows stronger. The optical properties of Ti, V, Co or Ni doped CrSi2 with different concentrations are calculated and analyzed, and the results show that the two-dimensional CrSi2 after being doped has good optical properties. For most of systems, their optical properties are improved and blue-shifted at the doping concentrations of 3.70 at% and 7.41 at%, but the absorption peak is red-shifted at the doping concentration of 11.1 at%. By studying the properties of doped two-dimensional CrSi2, it is found that the two-dimensional CrSi2 has excellent electronic structure and optical properties, and the electronic structure, magnetic and optical properties of the two-dimensional CrSi2 can be effectively changed by doping. Two-dimensional CrSi2 is expected to be a promising material for preparing new high reliability and high stability spintronic devices, and the present research provides an effective theoretical basis for developing the two-dimensional CrSi2 based devices. -
Keywords:
- two-dimensional CrSi2 materials /
- electronic structure /
- magnetic properties /
- optical properties
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图 4 不同浓度下Ti掺杂二维CrSi2的模型 (a)原子百分比为3.70%; (b) 原子百分比为7.41 %; (c) 原子百分比为11.1%
Fig. 4. Model of Ti doped two-dimensional CrSi2 at different concentrations: (a) Atomic percentage is 3.70%; (b) atomic percentage is 7.41%; (c) atomic percentage is 11.1%.
图 6 能带结构图 (a)三维CrSi2的能带结构图; (b)二维CrSi2的上旋电子能带结构; (c)二维CrSi2的下旋电子能带结构
Fig. 6. Energy band structure diagram: (a)Energy band structure diagram of three-dimensional CrSi2; (b) spin up electron band structure of two-dimensional CrSi2; (c) spin down electron band structure of two-dimensional CrSi2.
图 7 Ti, V, Co和Ni在3.70%, 7.41%, 11.1%浓度掺杂下二维CrSi2的能带结构 (a)上旋电子能带结构; (b)下旋电子能带结构
Fig. 7. Band structure of Ti, V, Co and Ni in two-dimensional CrSi2 doped with the concentration of 3.70%, 7.41% and 11.1%: (a) Spin up electron band structure; (b) spin down electron band structure.
图 8 CrSi2的态密度图 (a)三维CrSi2; (b)二维CrSi2
Fig. 8. Density of state of CrSi2: (a) Three dimensional CrSi2; (b) two dimensional CrSi2.
图 10 不同浓度掺杂后二维CrSi2的态密度图 (a) Ti-3.70%; (b) V-3.70%; (c) Co-3.70%; (d) Ni-3.70%; (e) Ti-7.41%; (f) V-7.41%; (g) Co-7.41%; (h) Ni-7.41%
Fig. 10. Density of states of two-dimensional CrSi2 doped with different concentrations: (a) Ti-3.70%; (b) V-3.70%; (c) Co-3.70%; (d) Ni-3.70%; (e) Ti-7.41%; (f) V-7.41%; (g) Co-7.41%; (h) Ni-7.41%.
图 11 二维CrSi2未掺杂及掺杂不同浓度的Ti, V, Co, Ni元素的磁矩
Fig. 11. Magnetic moments of two-dimensional CrSi2 undoped and doped with Ti, V, Co and Ni elements of different concentrations.
图 12 三维及二维CrSi2的复介电函数图
Fig. 12. Three-dimensional and two-dimensional complex dielectric function diagrams of CrSi2.
图 13 3.70%及7.41%浓度下掺杂后的复介电函数图 (a) Ti; (b) V; (c) Co; (d) Ni
Fig. 13. Complex dielectric function diagrams of doping at 3.70% and 7.41% concentrations: (a) Ti; (b) V; (c) Co; (d) Ni.
图 14 11.1%浓度下掺杂后的复介电函数图 (a) Ti, V; (b) Co, Ni
Fig. 14. Complex dielectric function of doping at 11.1 % concentration: (a) Ti, V; (b) Co, Ni.
图 15 三维和二维CrSi2的吸收系数
Fig. 15. Absorption coefficient of three-dimensional and two-dimensional CrSi2.
图 16 3.70%及7.41%浓度下掺杂后的吸收系数 (a) Ti; (b) V; (c) Co; (d) Ni
Fig. 16. Absorption coefficient of doping at 3.70 % and 7.41% concentrations: (a) Ti; (b) V; (c) Co; (d) Ni.
图 17 三维和二维CrSi2的反射系数
Fig. 17. Reflection coefficient of CrSi2 in three and two dimensions.
图 18 3.70%及7.41%浓度下掺杂后的反射系数 (a) Ti; (b) V; (c) Co; (d) Ni
Fig. 18. Reflection coefficient of doping at 3.70% and 7.41% concentrations: (a) Ti; (b) V; (c) Co; (d) Ni.
图 19 三维和二维CrSi2的能量损失函数
Fig. 19. Energy loss function diagrams of three-dimensional and two-dimensional CrSi2.
图 20 3.70%及7.41%浓度下掺杂后的能量损失函数 (a) Ti; (b) V; (c) Co; (d) Ni
Fig. 20. Energy loss function after doping at the concentration of 3.70% and 7.41%: (a) Ti; (b) V; (c) Co; (d) Ni.
表 2 三维及二维CrSi2的结构优化结果
Table 2. Structural optimization results of three-dimensional and two-dimensional CrSi2.
Model a/nm b/nm c/nm Vo/nm3 3D-CrSi2 0.438 0.438 0.632 0.107 2D-CrSi2 0.441 0.441 1.5 2.274 
下载: 导出CSV
表 3 过渡金属元素3d壳层的电子结构
Table 3. Electronic structure of 3d shell of transition metal elements.
原子序数 21 22 23 24 25 26 27 28 29 30 元素名 Sc Ti V Cr Mn Fe Co Ni Cu Zn 磁性 顺磁性 顺磁性 顺磁性 反铁磁性 反铁磁性 铁磁性 铁磁性 铁磁性 无磁性 无磁性 轨道结构 3d14s2 3d24s2 3d34s2 3d54s1 3d54s2 3d64s2 3d74s2 3d84s2 3d104s1 3d104s2 3d电子数及其自旋排布 ↑ ↑
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↑↓4s轨道电子数 2 2 2 1 2 2 2 2 1 2
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