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采用第一性原理计算方法研究了MoSi2N4/GeC异质结, 对其进行结构、电子及光学特性的计算, 并探究施加不同双轴应变和垂直电场对异质结能带结构及光吸收特性的影响, 研究表明: MoSi2N4/GeC异质结是一种带隙为1.25 eV的间接带隙半导体, 具有由GeC层指向MoSi2N4层的内建电场. 此外, 其光生载流子转移机制符合S型异质结机理, 从而提高了光催化水分解的氧化还原电位, 使其满足pH = 0—14范围内的光催化水分解要求. 双轴应变下, 带隙随压缩应变的增加而先增大再减小, 且在紫外区域的光吸收性能随压缩应变的增加而增强. 带隙随拉伸应变的增大而减小, 且可见光区域的光吸收性能较压缩应变时增强. 垂直电场下, 带隙随正电场的的增加而增大, 随负电场的增大而减小. 综上, MoSi2N4/GeC异质结可以作为一种高效的光催化材料应用于光电器件及光催化等领域.In this article, the first principles calculation method is used to study the MoSi2N4/GeC heterostructures, and calculate its structural, electronic, and optical properties. And the effects of different biaxial strains and vertical electric fields on the band structure and optical absorption characteristics of the heterostructures are also investigated. MoSi2N4/GeC heterostructure is an indirect bandgap semiconductor with a bandgap of 1.25 eV, with the built-in electric field direction pointing from the GeC layer to the MoSi2N4 layer. In addition, its photogenerated carrier transfer mechanism conforms to the S-type heterostructures mechanism, thus improving the oxidation reduction potential of photocatalytic water decomposition, making it fully meet the requirements of photocatalytic water decomposition with pH = 0–14. Under biaxial strain, the band gap first increases and then decreases with the increase of compressive strain, and the light absorption performance in the ultraviolet region increases with compressive strain increasing. The band gap decreases as tensile strain increases, and the light absorption performance in the visible light region is enhanced in comparison with its counterpart under compressive strain. Under a vertical electric field, the band gap increases with positive electric field increasing, and decreases with negative electric field increasing. In summary, MoSi2N4/GeC heterostructures can be used as an efficient photocatalytic material in some fields such as optoelectronic devices and photocatalysis.
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Keywords:
- S-type heterostructures /
- photocatalytic water decomposition /
- biaxial strain regulation /
- vertical electric field regulation
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图 1 MoSi2N4和GeC单层的俯视图和侧视图 (a) MoSi2N4; (b) GeC
Fig. 1. Top and side views of MoSi2N4 and GeC monolayer: (a) MoSi2N4; (b) GeC.
图 2 各单层材料的能带结构 (a) MoSi2N4; (b) GeC
Fig. 2. Band structure of each monolayer material: (a) MoSi2N4; (b) GeC.
图 3 不同堆垛方式的MoSi2N4/GeC vdWs异质结模型
Fig. 3. MoSi2N4/GeC vdWs heterostructure model with different stacking methods.
图 4 MoSi2N4/GeC vdWs异质结的电子特性 (a) 能带结构; (b) CBM的局域电荷密度; (c) VBM的局域电荷密度
Fig. 4. Electronic properties of MoSi2N4/GeC vdWs heterostructure: (a) Band structure; (b) local charge density of CBM; (b) local charge density of VBM.
图 5 MoSi2N4/GeC vdWs异质结沿Z方向的电子特性 (a) 静电势图 (蓝色虚线表示费米能级); (b) 平均平面电荷密度图 (插图是差分电荷密度图, 红色和黄色分别代表电荷的积累和消耗)
Fig. 5. Electronic properties of MoSi2N4/GeC vdWs heterostructure along Z direction: (a) Electrostatic potential diagram (Blue dotted line indicates Fermi energy level); (b) average plane charge density diagram (Inset is a differential charge density plot with red and yellow representing charge accumulation and consumption, respectively).
图 6 S型MoSi2N4/GeC vdWs异质结光生载流子的转移机制
Fig. 6. Transfer mechanism of S-type MoSi2N4/GeC vdWs heterostructure photogenerated carriers.
图 7 MoSi2N4, GeC和S型MoSi2N4/GeC vdWs异质结的光学特性 (a) 光吸收图谱; (b)在不同pH环境下的氧化还原电位
Fig. 7. Photocatalytic performance of MoSi2N4, GeC and MoSi2N4/GeC vdWs heterostructure: (a) Optical absorption spectra; (b) redox potential under different pH environments.
图 8 MoSi2N4/GeC vdWs异质结在不同双轴应变(a)和垂直电场(b)下的带隙变化
Fig. 8. Band gap change of MoSi2N4/GeC vdWs heterostructure are applied with different biaxial strains (a) and vertical electric field (b).
图 9 不同双轴应变下MoSi2N4/GeC vdWs异质结的能带结构 (a) ε = –8%; (b) ε = –6%; (c) ε = –4%; (d) ε = –2%; (e) ε = 2%; (f) ε = 4%; (g) ε = 6%; (h) ε = 8%
Fig. 9. Band structures of MoSi2N4/GeC vdWs heterostructure under different biaxial strains: (a) ε = –8%; (b) ε = –6%; (c) ε = –4%; (d) ε = –2%; (e) ε = 2%; (f) ε = 4%; (g) ε = 6%; (h) ε = 8%.
图 10 不同电场下MoSi2N4/GeC vdWs异质结的能带结构 (a) E = –0.4 V/Å; (b) E = –0.3 V/Å; (c) E = –0.2 V/Å; (d) E = –0.1 V/Å; (e) E = 0.1 V/Å; (f) E = 0.2 V/Å; (g) E = 0.3 V/Å; (h) E = 0.4 V/Å
Fig. 10. Band structure of MoSi2N4/GeC vdWs heterostructures under different field: (a) E = –0.4 V/Å; (b) E = –0.3 V/Å; (c) E = –0.2 V/Å; (d) E = –0.1 V/Å; (e) E = 0.1 V/Å; (f) E = 0.2 V/Å; (g) E = 0.3 V/Å; (h) E = 0.4 V/Å.
图 11 MoSi2N4/GeC vdWs异质结在不同双轴应变(a)和垂直电场(b)下的光吸收图谱
Fig. 11. Optical absorption spectra of MoSi2N4/GeC vdWs heterostructure under different biaxial strains (a) and vertical electric fields (b).
表 1 MoSi2N4和GeC的带隙(Eg)、功函数(Φ)、晶格常数(a)以及Ge—C, Mo—N和两种不同Si—N的键长dg (T1和T2分别代表两种不同的Si—N键键长)
Table 1. Band gap (Eg), work function (Φ), lattice constants (a) of MoSi2N4 and GeC and Ge—C, Mo—N and two different Si—N bond lengths (dg) (T1 and T2 represent two different Si—N bond lengths, respectively).
Eg/eV Φ/eV a/Å dg/Å Ge—C Mo—N T1 T2 MoSi2N4 1.80 5.20 2.910 — 2.096 1.747 1.755 GeC 2.07 4.63 3.265 1.883 — — — 
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[1] 熊子谦, 张鹏程, 康文斌, 方文玉 2020 物理学报 69 166301
Google Scholar
Xiong Z Q, Zhang P C, Kang W B, Fang W Y 2020 Acta Phys. Sin. 69 166301
Google Scholar
[2] Cai X F, Huang Y W, Hu J Z, Zhu S W, Tian X H, Zhang K, Ji G J, Zhang Y X, Fu Z D, Tan C L 2020 J. Catal. 10 1208
Google Scholar
[3] Yang K, Huang W Q, Xu L, Luo W K, Yang Y C, Huang G F 2016 Mater. Sci. Semicond. Process. 41 200
Google Scholar
[4] Sun Z Y, Xu J, Nsajigwa M, Yang W X, Wu X W, Yi Z, Chen S J, Zhang W B 2022 Commun. Theor. Phys. 74 015503
Google Scholar
[5] Bohayra M, Brahmanandam J, Fazel S, Rabczuk T, Shapeev A V, Zhuang X Y 2021 Nano Energy 82 105716
Google Scholar
[6] Hong Y L, Liu Z B, Wang L, Zhou T Y, Ma W, Xu C, Feng S, Chen L, Chen M L, Sun M D, Chen X Q, Cheng M H, Ren W C 2020 Science 369 670
Google Scholar
[7] Cao L M, Zhou G H, Wang Q Q, Ang L K, Ang Y S 2021 Appl. Phys. Lett. 8 013106
[8] Li Y H, Ho W K, Lü K L, Zhu B C, Li C S 2018 Appl. Surf. Sci. 430 380
Google Scholar
[9] Zhu Z, Tang X, Wang T, Fan W Q, Liu Z, Li C X, Huo P W, Yan Y S 2018 Appl. Catal. B 241 319
[10] Li S J, Li Y Y, Shao L X, Wang C D 2021 Chemistry Select 6 181
[11] Chen H, Li Y, Huang L, Li J B 2015 J. Phys. Chem. C 119 29148
Google Scholar
[12] King’ori G W, Ouma C N M, Mishra A K, Amolo G O, Makau N W T 2020 RSC Adv. 10 30127
Google Scholar
[13] Chen Y C, Tang Z Y, Shan H L, Jiang B, Ding Y L, Luo X, Zheng Y 2021 Phys. Rev. B 104 075449
Google Scholar
[14] Zhang X, Chen A, Zhang Z H, Jiao M G, Zhou Z 2019 Nanoscale Adv. 1 154
Google Scholar
[15] He Y, Zhang M, Shi J J, Cen Y L, Wu M 2019 J. Phys. Chem. C 123 12781
[16] Zhang K A, Zhang T N, Cheng G H, Li T X, Wang S X, Wei W, Zhou X H, Yu W W, Sun Y, Wang P, Zhang D, Zeng C G, Wang X J, Hu W D, Fan H J, Shen G Z, Chen X, Duan X F, Chang K, Dai N 2016 ACS Nano 10 3852
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[17] Jacobs D A, Langenhorst M, Sahli F, Richards B S, Paetzold U W 2019 J. Phys. Chem. Lett. 10 3159
Google Scholar
[18] He C, Zhang J H, Zhang W X, Li T T 2019 J. Phys. Chem. Lett. 10 3122
Google Scholar
[19] Fang L, Ni Y, Hu J S, Tong Z F, Ma X G, Lü H, Hou S C 2022 Phys. E 143 115321
Google Scholar
[20] Liu C Y, Wang Z W, Xiong W Q, Zhong H X, Yuan S J 2022 J. App. Phys. 131 163102
Google Scholar
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Google Scholar
Luo C, Long Q, Cheng B, Zhu B C, Wang L X 2023 Acta Phys. Chim. Sin. 39 2212026
Google Scholar
[22] 梅子慧, 王国宏, 严素定, 王娟 2021 物理化学学报 37 2009097
Google Scholar
Mei Z H, Wang G H, Yan S J, Wang J 2021 Acta Phys. Chim. Sin. 37 2009097
Google Scholar
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Google Scholar
[24] Ji Y J, Dong H L, Hou T J, Li Y Y 2018 J. Mater. Chem. A 6 2212
Google Scholar
[25] Fan X P, Jiang J W, Li R, Guo L, Mi W B 2022 Chem. Phys. Lett. 805 139968
[26] Kresse G, Furthmüller J 1996 Comp. Mat. Sci. 54 11169
Google Scholar
[27] Kresse G, Joubert D 1999 Phys. Rev. B 59 1758
Google Scholar
[28] Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865
Google Scholar
[29] Shi J Y, Ou Y, Max A M, Wang H Y, Li H, Zhang Y, Gu Y S, Zou M Q 2019 Comput. Mater. Sci. 160 301
Google Scholar
[30] Guo R, Luan L J, Cao M Y, Zhang Y, Wei X, Fan J B, Ni L, Liu C, Yang Y, Liu J, Tian Y, Duan L 2023 Phys. E 149 115628
[31] Li R X, Tian X L, Zhu S C, Mao Q H, Ding J, Li H D 2022 Phys. E 144 115443
[32] Yang F, Zhuo Z G, Han J N, Cao X C, Tao Y, Zhang L, Liu W J, Zhu Z Y, Dai Y H 2021 Superlattice. Microst. 156 106935
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Google Scholar
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Google Scholar
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Google Scholar
Luan L J, He Y, Wang T, Liu Z W 2021 Acta Phys. Sin. 70 166302
Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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