二维半金属/硅异质结中肖特基势垒高度的准确高效预测

doi:10.1016/j.actphy.2025.100078

物理化学学报 >> 2025, Vol. 41 >> Issue (7): 100078.doi: 10.1016/j.actphy.2025.100078

所属专题：新型光电功能材料

二维半金属/硅异质结中肖特基势垒高度的准确高效预测

诸海渝¹^,², 文卓群²^,³^,⁴, 熊稳³^,⁴^,*(), 魏兴战²^,³^,⁴^,*(), 王峙⁵^,*()

¹ 重庆邮电大学光电工程学院, 重庆 400065
² 中国科学院大学重庆学院, 重庆 400714
³ 中国科学院重庆绿色智能技术研究院, 重庆 400714
⁴ 中国科学院大学, 北京 100049
⁵ 中国科学院半导体研究所, 半导体芯片物理与技术全国重点实验室, 北京 100083

收稿日期:2025-01-17 修回日期:2025-03-02 录用日期:2025-03-04 发布日期:2025-05-22
通讯作者: Email: xiongwen@cigit.ac.cn (Zhi Wang)weixingzhan@cigit.ac.cn (魏兴战)wangzhi@semi.ac.cn (王峙)
基金资助:
国家自然科学基金(12174380); 国家自然科学基金(11904359); 国家自然科学基金(62074021); 重庆市自然科学基金(CSTB2023NSCQ-LZX0087); 重庆市自然科学基金(cstc2020jcyj-msxmX0822)

Accurate and efficient prediction of Schottky barrier heights in 2D semimetal/silicon heterojunctions

Haiyu Zhu¹^,², Zhuoqun Wen²^,³^,⁴, Wen Xiong³^,⁴^,*(), Xingzhan Wei²^,³^,⁴^,*(), Zhi Wang⁵^,*()

¹ School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
² Chongqing School, University of Chinese Academy of Sciences, Chongqing 400714, China
³ Chongqing Institute of Green and Intelligent Technology, Chinese Academy of Sciences, Chongqing 400714, China
⁴ University of Chinese Academy of Sciences, Beijing 100049, China
⁵ State Key Laboratory of Semiconductor Physics and Chip Technologies, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, China

Received:2025-01-17 Revised:2025-03-02 Accepted:2025-03-04 Published:2025-05-22
Contact: Email: xiongwen@cigit.ac.cn (Wen Xiong)weixingzhan@cigit.ac.cn (Xingzhan Wei)wangzhi@semi.ac.cn (Zhi Wang)
Supported by:
the National Natural Science Foundation of China(12174380); the National Natural Science Foundation of China(11904359); the National Natural Science Foundation of China(62074021); the Natural Science Foundation of Chongqing, China(CSTB2023NSCQ-LZX0087); the Natural Science Foundation Project of CQ CSTC, China(cstc2020jcyj-msxmX0822)

摘要/Abstract

摘要：

肖特基势垒高度(SBH)的准确预测对优化半金属/半导体异质结器件的性能至关重要。目前，二维半金属/半导体异质结构已在实验上得到广泛研究。然而，基于第一性原理的SBH预测通常需要在包含超过10³个原子的超胞中求解从头算哈密顿量。计算复杂度的增加不仅导致效率极低，还限制了异质结器件的设计和优化。本研究采用密度泛函理论结合核心能级对准方法，将过渡金属二碲化物半金属/硅异质结的超胞尺寸减少了一个数量级，计算得到的SBH与实验结果一致。进一步研究了多种二维半金属化合物，结果表明候选材料的空穴SBH均低于电子SBH，此外，厚度效应在三到五层后变得可以忽略不计。本研究为复杂异质结构中SBH计算提供一种高效的计算框架，能够为高性能二维半金属异质结器件的优化设计提供理论依据。

关键词: 肖特基势垒高度, 半金属/硅异质结构, 核心能级对准方法, 第一性原理, 晶格失配

Abstract:

The accurate prediction of the Schottky barrier height (SBH) holds significant importance for optimizing the performance of semimetal/semiconductor heterojunction devices. Two-dimensional semimetal/semiconductor heterostructures have now been extensively studied experimentally. However, first-principles predictions of the corresponding SBH typically require solving the ab initio Hamiltonian in supercells containing more than 10³ atoms. This high computational complexity not only results in extremely low efficiency but also hinders the design and optimization of heterojunction devices. Herein, we apply density functional theory with a core-level energy alignment method for transition-metal-ditelluride semimetal/silicon junctions, which enables a reduction in supercell size by one order of magnitude. The predicted SBHs show excellent agreement with experiment. We further investigate different 2D semimetal compounds, finding that all candidates exhibit lower SBHs for holes than electrons, with thickness effects becoming negligible beyond three to five layers. This study presents an efficient framework for calculating SBH in complex heterostructures and provides theoretical guidance for the efficient design of high-performance 2D semimetal heterojunction devices.

Key words: Schottky barrier height, Semimetal/silicon heterostructure, Core-level energy alignment method, First principles, Lattice mismatch

诸海渝, 文卓群, 熊稳, 魏兴战, 王峙. 二维半金属/硅异质结中肖特基势垒高度的准确高效预测[J]. 物理化学学报, 2025, 41(7), 100078. doi: 10.1016/j.actphy.2025.100078

Haiyu Zhu, Zhuoqun Wen, Wen Xiong, Xingzhan Wei, Zhi Wang. Accurate and efficient prediction of Schottky barrier heights in 2D semimetal/silicon heterojunctions[J]. Acta Phys. -Chim. Sin. 2025, 41(7), 100078. doi: 10.1016/j.actphy.2025.100078

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100078

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I7/100078

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参考文献 53

1	Chang, C. C.; Sharma, Y. D.; Kim, Y. S.; Bur, J. A.; Shenoi, R. V.; Krishna, S.; Huang, D.; Lin, S. Y. Nano. Lett. 2010, 10, 1704. doi: 10.1021/nl100081j
2	Tan, C. L.; Mohseni, H. Nanophotonics 2018, 7, 169. doi: 10.1515/nanoph-2017-0061
3	Tyagi, D.; Wang, H.; Huang, W.; Hu, L.; Tang, Y.; Guo, Z.; Ouyang, Z.; Zhang, H. Nanoscale 2020, 12, 3535. doi: 10.1039/c9nr10178k
4	Liu, C. Y.; Guo, J. S.; Yu, L. W.; Li, J.; Zhang, M.; Li, H.; Shi, Y. C.; Dai, D. X. Light Sci. Appl. 2021, 10, 123. doi: 10.1038/s41377-021-00551-4
5	Zhang, K. X.; Zhang, L. B.; Han, L.; Wang, L.; Chen, Z. Q. Z.; Xing, H. Z.; Chen, X. S. Nano Ex. 2021, 2, 012001. doi: 10.1088/2632-959X/abd45b
6	Long, M. S.; Wang, P.; Fang, H. H.; Hu, W. D. Adv. Funct. Mater. 2018, 29, 1803807. doi: 10.1002/adfm.201803807
7	Zha, J. J.; Luo, M. C.; Ye, M.; Ahmed, T.; Yu, X. C.; Lien, D. H.; He, Q. Y.; Lei, D. Y.; Ho, J. C.; Bullock, J.; et al. Adv. Funct. Mater. 2021, 32, 2111970. doi: 10.1002/adfm.202111970
8	Jiang, H.; Wang, M.; Fu, J.; Li, Z.; Shaikh, M. S.; Li, Y.; Nie, C.; Sun, F.; Tang, L.; Yang, J.; et al. ACS Nano 2022, 16, 12777. doi: 10.1021/acsnano.2c04704
9	Jiang, H.; Wei, J.; Sun, F.; Nie, C.; Fu, J.; Shi, H.; Sun, J.; Wei, X.; Qiu, C. W. ACS Nano 2022, 16, 4458. doi: 10.1021/acsnano.1c10795
10	Fu, J.; Guo, Z.; Nie, C.; Sun, F.; Li, G.; Feng, S.; Wei, X. Innovation 2024, 5, 100600. doi: 10.1016/j.xinn.2024.100600
11	Xie, C.; Zeng, L.; Zhang, Z.; Tsang, Y. H.; Luo, L.; Lee, J. H. Nanoscale 2018, 10, 15285. doi: 10.1039/c8nr04004d
12	Wu, Y.; Nie, C.; Sun, F.; Jiang, X.; Zhang, X.; Fu, J.; Peng, Y.; Wei, X. ACS Appl. Mater. Interfaces 2024, 16, 22632. doi: 10.1021/acsami.4c00827
13	Chen, B.; Xu, S.; Cheng, R.; Zhao, Y. IEEE Electron Device Lett. 2019, 40, 632. doi: 10.1109/led.2019.2897817
14	Huang, Z. W.; Yu, C. Y.; Chang, A. L.; Zhao, Y. M.; Huang, W.; Chen, S. Y.; Li, C. J. Mater. Sci. 2020, 55, 8630. doi: 10.1007/s10853-020-04625-3
15	Tersoff, J. Phys. Rev. B 1984, 30, 4874. doi: 10.1103/PhysRevB.30.4874
16	Tersoff, J. Phys. Rev. B 1985, 32, 6968. doi: 10.1103/physrevb.32.6968
17	Chiappe, D.; Scalise, E.; Cinquanta, E.; Grazianetti, C.; Van den Broek, B.; Fanciulli, M.; Houssa, M.; Molle, A. Adv. Mater. 2014, 26, 2096. doi: 10.1002/adma.201304783
18	Van, B. R.; Yao, Q.; Banerjee, S.; Cakir, D.; Oncel, N.; Zandvliet, H. J. W. Beilstein J. Nanotechnol 2017, 8, 1952. doi: 10.3762/bjnano.8.196
19	Zhou, S. R.; Wen, S. F.; Fan, H. D.; Wei, Y. Y.; Yin, Y.; Lan, C. Y.; Li, C.; Liu, Y. ACS Photonics 2024, 11, 1810. doi: 10.1021/acsphotonics.4c00331
20	Choi, H.; Min, K. A.; Cha, J.; Hong, S. Phys. Chem. Chem. Phys. 2018, 20, 25240. doi: 10.1039/c8cp05201h
21	Fang, P. X. W.; Nihtianov, S.; Sberna, P.; De Wijs, G. A.; Fang, C. M. J. Phys. Commun. 2022, 6, 085010. doi: 10.1088/2399-6528/ac8854
22	Mott, N. F. Proc. R. Soc. (London) A 1939, 171, 27. doi: 10.1098/rspa.1939.0051
23	Schottky, W. Z. Phys. 1939, 113, 367. doi: 10.1007/BF01340116
24	Bardeen, J. Phys. Rev. 1947, 71, 717. doi: 10.1103/PhysRev.71.717
25	Skachkov, D.; Liu, S. L.; Wang, Y.; Zhang, X. G.; Cheng H. P. Phys. Rev. B 2021, 104, 045429. doi: 10.1103/PhysRevB.104.045429
26	Nangoi, J. K.; Palmstrom, C. J.; Van de Walle, C. G. Phys. Rev. B 2024, 110, 035302. doi: 10.1103/PhysRevB.110.035302
27	Chin, K. K.; Cao, R.; Kendelewicz, T.; Miyano, K.; Williams, M. D.; Doniach, S.; Lindau, I.; Spicer, W. E. MRS Online Proc. Libr. 1986, 77, 297. doi: 10.1557/PROC-77-297
28	Kim, H.; Kumar, M. D.; Kim, J. Sensor Actuat A-phys 2015, 233, 290. doi: 10.1016/j.sna.2015.07.026
29	Taffelli, A.; Dirè, S.; Quaranta, A.; Pancheri, L. Sensors 2021, 21, 2758. doi: 10.3390/s21082758
30	Wei, S. H.; Alex, Z. Appl. Phys. Lett. 1998, 72, 2011. doi: 10.1063/1.121249
31	Li, Y. H.; Walsh, A.; Chen, S. Y.; Yin, W. J.; Yang, J. H.; Li, J. B.; Da Silva, J. L. F.; Gong X. G.; Wei, S. H. Appl. Phys. Lett. 2009, 94, 212109. doi: 10.1063/1.3143626
32	Lang, L.; Zhang, Y. Y.; Xu, P.; Chen, S. Y.; Xiang, H. J.; Gong, X. G. Phys. Rev. B 2015, 92, 075102. doi: 10.1103/PhysRevB.92.075102
33	Hu, Y. Y; Qiu, C.; Shen, T.; Yang, K. K.; Deng, H. X. J. Semicond. 2021, 42, 112102. doi: 10.1088/1674-4926/42/11/112102
34	Kresse, G.; Furthmüller, J. Comput. Mater. Sci. 1996, 6, 15. doi: 10.1016/0927-0256(96)00008-0
35	Kresse, G.; Furthmüller, J. Phys. Rev. B 1996, 54, 11169. doi: 10.1103/PhysRevB.54.11169
36	Kresse, G.; Joubert, D. Phys. Rev. B 1999, 59, 1758. doi: 10.1103/PhysRevB.59.1758
37	Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865. doi: 10.1103/PhysRevLett.77.3865
38	Heyd, J.; Scuseria, G. E.; Ernzerhof, M. J. Chem. Phys. 2003, 118, 8207. doi: 10.1063/1.1564060
39	Heyd, J.; Scuseria, G. E.; Ernzerhof, M. J. Chem. Phys. 2006, 124, 219906. doi: 10.1063/1.2204597
40	Leendertz, C.; Mingirulli, N.; Schulze, T. F.; Kleider, J. P.; Rech, B.; Korte, L. Appl. Phys. Lett. 2011, 98, 2002108. doi: 10.1063/1.3590254
41	Zeng, L. H.; Wu, D.; Jie, J. S.; Ren, X. Y.; Hu, X.; Lau, S. P.; Chai, Y.; Tsang, Y. H. Adv. Mater. 2020, 32, 2004412. doi: 10.1002/adma.202004412
42	Wei, S. H.; Zunger, A. Phys. Rev. B 1999, 60, 5404. doi: 10.1103/PhysRevB.60.5404
43	Li, Y. H.; Gong X. G.; Wei, S. H. Appl. Phys. Lett. 2006, 88, 042104. doi: 10.1063/1.2168254
44	Zhang, L.; Zhu, X. D.; Ling, L. S.; Zhang, C. J.; Pi, L.; Zhang, Y. H. Philos. Mag. 2013, 94, 439. doi: 10.1080/14786435.2013.855333
45	Qi, M. Y.; An, C.; Zhou, Y. H.; Wu, H.; Zhang, B. W.; Chen, C. H.; Yuan, Y. F.; Wang, S. Y.; Zhou, Y.; Chen, X. L.; et al. Phys. Rev. B 2020, 101, 115124. doi: 10.1103/PhysRevB.101.115124
46	Noh, H. J.; Jeong, J.; Cho, E. J.; Kim, K.; Min, B. I.; Park, B. G. Phys. Rev. Lett. 2017, 119, 016401. doi: 10.1103/PhysRevLett.119.016401
47	Ma, H. F.; Chen, P.; Li, B.; Li, J.; Ai, R. Q.; Zhang, Z. W.; Sun, G. Z.; Yao K. K.; Lin, Z. Y.; Zhao, B.; et al. Nano Lett. 2018, 18, 3523. doi: 10.1021/acs.nanolett.8b00583
48	Zahir, M.; Muhammad, Z.; Sami, U.; Zhang, B.; Lu, Q. X.; Zhu, L.; Hu, R. Inorg. Chem. Front. 2021, 8, 3885. doi: 10.1039/d1qi00553g
49	Li, P. F.; Li, L.; Zeng, X. C. J. Mater. Chem. C 2016, 4, 3106. doi: 10.1039/c6tc00130k
50	Yu, M.; Trinkle, D. R. J. Chem. Phys. 2011, 134, 064111. doi: 10.1063/1.3553716
51	Jan, G.; McMillan, P. F.; Marzke, R. F.; Ramachandran, G. K.; Patton, D.; Deb, S. K.; Sankey, O. F. Phys. Rev. B 2000, 62, R7707. doi: 10.1103/PhysRevB.62.R7707
52	Villaos, R. A. B.; Crisostomo, C. P.; Huang, Z. Q.; Huang, S. M.; Padama, A. A. B.; Albao, M. A.; Lin, H.; Chuang, F. C. NPJ 2D Mater. Appl. 2019, 3, 2. doi: 10.1038/s41699-018-0085-z
53	Yan, M.; Huang, H.; Zhang, K.; Wang, E.; Yao, W.; Deng, K.; Wan, G.; Zhang, H.; Arita, M.; Yang, H.; et al. Nat. Commun. 2017, 8, 257. doi: 10.1038/s41467-017-00280-6

2D material	Equilibrium lattice constant (hexagonal) (Å)				2D/Si(001) heterojunction strain applied on 2D (%)
	This work		Exp.		2D/Si(001) heterojunction strain applied on 2D (%)
	a = b	c	a = b	c	along (100)	along (010)
IrTe₂	3.959	5.419	3.929 ^a)	5.405 ^a)	10.7	−3.1
NiTe₂	3.860	5.177	3.878 ^b)	5.265 ^b)	13.0	−0.5
PdTe₂	4.028	5.128	4.036 ^c)	5.126 ^c)	8.3	−5.9
PtTe₂	4.048	5.113	4.026 ^d)	5.221 ^d)	8.7	−5.4
ZrTe₂	3.909	6.683	3.940 ^e)	6.630 ^e)	11.8	−1.8

Thickness	IrTe₂/Si	NiTe₂/Si	PdTe₂/Si	PtTe₂/Si	ZrTe₂/Si
1L	0.813	0.725	0.681	–	0.797
2L	0.872	0.826	0.781	0.640	0.811
3L	0.861	0.850	0.828	0.707	0.845
4L	0.859	0.823	0.819	0.691	0.849
5L	0.858	0.826	0.797	0.702	0.854
Bulk	0.849	0.828	0.808	0.697 (exp.: 0.733*)	0.859

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二维半金属/硅异质结中肖特基势垒高度的准确高效预测

Accurate and efficient prediction of Schottky barrier heights in 2D semimetal/silicon heterojunctions

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