Stability and electronic structure of hydrogenated two-dimensional transition metal dichalcogenides: First-principles study

Wang Dan; Zou Juan; Tang Li-Ming

doi:10.7498/aps.68.20181597

Abstract

Chemical functionalization of two-dimensional transition metal dichalcogenides (TMDs) with hydrogen is an effective and economical method to synthesize monolayer TMDs and tune their electronic properties. We theoretically study the stabilities and electronic properties of chemisorbed H atoms on monolayer TMDs by using density-functional theory calculations. The result shows that there exists a more stable adsorption site in the layers of the monolayer MX₂ (M = Mo, W; X = S, Se, Te) than its surface for hydrogen. In the case of the same cation, with the increase of the anion (X²⁻) atomic number, the stronger the bonding between the H atom and the MX₂ layer, the more stable the structure of the hydrogenated monolayer MX₂ is. However, in the case of the same anion, the binding between the H atom and the MX₂ layer becomes weaker as the atomic number of the cations increases. H atoms passes through one surface of the MS₂ to the other surface with a relatively small diffusion barrier of about 0.9 eV. So the H atoms can more easily go through the barrier. And for the H atom to go through the other monolayer MX₂ (M = Mo, W; X = Se, Te), the diffusion barrier is about 1.2 eV. H atoms are difficult to pass through the barrier at this time. The singular diffusion behavior of H atoms in monolayer MX₂ is conducible to understanding the stability of hydrogenated two-dimensional transition metal sulfide system. In addition, the surface hydrogenation and interlaminar hydrogenation have different effects on the electronic properties of monolayer MX₂, and mainly manifest themselves in the fact that the surface hydrogenation induces spontaneous magnetism and sharply reduces the band gap, but still retains the semiconductor properties of the original monolayer MX₂. However, interlaminar hydrogenation enables monolayer MX₂ to directly realize the transition from semiconductor to metal. Interlaminar hydrogenation monolayer MX₂ (M = Mo, W; X = S, Se) make the system generating magnetism, while when the anion is Te²⁻, the magnetism almost disappears. These results can provide theoretical guidance in understanding hydrogen functionalization of MX₂ layer, and also present a certain theoretical basis for realizing the application of MX₂ in nano-electronic devices.

Keywords:

hydrogenation /
two-dimensional transition metal dichalcogenides /
stability /
electronic properties

Authors and contacts

1.
College of Science, Central South University of Forestry and Technology, Changsha 410004, China
2.
School of Physics and Electronics, Hunan University, Changsha 410082, China

Corresponding author: Tang Li-Ming, lmtang@hnu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 11674090, 11347022, 11447224).

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References

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Cited By

图 1 单层MX₂的结构模型及可能的H吸附位点示意图, 其中蓝色, 橙色和粉色分别表示阴离子(X²⁻)、阳离子(M⁴⁺)和氢原子; A—F表示氢原子可能的吸附位点

Figure 1. Structural model and possible H adsorption sites of single-layer MX₂. Blue, orange and pink balls correspond to anions (X²⁻), cations (M⁴⁺) and hydrogen atoms, respectively. A−F shows a possible adsorption site for hydrogen atom.

DownLoad: Full-Size Img PowerPoint

图 2 单层MX₂的稳定吸附位点结合能统计图

Figure 2. Binding energy of the stable adsorption sites of single-layer MX₂.

DownLoad: Full-Size Img PowerPoint

图 3 氢原子穿过单层MX₂的扩散势垒(扩散路径为从单层MX₂表面D点穿过层间E点扩散到另一个表面D'点)

Figure 3. Diffusion barrier of hydrogen atoms through a single layer of MX₂. The diffusion path is from the D point of surface through the interlayer E point to the other surface D' point.

DownLoad: Full-Size Img PowerPoint

图 4 氢原子稳定吸附在单层 MX₂的电荷转移分布图(计算的电荷转移为MX₂层E位点的转移情况, 箭头指示电荷转移的方向)

Figure 4. Charge transfer profile of hydrogen atoms adsorbed on a single-layer MX₂. The calculated charge transfer is the transfer of the E site of the MX₂ layer, and the arrows indicate the direction of charge transfer.

DownLoad: Full-Size Img PowerPoint

图 5 4 × 4单层MX₂ (1L-MX₂)超胞的能带结构图(费米能级用黑色虚线表述并设为0 eV)

Figure 5. Band structures of 4 × 4 monolayer MX₂ (1L-MX₂) supercell. The fermi level is represented by dotted black line and set as 0 eV.

DownLoad: Full-Size Img PowerPoint

图 6 表面氢化MX₂能带结构图(蓝色和红色线分别表示自旋向上和自旋向下)

Figure 6. Band structures of surface hydrogenation MX₂. Blue and red correspond to spin-up and spin-down, respectively.

DownLoad: Full-Size Img PowerPoint

图 7 层间氢化MX₂能带结构图(蓝色和红色线表示自旋向上和自旋向下)

Figure 7. Band structures of interlayer hydrogenation MX₂. Blue and red correspond to spin-up and spin-down, respectively.

DownLoad: Full-Size Img PowerPoint

表 1 氢原子吸附在单层MX₂上的可能吸附位点(AS)的结合能, 及氢原子与阳离子(M⁴⁺ = Mo, W)的键长

Table 1. Binding energy of possible adsorption sites (AS) of hydrogen atoms adsorbed on single-layer MX₂, and M—H (M⁴⁺ = Mo, W) bond lengths.

AS	Binding energy/eV						M—H键长/Å
AS	A	B	C	D	E	F	M—H键长/Å
MoS₂	−0.38	−0.41	0.21	−0.27	−0.44	0.99	1.893
MoSe₂	−0.19	−0.16	−0.26	−0.30	−0.91	0.47	1.950
MoTe₂	−0.10	−0.35	−0.10	−0.52	−1.42	−0.19	1.996
WS₂	−0.09	−0.16	0.30	−0.06	−0.26	1.58	1.901
WSe₂	−0.01	−0.09	0.50	−0.18	−0.80	0.69	1.970
WTe₂	0.09	−0.05	−0.64	−0.45	−1.39	−0.18	2.005

DownLoad: CSV

map

[1]	Tang L P, Tang L M, Wang D, Deng H X, Chen K Q 2018 J. Phys.: Condens. Matter 30 465301 Google Scholar
[2]	Xie G F, Ding D, Zhang G 2018 Adv. Phys. X 3 1480417 Google Scholar
[3]	Wang D, Tang L M, Jiang X X, Tan J Y, He M D, Wang X J, Chen K Q 2018 Adv. Electron. Mater. DOI: 10.1002/aelm.201800475
[4]	Koppens F H, Mueller T, Avouris P, Ferrari A C, Vitiello M S, Polini M 2014 Nat. Nanotechnol. 9 780 Google Scholar
[5]	Schwierz F, Pezoldt J, Granzner R 2015 Nanoscale 7 8261 Google Scholar
[6]	Dean C R, Young A F, Meric I, Lee C, Wang L, Sorgenfrei S, Watanabe K, Taniguchi T, Kim P, Shepard K L, Hone J 2010 Nat. Nanotechnol. 5 722 Google Scholar
[7]	Zhang Y, Tang T T, Girit C, Hao Z, Martin M C, Zettl A, Crommie M F, Shen Y R, Wang F 2009 Nature 459 820 Google Scholar
[8]	Zhang W, Lin C T, Liu K K, Tite T, Su C Y, Chang C H, Lee Y H, Chu C W, Wei K H, Kuo J L, Li L J 2011 ACS Nano 5 7517 Google Scholar
[9]	Flores M Z, Autreto P A, Legoas S B, Galvao D S 2009 Nanotechnology 20 465704 Google Scholar
[10]	Sofo J O, Chaudhari A S, Barber G D 2007 Phys. Rev. B 75 153401 Google Scholar
[11]	Wang H, Yu L, Lee Y H, Shi Y, Hsu A, Chin M, Li L J, Dubey M, Kong J, Palacios T 2012 Nano Lett. 12 4674 Google Scholar
[12]	Radisavljevic B, Radenovic A, Brivio J, Giacometti V, Kis A 2011 Nat. Nanotechnol. 6 147 Google Scholar
[13]	Kang K, Xie S, Huang L, Han Y, Huang P Y, Mark K F, Kim C J, Muller D, Park J 2015 Nature 520 656 Google Scholar
[14]	Tang L P, Tang L M, Geng H, Yi Y P, Wei Z, Chen K Q, Deng H X 2018 Appl. Phys. Lett. 112 012101 Google Scholar
[15]	Xue X X, Feng Y X, Liao L, Chen Q J, Wang D, Tang L M, Chen K Q 2018 J. Phys.: Condens. Matter 30 125001 Google Scholar
[16]	颜送灵, 唐黎明, 赵宇清 2016 65 077301 Google Scholar Yan S L, Tang L M, Zhao Y Q 2016 Acta Phys. Sin. 65 077301 Google Scholar
[17]	李立明, 宁锋, 唐黎明 2015 64 227303 Google Scholar Li L M, Ning F, Tang L M 2015 Acta Phys. Sin. 64 227303 Google Scholar
[18]	Bernardi M, Palummo M, Grossman J C 2013 Nano Lett. 13 3664 Google Scholar
[19]	Lopezsanchez O, Lembke D, Kayci M, Radenovic A, Kis A 2013 Nat. Nanotechnol. 8 497 Google Scholar
[20]	Bertolazzi S, Brivio J, Kis A 2011 ACS Nano 5 9703 Google Scholar
[21]	Eda G, Yamaguchi H, Voiry D, Fujita T, Chen M, Chhowalla M 2011 Nano Lett. 11 5111 Google Scholar
[22]	Ning F, Wang D, Feng Y X, Tang L M, Zhang Y, Chen K Q 2017 J. Mater. Chem. C 5 9429 Google Scholar
[23]	Cao T, Wang G, Han W, Ye H, Zhu C, Shi J, Niu Q, Tan P, Wang E, Liu B, Feng J 2012 Nat. Commun. 3 887 Google Scholar
[24]	Li Q, Tang L, Zhang C, Wang D, Chen Q J, Feng Y X, Tang L M, Chen K Q 2017 Appl. Phys. Lett. 111 171602 Google Scholar
[25]	Xu Y, Li Y, Chen X, Zhang C, Zhang R, Lu P 2016 AIP Adv. 6 075001 Google Scholar
[26]	Kam K K, Parkinson B A 1982 J. Phys. Chem. 86 463 Google Scholar
[27]	Chen J, Li S L, Xu Q, Tanaka K 2002 Chem. Commun. 16 1722 Google Scholar
[28]	Cheng F Y, Chen J, Gou X L 2006 Adv. Mater. 18 2561 Google Scholar
[29]	Karunadasa H I, Montalvo E, Sun Y, Majda M, Long J R, Chang C J 2012 Science 335 698 Google Scholar
[30]	Mouri S, Miyauchi Y, Matsuda K 2013 Nano Lett. 13 5944 Google Scholar
[31]	Chhowalla M, Amaratunga G A 2000 Nature 407 164 Google Scholar
[32]	Muratore C, Voevodin A A 2006 Surf. Coat. Technol. 201 4125 Google Scholar
[33]	Stefanov M, Enyashin A N, Heine T, Seifert G 2008 J. Phys. Chem. C 112 17764 Google Scholar
[34]	Mak K F, Lee C, Hone J, Shan J, Heinz T F 2010 Phys. Rev. Lett. 105 136805 Google Scholar
[35]	Elias D C, Nair R R, Mohiuddin T M G, Morozov S V, Blake P, Halsall M P, Ferrari A C, Boukhvalov D W, Katsnelson M I, Geim A K, Novoselov K S 2009 Science 323 610 Google Scholar
[36]	Zou J, Tang L M, Chen K Q, Feng Y X 2017 J. Phys.: Condens. Matter 30 065001 Google Scholar
[37]	Zhang W, Zhang Z, Yang W 2015 J. Nanosci. Nanotechnol. 15 8075 Google Scholar
[38]	van der Marel D, Molegraaf H J A, Zaanen J, Nussinov Z, Carbone F, Damascelli H, Eisaki H, Greven M, Kes P H, Li M 2003 Nature 425 271 Google Scholar
[39]	Sundberg P, Moyes R B, Tomkinson J 1991 Bull. Soc. Chim. Belg. 100 967 Google Scholar
[40]	Lozada-Hidalgo M, Zhang S, Hu S, Kravets V G, Rodriguez F J, Berdyugin A, Grigorenko A, Geim A K 2018 Nat. Nanotechnol. 13 300 Google Scholar
[41]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[42]	Blöchl P E 1994 Phys. Rev. B 50 17953 Google Scholar
[43]	Henkelman G, Uberuaga B P, Jónsson H 2000 J. Chem. Phys. 113 9901 Google Scholar
[44]	Koh E W K, Chiu C H, LimY K, ZhangY W, Pan H 2012 Int. J. Hydrogen Energy 37 14323 Google Scholar
[45]	Özçelik V O, Azadani J G, Yang C, Koester S J, Low T 2016 Phys. Rev. B 94 035125 Google Scholar

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