Tuning electronic and magnetic properties in monolayer MoSe2 by metal adsorption

Accepted Manuscript Research paper Tuning electronic and magnetic properties in monolayer MoSe2 by metal adsorption Songlei Huang, Quan Zhang, Shuai Liu, Hongping Li, Changsheng Li, Jian Meng, Yi Tian PII: DOI: Reference:

S0009-2614(17)30837-0 http://dx.doi.org/10.1016/j.cplett.2017.08.064 CPLETT 35074

To appear in:

Chemical Physics Letters

Received Date: Revised Date: Accepted Date:

23 July 2017 24 August 2017 30 August 2017

Please cite this article as: S. Huang, Q. Zhang, S. Liu, H. Li, C. Li, J. Meng, Y. Tian, Tuning electronic and magnetic properties in monolayer MoSe2 by metal adsorption, Chemical Physics Letters (2017), doi: http://dx.doi.org/ 10.1016/j.cplett.2017.08.064

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Tuning electronic and magnetic properties in monolayer MoSe 2 by metal adsorption Songlei Huang,a Quan Zhang,a Shuai Liu,a Hongping Li,a,* Changsheng Li,a Jian Meng,b Yi Tianc,** a Institute for Advanced Materials, School of Materials Science and Engineering, Jiangsu University, Zhenjiang, 212013, P. R. China b State Key Laboratory of Rare Earth Resources Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, P. R. China c

Department of Chemistry, National University of Singapore, 3 Science Drive 3, 1175 43, Singapore

Abstract We have systematically explored the electronic structures and magnetic properties of metal Pd, Pt, Cu, Ag, Au and Zn adsorbed MoSe2 monolayer by means of first-principles calculations. It reveals that stable chemical adsorption has been formed between the adatoms Pd, Pt, Cu, Ag, Au and MoSe2 monolayer, however, weak physical interaction is found between Zn and MoSe2 monolayer owing to the small adsorption energy. Both the framework structure and electronic property of the metal adsorbed MoSe2 monolayer are slightly tuned by the adatoms. More importantly, magnetic character is introduced in Cu, Ag and Au systems. Keywords: MoSe2 monolayer; metal adsorption; electronic and magnetic properties; First-principles calculations 1. Introduction Since the discovery of graphene in 2004, two-dimensional layered materials have inspired a surge of interests [1-3]. Among them, layered transition-metal dichalcogenides (LTMDs) have attracted a great deal of attention owing to their 1

unique electronic, optical, lubricating and catalytic properties [4-7]. In particular, their band gap can transfer from indirect to direct when their size down to monolayer, which provides promising applications in the next-generation nanoelectronic devices. Recent advances in synthesis techniques, such as chemical vapor deposition [8], liquid exfoliation [9], electron irradiation [10], offer fertile new grounds for fabricating high quality few layers or even a large area single layer samples, opening up avenues to explore these ultrathin LTMDs so as to improve their physical properties. As two-dimensional (2D) layered materials have a very high surface area, surface decorating can be an effective strategy to manipulate the electronic structure and band structure engineering at the atomic-scale. For example, it is reported that the group I (Li, Na, K) and group II metals (Mg, Ca) are the most effective adatoms to enhance the n-type mobile carrier density in monolayer MoS2 by shifting of the Fermi level to the conduction band [11]. The electronic band structure of 2D monolayer MoS2 has been significantly modified by different atom adsorption, leading to metallic, semimetallic or semiconducting behavior in direct bandgap monolayer MoS2 [12]. Particularly, local or long-range magnetic moments have been attained in single-layer MoS2 upon adsorption of specific transition-metal atoms, silicon and germanium atoms [13]. Mn and Fe absorption on the disulfur vacancies of MoS2 monolayer are of high chemical stabilities as well as much enhanced magnetic anisotropic energies, which indicates the single transition-metal adatoms absorbed on the defects of MoS2 monolayers are very promising candidates for fabricating the 2

atomic-scale magnetic bit

for data storage [14]. Additionally, combining

high-resolution transmission electron microscopy with first-principles calculations, the atomic structures of noble metal Re and Au adsorbed MoS2 monolayer have been identified and the dynamic observations of the atomic structure evolution reveal the interaction of the dopant atoms with the host single-layered MoS2 sheet. This successful doping of MoS2 with Re and Au suggests the possibility of nano-electronic devices made of doped single-layered MoS2 [15]. Molybdenum diselenide (MoSe2), a representative member of LTMDs, is similar to MoS2 structurally and electronically. Therefore, its electronic structure and the corresponding physical properties should also be tailored by single atom adsorption approach. Indeed, adsorption of nonmetal elements can induce local magnetic moments on the host of MoSe2 monolayer, and H adsorption results in a large spatial extension of spin density [16]. However, up to now a systematic investigation of the interaction between metal atoms and MoSe2 monolayer at the atomic scale is still limited. Besides, it is elucidated that adsorption of noble metals on MoS2 monolayer can remarkably tune its properties [15], so that the knowledge of how noble atoms interact with the host MoSe2 crystal lattices is highly important in the context of both fundamental science and future device technology. Here, first-principles calculations within density functional theory (DFT) are performed to investigate the electronic structures and magnetic properties of metal Pd, Pt, Cu, Ag, Au, and Zn adsorbed MoSe2 monolayer. It reveals that the preferred adsorption sites are not exactly the same, which change from the Mo atom top site to the hollow site of the hexagonal 3

ring formed by the Se and Mo atoms. Different interaction mechanisms are found between metal and substrate MoSe2 monolayer. More importantly, magnetic character has been introduced in Cu, Ag and Au systems, which expands the utilization of MoSe2 in nanoelectronics and spintronics. 2. Computational methods First-principles calculations were carried out on the basis of the spin density-functional theory (DFT) using the projector-augmented wave (PAW) method [17], as implemented in the Vienna ab initio Simulation Package (VASP) [18]. The electron exchange correlation functional was processed by using the generalized gradient approximation (GGA) within the Perdew­Burke­Ernzerhof (PBE) scheme [19]. The wave functions of the valence electrons were described by a plane wave basis set within a cut-off energy of 400 eV. The Brillouin zone integration was carried out by using Monkhorst­Pack scheme [20] with a 6×6×1 k-point gird. The atomic positions and lattice constants were fully optimized using the conjugate gradient method until the convergence criterion of total energy was less than 1.0×10-5 eV/atom and maximum force on each atom was smaller than 0.01 eV/Å. Structurally, monolayer MoSe2 has a symmetry of P6m2 (D3h point group, as shown in Fig. 1(a)) owing to the absence of inversion symmetry [21]. The Mo layer is sandwiched in between two Se layers, forming edge-sharing MoSe6 octahedra with a strong covalent bonding in interlayer. To ignore adatom-adatom mutual interaction, 4×4×1 supercell was constructed to simulate the pristine and metal adsorbed systems, where the distance between two adjacent adatoms is 13.27 Å. A large 4

vacuum region of 15 Å along the Z-axis was embedded to eliminate the unwanted interaction between two adjacent slabs. To search the most stable configuration, three possible types of adsorption sites were considered: (i) the adatom occupies the site above the Se atom (TSe); (ii) the adatom occupies the site above the Mo atom (TMo); (iii) the adatom occupies the hollow site above the center of the hexagonal ring (H). The configurations of the metal adsorption systems are shown in Fig. 1(b). 3. Results and discussions 3.1 Adsorption energy To evaluate the relative stabilities of different adsorption systems, the adsorption energy (Eads) is calculated according to the below schematic-equation: Eads= Emonolayer+X－(Emonolayer＋EX) where Emonolayer+X is the energy of optimized equilibrium configuration for the system of MoSe2 sheet with adatom, Emonolayer is the energy of the isolated MoSe2 monolayer, and EX is the energy of the isolated adatom. The adsorption energies for adatoms adsorbed MoSe2 monolayer on the different positions are summarized in Table 1. It is found that the adsorption energies are different for diverse adatoms on the three adsorption sites, and stable chemical adsorption has been formed between the adatoms Pd, Pt, Cu, Ag, Au and MoSe2 monolayer. The most favorable adsorption position changes from the Mo atom top site to the hollow site of the hexagonal ring formed by the Se and Mo atoms, i.e., TMo is the most favorable surface adsorption position for Pd, Pt, Cu atoms, while Ag and Au atoms prefer to adsorb on the H site. Interestingly, although the Cu, Ag and Au adatoms belong to the same group, their preferred 5

adsorption sites are not exactly the same. Moreover, the energy difference for Ag and Au adsorbed systems between the different adsorption sites is very small, i.e., 0.05 eV between H and TMo for Ag case and 0.07 eV between H and TSe for Au case, suggesting the adatom easily moves from one site to another if under appropriate external stimuli, such as temperature, pressure, electron beam. This is quite similar to the experimentally observed migration behavior of the Au adsorption on the host single-layered MoS2 sheet [15]. However, things are totally changed when Zn atom absorbed on MoSe2 monolayer. The adsorption energy is very small, suggesting weak physical interaction between them. In addition, it is obvious that the adsorption energy of Pd-adsorbed TMo configuration is the smallest in all systems, which indicates that introduction of Pd above the Mo atom on MoSe2 monolayer is more thermodynamically preferred. 3.2 Optimized geometric structure Hereafter, we mainly discuss the results of the most energetically favorable adsorbed configurations for all investigated systems, and their optimized structural parameters are summarized in Table 2. The optimum lateral lattice constant for 4×4 ×1 MoSe2 monolayer is 13.27 Å, namely 3.32 Å for each unit, consistent with the previous calculation results [16,22], validating the application of our calculation method. As to the adsorbed systems, the adsorption of metal atoms does not yield any significant deformation, and the whole adsorbed systems nearly maintain trigonal prism symmetry after structural relaxation. The dX-Se (dX-Mo) is the distance between the adatom and the nearest Se (Mo) at the most stable configuration. It is found that 6

the X-Se bond length is very close to the sum of the covalent radii of adatoms (Pd, Pt, Cu, Ag and Au) and the nearest Se atom expect for Zn absorbed configuration, which indicates the presence of covalent interaction between them. Whereas, the X-Mo bond length in the Ag, Au and Zn adsorbed configuration is much bigger than that in the Pd, Pt and Cu adsorbed system, suggesting the weak interaction between them, in line with their relatively smaller adsorption energy in Ag, Au and Zn adsorbed cases. 3.3 Electronic structure and magnetic properties To gain insights into the impact of metal adsorption on the electronic structures and magnetic properties, we first briefly show the band structures and density of states (DOS) of pristine MoSe2 monolayer (shown in Fig. 2). Both the valance band maximum (VBM) and conduction band minimum (CBM) are located at the K point in the Brillouin zone, which unambiguously reproduces its semiconductor nature with a direct band gap of 1.44 eV, in agreement with pervious experimental as well as theoretical results [16,23]. Further partial density of states (PDOS) analysis discloses that its electronic structure is dominated by the hybridization between Mo 4d and Se 4p orbitals owing to their PDOS almost distributed at the same energy range, which is responsible for the strong covalent interaction between them. Furthermore, the calculated DOS display exactly symmetrical characteristic for the majority and minority spins, indicating the nonmagnetic nature of the pristine MoSe2 monolayer. To shed light on the magnetic behavior of MoSe2 monolayer sheet via adsorption of metal atoms, both the non-spin-polarized and spin-polarized calculations were performed. For Pd, Pt and Zn absorbed cases, equivalent total energies are obtained 7

for the two states and no magnetic moments have been found in the spin-polarized calculations (shown in Table 1). However, the spin-polarized states are energetically favorable than the non-spin-polarized ones in Cu, Ag and Au adsorbed systems, and the adatoms possess obviously magnetic moments, regardless of the adsorption positions. This suggests Cu, Ag and Au adatoms can trigger magnetic behavior on the nonmagnetic MoSe2 surface, so that the introduction of metal impurities may lead to new functionalities of MoSe2. In addition, it is noteworthy that the magnetic moments are associated with the adsorption sites. The energetically more favorable adsorbed configuration, the larger total magnetic moment. As listed in Table 1, the total magnetic moment of Cu, Ag and Au adsorbed MoSe2 monolayer at the most stable configuration is 0.70, 0.60 and 0.67 μB, respectively, and the corresponding magnetic moment of Cu, Ag and Au adatom is 0.13, 0.15 and 0.24 μB, i.e., the contributions of the adatoms Cu, Ag and Au to the total magnetic moments are 18.6%, 25% and 35.8%, respectively. Such differences are attributed to the fact that a small amount of magnetic moment is distributed not only to the nearest Se atoms but also the nearest Mo atoms. Figure 3 shows the band structures of metal adsorbed MoSe2 monolayer along the high symmetric directions for the most stable adsorption configurations. It is clear that energy level splitting occurs between the spin-up and spin-down channels near the Fermi level in Cu, Ag and Au adsorbed MoSe2 monolayer (Fig. 3(c), (d), (e)), which confirms that magnetism is induced by the adsorbed metal atom. Whereas, the utterly symmetric bands of Pd, Pt and Zn adsorbed MoSe 2 monolayer (Fig. 3(a), (b), 8

(f)) reflect their nonmagnetic properties, consistent with the above magnetic analysis. Interestingly, all the adsorption configurations retain semiconducting characters, nonetheless the band gap has been slightly modulated. More importantly, they still present direct band gap owing to both VBM and CBM located at the high symmetric K point, just as that of the pristine MoSe2 monolayer, which is crucial for the utilization in the nanoelectronic devices. In Cu, Ag and Au adsorbed cases, the Fermi level shifts to the high energy, i.e., from the top of valence band to the bottom of conduction band in Cu and Ag adsorbed cases and to the middle of the band gap in Au adsorbed case, which is a typical characteristic of the n-type doping. Besides, some impurity states are found around the CBM owing to the metal adsorption, especially in Pt, Cu, Ag and Au adsorbed systems, making the electronic transfer from VBM to CBM easier. However, the change of electronic structure in the Zn adsorbed system can nearly neglect owing to weak physical interaction between adatom Zn and MoSe2 monolayer. Furthermore, the corresponding total DOS and PDOS for all systems at their most stable configurations are shown in Fig. 4. For the Cu, Ag and Au adsorption cases (Fig. 4(c), (d) and (e)), an asymmetry configuration is seen in the spin-up and spin-down channels, verifying magnetic properties are triggered by Cu, Ag and Au adatoms, while Pd, Pt and Zn adsorbed cases are nonmagnetic (Fig. 4(a), (b) and (f)). Especially, the Fermi level shifts to high energy in Cu, Ag and Au adsorbed cases due to the charge transfer between the adatoms and MoSe2 monolayer. To give direct evidence of the charge transfer between the adatoms and MoSe2 monolayer, we show the isosurface plots of spin density difference for all the 9

adsorbed systems in Fig. 5. Obviously, the charge densities are reduced at the center of adatoms except Zn, while additional charges appear between adatoms and their neighboring Se and Mo atoms, verifying charge transfer from the adatoms to the MoSe2 monolayer. Meanwhile, the charge density spatially expands from adatoms to its nearest Se atoms along the bonding direction, which indicates the presence of a clear covalent-bonding character between them. Large spatial extensions of spin density have been observed in Pd and Pt adsorbed MoSe2 monolayer, while that in the Cu, Ag and Au adsorbed systems are relatively small, illustrating the strong interaction in the former two systems. This further proves the above adsorption energy results and structural analysis. Moreover, the charge transfer will result in the reductions in unpaired electrons of the adatoms and as a consequence magnetic moments are triggered, just as that in the Cu, Ag and Au absorbed systems. Our calculations reveal that the band structure and magnetic property of the MoSe2 monolayer can be tuned by adsorbing different atoms, which opens up an additional route to facilitate the design of spintronic devices. 4. Conclusion We have conducted systematically first-principles calculations of the electronic structures and magnetic properties of metal absorbed MoSe2 monolayer. Framework structure of the adsorbed systems is similar to that of the pristine MoSe2 monolayer, indicating that atomic arrangement did not significantly change with the adatoms. All the adatoms are chemically adsorbed on the MoSe2 monolayer expect for Zn, and the most favorable adsorption position changes from the Mo atom top site to the hollow 10

site of the hexagonal ring formed by the Se and Mo atoms, i.e., TMo is the most favorable surface adsorption position for Pd, Pt, Cu atoms, while Ag and Au atoms prefer to adsorb on the H site. Interestingly, all the adsorption configurations still retain semiconducting characters, and magnetic character has been introduced in Cu, Ag and Au systems with the total magnetic moments of 0.70, 0.60 and 0.67 μB, respectively, which expands the utilization of MoSe2 in nanoelectronics and spintronics. This finding indicates that metal adsorption may serve as a useful way to tune electronic structure and magnetic property of two-dimensional material for many device applications.

Acknowledgments

This work was supported by the National Natural Science Foundation of China (grant nos. 21301075, 51372244), the Specialized Research Fund for Doctoral Program of Higher Education (grant no. 20133227120003), and Research Foundation for Advanced Talents of Jiangsu University (grant no. 12JDG096). *Corresponding authors. E-mail: [email protected] (H. L.), [email protected] (Y. T.)

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Figure captions

Fig. 1 Geometric structures of pristine and metal adsorbed 4×4×1 MoSe2 monolayer. (a) pristine MoSe2 monolayer, (b) metal atoms absorbed MoSe2 monolayer. TSe, TMo and H stand for the adatoms adsorbed above the Se atom, Mo atom and the center of the hexagonal ring of the MoSe2 monolayer, respectively. X stands for the metal adatom.

Fig. 2 Band structure along the major symmetric directions (left) and DOS (right) of pristine MoSe2 monolayer supercell. The Fermi level is set to zero with a horizontal red dashed line.

Fig. 3 Band structures for metal adsorbed MoSe2 monolayer along the high symmetric directions at the most stable adsorption sites. (a) Pd-adsorbed, (b) Pt-adsorbed, (c) Cu-adsorbed, (d) Ag-adsorbed, (e) Au-absorbed, (f) Zn-absorbed MoSe2 monolayer. The black lines represent the spin-up bands, while the blue lines represent the spin-down bands. The Fermi level is set to zero with a horizontal red dashed line.

Fig. 4 The total DOS and the corresponding PDOS of (a) Pd-adsorbed, (b) Pt-adsorbed, (c) Cu-adsorbed, (d) Ag-adsorbed, (e) Au-absorbed, (f) Zn-absorbed MoSe2 monolayer at the most stable adsorption sites. The Fermi level is set to zero with a vertical red dashed line. 14

Fig. 5 The top and side views of the spin density difference of (a) Pd-adsorbed, (b) Pt-adsorbed, (c) Cu-adsorbed, (d) Ag-adsorbed, (e) Au-absorbed, (f) Zn-absorbed MoSe2 monolayer at the most stable adsorption sites. Yellow and blue distributions represent the positive and negative values, respectively. The isosurface value is 0.0015 e/Å3.

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Table 1 Calculated adsorption energies (Eads) of metal atoms adsorbed MoSe2 monolayer on three high symmetry positions (T Se, TMo and H sites), the total magnetic moments (Mtotal), and the magnetic moments of the introduced adatoms (MX).

Configuration Pd-MoSe2

Pt-MoSe2 Cu-MoSe2

Ag-MoSe2 Au-MoSe2 Zn-MoSe2

site TSe TMo H TSe TMo H TSe TMo H TSe TMo H TSe TMo H TSe TMo H

Eads (eV) -1.43 -3.28 -1.72 -2.11 -3.19 -2.17 -0.91 -1.41 -1.30 -0.51 -0.66 -0.71 -0.67 -0.63 -0.74 -0.03 -0.05 -0.04

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Mtotal (μB) 0 0 0 0 0 0 0.56 0.70 0.71 0.48 0.58 0.60 0.62 0.65 0.67 0 0 0

MX (μB) 0 0 0 0 0 0 0.21 0.13 0.13 0.19 0.16 0.15 0.29 0.27 0.24 0 0 0

Table 2 The optimized structural parameters for pure and adsorbed MoSe2 monolayer supercells at the most stable adsorption sites. The dX-Se and dX-Mo stands for the distance between the adatom X and the nearest Se and Mo atoms, respectively. dX-Mo (Å) -

α (°)

β(°)

γ(°)

13.27 13.27

dX-Se (Å) -

90.00

90.00

120.00

TMo

13.31 13.31

2.45(3)

2.92(1)

89.97

90.03

119.99

Pt-MoSe2

TMo

13.32 13.32

2.42(3)

2.80(1)

89.99

90.01

120.00

Cu-MoSe2

TMo

13.29 13.29

2.38(3)

2.98(1)

89.98

90.02

120.00

Ag-MoSe2

H

13.28 13.28

2.87(3)

4.26(3)

89.96

90.04

120.00

Au-MoSe2

H

13.28 13.28

2.85(3)

4.23(3)

90.00

90.00

120.00

Zn-MoSe2

TMo

13.27 13.27

3.78(3)

4.93(1)

89.90

90.10

120.00

Configuration

site

a (Å)

MoSe2

-

Pd-MoSe2

b (Å)

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Fig. 1

Fig. 2

18

Fig. 3

19

Fig. 4

20

Fig. 5

21

Graphical abstract

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Highlights



Stable chemical adsorption has been formed between adatoms Pd, Pt, Cu, Ag, Au and MoSe2 monolayer.



Weak physical interaction is found between Zn and MoSe2 monolayer.



A pronounced magnetic character has been introduced in Cu, Ag and Au systems.



The framework structure and electronic property are slightly tuned by the adatoms.

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