APPLIED PHYSICS LETTERS 97, 123103 2010

Theoretical investigation of Mbius strips formed from graphene

Xianlong Wang, Xiaohong Zheng, Meiyan Ni, Liangjian Zou, and Zhi Zenga
Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, Peoples Republic of China

Received 1 June 2010; accepted 26 August 2010; published online 23 September 2010 First-principle calculations are performed on the formation of graphene Mbius strips and their shape evolution as a function of the strip width. Results show that Mbius strips formed from graphene nanoribbons with xed length and different widths are stable. With the increase in the width, one planar triangular region appears, and nally, the strip evolves into three equilateral triangles stacked together. Physical properties such as deformation energy density, strain effects, and edge magnetism are discussed. As a result from the special topology, unlike zigzag-edged graphene nanoribbons, Mbius strips are ferromagnets with nonzero total magnetic moments observed at the edge. 2010 American Institute of Physics. doi:10.1063/1.3489982 The structural and physical properties of Mbius strips obtained by joining two ends of a strip with a single halftwist have been widely investigated experimentally13 and theoretically.48 Topologically, the most prominent feature of a Mbius strip is that it has only one edge and one surface. As for this special topology, it has many important applications. Good examples are sanding belts and recording tapes. Sanding belt or drive belt made from a Mbius strip is worn evenly on both sides and thus their lifetime is doubled in comparison to the ordinary belt. A Mbius recording tape is recorded on both sides, so more information can be stored. So far, researchers have been trying to synthesize different kinds of microscopic Mbius strip, such as Mbius aromaticity. The possibility of forming Mbius aromaticity was rst predicted in 1964,7 and it was realized experimentally recently.2,3 At a much larger scale, another kind of Mbius strips were synthesized by NbSe2 crystals under certain growth conditions.1 In the meantime, the physical properties of Mbius strips were studied theoretically. Using a simple model of Mbius ladder, Zhao et al.5 predicted some observable effects, such as the topology-induced optical spectral splitting and higher energy band suppression of the transmission. The work by Ballon and Voss6 shows that Mbius topology may play an import role in the design of novel materials and electronic instrumentation. Recently, graphene has received extensive attention due to its remarkable structural and electronic properties.911 It is a single layer of graphite and has planar structure like paper. One interesting point about graphene is that it has similar mechanical properties as paper or plastic, and the bulk modulus along the plane of graphene is huge. Moreover, this material can be easily curved. Actually, graphene can be wrapped into carbon nanotubes which possess excellent properties. These features qualify graphene as a promising material to build Mbius strips. Therefore, in this work, we use a set of zigzag-edged graphene nanoribbons ZGNRs with the same length and different width to construct Mbius strips by rst-principles simulations. We are interested in ZGNRs since these kinds of nanoribbons have more interesting properties than the ones with armchair edges. For exa

ample, ZGNRs have localized edge states and edge magnetism,12,13 which do not appear in the armchair edged graphene nanoribbons. Furthermore, Mbius strips formed by ZGNRs behaves as a topological insulator14 and possess topology-induced thermal15 and magnetic properties.16 However, the structural properties of graphene Mbius strips have not been fully addressed yet. Thus, in this work, we report our systematic investigation about the shape evolution process of ZGNR-based Mbius strips with the increase of the ribbon width, as well as their physical properties such as deformation energy density DED , strain effects, and edge magnetism. The width and length of the ZNGRs used to build Mbius strips are characterized by the number of zigzag chains across the nanoribbon Nz and the number of unit cells along the nanoribbons Na . In our calculations, the length Na of ZGNRs is xed to 30, while the width Nz is gradually increased from 2 to 14. The calculations of geometrical and electronic properties are performed with an ab initio code SIESTA which employs norm-conserving pseudopotentials and linear combinations of atomic orbitals as basis sets.17,18 After full relaxation, for all the cases concerned, the structures with Mbius geometry are obtained as shown in Fig. 1. The nal structures of Mbius strips formed by graphene are stable and their shapes are highly dependent on the ratio between the width and the length. It is interesting to

Author to whom correspondence should be addressed. Electronic mail: zzeng@theory.issp.ac.cn. FAX: 86-551-5591434.

FIG. 1. Color online The structures of the Mbius strips formed by graphene nanoribbons. The Arabic numerals in the square brackets indicate the width Nz . 2010 American Institute of Physics

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FIG. 2. Color online The inverse radius of the sphere determined by a carbon atom and its three nearest neighbors for the Nz = 8 a . The bond lengths in unit of angstrom of three typical areas are shown in b . Sign change of curvature at the vertex of planar triangle is shown c .

nd that a planar triangular region displayed in red appears and enlarges as the width increases. When the ratio between the width and the length is increased to w / L = 3 / 6.429, one double-layered triangle is formed in the strip with a curly taper located at the top see Fig. 1 e . As the ratio exceeds the critical value w / L = 3 / 6 Ref. 8 and reaches w / L = 3 / 5.294, as shown in Fig. 1 f , the Mbius strip evolves into a triple-layered triangle. All the calculated geometrical features agree with the Mbius strips mathematical models shown in Fig. 2 of Starostin and Van der Heijdens paper.8 Thus, the mathematical models of the Mbius strips are realized physically with a real material and a demonstration of the correctness of Starostin and Van der Heijdens equations is provided. Starostin and Van der Heijden also pointed out that the shape of the Mbius strip is determined by the ratio between the length and the width of the sheet material it is made of. Based on this, it can be predicted that the structural features of larger graphene Mbius strips will be the same so long as the ratio between the width and the length is kept xed. In order to clearly quantify the agreement between the optimized structures and mathematical model, the curvature at each carbon position of the strip surface is dened by the inverse radius of the sphere determined by each carbon atom and its three nearest neighbors. Specically, the curvature distribution for Nz = 8 is displayed in Fig. 2 a . Compared with the results of Starostin and Van der Heijden8 see Fig. 1 of their paper , a good agreement is achieved. For example, the appearance of a planar triangular region is conrmed by the black region in Fig. 2 a . Further, we investigate the strain effects of Mbius strips. Since the strain effects are well reected in the changes of the bond lengths and they are more prominent at the edge than inside the ribbon, we show the bond lengths of three typical edge areas in Fig. 2 b . It is found that, at the A area where the curvature is the largest, the bond length is 1.417 , which is decreased from that 1.421 of the 30,0 carbon nanotube, thus compression happens here. At the B area where the curvature sign changes shown in Fig. 2 c , the bond length is elongated, with the largest bond length 1.439 obtained at the vertex of the triangle, thus a large strain is introduced here. This is similar to what has been shown by Starostin and Van der Heijden: when we try to tear a sheet of paper, one planar triangle is created in the middle of the paper, and the crack starts at the vertex of the triangle.8 The edge bond lengths in other parts are between 1.417 and 1.439 , as shown in the B area of Fig. 2 b . To gain a further insight into the formation of ZGNRbased Mbius structures, the DED, which comes from bending, is calculated by the following formula: EMF = E M 60 EH 60 Nz EC , 1

EDED =

E MF EGF , 60 Nz

where E M is the energy of the Mbius strip, EH and EC represent the energy of H and C atoms, respectively. EMF and EGF is the formation energy of Mbius and graphene strips with the width of Nz. The DED increases rapidly with Nz at the beginning and slows down with Nz increasing see Fig. 3 . When Nz 8, the EDED gradually saturates to a constant value. These results indicate that, as the width increases, it becomes more and more difcult to synthesize the Mbius structures by graphene nanoribbons. It is well known that localized edge states and edge magnetism are formed at the edges of ZGNRs. In ZGNRs, although the local magnetic moments in each edge are ferromagnetically arranged, there are two possible magnetic congurations between the two edges, namely, ferromagnetic FM and antiferromagnetic AFM . The properties of ZGNRs depend strongly on their magnetic states. For example, the FM ZGNRs are metals while the AFM ZGNRs are semiconductors. Overall, the AFM state is the energetically more stable one, with total energy smaller than that of the FM state 2 meV smaller per edge atom for the ZGNR with Nz = 8 . Thus the total magnetic moment TMM of ZGNRs is zero.10 We want to emphasize that, for ZGNRs, comparing with the FM interaction inside one edge, the AFM interaction between two edges is rather weak.13 In Mbius strips, all the edge carbon atoms are ferromagnetically coupled and a nonzero TMM is observed. The same phenomenon has been reported by Jiang and Dai.16 It is easy to understand, as the two edges meet each other in Mbius structures, and actually, we just have only one edge. Thus all edge carbon atoms will be ferromagnetically arranged. In the inset of Fig. 3, the TMM of Mbius strips as a function of the ribbon width are shown. For Nz = 2, the TMM

FIG. 3. Color online The DED as a function of the width Nz of the Mbius strips formed by graphene nanoribbons. The TMMs of Mbius strips are shown in the inset.

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FIG. 4. Color online The AMMs of edge carbons are shown in a . The spin polarized density of states and spin density for Mbius molecule formed by graphene nanoribbons with Nz = 8 are shown in b and c , respectively.

is almost equal to zero because the edge magnetism directly arises from the localized edge states while no edge states are formed when the width of the ribbon is as small as 2. With the increase in the ribbon width, edge states are developed and the density of states becomes spin polarized see Fig. 4 b . With the increase in the ribbon width, the magnetic moment increases monotonously until it reaches the maximum 16 B when Nz = 8. The spin density shown in Fig. 4 c indicates that the interaction between the edge carbon atoms is FM but they are antiferromagnetically coupled with their nearest neighbors. Since the opposite magnetic moment at the nearest neighbors is very small, the TMM is nonzero. Furthermore, the atomic magnetic moment AMM of each edge carbon atom is shown in Fig. 4 a . The AMM of Nz = 4, 6, and 8 are approximately 0.25 B, 0.27 B, and 0.30 B, respectively. This means that the AMM in the graphene Mbius strips increases with the ribbon width and the increase stops when a critical width is reached, which is very similar to the ZGNRs where the same trend is observed. Note that the TMM is greatly affected by the curvature and strain effects. It is found that, at the edge sites where the curvature and strain effects are the most prominent, the AMM is greatly reduced from other edge sites see Fig. 4 a . This results in the decrease in the TMM after Nz 10 since the strain and curvature effects become more and more important. This does not happen in ZGNRs because of the absence of the curvature and strain effects. In summary, the structures of ZGNR-based Mbius strips with xed length and different widths are investigated theoretically. We nd that, the Mbius strips constructed with ZGNRs are quite stable. With the increase in the ribbon width, a planar triangular region appears, and nally, the strip evolves into three equilateral triangles stacked together. As a result from the special topology, the electronic properties in the Mbius strips are quite different from those of ZGNRs. For example, FM ground state with nite TMM is observed in the Mbius strips while AFM state is the ground state in ZGNRs and the TMM is zero. Furthermore, the strain effects in Mbius strips are very important which results in

the decrease in the TMM after some critical width while it never decreases with the width in the ZGNRs. Such magnetic properties that are different from the ZGNRs may make the Mbius strips graphene building blocks in spintronic devices. This work was supported by the National Science Foundation of China under Grant Nos. 10774148 and 10904148, the Special Funds for Major State Basic Research Project of China 973 under Grant No. 2007CB925004, 863 Project, Knowledge Innovation Program of Chinese Academy of Sciences under Grant No. KJCX2YW-W07, and Director Grants of CASHIPS. Part of the calculations was performed in Center for Computational Science of CASHIPS and the Shanghai Supercomputer Center.
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