CARBON 7 1 ( 2 0 1 4 ) 1 5 0 –1 5 8

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First-principles study on electronic and magnetic

properties of twisted graphene nanoribbon
and Möbius strips

Sheng-Ying Yue a, Qing-Bo Yan b, Zhen-Gang Zhu c,*

, Hui-Juan Cui a,
Qing-Rong Zheng a,*, Gang Su a,*
a
Theoretical Condensed Matter Physics and Computational Materials Physics Laboratory, School of Physics,
University of Chinese Academy of Science, Beijing 100049, China
b
College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China
c
School of Electronic, Electrical and Communication Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

A R T I C L E I N F O A B S T R A C T

Article history: The geometric, electronic, and magnetic properties of twisted zigzag-edged graphene
Received 30 August 2013 nanoribbons (ZGNRs) and novel graphene Möbius strips (GMS) are systematically investi-
Accepted 17 January 2014 gated with the first-principles calculations based on the density functional theory. All
Available online 24 January 2014 the structures of ZGNRs and GMS are optimized, and their structural stabilities are exam-
ined. The molecular energy levels and the spin polarized density of states of ZGNRs are also
calculated. It is found that the atomic bonding energies of the twisted ZGNRs decrease qua-
dratically with the increase of the twisted angle, and the gaps between the lowest unoccu-
pied molecular orbital and the highest occupied molecular orbital are varied with the
twisted angle. The spin densities of ZGNRs and GMS reveal that the ground states with
antiferromagnetic edges persist during the twisting, and the spin flip at some positions
of the zigzag edges of GMS can be observed.
Ó 2014 Elsevier Ltd. All rights reserved.

1. Introduction Especially, to make spintronic nanodevices the materials

are required to bear net spin and magnetism. This
Carbon nanostructures such as fullerene, nanotube, and stimulates extensive exploration of magnetism of carbon-
graphene have attracted great interest in basic research based materials. Apart from graphene, some carbon-based
and industrial applications. The techniques for growth and materials such as one-dimensional and two-dimensional
preparation of carbon nanostructures have gained a remark- (2D) organic polymers with high spin have been synthesized
able progress, and the scope of feasible applications of car- and explored currently [12]. However, it is still difficult to
bon nanostructures has been enlarged dramatically [1,2]. synthesize organic polymers with macroscopic magnetiza-
Since the first successful isolation of graphene, a single layer tion. In fact, these materials exhibit macroscopic diamagne-
of graphite, the graphene-based materials have attracted tism because of the interactions between molecules that
much attention because a new generation of nanodevices may cause the cancellation of magnetism [12]. Therefore,
[1–6] such as the graphene field-effect transistor [7,8], the in order to obtain the magnetic organic materials, it is
electromechanical resonators from graphene sheets [9], important to perform relevant researches on the nature of
spintronic nanodevices [10,11] and so on, are expected. graphene at the atomic level, including the electronic and

* Corresponding authors: Fax: +86 10 8825 6006.

E-mail addresses: zgzhu@ucas.ac.cn (Z.-G. Zhu), qrzheng@ucas.ac.cn (Q.-R. Zheng), gsu@ucas.ac.cn (G. Su).
0008-6223/$ - see front matter Ó 2014 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.carbon.2014.01.023
 CARBON 7 1 (2 0 1 4) 1 5 0–15 8 151

magnetic properties of carbon-based molecules and [37] known as PW91. We have used projector augmented wave
nanostructures. potentials [38,39] to describe the core (1s2 ) electrons, with the
It is well known that there are two types of edges in graph- 2s2 and 2p2 electrons of carbon considered as valence elec-
ene nanoribbons [3]: armchair and zigzag edges. Localized trons. The kinetic energy cutoff is 400 eV. Only CPoint is used
electronic edge states of the zigzag-edged graphene nanorib- for k- sampling. The force tolerance is set as 0.025 eV/Å. The
bons (ZGNRs) have been reported theoretically [13,14], and la- total spin densities are calculated by taking the difference be-
ter confirmed experimentally by scanning tunneling tween a and b spin densities. The supercells are created by
microscopy and spectroscopy [15,16]. Recently, a number of including a vacuum layer with thickness larger than 10 Å. In
works have predicted the ground state with antiferromag- order to show the edge magnetic properties more clearly,
netic (AFM) edges that lays a spin (up-spin) at one edge and the zigzag edges of the ZGNRs and GMS are not hydrogenated.
b spin (down-spin) at the opposite edge of a ZGNR [17–23].
The armchair-edged graphene nanoribbon does not have 3. Results and discussion
such a magnetic property. Although the AFM ground state
of ZGNR has not been confirmed experimentally, Enoki and 3.1. Structures and stability
coworkers have observed the localized spins in graphite nan-
odomains of activated carbon fibers, and attributed the First we shall generate ZGNRs with specific sizes from
underlying physics to the zigzag edge [24,25]. However, the graphene, and then twist them with different angles. For a
above-mentioned theoretical and experimental works did comparison, the structure of an untwisted ZGNR with the
not included the magnetic properties of the twisted ZGNRs. number of carbon atoms N ¼ 96, the length L ¼ 12 and the
If we connect the two ends of a twisted ZGNR, a graphene width W ¼ 4 is also included, as shown in Fig. 1(a). The
Möbius strip (GMS) could be formed. In 1982, the molecules twisted ZGNRs with twisted angles h ¼ 60 and 180 are pre-
with the shape of a half-twisted Möbius strip have been syn- sented in Fig. 1(b) and (c), respectively. To investigate the
thesized for the first time [26]. In 1998, Mauksch et al. [27] twisted ZGNRs systematically, various twisted structures of
have presented a computational reinterpretation of experi- ZGNRs are considered, ranging from L = 6 to 12, h = 0° to
mental data, showing that ðCHÞþ 9 could be a Möbius aromatic 180°, and N=48 to 96, while W is kept at 4. All of the geometric
cyclic annulene with 4n p-electrons. Also, the electronic prop- structures of twisted ZGNRs are relaxed, except for the atoms
erties of ring compounds were discussed theoretically in on the armchair edges (the two ends of ZGNRs), as simulating
connection with Möbius aromatic properties in some works the experimental situations the end-site atoms should be
[28–31]. Martı́n-Santamaria and Rzepa[28] presented an anal- fixed.
ysis of the main features of Möbius annulenes by considering
the p-molecular orbital correlation between the planar Hückel
configuration and the twisted C2 symmetric Möbius system.
10 11 12
The synthesis of a stable Möbius aromatic hydrocarbon has (a) 1 2 3 4 5 6 7 8 9
1
been obtained for the first time in 2003 by Ajami et al. [32]
who combined a normal aromatic structure (such as benzene, 2
3 W
with trigonal planar sp2-hybridized atoms) and a belt-like aro-
matic structure (such as the surface of a carbon nanotube, 4
with pyramidalized sp2 atoms), creating a Möbius compound 13 14 15 16 17 18 19 20 21 22 23 24
stabilized by an extended p-system. In 2008, Caetano et al. L
0
have investigated theoretically the structural stability, geo- θ= 0
metrical optimization and electronic properties of twisted
GNRs and GMS [33], but magnetic edge states have not been (b)
touched. Recently, Wang et al. have studied some specific
graphene Möbius structural models theoretically [34].
In this paper, the geometric, electronic and magnetic prop- θ= 60 0
erties of twisted ZGNRs and GMS are investigated systemati-
cally by the first principles calculations. For the ZGNRs, the 0
effects of size and twisted angle on the physical properties θ= 60
are studied. The main focus is targeted to reveal how the
electronic and magnetic properties of ZGNRs changing with (c)
different twisted curvatures. In addition, a series of GMS
derived from ZGNRs are generated, and their electronic and
magnetic properties are studied as well.
0
θ= 180
2. Computational details
Fig. 1 – The structures of untwisted and twisted ZGNRs,
All calculations have been performed using the Vienna Ab- where L and W are the length and width of ZGNRs, and h is
initio Simulation Package (VASP) [35,36] code, implementing the twisted angle as indicated in the inset of (b). (a) h ¼ 0 ; (b)
the spin-polarized density functional theory (DFT) and the h ¼ 60 ; (c) h ¼ 180 . (A colour version of this figure can be
generalized gradient approximation of Perdew and Wang viewed online.)
152 CARBON 7 1 ( 2 0 1 4 ) 1 5 0 –1 5 8

If the two armchair ends of the twisted ZGNRs are con- deformations occur during this process. It is interesting that
nected together through carbon–carbon (C–C) bonds, the a new metastable structure with Nt ¼ 0 is unveiled in the
GMS structures are thus generated, as shown in Fig. 2(a). simulated annealing process (the second one of Fig. 2(b)).
Obviously, different twisted angles of the generating process When the final structures of the twisted ZGNRs and GMS
give rise to different geometric topologies, which could be ex- are obtained, the DFT optimizations are performed and the
pressed by the half twisted times Nt , and the twisted angle relative energies of the structures are obtained. To compare
h ¼ Nt  180 . If Nt ¼ 0, a short carbon nanotube could be the relative energies of structures with different number of
formed, as indicated in Fig. 2(b). If Nt ¼ 1, the conventional carbon atoms, the atomic bonding energy Eb is a proper quan-
Möbius strip is obtained. Furthermore, Fig. 2(b) also presents tity, which is defined as: Eb ¼ ENtot  Ec , where Etot is the total
other GMS with higher twisted times Nt ¼ 2; 3, and 4. The free energy of the system, N is the total number of atoms, and
structures of Nt ¼ 0 to 4; L ¼ 30 to 40; W ¼ 4; N ¼ 240 to 320 Ec is the energy of an isolated carbon atom. The structure is
are also considered (here only the structure with N ¼ 240 is more stable for a lower Eb (or a larger Eb ).
shown in Fig. 2(b)). To check the geometric stability, the The atomic bonding energies of the untwisted and twisted
molecular dynamics (MD) calculation has been performed to ZGNRs are given in Table 1. Fig. 3(a) shows the twisted angle
simulate the annealing process from 1000 to 300 K. It turns dependence of Eb for the twisted ZGNRs with the length
out that all generated structures are stable, and only small from L = 6 to 12. It is obvious that Eb of the twisted ZGNRs

(a)

(b)

Fig. 2 – (a) An illustration how to generate Nt ¼ 2 GMS by using a twisted ZGNR (L = 30, W = 4, and N = 240). (b) Several GMS
generated with twisted ZGNRs (L = 30, W = 4, and N = 240), where Nt is the half twisted times. When Nt ¼ 0, there are two
stable GMS structures. All structures presented here are optimized with the MD simulated annealing and the DFT method.
 CARBON 7 1 (2 0 1 4) 1 5 0–15 8 153

Table 1 – The atomic bonding energy Eb (eV) of untwisted and twisted ZGNRs with the number of atoms N = 48–96.
Twisted angle N = 48 N = 56 N = 64 N = 72 N = 80 N = 88 N = 96

h¼0 6.882 6.954 6.992 7.021 7.044 7.062 7.077
h ¼ 30 6.880 6.953 6.989 7.020 7.043 7.062 7.076
h ¼ 60 6.866 6.948 6.986 7.018 7.040 7.059 7.074
h ¼ 90 6.831 6.937 6.977 7.008 7.032 7.052 7.071
h ¼ 120 6.754 6.923 6.966 6.999 7.025 7.045 7.063
h ¼ 150 6.624 6.908 6.953 6.985 7.015 7.037 7.056
h ¼ 180 6.450 6.727 6.926 6.968 7.001 7.024 7.045

(a) are increased in a quadratic way with increasing the twisted

angle h. After the geometric optimization of the twisted
ZGNRs, the bond angle and the bond length are both changed
for different angles. Hence, it appears that the strain-depen-
dence of potential energy is related to both bending modulus
and Young’s modulus. In the study of Lu et al. [40], the strain
energy per atom of graphene with bending curvature can be
expressed as W ¼ 12 Dj2 , where D is the bending modulus
and j is the curvature. Similarly, the elastic potential energy
per unit volume of graphene could also be expressed as
U ¼ 12 E2 , where E is Young’s modulus of graphene that was
studied by Jiang et al. [41] in 2009 and measured by Lee
et al. in 2012 with Raman spectroscopy [42]. As shown in
Fig. 3(a), one may look at that the changes of Eb of the
twisted ZGNRs with the twisted angle h are also in a quadratic
(b) way. Hence, we could assume that Eb can be expressed as
Eb ¼ 12 Th2 , where T describes the stress per atom with unit
in eV. A higher T means a stronger stress. Using the polyno-
mial fitting method based on the data in Table 1, we can ob-
tain T of different ZGNRs, as listed in Table 3. We may see
that a smaller ZGNRs has a higher T. This means that when
the twisted angle is the same, the atoms of smaller ZGNRs
will feel greater stress and thus release a larger strain. This
may be the reason that a higher bonding energy for a smaller
twisted ZGNR shown in Table 1 can be observed. It is clear
that a longer ZGNR is more stable, and the twisting tends to
reduce the stability of ZGNRs.
The atomic bonding energy Eb of GMS with half twisted
times from Nt ¼ 0 to 4 and the number of atoms from
N ¼ 240 to 360 are listed in Table 2. Generally, Eb with the
Fig. 3 – (a) The negative atomic bonding energy Eb of the same Nt are decreasing with the increase of the number of
twisted ZGNRs versus the twisted angle h for different atoms N, and Eb with larger Nt grows steeper than those with
length L. (b) The negative atomic bonding energy Eb of the smaller Nt [Fig. 3(b)], which could be attributed to the fact that
GMS versus the number of carbon atoms N for different a larger twisted times brings a higher strain to a strip. For
twisted times Nt , where the width is fixed to W ¼ 4. (A Nt ¼ 0, the bonding energies Eb are much larger than those
colour version of this figure can be viewed online.) in the cases of Nt > 0.

Table 2 – The atomic bonding energy Eb (eV) of GMS with the number of atoms N = 240–320 and the twisted times Nt ¼ 0–4.
N Nt ¼ 0 ðIÞ Nt ¼ 0 ðIIÞ Nt ¼ 1 Nt ¼ 2 Nt ¼ 3 Nt ¼ 4

240 7.973 7.972 7.800 7.797 7.782 7.752

256 7.973 7.952 7.792 7.798 7.789 7.766
272 7.973 7.973 7.804 7.799 7.793 7.774
288 7.974 7.963 7.804 7.803 7.797 7.782
304 7.974 7.963 7.807 7.798 7.800 7.788
320 7.975 7.974 7.808 7.801 7.803 7.793
154 CARBON 7 1 ( 2 0 1 4 ) 1 5 0 –1 5 8

Table 3 – The parameter T (eV) of ZGNRs with different number of atoms N.

N 48 56 64 72 80 88 96

T 0.06613 0.04149 0.00745 0.00588 0.00403 0.00411 0.00381

It can be seen from Fig. 3(b) that the new stable structure As a result, the pz orbitals at the ribbon edge are no longer
(as labeled in Fig. 2 with Nt ¼ 0 (II)) and the nanotube (as in orthogonal to the r orbitals, and are not exactly parallel to
Fig. 2 with Nt ¼ 0 (I)) are highly competitive in energy Eb, each other among themselves with increasing the twisted
and vary with N in a similar trend. For GMS with Nt > 0, a lar- angle. When this happens, the magnitudes of the two small
ger Nt leads to a less stable structure (with a larger Eb ). For a peaks just above and just below the Fermi level are increased
fixed Nt , we observe that the structures with smaller N are and the peaks are sharpened.
more unstable because a smaller GMS bears a larger strain
from the twisting process. This is also manifested in Eb that
tends to a common value for a bigger GMS since the strain ef- (a)
fect becomes smaller in the larger system. We should point
out that all the structures studied here are optimized by the
first-principles calculations.

3.2. Electronic structures of twisted ZGNRs

The electronic structures of twisted ZGNRs are also investi-

gated. The molecular energy levels and density of states
(DOS) with different twisted angle h are shown in Fig. 4. It
is known that the two edges of ZGNR, one on A-sublattice
and the other on B-sublattice, have different potentials due
to the AFM coupling, which opens a finite gap with spin
polarization [11]. The energy gap, which is defined by an en-
ergy difference between the lowest unoccupied molecular
orbital (LUMO) and the highest occupied molecular orbital
(HOMO) of the ZGNRs, is obtained for various structures.
(b)
The smallest gap 0.074 eV occurs at the twisted angle
h ¼ 30 , while the largest energy gap is 0.397 eV, which ap-
pears at the twisted angle h ¼ 120 [Fig. 4(a)]. Generally, the
energy gap becomes larger and then decreases as the twisted
angle grows. The results of the LUMO–HOMO gap reveal that
the twisted ZGNRs could be tunable organic semiconductor
materials. We note that in 2011, Sadrzadeh et al. [43] have
studied the electronic properties of twisted armchair edged
graphene nanoribbons (AGNRs), where the band gap as a
function of the twisted angle was discussed for the H-termi-
nated AGNRs. However, the AGNR structures are different
from those of the ZGNRs, and the spin polarized calculations
should be invoked to take into account the AFM edge states of
the ZGNRs [10].
In Fig. 4(b), the DOS of electrons with a spin (red dashed
lines) and b spin (green solid lines) are shown for the twisted
angle h ¼ 0 ; 60 ; 120 and 180 . It is seen that the magnitudes
of DOS for up and down spins coincide with each other for
different twisted angles, implying that the ground states of
the ZGNRs are AFM or nonmagnetic. The DOS profile reveals
that the small peaks in the a subbands just above and below
the Fermi level move away from the Fermi level upon apply- Fig. 4 – (a) The molecular energy levels of the ZGNRs versus
ing the twist. This could be caused by the charge transfer the twisted angle h, where the LUMO–HOMO gaps are
from the local edge to the middle of the graphene nanoribbon. indicated. (b) The spin polarized DOS of the ZGNRs for
The reason is that the strain induced by the twist changes the different twisted angle h, where the red dot lines represent
bond length and the bond angles. In accordance with this the DOS of electrons with a spin and the green solid lines for
change, the charge may be transferred from one carbon atom the electrons with b spin. The Fermi level is set to zero, and
to others since the originally orthogonal orbitals are hardly to L = 12, W = 4 and N = 96. (A colour version of this figure can
maintain themselves in the same orientation after relaxation. be viewed online.)
 CARBON 7 1 (2 0 1 4) 1 5 0–15 8 155

θ = 00

θ = 30 0 θ = 60
0

0 0
θ = 90 θ =120

0
θ =150
0
θ = 180
Fig. 5 – Spin densities of the twisted ZGNRs with L = 12, W = 4, and N = 96 for different twisted angles, where the green
isosurface represents the a spin density, and the red isosurface represents the b spin density. The isovalue of isosurface is
0.0056. (A colour version of this figure can be viewed online.)

3.3. Edge magnetism of twisted ZGNRs and GMS AFM edges that are manifested by the opposite net spin
densities at zigzag edges during twisting, whenever the
The charge transfer may lead to the redistribution of not only twisted angle is small or large, where the spin density is ob-
charge but also the local magnetic moments in real space. tained by integrating spd-projected DOS up to the Fermi level.
The latter could manifest itself in a variation of the original This result is also well consistent with the spin-polarized DOS
AFM edge magnetism of the ZGNRs. In this subsection, the ef- in Fig. 4(b), showing that the twist does not have a qualitative
fect of twisting on the spin density distribution (q"  q# ) of the effect on the AFM ground states of the ZGNRs.
twisted ZGNRs and GMS are explored, where q" and q# are the There are also a few previous studies on spin polarized
charge densities of electrons with a and b spin, respectively. properties [20] and structural stability [33] of the GMS. How-
The results are presented in Figs. 5 and 6. It is known that ever, the spin-resolved edge states of the GMS with higher
each carbon atom at zigzag edge of graphene possesses four twisted times have not yet been reported. Therefore, it is
valence electrons, two of which participate in the r covalent interesting to pay attention to a nontrivial question whether
bonds forming the honeycomb structure of graphene, while the twisting can affect the magnetic property of a zigzag-
the other two are unpassivated electrons, one of which forms edged GMS, particularly the GMS with odd twisted times
the dangling sp2 bond, and another is in the dangling pz (odd Nt ) that has only a single edge in a topological sense.
orbital. Without twisting, this pz orbital is orthogonal to the The calculated results are given in Fig. 6. When Nt is odd,
surface orbitals and localized at the edges. The dangling sp2 the GMS also remains in the AFM ground states, but the spin
bond is probably spin-polarized slightly [44]. flipping can happen at some contrapositions of the two
The magnetic properties of the ZGNRs were discussed pre- nanoribbon edges, as indicated by the blue-dashed circles in
viously [22,23]. Following Lieb’s theorem [45], the spins on the Fig. 6. Such a flip could be understood by the geometric rule
same sublattice (A or B) are FM coupled and on the different proposed in Ref. [22] which states that the two zigzag edges
sublattices (A versus B) are AFM coupled. This generic geo- may be AFM-coupled when the angle between their normal
metric rule still applies to our case. Fig. 5 demonstrates the directions is 180 .
spin densities of the ZGNRs with different twisted angles. When Nt is even, the GMS still retains the AFM ground
We can see that the ZGNRs always take the ground states with states, and the spin flips can also appear at some positions.
156 CARBON 7 1 ( 2 0 1 4 ) 1 5 0 –1 5 8

N t=0 N t=0

N t=1 N t=2

N t=3 N t=4

Fig. 6 – Spin densities of the zigzag-edged graphene Möbius-like nano-strips (with L = 30, W = 4, N = 240) for different
geometric topologies, where the green isosurface represents the a spin density, and the red isosurface represents the b spin
density. The isovalue of isosurface is 0.0056. (A colour version of this figure can be viewed online.)

However, the spin flip in this case appears not at the contra- twisting on nanoribbons. Our study shows that the twisted
positions of the edges but at those positions where two ZGNRs could be taken as tunable organic semiconductor
carbon atoms are the closest to each other in real space after materials. The energy of the GMS was uncovered to increase
relaxation, which are marked by the blue-long-dashed circles with the twisted times Nt , and the effect induced by the twist-
for Nt ¼ 0; 2 in Fig. 6. This phenomenon may be caused by the ing process is degraded with increasing the number of atoms.
electronic interactions of carbon atoms. By using the simulating annealing process in MD and the DFT
optimization, we also uncovered a new stable structure of the
4. Summary GMS with Nt ¼ 0 (type II). The spin-polarized DFT calculations
show that the AFM ground states of the twisted ZGNRs and
In this work we have investigated the geometric, electronic GMS are persistent during the twisting. In addition, the spin
and magnetic properties of the ZGNRs as well as the GMS states on the zigzag edges of GMS were observed to flip at
built on ZGNRs by using the first-principles DFT calculations. some positions. For the GMS with odd Nt , the spin flip occurs
The stability of these novel structures was examined. The at the contrapositions of the two zigzag edges. For the strips
molecular energy levels and the spin polarized DOS were ob- with Nt ¼ 0 and 2, the spin flip takes place at those where
tained. It is found that the atomic bonding energy of the two carbon atoms are placed at the closest positions after a
twisted ZGNRs decreases quadratically with increasing the structural optimization. Our present study might be helpful
twisted angle. The LUMO–HOMO energy gap was calculated, to understand further the properties of graphene at atomic
and found to vary with the twisted angle as well. A charge scales, and is useful for future designs of spintronic
transfer was observed, which may be due to the applied nanodevices.
 CARBON 7 1 (2 0 1 4) 1 5 0–15 8 157

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