ARTICLES

PUBLISHED ONLINE: 9 MARCH 2014 | DOI: 10.1038/NMAT3888

Electro-optical switching of graphene oxide liquid

crystals with an extremely large Kerr coefficient
Tian-Zi Shen†, Seung-Ho Hong† and Jang-Kun Song*

The sensitive response of the nematic graphene oxide (GO) phase to external stimuli makes this phase attractive for extending
the applicability of GO and reduced GO to solution processes and electro-optic devices. However, contrary to expectations,
the alignment of nematic GO has been difficult to control through the application of electric fields or surface treatments. Here,
we show that when interflake interactions are sufficiently weak, both the degree of microscopic ordering and the direction of
macroscopic alignment of GO liquid crystals (LCs) can be readily controlled by applying low electric fields. We also show that
the large polarizability anisotropy of GO and Onsager excluded-volume effect cooperatively give rise to Kerr coefficients that
are about three orders of magnitude larger than the maximum value obtained so far in molecular LCs. The extremely large
Kerr coefficient allowed us to fabricate electro-optic devices with macroscopic electrodes, as well as well-aligned, defect-free
GO over wide areas.

G
O-LCs with controllable alignments may provide a new
way to make use of the many advantages of carbon-based
materials1–5 . In particular, chemical-reduction techniques
can combine the attractive properties of graphene—which has
outstanding electrical, thermal and mechanical properties—
with the merits of self-assembled GO-LCs (refs 6,7). The wide
applicability and commercial success of molecular LCs are largely
attributed to the easy, fine and dynamic control of their alignment
by application of electric fields, which is regarded as an intrinsic
advantage of the fluidic liquid nature of LCs (refs 8,9). However, it
was reported that the application of electric fields does not induce
GO-LC switching, but instead causes electrophoretic drift and
reduction of the GO, along with electrolysis of water10 . Although
a couple of methods to align GO-LCs using the capillary effect
and magnetic fields have been suggested10,11 , these methods have
clear limitations that prevent the fine and arbitrary control of
GO alignment. The insensitivity to electric fields seems to arise
from viscous rheology similar to polymeric liquid crystals, and is
considered as an intrinsic limitation1,10 . Meanwhile, the alignment
and electrical switching of carbon nanotubes and graphene flakes
were demonstrated by using dispersions in a calamitic nematic LC
host and exploiting its dynamics12–14 .
Onsager’s theory, based on excluded volume, predicts the
transition from an isotropic to a nematic phase passing through
a biphase (coexistence of isotropic and nematic phases) as the
concentration increases in colloidal dispersions of rod-like carbon
nanotubes or plate-like GOs. The location of this transition will
depend sensitively on the aspect ratio (length/diameter for rods or
diameter/thickness for plates)15,16 . Whereas a typical aspect ratio
for carbon nanotube LCs is usually less than 50 because of their
rather thick diameters and easy entanglement of excessively long
carbon nanotubes1,17 , the aspect ratio of GO-LCs with monoatomic
thickness can be up to the order of 10,000 (ref. 11). As a result, the
biphase is theoretically predicted to appear at an order of 1–10 vol%
for carbon nanotube LCs (ref. 17) and around 0.01 to 0.1 vol% for
GO-LCs (refs 10,18). The viscosities of these biphases were reported
to be about 500 Pa s for carbon nanotube LCs (ref. 19) and less than
1 Pa s for GO-LCs (ref. 18). Thus, GO is a better material than carbon
nanotubes to form a nematic phase with a large anisotropy and
good fluidity.
LC phase sequence of GO dispersions
By analysing the aqueous GO flakes used in our experiments
(Methods and Supplementary Fig. 1), we verified that they were
mostly single-layered and had a mean size of 3.2 µm (refs 2,7,18,
20,21), which means that the average aspect ratio was about 3,200.
Using Onsager’s theory (Supplementary Fig. 2), we determined the
theoretical concentrations for phase transitions from the isotropic
phase to the biphase (CIB T = 0.04 vol%), and from the biphase to the
nematic phase (CBN T = 0.17 vol%). By observing the macroscopic
birefringence pattern (Supplementary Fig. 3), we also determined
that the experimental values of CIB E and CBN E were approximately
0.08 and 0.2 vol%, respectively, which were only slightly larger than
the theoretical values. This difference may be due to the excessive
flexibility of the GO flakes22 . By measuring the volume fraction of
the high-concentration nematic phase relative to that of the low-
concentration isotropic phase in a bottle stored for several weeks,
the heterogeneous volume-fraction diagram was also determined
(Fig. 1b)10 . It was found that the heterogeneous biphase (BPH )
appeared in a wider concentration range.
Flow- and field-induced birefringence
Interestingly, flow-induced optical birefringence was observed
in the GO dispersions below CIB E , indicating the transition
from the isotropic to an ordered state. As shown in the inset
image in Fig. 1b and Supplementary Fig. 4, the aqueous GO
dispersions in a bottle and in a Petri dish looked isotropic initially,
but bright birefringence patterns were induced under crossed
polarizers after the bottle was shaken or a magnet bar was rotated
in the Petri dish. A clearer visualization of the flow-induced
birefringence is provided in Supplementary Video 1. The flow-
induced birefringence disappeared after a while when the dispersion
stopped flowing, and the persistence time of the flow-induced
birefringence in a Petri dish test was recorded as a function of
concentration. The persistence time increased sharply from the
concentration of 0.04 vol%, indicating the existence of nematic

School of Information and Communication Engineering, Sungkyunkwan University, Jangan-Gu, Suwon, Gyeonggi-do 440-746, Korea. †These authors
contributed equally to this work. *e-mail: jk.song@skku.edu

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NATURE MATERIALS DOI: 10.1038/NMAT3888 ARTICLES
a
Isotropic BPU Nematic
Uniform
phase
sequence

100 µm

Macroscopic CIB_E CBN_E

transition concent 0.08 0.2

Theoretical CIB_T CBN_T

transition concent 0.04 0.17

b
8 100

80
FIB persistence time (min)

N volume fraction (%)

6

60
BPH N
4
40

2
20

0 0
0.0125 0.0250 0.0500 0.1000 0.2000 0.4000 0.8000
Concentration (vol%)

Figure 1 | Phase sequence, nematic volume-fraction diagram and flow-induced birefringence. a, The uniform sequence of phases was determined
experimentally (corresponding phase transition concentrations: CIB E , CBN E ) and theoretically (CIB T , CBN T ; Supplementary Figs 2 and 3 for details). The
polarized optical microscopy images exhibit different birefringence patterns (brushes) depending on the phase. BPU and BPH represent the biphases with
uniform concentration throughout the vessel and with heterogeneous concentrations in a stored bottle, respectively. b, The volume fraction of the nematic
phase as a function of GO concentration (red squares) was obtained from bottles stored for two weeks. The persistence time of the field-induced
birefringence (FIB, inset image) after the shaking stopped is also plotted (blue circles). It rose sharply as the concentration increased above 0.04 vol%.

ordering interactions even in the macroscopically isotropic phase
below CIB E , as shown in Fig. 1b.
More interestingly, electric-field-induced birefringence was
observed in the low-concentration nematic phase, the biphase and
the isotropic phase (Fig. 2a). Chemical reduction and electrolysis10 ,
which were observed only under the application of a low-frequency
electric field (below 0.5 kHz) with a sufficiently high amplitude,
were avoided when a 10 kHz electric field was applied, even
without any insulation layer (Supplementary Fig. 5). We fabricated
a 0.1 vol% aqueous GO cell using Cell Type A in Fig. 2a. Clear
birefringence was induced by the application of a 5 V mm−1 electric
field, which is roughly three orders of magnitude weaker than
the field for usual molecular LC switching. After the voltage was
switched off, the field-induced birefringence slowly disappeared,
although some weak nematic ordering partially remained (the
last image in Fig. 2a–i). In contrast, no change was observed in a
1.1 vol% nematic GO cell up to 20 V mm−1 (Fig. 2a–ii).
The field-induced birefringence was measured optically using
Cell Type B, as shown in Fig. 2b, where the vertical axis represents
the induced birefringence obtained by subtracting the initial
birefringence at 0 V mm−1 from the measured birefringence.
The plots of field-induced birefringence were without thresholds,
showed large hysteresis and depended sensitively on the GO
concentration23,24 . Because the induced birefringence can be
expressed as 1n = 1nSAT × S × Cv (Supplementary Equation (10)),
where 1nSAT is the specific birefringence, S is the order parameter
and Cv is the concentration, the magnitude of 1n at 20 V mm−1
increased as the concentration was increased to 0.1 vol%. However,
it decreased when the concentration was increased above 0.1 vol%,
indicating that the sensitivity to external fields quickly became
muted as the mean interflake distance shrank. The nematic GO
with a concentration over 0.56 vol% was almost unresponsive to an
applied voltage up to 20 V mm−1 (Fig. 2b).
Extremely large Kerr coefficients
Finally, to determine accurately the Kerr coefficient, a measure
of optical sensitivity to external fields, a cuvette with parallel
electrodes on two opposite walls and a beam-path length of 5 mm
was used. Because of the appearance of a large initial birefringence
in high-concentration GO dispersions in the cuvette, Cell Type B
was used instead of the cuvette in the experiments represented
by the red square data points in Fig. 3a (Supplementary Figs 6
and 7 for details). The maximum Kerr coefficient was found to
be approximately 1.8 × 10−5 mV−2 (Fig. 3a). Note that the Kerr
coefficients of nitrobenzene and aqueous 2D gibbsite platelet
suspensions are of the order of 10−12 and 10−9 mV−2 respectively25 .
Recently, Ashok et al. reported a giant Kerr coefficient of the order
of 10−6 mV−2 using thermal rubidium vapour26 . Blue-phase LCs
have also attracted substantial interest owing to their large Kerr
coefficient on the order of 10−9 –10−8 mV−2 (refs 9,27,28). Thus, the
observed Kerr coefficient of GO-LCs on the order of 10−5 mV−2 is
extraordinarily large compared to those of any other Kerr materials.
We next considered the microscopic mechanisms behind the
observed behaviour of GO-LCs. It has been well documented

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ARTICLES NATURE MATERIALS DOI: 10.1038/NMAT3888

a
0.1 vol%

1 mm

0 V mm–1 2 V mm–1 5 V mm–1 0 V mm–1

1.1 vol%

0 V mm–1 2 V mm–1 5 V mm–1 0 V mm–1

Cell Type A Cell Type B

ITO
Glass ITO

500 μm 300 μm 300 μm 500 μm

b 4.5

4.0
0.01 vol%
3.5
0.03 vol%
3.0
0.06 vol%
Δn (×10–5)

2.5

2.0 0.11 vol%

1.5 0.22 vol%

1.0 0.28 vol%

0.5 0.56 vol%

0
0 5 10 15 20
Electric field (V mm–1)

Figure 2 | Electric-field-induced birefringence. a, Top row: Field-induced birefringence was generated by applying electric fields (10 kHz) to Cell Type A
filled with an aqueous 0.1 vol% GO dispersion. When the field was switched off, the field-induced birefringence almost disappeared, with only slight
nematic aggregation remaining. Bottom row: In the same cell structure with a 1.1 vol% GO LC, no change was detected up to 20 V mm−1 . b, Field-induced
birefringence curves without thresholds were obtained by applying extremely low electric fields using Cell Type B. Part of the hysteresis curve is shown for
the 0.11 vol% sample.

that a GO flake in an aqueous dispersion will be negatively
charged, with H3 O+ ions forming an electrical double layer on its
surface29 , which can produce Maxwell–Wagner polarization orders
of magnitude larger than that obtained for the other dielectric
molecular modes. According to the Maxwell–Wagner–O’Konski
model30,31 , the anisotropy of the polarizability (1α) of a colloid
particle depends sensitively on the aspect ratio of the particle, its
volume and the ionic conductivity on its surface. As elucidated
in detail in Supplementary Fig. 8, we calculated the theoretical
1α value of a GO flake with an aspect ratio of 3,200 using the
known material parameters of GO flakes and H3 O+ ions. The
theoretical 1α was estimated to be −1.5 × 10−26 F m2 , which is two
or three orders of magnitude larger than that of any other plate-
like or rod-like particles31 . Here, the negative value of 1α indicates
that the normal direction of the GO plane is likely to be aligned
perpendicular to the electric field.
Onsager’s reorientational entropy can be introduced into
the field-induced Maxwell–Boltzmann distribution function for
dispersed particles to obtain the Kerr coefficient as32,33
1α C
K ≈ −1nSAT (1)
15kB T λ 1 − C/CIB
Here, (1 − C/CIB )−1 comes from Onsager’s excluded volume effect,
and if the concentration is very low and the interparticle interaction
is negligible, the Kerr coefficient is determined purely by the electric
potential energy and (1 − C/CIB )−1 ∼1 (Supplementary Equation
(22) in the discussion of Supplementary Fig. 8). Using the theoretical
1α obtained above, we plotted the Kerr coefficients obtained using
both the Straley and van der Beek model (equation (1)) and
the usual Boltzmann distribution without interflake interactions
(Supplementary Equation (22)) as a function of concentration in
Fig. 3a. The theoretical prediction based on the Onsager–Straley

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NATURE MATERIALS DOI: 10.1038/NMAT3888
a 3.0
2.5
Kerr coefficient(×10–5 m V–2)
2.0
1.5
1.0
0.5
CIB_E
0.0
0.00 0.04 0.08
Concentration (vol%)
b 4.5
No NaCl
4.0 1.71 × 10–4 M
3.5 1.02 × 10–3 M
5.80 × 10–3 M
3.0
1.71 × 10–2 M
Δn (× 10–5)
2.5
2.0
1.5
1.0
0.5
0.0
0 5
Electric field (V mm–1)
Figure 3 | Extremely large Kerr coefficient and the mechanisms involved.
a, Extremely large Kerr coefficients were measured using a cuvette filled
with a GO dispersion as the sample (Supplementary Fig. 6). Below CIB E ,
the Onsager–Staley model fitted well with the experimental results,
indicating that the nematic ordering interaction partially contributed to the
large Kerr coefficient. It decreased sharply above CIB E . The red squares
represent values calculated from the data in Fig. 2b (Supplementary Fig. 7).
b, The addition of NaCl ions decreased the sensitivity of the electro-optic
response to external fields, owing to decreases in |1α|.
model accords better with the experimental results below CIB E than
the traditional model (Supplementary Equation (22)). This clearly
demonstrates that Onsager’s excluded-volume effect contributed to
the large Kerr coefficient near CIB E . In other words, as the flow-
induced birefringence persistence time confirmed the existence of
nematic ordering interactions below CIB E in Fig. 1b, it can be
concluded that the nematic ordering interactions encouraged the
sensitivity to external fields below CIB E .
Desensitization of the Kerr effect
Meanwhile, the Kerr coefficient decreased with further increases
in concentration above CIB E , indicating an increase in interflake
friction. When the interflake distance became small, van der Waals
attractions due to deformed ionic clouds around the GO flakes
became dominant29 . Such attractive interflake interactions increased
the frictional effect, which quickly paralysed the extremely sensitive
GO dispersion and prevented the Kerr effect. The increase in
interflake friction with concentration can be also confirmed by the
exponentially increasing kinetic viscosity with GO concentration
shown in Supplementary Fig. 1c.
It was also found that addition of salt dramatically reduced
the sensitivity to external fields beyond a salt concentration
of 1 × 10−5 M (Fig. 3b) and, ultimately, further addition of salt
completely desensitized the GO-LCs to external fields. The addition
of salt gives rise to a decrease in |1α|, mainly due to a increase in
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ARTICLES
a
Exp_cuvette b
Cell Type C
Exp_Cell Type B
Onsager–Straley model
No inter-flake interaction
c
CBN_E Off state
ON state
0.12 0.16 0.20
Figure 4 | Electro-optic GO-LC device using simple macroscopic wire
10 15 20
electrodes. a, Substrate with two simple wire electrodes. The average
distance between the two electrodes was 5 mm. b, Photo of the device on a
back-light unit. The electrode was placed on a glass substrate and then
covered by another glass substrate, and the edge of the cell was sealed with
PDMS walls of thickness 2 mm. The cell was filled with 0.056 vol% GO-LC
and sandwiched between left and right circular polarizers. An electric field
of 20 V at 10 kHz was applied. c, Field-on and field-off states; the contrast
between the on and off states was 15:1.
electrolyte conductivity, and it enhances the interflake interactions
as well, which can be confirmed by the fact that rotational relaxation
slowed down with the addition of NaCl (10−4 to 10−3 M) and by the
observation of GO flocculation with further NaCl addition (0.17 M;
Supplementary Fig. 9). Although both the decrease in |1α| and
the increase in interflake interactions may influence the electrical
desensitization, the former seems to contribute more, considering
that the theoretical |1α| accurately explains the experimental result
and that the increase in kinetic viscosity with NaCl concentration is
one order of magnitude smaller than that from the increase of GO
concentration (Supplementary Fig. 9).
Optical devices and wide defect-free GO LC
To demonstrate the significance of the large Kerr coefficient, we
made an electro-optic device using two simple wire electrodes
separated by 5 mm (Cell Type C in Fig. 4). Note that interdigitated
electrodes are commonly used in liquid-crystal displays (LCDs)
including blue-phase LCDs (ref. 9), in which the distance between
two neighbouring electrodes is about 5 µm—one thousandth of that
in our sample. Interestingly, our simple optical device worked very
well under an applied voltage of just 20 V on the electrodes, as shown
in Fig. 4c, although its performance was not comparable to those of
commercial LCDs. Development of a real GO device may require
an intensive study to synthesize a high-concentration isotropic GO
dispersion for highly saturated birefringence, to control the ionic
influence and precipitation for long-term stability, and to develop
a new driving scheme suitable for electrolyte materials.
In Fig. 2, we demonstrated that order parameter switching was
achievable in a low-concentration GO dispersion, but the director
397
© 2014 Macmillan Publishers Limited. All rights reserved
ARTICLES NATURE MATERIALS DOI: 10.1038/NMAT3888

a D1 D2 Cell Type D Cell Type E

F C C 2 mm
0.5 mm 1 mm

S C S C S S

300 μm ITO GO droplet

F S C Aluminium

F C C b 0 V mm–1 20 V mm–1
0.056 vol% 0.056 vol%
S C S C S S

1 mm F S C
1 mm

Δn switching Drying about 1 h at room temp.

1.0 1.0 1.0 Director rotating
0.8 0.8 0V mm–1 20 V mm–1
Trans. (a.u.)

Trans. (a.u.)

After drying After drying

0.6 0.6
0.4 0.4
0.2 Δn switching 0.2
Director rotating
0.0 0.0
–2.5 0.0 2.5 5.0 7.5 10 –2.5 0.0 2.5 5.0 7.5 10
Time (s) Time (s)

Figure 5 | Director switching of induced GO-LC alignment and field-induced wide-area uniform nematic GO-LC phase. a, In Cell Type D, filled with
0.056 vol% GO dispersion, the director of the field-induced GO alignment rotated with changes in field direction. S, a.c. signal; C, common signal; F,
floating electrode. 1n switching curves on the bottom left and right represent the field-on (0 V → D1) and field-off (D1 → 0 V) times, respectively.
Director rotating curves correspond to the rising (D2 → D1) and falling (D1 → D2) times, respectively. The dynamics of the director rotating (D1 ↔ D2)
was faster than that of the order parameter or 1n switching (0 V ↔ D1). The rising and falling times between 10% and 90% luminance were
approximately 1.0 and 4.5 s, respectively, for director switching, and 6.5 and 120 s, respectively, for order-parameter switching. b, In Cell Type E, the
isotropic GO phase turned into the LC phase as the water content evaporated. Whereas the GO on the substrate without fields exhibited a deformed LC
director (left), the GO on the substrate with fields exhibited a well-controlled, uniform LC phase (right).

of the spontaneously aligned nematic GO-LCs was not switchable.
In contrast, we successfully controlled the director of the field-
induced GO alignment at a low concentration using a 0.056 vol%
GO cell (Fig. 5a). The director of the field-induced GO was easily
rotated by changing the direction of the electric fields and optical
switching behaviour similar to that of a typical nematic LC device
was obtained. Compared to the order-parameter switching, the
switching of the induced director was faster, as shown at the bottom
part of Fig. 5a.
Using Cell Type E with a single substrate, we obtained a
wide-area, electrically aligned, high-concentration nematic GO
dispersion by evaporating some of the water contained in isotropic
aqueous GOs while electric fields were applied (Fig. 5b). An
isotropic 0.056 vol% aqueous GO dispersion was released between
two electrodes on the substrate and left under ambient conditions to
allow the water content to slowly evaporate. The field-induced GO
alignment in the isotropic state was sustained after the GO changed
to the nematic phase as the dispersion dried, and the uniform
GO-LC alignment was not disturbed even after the fields were
switched off. In contrast, in the cell that dried without an applied
electric field, the GO formed a disordered LC alignment with many
brushes (left Fig. 5b). This clearly shows that GO-LC alignment
with arbitrary sizes and shapes can be achieved by designing an
appropriate electric field.
Methods
The preparation of the graphene oxide samples and their characterizations are
described in detail in Supplementary Fig. 1. The quality and dimensions of GO
flakes varied depending on the batch and the sonicating time, so we used a GO
sample with a mean size of 3.2 µm from a single batch to maintain consistency.
The determination of the sequence of uniform phases of the aqueous GO
dispersion, which had a second-order transition between the isotropic and
nematic phases, is described in Supplementary Fig. 3.
For the electro-dynamics experiments, the five different types of cells shown
in Fig. 2 (Cell Types A and B), Fig. 4 (Cell Type C) and Fig. 5 (Cell Types D and
E) were used. The substrates for these cells were transparent glass (0.5-mm
thickness) and the electrodes in Cell Types A, B and D were indium–tin–oxide
(ITO) layers with 100-nm thicknesses. Cell Type E had 0.5-mm-thick aluminium
electrodes. The dimensions are given in each illustration in Figs 2 and 5.
Depending on the purpose of the experiment, all the cells were designed to
produce different field profiles.
Received 26 August 2013; accepted 20 January 2014;
published online 9 March 2014
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Acknowledgements
This work was supported by the National Research Foundation of Korea (NRF) grants
funded by the Korea government (MSIP) (No. 2012R1A1A1012167 and No.
2013R1A1A2057455).
Author contributions
J-K.S. planned and supervised the project. T-Z.S. and S-H.H. carried out all the
experiments. All authors analysed the data and participated in writing the manuscript.
Additional information
Supplementary information is available in the online version of the paper. Reprints and
permissions information is available online at www.nature.com/reprints.
Correspondence and requests for materials should be addressed to J-K.S.
Competing financial interests
The authors declare no competing financial interests.
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