www.advopticalmat.

de
www.MaterialsViews.com

COMMUNICATION

Uniaxial-isotropic Metamaterials by Three-Dimensional

Split-Ring Resonators
Che-Chin Chen, Atsushi Ishikawa, Yu-Hsiang Tang, Ming-Hua Shiao,
Din Ping Tsai, and Takuo Tanaka*
Metamaterials introduce a new paradigm to create unprecedented optical functional materials using sub-wavelength
structures with tailored shape and material compositions.[14]
Analogous with atoms or molecules in natural materials, the
corresponding elemental unit for metamaterials is the metaatom, that is, a specially designed man-made structure to
create peculiarinteractions with electromagnetic (EM) waves.
An example of such unique optical functionalities is the negative index of refraction. The first negative index metamaterial
was demonstrated in the microwave regime by adopting splitring resonators (SRRs) as magnetic meta-atoms and metal
wires as electric ones.[5,6] This pioneering work brought the
metamaterial concept into reality and a lot of analogue shapes
of meta-atoms have been proposed and demonstrated, such
as rod pairs, fishnet structures, and closed nanorings.[710]
Although these meta-atoms were developed to create optical
magnetism,[1115] their EM interactions with light are explained
by antenna theory. Since no ideal isotropic antennas exist practically, their coupling properties are intrinsically asymmetric and
the resultant optical responses of the metamaterials are inevitably anisotropic, severely limiting their practical applications.
In contrast, lessons learned from the architecture of natural materials can show that, even if their element structure

Dr. C.-C. Chen, Y.-H. Tang, Dr. M.-H. Shiao

Instrument Technology Research Center
National Applied Research Laboratories
Hsinchu 30076, Taiwan
Prof. A. Ishikawa
Department of Electrical and Electronic Engineering
Okayama University
3-1-1 Tsushimanaka, Kitaku, Okayama 700-8530, Japan
Dr. C.-C. Chen, Prof. A. Ishikawa, Prof. T. Tanaka
Metamaterials Laboratory
RIKEN, 21 Hirosawa, Wako, Saitama 351-0198, Japan
E-mail: t-tanaka@riken.jp
Prof. D. P. Tsai
Department of Physics
National Taiwan University
Taipei 10617, Taiwan
Prof. D. P. Tsai
Research Center for Applied Sciences
Academia Sinica
Taipei 115, Taiwan
Prof. T. Tanaka
Research Institute for Electronic Science
Hokkaido University
N21W10 Kita-Ward
Sapporo, Hokkaido 001-0020, Japan

DOI: 10.1002/adom.201400316

Adv. Optical Mater. 2014,

DOI: 10.1002/adom.201400316

is anisotropic, overall isotropic responses will effectively arise

from the random arrangement of the elements. For instance,
water in a glass acts as an isotropic material for light, although
the water molecule itself has an asymmetric and anisotropic
structure. The isotropic properties of water arise from the
random and symmetric orientation of the water molecules.
In the same manner, isotropic metamaterials can be realized
by the highly symmetric arrangement of three-dimensional
(3D) meta-atoms. To date, according to this concept, isotropic
responses of metamaterials have been achieved at microwave
frequencies by employing symmetric 3D alignment of metaatoms. However, in the optical regime, such isotropic metamaterials have been elusive due to the challenge of 3D nanostructure fabrication.[1619] Few techniques have been reported
to fabricate 3D SRRs at optical frequencies, and the fabrication
processes were relatively complicated.[2028] Isotropic metamaterials remain a theoretical prediction.[1619]
Here, we report the first demonstration of an isotropic IR metamaterial consisting of fourfold-symmetric 3D SRRs. We have
developed a metal stress-driven self-folding method and it enables
us to mass-produce 3D metallic nanostructures (Figure 1a).[29]
The greatest advantage of our technique is that the assembled
3D stereostructures can be formed directly from two-dimensional (2D) templates through a self-folding process that is
spontaneously driven by pre-stressed films.[3032] This basic
principle, which is totally different from other approaches,[22,23]
enables the fabrication of electrically isolated 3D structures for
isotropic responses. We adopt Ni/Au (10/60 nm) as the bilayer
metals, and a series of the stress tests by varying the arm sizes
is carried out to determine the corresponding dimensions for
our 2D template (see Supporting Information, Figure S1). The
2D template of a SRR, which consists of two arms and a connection pad, was firstly fabricated using electron beam lithography, Ni/Au deposition, and lift-off techniques. The connection pad was purposefully designed to have a slightly larger
width compared to that of the arms, serving as an adhesive
area to the substrate in the self-folding process (see Supporting
Information, Figure S2a). Note that, after the stress tests, we
designed the arms with a width of 200 nm and a length of
2.5 m to expect a 3D SRR with a diameter of 2.4 m. The
sample was then completed by CF4 plasma dry-etching for
the Si substrate, where folding of the arms was spontaneously induced by bilayer residual stress. When the arms were
released from the Si substrate, the top Au film revealed higher
tensile stress than that of the back Ni film, thereby folding up
the arms away from the substrate.[33,34] Figure 1b shows a scanning electron microscopy (SEM) image of the as-fabricated
isotropic metamaterial with a total sample area of 4 4 mm2.

2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

wileyonlinelibrary.com

www.advopticalmat.de

COMMUNICATION

www.MaterialsViews.com

Figure 1. a) The fabrication process of a 3D SRR; spin-coating resist, electron beam lithography, Ni/Au (10/60 nm) deposition, lift-off, CF4 plasma
dry-etching, and self-folding (in sequence). The SRR diameter, d, height, h, and gap size, g, were 2.2 m, 1.8 m, and 1.5 m, respectively. Note that a
shadow effect of the arms in the dry-etching process produces protruding Si portions under the arms in the last two steps. b) SEM image of the fabricated isotropic metamaterial consisting of fourfold symmetric 3D SRRs. The inset shows a magnified image, and the total sample area was 4 4 mm2.

Since the folding forces were entirely programmed by the deposition conditions and structure design, the fabricated structures
were quite uniform over a sample area. Different from previous
reports,[29,34] our technique based on 2D templates of bilayer
metals demonstrates a robust approach for the realization of
large-scale 3D metamaterials.
We firstly characterized the fundamental optical properties
of the 3D SRR elements by measuring a rectangular array of
the SRRs, i.e., an anisotropic metamaterial (see Supporting
Information, Figure S2b), using Fourier-transform infrared

spectrophotometry (FTIR). The normalincidence transmittance

spectra for different sample rotations () are shown in Figure 2a.
Each spectrum was normalized by that of the bare substrate to
discuss only the dependences of the response of the metamaterials. At = 0, where the incident electric field is parallel
to the SRR gap, a typical resonant dip was clearly observed
at 27.52 THz. With increasing , the resonant dip gradually
decreased following the relations of the corresponding transmittance, i.e., T() = 1(1T = 0) |cos2|, and totally disappeared at = 90. To identify the resonant behavior of these

Figure 2. a) Measured normalincidence transmittance spectra for different sample rotations . The inset shows the sample configuration at = 0
where the incident electric field is parallel to the SRR gap. b) Numerically simulated transmittance spectra at = 0 and 90. The inset shows the corresponding Jz distribution in the 3D SRR at the resonance f = 30.2 THz. c) Real and imaginary parts of the retrieved effective parameters of 3D SRRs;
permittivity , permeability , bi-anisotropy parameter , and refractive index n.

wileyonlinelibrary.com

2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Adv. Optical Mater. 2014,

DOI: 10.1002/adom.201400316

www.advopticalmat.de
www.MaterialsViews.com

D 0
B =
i / c 0

i / c 0 E
0 H

(1)

where 0 (0) is the vacuum permittivity (permeability), ()

is the effective permittivity (permeability), c0 is the speed of
light, and is the bi-anisotropy parameter to describe the
excitation of electric dipoles by the magnetic field and vice
versa. Here, , , , and the complex refractive index n satisfy
the relationship: n2 = 2. With careful attention to this bianisotropic response, the effective parameters, , , , and n of
the 3D SRR array were retrieved from the simulated complex
transmittance and reflectance coefficients.[36] The results are
shown in Figure 2c. At the resonance, typical Lorentzian-like
responses are observed in and ; reaches a negative value
within a certain frequency range, while also shows values
away from 1.0. Despite the influence of bi-anisotropy (), which
dampens the oscillation of the refractive index, the real part of
the refractive index shows a large swing from 0.35 to 1.86 at
mid-IR frequencies.
We now turn to an isotropic metamaterial, i.e., a fourfoldsymmetric structure whose unit cell consists of total 12 SRRs
(see Supporting Information, Figures S2c and S2d). To thoroughly evaluate its isotropic properties, we systematically
changed the sample rotation (), incidence angle (), and p- or
s-polarization, as shown in the experimental setup of Figure 3a.
Figure 3b shows the measured transmittance map of the isotropic metamaterial as a function of frequency and sample
rotation for the normal incidence [transverse electromagnetic
(TEM) at = 0]. Surprisingly, the transmittance spectra manifested no dependence and a totally isotropic response of the
first mode, demonstrating our primary goal of realizing an isotropic IR metamaterial. Note that the spectral dip position and
intensity were slightly shifted and decreased compared to the

Adv. Optical Mater. 2014,

DOI: 10.1002/adom.201400316

COMMUNICATION

meta-atoms, a set of numerical simulations was carried out for

the configurations of = 0 and 90. The calculated spectra are
shown in Figure 2b and are in good agreement with the experimental results. The minor difference in the spectral dip position is due to the dimension deviation of the SRR between the
experiment and simulation; the dimensions of the simulation
model were determined by SEM observations. The final structure of 3D SRR is slightly smaller than the original design with
a few percent deviation. The inset of Figure 2b shows the current distribution along the z-axis (Jz), revealing the mode profile
of the resonant dip. An out-of-phase current flows between two
arms formed a circular current in the SRR, inducing a strong
magnetic dipole moment perpendicular to the ring (see Supporting Information, Figure S3a). Based on these results, we
designate the resonant dip at 27.52 THz as the fundamental
(first) mode of our 3D SRR.
Since the 3D SRR has a single gap, the inversion symmetry
is broken along the propagation direction. As a result, the SRRs
array behaves as a bi-anisotropic metamaterial, where electric
(magnetic) dipoles in the structure are excited by both magnetic and electric (electric and magnetic) fields of the incident
light.[35,36] For the simplest situation at = 0, the relationship
between the relevant EM fields of the Maxwell equation is
described by Equation (1)

Figure 3. a) Schematic of measurement setup. The illumination condition is specified using three variables; the sample rotation , incident
angle , and p- or s-polarization. b) Measured transmittance map of an
isotropic metamaterial as a function of frequency and sample rotation for
the normal incidence (TEM at = 0). The resonant dip position of the
first mode is indicated by the white dashed line.

rectangular SRR array (Figure 2a). This is due to the difference

in the periodicity, giving different effective capacitances and
densities, which affect the resonance behavior.
Since our isotropic metamaterial has only in-plane symmetry, no complete isotropic response might be expected for
the oblique incidence. However, we found that 3D stereostructures in the metamaterial effectively improved the symmetry
breaking along the z-axis and indeed exhibited a quasi-3-axisisotropic response, even for the oblique incidence. This condition is demonstrated in Figure 4, where the first mode remained
almost the same up to = 40 for both p- and s-polarizations.
It is worth noting that, since the transmission spectrum of the
isotropic metamaterial was almost the same as that of the simulated SRR array [Figure 2(a)], its refractive index should have
a similar value. For the p-polarization (Figure 4a), the second
mode, which has an in-phase current flow between two arms,
was also excited at a large incidence angle (see Supplemental
Information, Figure S3b).[37] Since this mode has only the electric dipole moment along the z-axis, the resonance dip became
more notable as the incidence angle increased. On the other
hand, the excitation of the second mode was not observed for
the s-polarization because of no electric field along the z-axis
(Figure 4b). Note that such quasi-isotropic responses are also
highly robust, even when the sample is rotated (see Supplemental Information, Figure S4). As a result, we conclude that
our metamaterial made of 3D SRRs is totally isotropic for any
lateral rotation, polarization, and incidence angle up to 40.
In conclusion, we have fabricated and characterized an isotropic IR metamaterial consisting of fourfold-symmetric 3D

2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

wileyonlinelibrary.com

www.advopticalmat.de

COMMUNICATION

www.MaterialsViews.com

metamaterials for mass-production purposes. Hence, it may

have great potential for realizing the practical applications of
3D optical metamaterials.

Experimental Section

Figure 4. a,b) Measured transmittance map of an isotropic metamaterial as a function of frequency and incident angle for the p- (a) and s(b) polarizations at = 0. The quasi-isotropic responses are robust even
for the sample rotation. (see Supplemental Information, Figure S4). The
resonant dip positions of the first and second modes are indicated by the
white dashed lines.

SRRs formed by a metal stress-driven self-folding method.

Unambiguous isotropic characteristics were demonstrated for
any lateral rotation and polarization at the normal incidence.
Despite the lack of symmetry in the third dimension of the
metamaterial, such isotropic responses were maintained for
incidence angles up to 40. The corresponding numerical simulations re-produced the experimental results well, revealing
that the interplay of electric and magnetic interactions of the
3D SRR plays a crucial role for the bi-anisotropic responses.
The fabrication technique presented here can in principle
be extended to multiple layers being stacked by depositing
multi-stressed metal layers and/or combining the planarization process, allowing the construction of more complex 3D
meta-atoms for more optical functionalities.[38] Tailored optical
responses could be expected as well by tuning the dimensions
of the 2D templates. Moreover, with suitable lithography techniques such as photolithography, electron beam lithography,
or nanoimpriting, one may fabricate desired spectrum band

wileyonlinelibrary.com

Sample Preparation: 3D SRRs were fabricated as follows. A bilayer

electron beam resist consisting of PMMA_MAA/PMMA was spin-coated
on a Si substrate with 4000 rpm for 40 s and baked at a 160 C for
30 min in succession. The 2D pattern template was exposed by using an
EBL system (Elionix ELS-7700H) with parameters of accelerate voltage
of 100 kV, beam current of 100 pA, field size of 300/60000 m/dot, and
exposure dosage of 1.5 s/dot, respectively. The exposed resist was then
developed using MIBK:IPA = 1:3 for 75 s and IPA for 25 s, respectively.
Ni/Au (10/60 nm) films were deposited using a thermal evaporator
SVC-700TM (Sanyu Electron) with coating rate of 0.5/0.8 /s under
a vacuum of about 3 103/9 103 Pa. A lift-off was achieved in an
acetone solvent to dissolve the resist on the substrate. The 3D SRRs on
the substrate were finally created by etching the underneath Si substrate
of the arms using the inductive coupled plasma reactive ion etching
system (RIE-200P, Samco) with parameters of CF4 plasma of flow rate
of 20 sccm, pressure of 0.15 Pa, ICP power of 500 W, and forward power
of 0 W for 320 s.
Sample
Characterization:
A
Fourier
transform
infrared
spectrophotometer (FT/IR-6300FV, Jasco) with a high-intensity ceramic
lump and a liquid-N2 cooled MCT detector was used to characterize
the transmittance spectra of the sample. The sample was installed on a
rotatable and tiltable stage under a vacuum chamber to avoid CO2 and
H2O absorption in the atmosphere.
Numerical Simulations: The EM responses of 3D SRRs were calculated
using the finite-element method (FEM) software package, COMSOL, with
the dielectric constant of silicone = 3.5 and the empirical value for gold.[39]
The dimensions of 3D SRRs were determined from the SEM image as
shown in Figure 1b. The calculation volume was (x, y, z) = (5.7 m, 2.45 m,
7.5 m), including the silicone substrate with the thickness of 1.5 m,
on which a 3D SRR was placed. The periodic boundary conditions were
applied in the x- and y-axes to model the two-dimensional periodic array
of 3D SRRs. The input and output ports boundary was employed in
the z-axis to launch the polarized light toward the positive z direction.
Calculated transmittance was normalized by the corresponding result for
the bare substrate to compensate the effect of Fresnel reflection at the
air-substrate interface. From the calculated complex transmittance and
reflectance coefficients, the effective parameters of 3D SRRs, permittivity
, permeability , bi-anisotropy parameter , and refractive index n, were
retrieved following a method in the literature.[32]

Supporting Information
Supporting Information is available from the Wiley Online Library.

Acknowledgements
The authors thank nano-fabrication supports from the Metamaterials
Fabrication Platform of Instrument Technology Research Center and
Emergent Matter Science Research Laboratory of RIKEN. This work was
supported by grants from the National Science Council (NSC 1022221E-492033, 1022745-M-002005-ASP, 1002923-M-002007-MY3, and
1022221-E-492003), the Photonics Center Osaka Univ. joint research
R-3, the JSPS Asian CORE Program, and MEXT KAKENHI Grant-in-Aid
for Scientific Research on Innovative Areas Grant Number 22109006.
C.-C.C., A.I., and T.T. contributed equally to this work. C.-C.C. and D.P.T.
devised the 3D structure idea and initiated the project; C.-C.C., Y.-H.T.
and M.-H.S. performed the fabrication experiments; C.-C.C. and A.I.

2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Adv. Optical Mater. 2014,

DOI: 10.1002/adom.201400316

www.advopticalmat.de
www.MaterialsViews.com

Received: July 12, 2014

Revised: September 24, 2014
Published online:

[1]
[2]
[3]
[4]
[5]
[6]
[7]
[8]
[9]
[10]
[11]
[12]
[13]
[14]
[15]
[16]
[17]
[18]
[19]

D. R. Smith, J. B. Pendry, M. C. K. Wiltshire, Science 2004, 305, 788.

V. M. Shalaev, Nat. Photon. 2007, 1, 41.
N. Engheta, Science 2007, 317, 1698.
B. Lukyanchuk, N. I. Zheludev, S. A. Maier, N. J. Halas, P. Nordlander,
H. Giessen, C. T. Chong, Nat. Mater. 2010, 9, 707.
D. R. Smith, W. J. Padilla, D. C. Vier, S. C. Nemat-Nasser, S. Schultz,
Phys. Rev. Lett. 2000, 84, 4184.
R. A. Shelby, D. R. Smith, S. Schultz, Science 2001, 292, 77.
V. M. Shalaev, W. Cai, U. K. Chettiar, H. K. Yuan, A. K. Sarychev,
V. P. Drachev, A. V. Kildishev, Opt. Lett. 2005, 30, 3356.
G. Dolling, M. Wegener, C. M. Soukoulis, S. Linden, Opt. Lett. 2007,
32, 53.
J. Valentine, S. Zhang, T. Zentgraf, E. Ulin-Avila, D. A. Genov,
G. Bartal, X. Zhang, Nature 2008, 455, 376.
B. Kant, Y. S. Park, K. OBrien, D. Shuldman, N. D. LanzillottiKimura, Z. J. Wong, X. Yin, X. Zhang, Nature Commun. 2012, 3, 1180.
J. B. Pendry, A. J. Holden, D. J. Robbins, W. J. Stewart, IEEE Trans.
Microwave Theory Tech. 1999, 47, 2075.
T. J. Yen, W. J. Padilla, N. Fang, D. C. Vier, D. R. Smith, J. B. Pendry,
D. N. Basov, X. Zhang, Science 2004, 303, 1494.
S. Linden, C. Enkrich, M. Wegener, J. Zhou, T. Koschny, C. M. Soukoulis,
Science 2004, 306, 1351.
A. Ishikawa, T. Tanaka, S. Kawata, Phys. Rev. Lett. 2005, 95, 237401.
N. Liu, H. Liu, S. Zhu, H. Giessen, Nat. Photon. 2009, 3, 157.
T. Koschny, L. Zhang, C. M. Soukoulis, Phys. Rev. B 2007, 71,
121103.
J. D. Baena, L. Jelinek, R. Marqus, Phys. Rev. B 2007, 76, 245115.
D. . Guney, T. Koschny, M. Kafesaki, C. M. Soukoulis, Opt. Lett.
2009, 34, 506.
D. . Guney, T. Koschny, M. Kafesaki, C. M. Soukoulis, Opt. Express
2010, 18, 12348.

Adv. Optical Mater. 2014,

DOI: 10.1002/adom.201400316

COMMUNICATION

contributed to the sample characterization and simulation. C.-C.C., A.I.

and T.T. contributed to data analysis and manuscript preparation.

[20] S. Zhang, W. Fan, B. K. Minhas, A. Frauenglass, K. J. Malloy,

S. R. J. Brueck, Phys. Rev. Lett. 2005, 94, 037402.
[21] T. Tanaka, A. Ishikawa, S. Kawata, Appl. Phys. Lett. 2006, 88, 081107.
[22] M. S. Rill, C. Plet, M. Thiel, I. Staude, G. V. Freymann, S. Linden,
M. Wegener, Nat. Mater. 2008, 7, 543.
[23] J. K. Gansel, M. Thiel, M. S. Rill, M. Decker, K. Bade, V. Saile,
G. V. Freymann, S. Linden, M. Wegener, Science 2009, 325,
1513.
[24] D. B. Burckel, J. R. Wendt, G A. T. Eyck, J. C. Ginn, A. R. Ellis,
I. Brener, M. B. Sinclair, Adv. Mater. 2010, 22, 5053.
[25] K. Fan, A. C. Strikwerda, H. Tao, X. Zhang, R. D. Averitt, Opt. Express
2011, 19, 12619.
[26] W. T. Chen, C. J. Chen, P. C. Wu, S. Sun, L. Zhou, G. Y. Guo,
C. T. Hsiao, K. Y. Yang, N. I. Zheludev, D. P. Tsai, Opt. Express 2011,
19, 12837.
[27] C. M. Soukoulis, M. Wegener, Nat. Photon. 2011, 5, 523.
[28] A. Radke, T. Gissibl, T. Klotzbcher, P. V. Braun, H. Giessen,
Adv. Mater. 2011, 23, 3018.
[29] C. C. Chen, C. T. Hsiao, S. Sun, K. Y. Yang, P. C. Wu, W. T. Chen,
Y. H. Tang, Y. F. Chau, E. Plum, G. Y. Guo, N. I. Zheludev, D. P. Tsai,
Opt. Express 2012, 20, 9415.
[30] E. J. Smith, Z. Liu, Y. Mei, O. G. Schmidt, Nano Lett. 2010, 10, 1.
[31] E. J. Smith, Z. Liu, Y. F. Mei, O. G. Schmidt, Appl. Phys. Lett. 2009,
95, 083104.
[32] Y. Mei, G. Huang, A. A. Solovev, E. B. Urea, I. Mnch, F. Ding,
T. Reindl, R. K. Y. Fu, P. K. Chu, O. G. Schmidt, Adv. Mater. 2008,
20, 4085.
[33] F. M. DHeurle, J. M. E. Harper, Thin Solid Films 1989, 171, 81.
[34] Y. V. Nastaushev, V. Y. Prinz, S. N. Svitasheva, Nanotechnology 2005,
16, 908.
[35] R. Marqus, F. Medina, R. Rafii-El-Idrissi, Phys. Rev. B 2002, 65,
144440.
[36] C. . Kriegler, M. S. Rill, S. Linden, M. Wegener, IEEE J. Sel. Topics
Quantum Electron. 2010, 16, 367.
[37] C. Enkrich, M. Wegener, S. Linden, S. Burger, L. Zschiedrich,
F. Schmidt, J. F. Zhou, Th. Koschny, C. M. Soukoulis, Phys. Rev. Lett.
2005, 95, 203901.
[38] N. Liu, H. Guo, L. Fu, S. Kaiser, H. Schweizer, H. Giessen, Nat.
Mater. 2008, 7, 31.
[39] P. B. Johnson, R. W. Christy, Phys. Rev. B 1972, 6, 4370.

2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

wileyonlinelibrary.com