Graphene as broadband terahertz antireflection coating

Yixuan Zhou, Xinlong Xu, Fangrong Hu, Xinliang Zheng, Weilong Li, Penghui Zhao, Jintao Bai, and Zhaoyu Ren

Citation: Applied Physics Letters 104, 051106 (2014); doi: 10.1063/1.4863838

View online: http://dx.doi.org/10.1063/1.4863838
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 APPLIED PHYSICS LETTERS 104, 051106 (2014)

Graphene as broadband terahertz antireflection coating

Yixuan Zhou,1 Xinlong Xu,1,a) Fangrong Hu,2 Xinliang Zheng,1 Weilong Li,1 Penghui Zhao,1
Jintao Bai,1 and Zhaoyu Ren1,a)
1
State Key Lab Incubation Base of Photoelectric Technology and Functional Materials, National Photoelectric
Technology, Functional Materials and Application of Science and Technology International Cooperation
Center, and Institute of Photonics & Photon-Technology, Northwest University, Xian 710069, China
2
School of Electronic Engineering and Automation, Guilin University of Electronic Technology,
Guilin 541004, China
(Received 13 November 2013; accepted 18 January 2014; published online 3 February 2014)
We examined the potential of stacked multilayer graphene as broadband terahertz (THz)
antireflection coating based on the impedance matching effect in experiment and theory. The
reflected pulses from the quartz and silicon substrates were observed to change with the layer
number and doping concentration of the graphene coating. Remarkable broadband impedance
matching was achieved due to optimized THz conductivity. Theoretical analysis based on Drude
model and thin film Fresnel coefficients have been used to explain the experimental phenomena,
which indicated the shift of Fermi level caused by chemical doping. This work paves the way for
graphene-based broadband THz antireflection coating. VC 2014 AIP Publishing LLC.

[http://dx.doi.org/10.1063/1.4863838]

As one of the most rapid growing field, terahertz (THz)
technology has stimulated many applications ranging from
time-domain spectroscopy (TDS), biological imaging, high
sensitive sensing, to radar and high-speed communications.1
Hence, there is an urgent demand of THz devices, such as
sources, detectors, and many other THz components for THz
wave manipulation.2,3 Among them, antireflection coatings
are needed to minimize the reflections at the interfaces of the
THz components, which suppress the unwanted Fabry-Perot
effects. This is especially useful for the THz-TDS system, as
the reflections limit the spectral resolution.
In visible-infrared region, quarter-wavelength dielectric
films are the mostly used antireflection coatings. However,
they are not suitable for THz wave due to the broadband char-
acteristics. Recently, impedance matching layers have been
demonstrated to be a good option as antireflection coatings.
Metal films, such as chromium and gold,4,5 oxide semicon-
ductor materials, such as zinc oxide, vanadium dioxide and
indium-tin-oxide,4,6,7 as well as metamaterials,8 have been
studied as THz impedance matching layers. However, for
THz applications, metal films still need to overcome the com-
plexity of fabrication and high cost, oxide semiconductor
materials are often unstable and their effects are often insuffi-
cient, and metamaterials work at narrow bandwidth. Thus,
new materials with better performances are still in great
demand.
Graphene as a two-dimensional atomic crystal has
excellent mechanical, electrical, optical, magnetic, and ther-
mal properties.9,10 Particularly, the electrical and optical
properties of graphene are determined by the unique Dirac
cone structure with a linear dispersion relation.11,12 The
extraordinary carrier nature as well as the pronounced ambi-
polar electric field effect have made it widely useful for the
next-generation of photonics and optoelectronics.10,12 In the
a)
Authors to whom correspondence should be addressed. Electronic
addresses: xlxuphy@nwu.edu.cn and rzy@nwu.edu.cn.
THz regime, the optical conductivity of graphene is deter-
mined by the intraband transition and follows the Drude
model.13,14 What is more, efficient THz wave manipulation,
such as THz modulator, switch, isolator, and polarizer, etc.,
has been proved.1518 However, the impedance matching
property of graphene has not been mentioned.
In this paper, we present the impedance matching proper-
ties of graphene in both theory and experiment. Graphene
samples are synthesized by chemical vapor deposition
(CVD), and multi-layer graphene is fabricated by layer-by-
layer random stack on both quartz and silicon substrates. The
lateral size of a single graphene layer is approximate
1  1 cm2. After stacking, the overlapping area is no less than
5  5 mm2, which is larger than the wavelength of the broad-
band THz pulse. Chemical doping by HNO3 can be used to
optimize the THz sheet conductivity of multilayer graphene.
The amplitude and phase of the internal reflected pulses from
the substrates are observed to change with the layer number
and doping concentration. After chemical doping, broadband
THz-wave impedance matching can be achieved with 2-layer
graphene on quartz and 5-layer graphene on silicon.
Theoretical calculation with a Drude model and thin film
Fresnel coefficient further suggests that the Fermi level of
graphene drops from 0.11 eV to 0.25 eV after chemical
doping. This work verifies the potential application of
graphene-based broadband THz antireflection coating.
The graphene samples were fabricated by CVD on cop-
per foils as described in our previous work.19 Thin poly-
methyl methacrylate (PMMA) films were then spin coated
on top of them. After wet-etching of the copper foils,
PMMA/graphene films were transferred onto different sub-
strates. Subsequently, the PMMA films were dissolved with
acetone. The aforementioned processes were repeated N
times to fabricate an N-layer graphene sample. Both quartz
and high-resistivity silicon are used as substrates, and multi-
layer graphene with N 1, 2, 3, 5, 7 is obtained in this work.
This kind of randomly stacked graphene has been proved to

0003-6951/2014/104(5)/051106/5/$30.00 104, 051106-1 C 2014 AIP Publishing LLC

V

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 051106-2 Zhou et al.
be different with exfoliated one, as the electrical decoupling
between layers makes it behave like isolated monolayer
graphene.2022 Chemical doping was achieved by dipping
the N-layer graphene/substrate into HNO3 (68%) for 5 min.
HNO3 is a p-type dopant in graphene. It can make electron
transfer from graphene to the nitric acid and result in the
shift of the Fermi level.23
Before and after the doping process, commercial THz-
TDS system (Zomega Z-3) was employed to measure the
THz transmission of these samples at normal incidence. In
general, THz pulses were generated by a photoconductive
antenna under the excitation of a 100-fs laser (FemtoFiber
pro NIR, TOPTICA Photonics) with a center wavelength of
790 nm and the average power of 140 mW at a repetition
rate of 80 MHz. THz pulses are detected by electro-optic
sampling with a ZnTe(110) crystal. The optical path from
THz generation to THz detection is purged with dried air to
avoid the effect of the humidity.
Figs. 1(a) and 1(b) show the measured THz signal
transmitted through N-layer graphene on quartz (1 mm in
thickness) before and after the chemical doping process.
Corresponding results for silicon substrate (0.5 mm in thick-
ness) are presented in Figs. 1(c) and 1(d). For quartz sub-
strate, the main pulse appears at 8.4 ps, and the reflection
pulse (circumscribed by a dotted window in Fig. 1) appears
at 21.5 ps, while the main pulse appears at 9.2 ps and
the reflection pulse at 20.5 ps for silicon substrate. The
reflection pulses are notorious limitation of spectral
FIG. 1. Transmitted THz pulses through (a) N-layer (1,3,5,7) graphene on
quartz before doping; (b) N-layer (1,2,5,7) graphene on quartz after doping; (c)
N-layer (1,3,5,7) graphene on silicon before doping; and (d) N-layer (1,3,5,7)
graphene on silicon after doping. The results of uncoated substrates are shown
as references (ref.).
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Appl. Phys. Lett. 104, 051106 (2014)
resolution in THz-TDS. We focus on the reflection pulses
when the layer number increases. With layer number
increasing, the reflection pulse is observed to suppress at 3-
layer for quartz substrate (Fig. 1(a)) and at 7-layer for sili-
con substrate (Fig. 1(c)). After chemical doping, the sup-
pression appears at 2-layer for quartz substrate (Fig. 1(b))
and 5-layer for silicon substrate (Fig. 1(d)). All these are
due to the impedance matching properties from graphene
layer. In particular, for uncoated substrate, the reflection
pulse has a valley-peak shaped resonance, which is weak-
ened by graphene for all conditions. We also observed the
polarity reversal of the reflection pulses as shown in Figs.
1(a), 1(b), and 1(d), due to the phase change of the imped-
ance matching layer.
We present a propagation model to analyze the effect as
shown in Fig. 2. Pulse 1 represents the main pulse and pulse
m (2, 3, 4) represents the reflection pulse. N-layer gra-
phene is placed at the interface between air and substrate
(dsub in thickness) with refractive indices n1 nair and
n3 nsub . Graphene is a two-dimensional material with a
thickness dgra  0.335 nm.24 Thus even when N 30, the
film is sub-10 nm and much thinner than the skin depth of
THz wave. Therefore, it can be treated as a zero-thickness
conductive film with the transmission and reflection at the
interface given by5
2n1
tgra ; (1)
n1 n3 Z0 rtotal
n3  n1  Z0 rtotal
rgra ; (2)
n1 n3 Z0 rtotal
where Z0 377X is the impedance of free space and rtotal
the optical sheet conductivity of N-layer graphene.
The Fresnel coefficients tij 2ni =ni nj and rij
ni  nj =ni nj are used to describe the transmission
and reflection at the interface between air and the substrate.
At normal incidence, the transmission coefficient of the m-th
pulse can be expressed as follows:
Etm x
tm m1 m1
tgra t34 rgra r34 pair
ETHz x
 x; dsub psub x; dsub 2m1 ; (3)
FIG. 2. Schematic of THz pulse propagation through N-layer graphene on
substrate (quartz or silicon). The incident THz pulse and the main transmit-
ted pulse (pulse 1) are indicated by red color, while the internal reflections
in the substrate are blue, with only the first two pulses (pulses 2 and 3)
shown.
 051106-3 Zhou et al. Appl. Phys. Lett. 104, 051106 (2014)

where x is the angular frequency; ETHz , Etm are electric

fields of the incident and transmitted THz waves;
and pair x; dsub expixdsub nair =c and psub x; dsub
expixdsub nsub =c are propagation factors in air and the
substrate. The corresponding transmission coefficient of
m
uncoated substrate is defined as tsub , which shows a similar
expression as Eq. (3) by replacing tgra and rgra to t13 and r31 .
For pulse 1 (m 1), t1 is in direct proportion to tgra and
inversely proportional to the optical sheet conductivity of N-
layer graphene. Differently, t2 is proportional to rgra besides
tgra , which is intrinsic related to optical sheet conductivity of
the coated layer.
It implies that the internal reflection can significantly be
reduced by decreasing the impedance mismatch. When the
THz wave travels from the substrate to air (n3 > n1 ), the
phase of pulse 2 will be dominated by rtotal (Eq. (2)). When
rtotal < n3  n1 =Z0 (rgra > 0), pulse 2 has the same phase
as the incident pulse. When rtotal > n3  n1 =Z0 (rgra < 0),
pulse 2 shows a p phase shift. When rtotal n3  n1 =Z0
FIG. 3. THz sheet conductivity obtained from pulse 1 for (a) N-layer (1,3,5,7)
(rgra 0), impedance matching condition can be achieved graphene on quartz before doping; (b) N-layer (1,2,5,7) graphene on quartz after
and the reflection is suppressed. The amplitude and phase of doping; (c) N-layer (1,3,5,7) graphene on silicon before doping; and (d) N-layer
the reflection can be controlled by the sheet conductivity of (1,3,5,7) graphene on silicon after doping.
the coated graphene-layer.
As a qualitative analysis, Fig. 1 can be explained as fol- Before doping, the average sheet conductivity values of 1, 3,
lows. Firstly, the optical sheet conductivity rises with the 5, 7-layer graphene are approximate 0.6, 2.0, 3.2, and 4.8 mS,
graphene layer number increasing, the proportional relation- thus the perfect impedance matching is expected to occur
ship with main pulse leads to the reduction of the amplitude between 3 and 5 layers. After doping, the average optical
in all conditions. Secondly, when pulse 2 is suppressed, it sheet conductivities for 1, 2, 5, 7-layer graphene are around
means impedance matching condition is approaching ful- 1.0, 3.2, 7.2, and 10.5 mS, and the ideal impedance matching
filled. Similarly, when pulse 2 shows a p phase shift, it sug- layer number reduces to between 1 and 2. For silicon, the im-
gests the conductivity of the stacked graphene is beyond the pedance matching sheet conductivity is calculated to be 6.42
impedance matching value. Specifically, 3-layer and 2-layer mS with nsilicon 3.42. Before doping, the average optical
graphene on quartz before and after doping, 7-layer and 5- sheet conductivities of 1, 3, 5, 7-layer graphene are about 1.0,
layer graphene on silicon before and after doping in experi- 1.5, 2.8, and 5.7 mS, and the ideal impedance matching con-
ments, are most approximative to the impedance matching dition cannot be reached even with layer number 7. After
condition, respectively. Thirdly, as proved in previous doping, the average optical sheet conductivities become
works,18,23,25 the chemical doping by HNO3 improves the around 1.8, 4.4, 7.1, and 11.7 mS and 5-layer graphene has
optical sheet conductivity of graphene on either quartz or sil- the optimized sheet conductivity as shown in Fig. 1.
icon. It leads to optimize impedance matching condition due We begin the discussion with the optical sheet conduc-
to the increasing conductivity. Lastly, as the refractive index tivity of N-layer graphene. In THz region where intraband
of quartz (nquartz 1.955) is much lower than the refractive transitions dominate, the optical conductivity of monolayer
index of silicon nsilicon 3.42, the impedance matching con- graphene follows a Drude model.14,15,26 In consideration of
dition is easier to achieve on quartz than on silicon. the carrier density dependence, the intraband conductivity
We define the amplitudes of the transmission through has a full description as follows:14
substrate and N-layer graphene/substrate for the m-th pulse     
m m
as ANlayer and Aref in frequency domain, which have a rela- 2e2 kB T EF EF
m
rg x 2 ln exp  exp ;
tionship with the transmission coefficients tm =tsub ph C  ix 2kB T 2kB T
m m
ANlayer =Aref . Combined with Eqs. (1)(3), optical sheet (5)
conductivity can be simplified from pulse 1:
where e and h are the elementary charge and Planck con-
0 1
1 stant. T and kB are the temperature and Boltzmann constant.
n1 n3 @ Aref
rtotal 1
 1A: (4) C and EF are the scattering rate and the Fermi energy. The
Z0 ANlayer Fermi energy is related to the carrier density Nc by
p
EF 6hvF pjNc j26 with negative (positive) corresponds to
The calculated THz sheet conductivity of graphene is shown hole (electron) doping. vF 1:1  106 m=s is the Fermi ve-
in Fig. 3, which is flat and featureless from 0.2 to 1.2 THz, locity. Room temperature T 300 K can be set to a constant.
consistent with the previous results.13,14,21 The nearly con- Therefore, the optical conductivity of monolayer graphene
stant THz conductivity leads to a broadband response as depends on the frequency, the quality of the sample (C), and
applications. For quartz, the impedance matching sheet con- the carrier density (or Fermi energy) as suggested in Eq. (5).
ductivity is calculated to be 2.53 mS with nquartz 1.955. With the same fabrication method, C can be expected to be
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 051106-4 Zhou et al.
constant. The conductivity is almost frequency independent
in THz frequency range. Therefore, the carrier density
becomes the key issue to tune the sheet conductivity with
graphene. However, although the electrons and holes can be
tuned up continuously in concentration as high as
1013 cm2,9 it still cannot match the requirement of imped-
ance matching with high refractive index substrate, such as
silicon. Therefore, stacked multilayer graphene combined
with chemical doping method is expected in order to opti-
mize the THz sheet conductivity.
It has been demonstrated that the THz wave absorption
of multilayer graphene has a strong dependence on the
stacking arrangements and misorientation angles between
N n1 Z0 rg n3 Z0 rg
rtotal M1  M2 expikg dgra M3  M4 expikg dgra 
M1 M2 expikg dgra M3 M4 expikg dgra 
M1  M2 expikg dgra  M3  M4 expikg dgra 
M1 M2 expikg dgra  M3 M4 expikg dgra 
p
where kg x eg =c is the propagating vector in graphene, and the coefficients M1 , M2 , M3 , and M4 have the following expres-
sion as follows:
0 !
Z0 rg
  B 1 p expikg dgra
B 2 eg
M1 M2
B
B
M3 M4 @ Z0 rg
 p expikg dgra
2 eg
We define the relative amplitude transmission for THz
m 1
pulse m as ANlayer =Aref . The theoretical calculated relative
amplitude with parameter C 100 cm1, combined with the
corresponding experimental data, is shown in Fig. 4. The ex-
perimental data at 0-layer in Fig. 4 represent the relative
amplitudes of pulse 2 for uncovered substrates. The close
matching of the experiments and theoretical calculation con-
firms the tunability of impedance matching with graphene
layer. For quartz, the relative amplitude transmission of
pulse 2 is 0.104. Before doping, the experimental data show
the relative amplitude transmission of pulse 2 can be sup-
pressed to 0.028 with 3-layer graphene and further reduced
to 0.013 with 4-layer one in theory. After doping, the relative
amplitude transmission of pulse 2 can be suppressed to
0.0025, a little higher than the theoretical calculated 0.017.
As suggested from Eq. (5), the Fermi energy drops from
0.11 to 0.25 eV after chemical doping. It also suggests
that the samples before chemical doping are also slightly
hole-doped by the substrate or the transfer process, which
has been confirmed in some previous works.14,15,26 For sili-
con, the relative amplitude of pulse 2 can reach 0.300.
Before doping, the ideal impedance matching condition
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Appl. Phys. Lett. 104, 051106 (2014)
layers.22 However, randomly stacked sample shows an elec-
tronically decoupling, which makes it behave like isolated
monolayer graphene.20 In THz regime, this conclusion has
been further testified by THz-TDS.21 The transmission coef-
ficient of multilayer graphene can be calculated with a
layer-by-layer model used in previous works,21,24 in which
the multilayer graphene is regarded as homogeneous dielec-
tric layer with a thickness N  1dgra . We assume all the
graphene layers have the same scattering rate and the same
Fermi energy for simplicity. Thus, the relationship between
the optical sheet conductivity of the N-layer (N > 1) sample
and the monolayer graphene can be obtained combined with
Eq. (1) as follows:
p
2Z0 eg
n1 Z0 rg
2Z0
n3 Z0 rg
2Z
p 0
eg n1 n3
 ; (6)
2Z0 Z0
1N2
Z0 rg
p expikg dgra C
2 eg C
!
C
C : (7)
Z0 rg A
1  p expikg dgra
2 eg
cannot be reached even with 7-layer graphene. After doping,
5-layer graphene can be used as antireflection layer with a
suppressed relative amplitude as low as 0.028. The Fermi
energy in the theoretical model from Eq. (5) also drops from
0.11 eV to 0.25 eV.
These results suggest the reflection properties of the
substrate can be changed by the layer number of graphene
and impedance matching can be achieved with suitable
layers. Furthermore, chemical doping is proved to be a good
solution to drive the Fermi level down, which will greatly
optimize impedance matching properties of graphene layer.
The combination provides a simple and effective method to
fabricate graphene-based broadband THz antireflection
coating. From Fig. 4, the decrease in main pulses in ampli-
tudes suggests that graphene still cannot overcome the draw-
back of absorption losses as observed in metallic layers.4,5
However, graphene is still superior than metal and semicon-
ductor as THz impedance matching layer. Due to the high
THz conductivity, graphene is more suitable for substrates
with high refractive index, when the impedance matching
layer might be too thick to fabricate with metal and semi-
conductor. Compared with metal,5 graphene also has
 051106-5 Zhou et al. Appl. Phys. Lett. 104, 051106 (2014)

Department (13JS101), National Key Basic Research Program

(2012CB723407, 2014CB339800), Research Fund for the
Doctoral Program of Higher Education (20106101110017,
20136101110007), International Cooperative Program
(201410780), and Program for Innovative Research Team of
Guilin University of Electronic Technology.

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