PHYSICAL REVIEW B 76, 153410 共2007兲

Optical far-infrared properties of a graphene monolayer and multilayer

L. A. Falkovsky1,2 and S. S. Pershoguba3,4

1L.D.Landau Institute for Theoretical Physics, Moscow 117334, Russia
2Institute
of the High Pressure Physics, Troitsk 142190, Russia
3
Moscow Institute of Physics and Technology, Dolgoprudniy 147100, Russia
4G.V. Kurdyumov Institute for Metal Physics, Kyiv 03142, Ukraine

共Received 10 July 2007; revised manuscript received 20 September 2007; published 31 October 2007兲
We analyze the features of the graphene mono- and multilayer reflectance in the far-infrared region as a
function of frequency, temperature, and carrier density taking the intraband conductance and the interband
electron absorption into account. The dispersion of plasmon mode of the multilayers is calculated using
Maxwell’s equations with the influence of retardation included. At low temperatures and high electron densi-
ties, the reflectance of multilayers as a function of frequency has the sharp downfall and the subsequent deep
well due to the threshold of electron interband absorption and plasmon excitations.

DOI: 10.1103/PhysRevB.76.153410 PACS number共s兲: 81.05.Uw, 78.67.Ch, 78.67.Pt, 78.66.⫺w

Monolayer and bilayer graphenes1–3 are gapless two-
dimensional 共2D兲 semiconductors4–6 whereas its three-
dimensional 共3D兲 predecessor, graphite, is a semimetal.7–9
Hence, the dimensionality effects for the unique substance
can be studied.10 Monolayer graphene has a very simple
electron band structure. Near the energy ␧ = 0, the energy
bands are cones ␧1,2共p兲 = ± v p at the K points in the 2D Bril-
obtained in our previous paper18 and is valid under a restric-
tion that the collision rate of carriers is less than the fre-
quency and spatial dispersion of the electric ac field, ␶−1
Ⰶ ␻ , kv. In limiting cases, our result coincides with the for-
mulas of Ref. 24. For high frequencies, when one can also
ignore the spatial dispersion of the ac field, ␻ Ⰷ kv , ␶−1, the
complex conductivity 关see Eq. 共8兲 in Ref. 18兴 is given by

冋冕 册
louin zone with the constant velocity parameter v
= 108 cm/ s. Such a degeneration is conditioned by symmetry
because the small group C3v of the K points has a two-
dimensional representation.
␴共␻兲 =
e 2␻
i␲ប −⬁
+⬁
d␧
兩␧兩 df 0共␧兲
␻2 d␧
− 冕
0
+⬁
d␧
f 0共− ␧兲 − f 0共␧兲
共␻ + i␦兲2 − 4␧2
.

While the carrier concentration decreases in the field gate 共1兲

experiment, the graphene conductivity at low temperatures
goes to the finite minimal values.1,2 Much theoretical Here, the first term corresponds to the intraband electron-
efforts11–14 have been devoted to evaluate the minimal con- photon scattering processes. One can obtain it from the
ductivity in different approaches. Theoretical15–17 and experi- Drude-Boltzmann expression 共for a case 1 / ␶ = 0兲 and write
mental researches show that the main mechanism of the car- explicitly
rier relaxation is provided by the charged impurities and
gives the collision rate ␶−1 ⬃ 2␲2e4nimp / ប⑀2g␧, where ⑀g is the 2e2T
dielectric constant of graphene, ␧ is the characteristic elec- ␴intra共␻兲 = i ln关2 cosh共␮/2T兲兴. 共2兲
␲ប␻
tron energy 共of the order of the Fermi energy or tempera-
ture兲, and nimp is the density of charged impurities per unit
The second term in Eq. 共1兲, where ␦ → 0 is the infinitesimal
surface. Plasmons in graphene are considered in Refs.
quantity determining the bypass around the integrand pole,
18–20; surface wave propagation along graphene located at
owes its origin to the direct interband electron transitions.
interfaces between two dielectrics is studied in Ref. 21. The
The real part of this contribution is reduced to the expression
optical visibility of both monolayer and bilayer graphene is
for the absorbed energy due to the interband transitions.
studied in Ref. 22 focusing on the role of the underlying
Since there is no gap between the conduction band and va-
substrate.
lence band, these two terms can compete and the interband
In the present Brief Report, we analyze the spectroscopy
contribution becomes larger at high frequencies ␻ ⬎ T , ␮. In
of the graphene monolayer and multilayers in the infrared
the opposite case, the intraband contribution plays the lead-
region. In order to calculate the reflection coefficient for the
ing role.
multilayers, we follow the method used in Ref. 23 and de-
The difference of the Fermi functions in the second inte-
termine the spectrum of electromagnetic excitations—
grand equals
plasmons. We use the appropriate boundary conditions at in-
terfaces and the complex conductivity ␴ as a function of
frequency ␻, temperature T, and chemical potential ␮. The sinh共␧/T兲
G共␧兲 = .
chemical potential of ideal pure graphene equals zero at any cosh共␮/T兲 + cosh共␧/T兲
temperature. With the help of the gate voltage, one can con-
trol the density and type 共n or p兲 of carriers varying their Extracting the principal value of the integral, we arrive at the
chemical potential. integral without singularities and write the interband conduc-
The general expression for the conductivity used here is tivity in the form available for numerical calculations,

1098-0121/2007/76共15兲/153410共4兲 153410-1 ©2007 The American Physical Society

BRIEF REPORTS PHYSICAL REVIEW B 76, 153410 共2007兲

500 current j has only the in-layer x component 关see Fig. 1共b兲兴.
(a) (b) 共i兲 Optics of a monolayer. Consider the graphene mono-
400 layer at z = 0 with ⑀0 = ⑀g deposited on the substrate 共z ⬎ 0兲
Chemical potential (K)
with the dielectric constant ⑀0 = ⑀s. In the vacuum, z ⬍ 0, the
300 ac field is given by the sum of incident and reflected waves
11 −2
n0 = 10 cm and by the transmitted wave in the substrate. In the geometry
x
200 considered, the current in the graphene monolayer can be
10 −2 written in the form
10 cm d
100
jx = ␴␦共z兲Ex . 共8兲
9 −2 z
10 cm
0
50 150 250
Making use of the Fourier transformations with respect to
Temperature (K) the x coordinate, E ⬀ eikxx, we rewrite the Maxwell equations
关Eq. 共7兲兴 as follows:
FIG. 1. 共Color online兲 共a兲 Chemical potential 共in K兲 as a func-
tion of temperature at carrier densities noted at curves. 共b兲 dEz d2Ex ␻2 4␲i␻
ikx − 2 − ⑀0 2 Ex = jx ,
Multilayer sample and geometry of wave scattering. dz dz c c2

␴ 共␻兲 =
inter e2
4ប
G共␻/2兲 −
4␻
i␲ 冋 冕 0
+⬁
d␧
G共␧兲 − G共␻/2兲
␻2 − 4␧2
.册 ikx
dEx
dz
冉 ␻2
+ k2x − ⑀0 2 Ez = 0.
c
冊 共9兲

共3兲 The boundary conditions for these equations at z = 0 are

the continuity of the field component Ex and the jump of the
Here, the first term is given asymptotically by electric-induction z component ⑀Ez at the sides of the mono-

G共␻/2兲 = 再 tanh共␻/4T兲, ␮ Ⰶ T
␪共␻ − 2␮兲, ␮ Ⰷ T,
冎 共4兲
layer,

⑀s兩Ez兩z=+0 − 兩Ez兩z=−0 = 4␲ 冕 +0
␳共␻,kx,z兲dz. 共10兲
where the step function ␪共␻ − 2␮兲 expresses the condition for −0

the interband electron transitions at low temperatures. The The carrier density is connected to the current in Eq. 共8兲
integral in Eq. 共3兲 represents the imaginary interband correc- according to the continuity equation
tion to the intraband conductivity. With the help of Eq. 共4兲,
we find for low temperatures 共T Ⰶ ␮兲 ␳共␻,kx,z兲 = jx共␻,kx,z兲kx/␻ .

␴inter共␻兲 =
e2
冋
␪共␻ − 2␮兲 −
i
ln
共␻ + 2␮兲2
2␲ 共␻ − 2␮兲2 + 共2T兲2
. 册 Substituting Ez from the second equation in Eq. 共9兲 into Eq.
共10兲, we find the second boundary condition

冏 冏 冏 冏 冏 冏
4ប
共5兲 ⑀s dEx 1 dEx 4␲␴共␻兲
− = Ex ,
ks2 dz z=+0 共kzi兲2 dz z=−0 i␻ z=0
This expression shows that the interband contribution plays
the leading role comparatively with the intraband term 共11兲
around the absorption threshold ␻ ⯝ 2␮, where the logarith-
where ks = 冑⑀s共␻ / c兲2 − k2x , kzi = 冑共␻ / c兲2 − k2x .
mic singularity is cut off with temperature 共or scattering rate
Using the boundary conditions, we find the reflection am-
while considered兲.
plitude
By using the gate voltage, one can control the density of
electrons 共n0兲 or holes 共−n0兲. Then, the chemical potential is 1−C
determined by the condition r= , 共12兲
1+C

n0 =
2
␲共បv兲2
冕 0
+⬁
␧关f 0共␧ − ␮兲 − f 0共␧ + ␮兲兴d␧. 共6兲 where C = kzi关4␲␴共␻兲 / ␻ + 共⑀s / ks兲兴.
The reflection coefficient 兩r兩2 calculated with the help of
Eqs. 共1兲–共6兲 and 共12兲 for normal incidence is shown in Figs.
From this expression and Fig. 1共a兲, one can see that the 2 and 3 as a function of frequency, temperature, and carrier
chemical potential goes to zero while the temperature in- concentration. Notice that the carriers have a pronounced
creases. 共intraband兲 effect on reflectance only at low frequencies
In order to calculate the graphene reflectance, we apply where the dimensionless parameter e2 max共T , ␮兲 / បc␻ is of
Maxwell’s equations the order of unity. With increasing temperature, the carriers
␻2 4␲i␻ occupy a more expanded energy interval, but the chemical
ⵜ共ⵜ · E兲 − ⵜ2E = ⑀0 2E+ j, 共7兲 potential decreases. This results in the nonmonotonic behav-
c c2
ior of reflectance as a function of temperature shown in Fig.
where ⑀0 is the ion contribution into the dielectric constant 3.
and j is the conductivity current. We consider the case of the The optical properties of the graphene bilayer can be con-
p polarization, when the field E lies in the xz plane and the sidered in a similar way. Here, we do not present the corre-

153410-2
BRIEF REPORTS PHYSICAL REVIEW B 76, 153410 共2007兲

1 1 1 1
8
n0=10 cm
−2 10 −2 graphene multilayers
0.9 0.9 10 cm
0.8 0.8 n =10 10
cm −2
0.8 1011 cm−2
0
Reflection coefficient

0.8

Reflection coefficient
0.7 T=300 K 0.7 300 K 50 K 200 K
0.6 100 K 0.6 100 K 300 K 0.6

0.5 10 K 0.5 10 K 0.6 10 K

0.4 0.4 0.4
50 K
0.3 0.3 10 K
0.4
0.2 0.2 0.2

0.1 0.1

0 0 0.2 0
0 5 10 0 10 20 0 2.5 5 7.5 10 0 0.5 1 1.5 2
Frequency (K) Frequency (K) Frequency (103 K)

FIG. 2. 共Color online兲 Reflectance from the graphene monolayer FIG. 4. 共Color online兲 Reflectance from the graphene monolayer
with carrier densities n0 = 108 cm−2 共left兲 and n0 = 1010 cm−2 共right兲 with the carrier density n0 = 1010 cm−2 共left兲 and multilayers with
versus the frequency at temperatures noted at the curves: normal n0 = 1011 cm−2 in a layer and distance d = 3 Å between layers 共right兲;
incidence. temperatures are noted at curves and the incidence angle is 80°.

sponding results, and we investigate another 3D example—

e1,2共z兲 = e±ikznd兵sin ks共z − nd兲 − e⫿ikzd sin ks关z − 共n + 1兲d兴其,
the graphene multilayers.
共ii兲 Spectroscopy of graphene multilayers. Let the multi- nd ⬍ z ⬍ 共n + 1兲d, 共14兲
layers cross the z axis at points zn = nd, where d is the dis-
with the quasimomentum kz determined from the dispersion
tance between the layers 关see Fig. 1共b兲兴. Such a system can
equation
be considered as a model of graphite since the distance d
= 3 Å in graphite is larger than the interatomic distance in the cos kzd = cos ksd − D sin ksd. 共15兲
layer. So, we describe the carrier interaction in the presence
of ac electric field with the help of self-consistent Maxwell’s The dispersion equation describes the electric field excita-
equations 关Eq. 共7兲兴. For the x component of the field Ex, they tions of the system, i.e., plasmons. The quasimomentum kz
give can be restricted to the Brillouin half-zone 0 ⬍ kz ⬍ ␲ / d, if
the parameter D is real. In the general case, while taking the

冋 d2
dz2
+ ks2 + 2ksD 兺 ␦共z − nd兲 Ex = 0,
n
册 共13兲
interband absorption into account, we fix the choice of the
eigenfunctions in Eq. 共14兲 by the condition Im kz ⬎ 0 so that
the solution e1 decreases in the positive direction z. In the
where D = 2i␲␴共␻兲ks / ⑀g␻ and ks = 冑⑀g共␻ / c兲2 − k2x . long-wave approximation, kz , ks Ⰶ 1 / d, the dispersion equa-
tion 关Eq. 共15兲兴 takes the form
For the infinite number of layers in the stack, the solutions
of Eq. 共13兲 represent two Bloch states kz2 ␴共␻兲
= 1 + 4␲i . 共16兲
ks2 ␻ ⑀ gd
1 1
9 −2
0.9
n =10 cm
0 0.9
n =1010 cm−2 Reflectance from the multilayers that occupied the semi-
0
space z ⬎ 0 can be calculated similarly to the reflectance of a
0.8 0.8
monolayer. The electric field is given by the decreasing so-
Reflection coefficient

0.7 ω=1 K 0.7 ω=1 K lution e1 inside the sample and by the sum of incident and
0.6 0.6 reflected waves in the vacuum, z ⬍ 0, with the same value of
0.5 0.5
the component kx.
Using the boundary condition, Eq. 共11兲, with the dielectric
0.4 ω=5 K 0.4 ω=5 K constant of graphene ␧g instead of ␧s, we find the reflected
0.3 0.3 amplitude
0.2 0.2
ω=30 K ω=30 K i sin共ksd兲 − Z
0.1 0.1 r= ,
i sin共ksd兲 + Z
0 0
0 100 200 300 0 100 200 300
Temperature (K) where
kzi
FIG. 3. 共Color online兲 Reflectance from the graphene monolayer Z = ⑀g 关cos共ksd兲 − e−ikzd兴,
ks
with carrier concentrations n0 = 109 cm−2 共left兲 and 1010 cm−2
共right兲 versus temperature for frequencies noted at curves: normal kzi is the normal component of wave vector in the vacuum,
incidence. and kz is the quasimomentum determined by the dispersion

153410-3
BRIEF REPORTS
equation 关Eq. 共15兲兴 at fixed values of ␻ and kx.
In Fig. 4, the reflection coefficient calculated for multilay-
ers is shown in comparison with the reflection coefficient of
the monolayer. The left panel in this figure differs from the
right one in Fig. 2 only in the incidence angle, which is now
taken to be 80° in order to emphasize the multilayer features.
The main of them is the sharp downfall of reflectance at low
temperatures 共see the right panel in Fig. 4兲. This is the
threshold effect of the direct interband transitions at ␻ 艌 2␮,
which is sharp when temperature T → 0 关see Eq. 共4兲兴. Just at
the downfall, the reflectance has the deep well which disap-
pears while the temperature increases. This is an effect of
plasmon excitations. As one can see from Eq. 共16兲, the plas-
mon excitations with the real kz are possible if the imaginary
part of conductivity is negative. This can be realized if the
interband contribution described by the second term in Eq.
共5兲 is larger than the intraband term. Contrary to the mono-
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153410-4
PHYSICAL REVIEW B 76, 153410 共2007兲
layer, the peculiarities of reflectance from multilayers take
place at larger frequencies ␻ ⯝ 2␮ because they are governed
by the dimensionless parameter 共e2 / ប⑀g␮d兲ln共␮ / kBT兲, where
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In conclusion, we have developed the detailed micro-
scopic theory of the graphene mono- and multilayer spec-
troscopy. We have shown that the nonmonotonic temperature
behavior of reflectance from the monolayer in the infrared
region is expected. We have argued that at low temperatures
and high electron densities, the reflectance from multilayers
has the sharp downfall with the subsequent deep well. They
are caused by the direct interband electron transitions.
This work was supported by the Russian Foundation for
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