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Plasmonics in Graphene at Infrared Frequencyies
Plasmonics in Graphene at Infrared Frequencyies
FIG. 1. 共Color online兲 共a兲 Schematic description of a surface plasmon 共SP兲 on metal-dielectric interface. 共b兲 SP dispersion curve 共solid
blue line兲 for Ag-Si interfaces; dotted blue is the light line in Si; dashed red line denotes the SP resonance. 共c兲 Wave localization and
propagation length for SPs at Ag-Si interface 共experimental Ag losses are taken into account兲.
dielectric 关see Fig. 1共a兲兴; these are transverse magnetic 共TM兲 the Fermi energy. The band structure, calculated in the tight
modes accompanied by collective oscillations of surface binding approximation is shown in Fig. 2共b兲 共see Ref. 25 and
charges, which decay exponentially in the transverse direc- references therein兲; for low energies the dispersion around
tions 共see, e.g., Refs. 1 and 2 and references therein兲. Their the Dirac point can be expressed as En,k = nvFប兩k兩, where the
dispersion curve is given by Fermi velocity is vF = 106 m / s, n = 1 for conduction, and n
冑
= −1 for the valence band. Recent experiments32 have shown
⑀ r⑀ 共 兲 that this linear dispersion relation is still valid even up to the
qsp = 共1兲
c ⑀r + ⑀共兲 energies 共frequencies兲 of visible light, which includes the
regime we are interested in.
关see Fig. 1共b兲兴; note that close to the SP resonance Here, we consider TM modes in geometry depicted in Fig.
共 = SP兲, the SP wave vector 关solid blue line in Fig. 1共b兲兴 is 2共a兲, where graphene is surrounded with dielectrics of con-
much larger than the wave vector of the same frequency stants ⑀r1 and ⑀r2. Throughout the paper, for definiteness we
excitation in the bulk dielectric 关dotted blue line in Fig. use ⑀r1 = 4 corresponding to SiO2 substrate, and ⑀r2 = 1 for air
1共b兲兴. As a result, a localized SP wave packet can be much on top of graphene, which corresponds to a typical experi-
smaller than a same frequency wave packet in a dielectric. mental setup. TM modes are found by assuming that the
Moreover, this “shrinkage” is accompanied by a large trans- electric field has the form
verse localization of the plasmonic modes. These features are
considered very promising for enabling nanophotonics,1–4 as Ez = Aeiqz−Q1x, Ey = 0, Ex = Beiqz−Q1x, for x ⬎ 0,
well as high field localization and enhancement. A necessary
condition for the existence of SPs is ⑀共兲 ⬍ −⑀r 共i.e., ⑀共兲 is Ez = Ceiqz+Q2x, Ey = 0, Ex = Deiqz+Q2x, for x ⬍ 0.
negative兲, which is why metals are usually used. However, 共2兲
SPs in metals are known to have small propagation lengths,
which are conveniently quantified 共in terms of the SP wave- After inserting this ansatz into Maxwell’s equations and
length兲 with the ratio Rqsp / Iqsp; this quantity is a measure matching the boundary conditions 关which include the con-
of how many SP wavelengths can an SP propagate before it ductance of the 2D graphene layer, 共 , q兲兴, we obtain the
loses most of its energy. The wave localization 共or wave dispersion relation for TM modes:
“shrinkage”兲 is quantified as air / sp, where air = 2c / 共the ⑀r1 ⑀r2 共,q兲i
冑 冑
wavelength in air兲. These quantities are plotted in Fig. 1共c兲 + =− . 共3兲
for the case of Ag-Si interface, by using experimental data 2 ⑀r1 2
2 ⑀r2 2 ⑀0
q − 2 q − 2
共see Ref. 3 and references therein兲 to model silver 共metal c c
with the lowest losses for the frequencies of interest兲. Near
By explicitly writing the dependence of the conductivity on
the SP resonance, wave localization reaches its peak; how-
the wave vector q we allow for the possibility of nonlocal
ever, losses are very high there resulting in a small propaga-
effects, where the mean free path of electrons can be smaller
tion length l ⬇ 0.1sp ⬇ 5 nm. At higher wavelengths one can
than q−1.33 Throughout this work, we consider the nonre-
achieve low losses but at the expense of poor wave localiza-
tarded regime 共q Ⰷ / c兲, so Eq. 共3兲 simplifies to
tion.
⑀r1 + ⑀r2 2i
q ⬇ Q1 ⬇ Q2 ⬇ ⑀0 . 共4兲
III. PLASMONS AND THEIR LOSSES IN DOPED 2 共,q兲
GRAPHENE
Note that a small wavelength 共large q兲 leads to a high trans-
Graphene behaves as an essentially 2D electronic system. versal localization of the modes, which are also accompanied
In the absence of doping, conduction and valence bands meet by a collective surface charge oscillation, similar to SPs in
at a point 共called Dirac point兲 which is also the position of metals; however, it should be understood that, in contrast to
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PLASMONICS IN GRAPHENE AT INFRARED FREQUENCIES PHYSICAL REVIEW B 80, 245435 共2009兲
EF 1eV
z
y
FIG. 2. 共Color online兲 共a兲 Schematic of the graphene system and TM plasmon modes. Note that the profile of the fields looks the same
as the fields of an SP 关Fig. 1共a兲兴. 共b兲 Electronic band structure of graphene; to indicate the vertical scale we show the Fermi energy level for
the case EF = 1 eV. 共c兲 Sketch of the intraband 共green arrows兲 and interband 共red arrows兲 single particle excitations that can lead to large
losses; these losses can be avoided by implementing a sufficiently high doping. 共d兲 Plasmon RPA and semiclassical dispersion curves. Black
solid 共RPA兲 and black dot-dashed 共semiclassical兲 lines correspond to ⑀r1 = ⑀r2 = 1; Blue dashed 共RPA兲 and blue dotted 共semiclassical兲 lines
correspond to ⑀r1 = 4 and ⑀r2 = 1. The green 共lower兲 and rose 共upper兲 shaded areas represent regimes of intraband and interband excitations,
respectively.
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JABLAN, BULJAN, AND SOLJAČIĆ PHYSICAL REVIEW B 80, 245435 共2009兲
e2 ⑀r1 + ⑀r2 q
共q, 兲 = ⌸共q, 兲, 共8兲 ⑀RPA共q, 兲 = + 共q, 兲, 共11兲
q2 2 2⑀0
where
and
4 f共En2,k+q兲 − f共En1,k兲
⌸共q, 兲 = 兺
⍀ k,n1,n2 ប + En1,k − En2,k+q RPA共q, 兲 = − i共q, 兲. 共12兲
⫻兩具n1,k兩e−iq·r兩n2,k + q典兩2 . 共9兲 We note here that throughout the text only ––bands are
共E−EF兲/kBT taken into consideration; it is known that in graphite, higher
Here, f共E兲 = 共e −1
+ 1兲 is the Fermi distribution func-
––bands give rise to a small background dielectric
tion, EF is the Fermi energy and factor 4 stands for 2 spin
constant37 at low energies, which is straightforward to imple-
and 2 valley degeneracies. Note that in Eq. 共8兲 is given an
ment in the formalism. Using Eqs. 共4兲 and 共12兲 we obtain
infinitesimally small imaginary part which leads to the fa-
that the properties of plasmons 共i.e., dispersion, wave local-
mous Landau damping; that is, plasmons can decay by ex-
ization and losses兲 can be calculated by solving
citing an electron-hole pair 共interband and intraband scatter-
ing兲 as illustrated in Fig. 2共c兲. The effects of other types of
scattering 共impurities, phonons兲 can be accounted for by us- ⑀RPA共q, 兲 = 0, 共13兲
ing the relaxation-time as a parameter within the RPA-RT
approach,29 which takes into account conservation of local with complex wave vector q = q1 + iq2. The calculation is sim-
electron number. Within this approximation the 2D polariz- plified by linearizing Eq. 共13兲 in terms of small q2 / q1, to
ability is obtain,
1 1
I关⌸共q1, 兲兴 + R关⌸共q1, 兲兴 + R兵⌸共q1, 兲关1 − ⌸共q1, 兲/⌸共q1,0兲兴其
q2 = 共15兲
1
R关⌸共q1, 兲兴 − R关⌸共q1, 兲兴
q1 q1
yielding losses. Note that in the lowest order, the dispersion smaller than inter ⬇ 7.7 m, the system is in the regime of
relation 共and consequently air / p and the group velocity vg兲 high interband losses 共rose shaded region兲. Below the inter-
does not depend on . This linearization is valid when band threshold, both losses and wave localization obtained
q2 Ⰶ q1; as the plasmon losses increase, e.g., after entering by employing RPA-RT approach are quite well described by
the interband regime 关the rose area in Fig. 2共d兲兴, results from the previously obtained semiclassical formulas. Since the
Eqs. 共14兲 and 共15兲 should be regarded as only qualitative. frequencies below the interband threshold are 共for the as-
The characteristic shape of the plasmon dispersion is shown sumed doping level兲 also below the optical phonon fre-
in Fig. 2共d兲. Note that the semiclassical model and the RPA quency, the relaxation time can be estimated from DC mea-
model agree well if the system is sufficiently below the in- surements.
terband threshold 关for small q, 共q兲 ⬃ 冑q as in Eq. 共6兲兴. By At this point we also note that in all our calculations we
comparing Figs. 2共d兲 and 1共b兲 we see that the dispersion for have neglected the finite temperature effects, i.e., T ⬇ 0. To
SPs on silver-dielectric surface qualitatively differs from the justify this, we note that for doping values utilized in this
plasmon dispersion in graphene.34 While SPs’ dispersion re- paper the Fermi energies are 0.135 eV⬇ 5.2kBTr 共n = 1.35
lation approaches an asymptote 共 → SP兲 for large q values ⫻ 1012 cm−2兲 and 0.64 eV⬇ 25kBTr 共n = 3 ⫻ 1013 cm−2兲 for
关Eq. 共1兲兴, graphene plasmon relation gives 共q兲 which con- room temperature Tr = 300 K. The effect of finite tempera-
tinuously increases 关Fig. 2共d兲兴. ture is to slightly smear the sharpness of the interband
Theoretically predicted plasmon losses Rq / Iq and wave threshold, but only in the vicinity 共⬃kBTr兲 of the threshold.
localization air / p are illustrated in Fig. 3 for doping level By increasing the doping, EF increases, and the region of
EF = 0.135 eV and relaxation time = 1.35⫻ 10−13 s. We ob- interband plasmonic losses moves toward higher frequencies
serve that for this particular doping level, for wavelengths 共smaller wavelengths兲. However, by increasing the doping,
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PLASMONICS IN GRAPHENE AT INFRARED FREQUENCIES PHYSICAL REVIEW B 80, 245435 共2009兲
FIG. 3. 共Color online兲 Properties of plasmons in doped graphene. Solid-lines are obtained with the number-conserving RPA calculation,
and the dashed lines with the semiclassical approach. Losses 共a兲, field localization 共wave “shrinkage”兲 共b兲, and group velocity 共c兲 for doping
EF = 0.135 eV, and relaxation time = 1.35⫻ 10−13 s, which corresponds to the mobility of 10 000 cm2 / Vs. The upper scale in all figures
is frequency = / 2, whereas the rose shaded areas denote the region of high-interband losses.
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JABLAN, BULJAN, AND SOLJAČIĆ PHYSICAL REVIEW B 80, 245435 共2009兲
FIG. 5. 共Color online兲 Properties of plasmons in doped graphene. Solid-lines are obtained with the number-conserving RPA calculation,
and the dashed lines with the semiclassical approach. Losses 共a兲, field localization 共wave “shrinkage”兲 共b兲, and group velocity 共c兲 for doping
EF = 0.64 eV; losses are calculated by using the relaxation time −1 = DC−1
+ e−ph
−1
, where DC = 6.4⫻ 10−13 s, and e−ph is the relaxation time
from the electron-phonon coupling for the given parameters. In the white regions 共right regions in all panels兲, losses are determined by DC.
In the yellow shaded regions 共central regions in all panels兲, losses are determined by the optical phonon emission, i.e., e−ph. The rose shaded
areas 共left region in all panels兲 denote the region of high interband losses. Dotted vertical lines correspond to the optical phonon frequency
Oph ⬇ 0.2 eV. The upper scale in all figures is frequency = / 2. See text for details.
order of 10−14 – 10−13 s, indicating that optical phonons are acoustic phonons 共this decay channel is open at all frequen-
an important decay mechanism. cies兲; such a calculation would not affect losses for
It should be emphasized that the exact calculated values ⬎ Oph where optical phonons are dominant.
should be taken with some reservation for the following rea-
son: strictly speaking, one should calculate the relaxation IV. CONCLUSION AND OUTLOOK
times 共 , q兲 along the plasmon dispersion curve given by
Eq. 共14兲; namely the matrix elements which enter the calcu- In conclusion, we have used RPA and number-conserving
lation depend on q, whereas the phase space available for the relaxation-time approximation with experimentally available
excitations also differ for q = 0 and q ⬎ 0. Moreover, the ex- input parameters, and theoretical estimates for the relaxation-
act value of the matrix element for electron phonon coupling time utilizing electron-phonon coupling, to study plasmons
is still a matter of debate in the community 共e.g., see Ref. and their losses in doped graphene. We have shown that for
39兲. Therefore, the actual values for plasmon losses could be sufficiently large doping values high wave localization and
somewhat different for ⬎ Oph. Nevertheless, fairly small low losses are simultaneously possible for frequencies below
values of relaxation times presented in Fig. 4 for ⬎ Oph that of the optical phonon branch ⬍ Oph 共i.e., Eplasmon
indicate that emission of an optical phonon together with an ⬍ 0.2 eV兲. For sufficiently large doping values, there is an
electron-hole pair is an important decay mechanism in this interval of frequencies above Oph and below interband
regime. Precise calculations for q ⬎ 0 and ⬎ Oph are a threshold, where an important decay mechanism for plas-
topic for a future paper. mons is excitation of an electron-hole pair together with an
Plasmonic losses and wave localization calculated from optical phonon 共for ⬍ Oph this decay channel is inactive兲;
the RPA-RT approximation are illustrated in Fig. 5 for dop- the relaxation times for this channel were estimated and dis-
ing level EF = 0.64 eV and the relaxation time given by cussed. We point out that further more precise calculations of
−1 = DC
−1
+ e−ph
−1
, where DC = 6.4⫻ 10−13 s 共mobility plasmon relaxation times should include coupling to the sub-
10000 cm2 / Vs兲, whereas e−ph is frequency dependent and strate 共e.g., coupling to surface-plasmon polaritons of the
corresponds to electron-phonon coupling assuming very substrate兲, a more precise shape of the phonon dispersion
clean samples 关see dashed line in Fig. 4共b兲兴. Interband losses curves,28 and dependence of the relaxation time via electron-
关left 共rose shaded兲 regions in all panels兴 are active for wave- phonon coupling on q ⬎ 0 共see Sec. III C兲.
lengths smaller than inter ⬇ 1.7 m. In the frequency inter- The main results, shown in Figs. 3 and 5 point out some
val inter ⬎ ⬎ Oph 关central 共yellow shaded兲 regions in all intriguing opportunities offered by plasmons in graphene for
panels兴, the decay mechanism via electron phonon coupling the field of nanophotonics and metamaterials in infrared 共i.e.,
determines the loss rate, i.e., ⬇ e−ph. For ⬍ Oph 关right for ⬍ Oph兲. For example, we can see in those figures that
共white兲 regions in all panels兴, the DC relaxation time DC can high field localization and enhancement air / p ⬃ 200 关see
be used to estimate plasmon losses. Fig. 3共b兲兴 are possible 共resulting in p ⬍ 50 nm兲, while plas-
It should be noted that the mobility of 10000 cm2 / Vs mons of this kind could have propagation loss-lengths as
could be improved, likely even up to mobility long as ⬃10 p 关see Fig. 5共a兲兴; these values 共albeit at differ-
100 000 cm2 / Vs,13 thereby further improving plasmon ent frequencies兲 are substantially more favorable than the
propagation lengths for frequencies below the optical phonon corresponding values for conventional SPs, for example, for
frequency. However, for these larger mobilities the calcula- SPs at the Ag/Si interface air / p ⬃ 20, whereas propagation
tion of losses should also include in more details the fre- lengths are only ⬃0.1sp 关see Fig. 1共c兲兴. Another interesting
quency dependent contribution to the relaxation time from feature of plasmons in graphene is that, similar to usual
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PLASMONICS IN GRAPHENE AT INFRARED FREQUENCIES PHYSICAL REVIEW B 80, 245435 共2009兲
SP-systems,4 wave localization is followed by a group veloc- ulos, Pablo Jarillo-Herrero, Tony Heinz, Vladimir Shalaev,
ity decrease; the group velocities can be of the order vg Thomas Ebbesen, Ivan Kupčić, Antonio Šiber, Branko Gum-
= 10−3 – 10−2 c, and the group velocity can be low over a halter, Tobias Stauber, and Ivo Batistić, for many helpful
wide frequency range, as depicted in Figs. 3共c兲 and 5共c兲. This comments. This work was supported in part by the Croatian
is of interest for possible implementation of novel nonlinear Ministry of Science under Grant No. 119-0000000-1015.
optical devices in graphene, since it is known that small This work was also supported in part by the MRSEC pro-
group velocities can lead to savings in both the device length gram of National Science Foundation under Award No.
and the operational power;40 the latter would also be reduced DMR-0819762, in part by the U.S. Army Research Office
because of the large transversal field localization of the plas- through the institute of soldier nanotechnologies under Con-
mon modes. tract No. W911NF-07-D-0004, and also in part by the U.S.
Department of Energy office of science, office of basic en-
ACKNOWLEDGMENTS
ergy sciences, through S3TEC, which is a DOE energy fron-
We would like to thank Leonid Levitov, J. D. Joannopo- tier research center.
*mjablan@phy.hr 21
B. Wunsch, T. Sauber, F. Sols, and F. Guinea, New J. Phys. 8,
†
hbuljan@phy.hr 318 共2006兲.
‡soljacic@mit.edu 22 E. H. Hwang and S. Das Sarma, Phys. Rev. B 75, 205418
1 W. L. Barnes, A. Dereux, and T. W. Ebbesen, Nature 共London兲
共2007兲.
424, 824 共2003兲. 23 S. A. Mikhailov and K. Ziegler, Phys. Rev. Lett. 99, 016803
2 S. A. Maier and H. A. Atwater, J. Appl. Phys. 98, 011101
共2007兲.
共2005兲. 24
L. A. Falkovsky and S. S. Pershoguba, Phys. Rev. B 76, 153410
3 S. Vedantam, H. Lee, J. Tang, J. Conway, M. Staffaroni, and E.
共2007兲.
Yablonovitch, Nano Lett. 9, 3447 共2009兲. 25
A. Bostwick, T. Ohta, T. Seyller, K. Horn, and E. Rotenberg,
4 A. Karalis, E. Lidorikis, M. Ibanescu, J. D. Joannopoulos, and
Nat. Phys. 3, 36 共2007兲.
M. Soljačić, Phys. Rev. Lett. 95, 063901 共2005兲. 26
V. Ryzhii, A. Satou, and T. Otsuji, J. Appl. Phys. 101, 024509
5 V. G. Veselago, Sov. Phys. Usp. 10, 509 共1968兲.
共2007兲.
6 V. M. Shalaev, Nat. Photonics 1, 41 共2007兲. 27 S. Gangadharaiah, A. M. Farid, and E. G. Mishchenko, Phys.
7
J. B. Pendry, Phys. Rev. Lett. 85, 3966 共2000兲. Rev. Lett. 100, 166802 共2008兲.
8 D. R. Smith, J. B. Pendry, and M. C. K. Wiltshire, Science 305, 28 For simplicity here we assume Einstein model for optical
788 共2004兲. phonons, and assume that they form a branch at 0.2 eV. More
9 K. S. Novoselov, A. K. Geim, S. V. Morozov, D. Jiang, Y.
precisely one should take into account that electrons interact
Zhang, S. V. Dubonos, I. V. Grigorieva, and A. A. Firsov, Sci- with zone center phonons at ប⍀⌫ = 0.196 eV 共intravalley scat-
ence 306, 666 共2004兲. tering兲 and zone boundary phonons at ប⍀K = 0.161 eV 共interval-
10
K. S. Novoselov, D. Jiang, F. Schedin, T. J. Booth, V. V. Khot- ley scattering兲.
29 N. D. Mermin, Phys. Rev. B 1, 2362 共1970兲.
kevich, S. V. Morozov, and A. K. Geim, Proc. Natl. Acad. Sci.
U.S.A. 102, 10451 共2005兲. 30 Ch.-H. Park, F. Giustino, M. L. Cohen, and S. G. Louie, Phys.
11 K. S. Novoselov, A. K. Geim, S. V. Morozov, D. Jiang, M. I.
Rev. Lett. 99, 086804 共2007兲.
31
Katsnelson, I. V. Grigorieva, S. V. Dubonos, and A. A. Firsov, T. Stauber and N. M. R. Peres, J. Phys.: Condens. Matter 20,
Nature 共London兲 438, 197 共2005兲. 055002 共2008兲; see also T. Stauber, N. M. R. Peres, and A. H.
12 Y. Zhang, Y. W. Tan, H. L. Stormer, and P. Kim, Nature 共Lon-
Castro-Neto, Phys. Rev. B 78, 085418 共2008兲.
don兲 438, 201 共2005兲. 32
R. R. Nair, P. Blake, A. N. Grigorenko, K. S. Novoselov, T. J.
13 A. K. Geim and K. S. Novoselov, Nature Mater. 6, 183 共2007兲.
Booth, T. Stauber, N. M. R. Peres, and A. K. Geim, Science
14
C. Berger, Z. Song, T. Li, X. Li, A. Y. Ogbazghi, R. Feng, Z. 320, 1308 共2008兲.
33 N. W. Ashcroft and N. D. Mermin, Solid State Physics 共Saun-
Dai, A. N. Marchenkov, E. H. Conrad, P. N. First, and W. A. de
Heer, J. Phys. Chem. B 108, 19912 共2004兲. ders, Philadelphia, PA, 1976兲.
15 C. Berger, Z. Song, X. Li, X. Wu, N. Brown, C. Naud, D. 34 W. H. Backes, F. M. Peeters, F. Brosens, and J. T. Devreese,
Mayou, T. Li, J. Hass, A. N. Marchenkov, E. H. Conrad, P. N. Phys. Rev. B 45, 8437 共1992兲.
First, and W. A. de Heer, Science 312, 1191 共2006兲. 35 G. W. Hanson, J. Appl. Phys. 104, 084314 共2008兲.
16
F. Wang, Y. Zhang, Ch. Tian, C. Girit, Alex Zettl, M. Crommie, 36
F. Stern, Phys. Rev. Lett. 18, 546 共1967兲.
and Y. R. Shen, Science 320, 206 共2008兲. 37 E. A. Taft and H. R. Philipp, Phys. Rev. 138, A197 共1965兲.
17 Z. Q. Li, E. A. Henriksen, Z. Jiang, Z. Hao, M. C. Martin, P. 38 K.-F. Mak, M. Y. Sfeir, Y. Wu, C.-H. Lui, J. A. Misewich, and T.
Kim, H. L. Stormer, and D. N. Basov, Nat. Phys. 4, 532 共2008兲. F. Heinz, Phys. Rev. Lett. 101, 196405 共2008兲.
18
O. Vafek, Phys. Rev. Lett. 97, 266406 共2006兲. 39
J. L. McChesney, A. Bostwick, T. Ohta, K. Emtsev, Th. Seyller,
19 V. Ryzhii, M. Ryzhii, and T. Otsuji, J. Appl. Phys. 101, 083114
K. Horn, and E. Rotenberg, arXiv:0809.4046 共unpublished兲.
共2007兲. 40
M. Soljačić and J. D. Joannopoulos, Nature Mater. 3, 211
20 F. Rana, IEEE Trans. NanoTechnol. 7, 91 共2008兲.
共2004兲.
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