Escolar Documentos
Profissional Documentos
Cultura Documentos
Nicolas Bonod,1,* Alexis Devilez,1 Brice Rolly,1 Sebastien Bidault,2 and Brian Stout1
1InstitutFresnel, CNRS UMR 6133, Ecole Centrale Marseille, Aix-Marseille Université,
Domaine Universitaire de Saint Jérôme, 13397 Marseille, France
2Institut Langevin, CNRS UMR 7587, ESPCI ParisTech, 10 rue Vauquelin, 75231 Paris Cedex 05, France
I. INTRODUCTION nantly in only one half space and can thus be characterized
as unidirectional.
Metallic nanostructures are key elements in the control of This paper is dedicated to studying how nearby spherical
light interaction with quantum emitters. They can both focus nanoparticles modify the angular distribution of light emitted
light in tiny volumes and enhance the radiative decay rates of by an oscillating dipole. In particular, we provide a thorough
nearby emitters.1–9 The latter property has been thoroughly study of the phase differences between the dipolar source
studied in the case of a single emitter coupled to a single and the dipolar mode induced in the particle. We emphasize
nanoparticle.10–20 It has been shown that the radiative decay that these phase differences must take into account the opti-
rates depend strongly on the distance between the emitter cal path between the emitter and the particle in addition to
and the nanoparticle. Furthermore, at very short distances the polarizability of the particle. We show that by tuning the
from the surfaces 共a few nanometers兲, nonradiative decay position of a single emitter from a single nanoparticle by a
channels dominate and the quantum efficiency drops. The few tens of nanometers, we can sufficiently modify the
coupling efficiency between emitters and optical antennas dephasing to control the reflective or collective properties of
also depends on the orientation of the dipolar source with the particle at a given frequency. When the phase difference
respect to the dipolar modes supported by the metallic par- between the exciting and induced dipoles is strictly equal to
ticles. A longitudinal-coupling geometry significantly en- , an equal part of the energy is radiated into each of the half
hances the emission decay rates while a transverse interac- spaces surrounding the emitter 共the separation plane being
tion leads to moderate enhancements.19–22 perpendicular to the axis containing the dipoles兲. We then
More recently, the ability of nanoantennas to control the apply these results to the design of highly unidirectional an-
angular emission of single molecules has been tennas composed of two nanospheres separated by a mere 50
investigated.23–25 This possibility is particularly important or 60 nm. The basic concept is similar to the idea underlying
since a high directivity facilitates both the excitation of a the design of Yagi-Uda optical antennas, which associate the
quantum emitter by a collimated beam as well as the collec- collective and reflective properties of nanoparticles27,28 but at
tion of the radiated light.26 Yagi-Uda antennas have been much smaller interparticle distances and in simpler geom-
successfully introduced at optical frequencies27,28 and their etries. Taking into account the phase lag induced by the dis-
high angular directivity has recently been confirmed tance between the emitter and the nanoparticle, highly direc-
experimentally.29 This antenna geometry combines a director tional antennas can be designed with only two nanoparticles.
element generally consisting of a finite chain of identical We will first emphasize the role of the distance between the
particles and a reflector element typically based on a slightly emitter and the nanoparticles by designing a directional an-
larger particle.30,31 A dipolar emitter can be coupled longitu- tenna composed of identical particles, i.e., with strictly iden-
dinally to the antenna by utilizing a nanoparticle located near tical polarizabilities. Furthermore, by tuning the relative size
the reflector element.32 In this configuration, the emitter is of the two particles, it is possible to design an antenna
off-axis. For an on-axis emitter, the weak transverse coupling smaller than / 2 that channels light radiated by a single
with the chain of particles can be reinforced by employing emitter in the angular aperture of commercial microscope
the so-called “super emitter”consisting of a dimer of nano- objectives.33
particles perpendicular to chain axis.12,31 Pakizeh and Kall32
have recently proposed an ultracompact antenna made of two II. RADIATION PROPERTIES OF A DIPOLAR EMITTER
identical metallic particles. The dipolar emitter is then COUPLED TO A SINGLE NANOPARTICLE
coupled to a dark mode characterized by opposite phase di-
polar modes induced in the two neighboring particles. In that We first investigate the radiation pattern of a single emit-
case, it has been shown that the emitter radiates predomi- ter located near a single 90 nm silver particle. The dipolar
z 90
z 1.0 120 60
0.8
Dipolar 0.6 150
emitter θ 30
r 0.4
x 0.2
y 0.0 180 0
0.2
x1= (-d-R)/2 x2= (d+R)/2 ϕ 0.4
1.3π 1.0 0.6 210 330
x 1.0π 0.8
0.9
0.8π 1.0 240 300
Reflected efficiency
2R d 0.5π 0.8 270
(a) (b)
0.3π 0.7 (b)
0.0π
∆Φ
90
0.6
FIG. 1. 共a兲 Sketch of a dipolar emitter oriented along the z axis -0.3π
0.5
1.0 120 60
-0.5π 0.8
and located at a distance d from the surface of a silver nanosphere. -0.8π 0.4 0.6 150 30
-1.0π 0.4
The refractive index of silver is taken from Ref. 37. Silver nano- -1.3π
0.3
0.2
spheres are embedded in a polymer of refractive index 1.5. 共b兲 The 0.3 0.4 0.5 0.6 0.7 0.8 0.9
0.0 180 0
λ (µm)
spherical coordinates used in the analytical expressions. 0.2
(a) 0.4
0.6 210 330
emitter is polarized along the z axis in order to provide a 0.8
1.0
transverse coupling with the nanoparticle as sketched in Fig. 240
270
300
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ULTRACOMPACT AND UNIDIRECTIONAL METALLIC ANTENNAS PHYSICAL REVIEW B 82, 115429 共2010兲
100 100
the nanoparticle reflects with a rather high efficiency the ra- 1
0.9 14
13
diated light since R reaches 90% at = 510 nm. 80
0.8
0.6 80 12
11
0.5 11
The emission pattern of the light radiated by the exciting 60
0.4
0.3 60
9.7
8.8
0.1
dipole at = 510 nm is reconstructed in Fig. 2共b兲 by plotting 7.9
d (nm)
1.0
d (nm)
0 7.1
-0.1 6.2
40 -0.2 40 5.3
the radial component of the Poynting vector normalized by -0.4 4.4
-0.5 3.6
the forward emission value as a function of the polar angle 20 -0.6
-0.7 20
2.7
1.8
-0.9
共in the plane xOz兲. This result demonstrates the good unidi- 500 600 700 800
-1
1.0 1.0
0.10
500 600 700 800
rectionality offered by a single nanoparticle. The angular λ (nm) λ (nm)
width of the emission pattern defined as the angle between (a) (b)
the on-axis maximum value and the direction of half maxi- 100 100
1 14
0.9 13
mum value is on the order of ⫾40°. Finally, it is interesting 80 0.8
0.6 80
12
11
0.5
to note that for = r, the ratio of the radiated energy in both 60
0.4
0.3
11
9.7
60 8.8
0.1
d (nm)
d (nm)
half spaces is precisely equal to 1. It may seem surprising 0 1.0
7.9
7.1
-0.1
that a highly asymmetric environment 共a single particle at the 40 -0.2
-0.4
40 6.2
5.3
4.4
-0.5 3.6
left of the emitter兲 results in perfectly symmetric radiation 20 -0.6
-0.7 20 2.7
1.8
关see the radiation pattern in Fig. 2共c兲兴. To fully understand -0.9
-1
.0 1.0
0.10
500 600 700 800 500 600 700 800
this counter-intuitive result, let us consider the analytic ex- λ (nm) λ (nm)
pression of the emission of two dipoles with moments de- (c) (d)
noted p1 and p2. They are placed along the x axis with sepa-
ration d + a, and oriented along the z axis 关see Fig. 1共a兲兴. Let FIG. 3. 共a兲 Phase differences normalized by between the di-
us note x1 = −共d + a兲 / 2 and x2 = 共d + a兲 / 2 the positions of the polar emitter and the induced dipolar moment of the nanoparticle
dipoles along the x axis. We consider that in the far-field and 共b兲 reflection ratio defined as the ratio of the power emitted
limit 共r Ⰷ 兲, toward the right and left half spaces respectively as a function of the
wavelength of emission and the distance d between the emitter and
兩r − x j兩 − r = 冑共x − x j兲2 + y 2 + z2 − r the metallic surface of a 90 nm silver sphere. 共c兲 and 共d兲 show
similar results as 共a兲 and 共b兲, respectively, but for a 60 nm sphere.
⬇ r共冑1 − 2xx j/r2 − 1兲
⬇ − x j共x/r兲 ⬇ − x j sin共兲cos共兲. the sum of the Poynting vectors in one direction and in the
opposite direction
The electric and magnetic fields produced in the far field by
p1 共j = 1兲 and p2 共j = 2兲 then write ⌬P共r, , 兲 = P共r, , 兲 + P共r, − , + 兲 共7兲
E j共r, , 兲 = 冉冊
c
2
1
4r⑀0
eik兩r−x j兩关共er ⫻ p j兲 ⫻ er兴 共1兲
=
3k
Re兵2ip1 pⴱ2 sin关k共d + a兲sin共兲cos共兲兴其sin2共兲er .
162⑀0c2r2
= 冉冊
c
2
1
4r⑀0
eikre−ikx j sin共兲cos共兲 p j sin共兲共− e兲, 共2兲
In our case, we are interested by the evolution of ⌬P with
共8兲
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BONOD et al. PHYSICAL REVIEW B 82, 115429 共2010兲
Reflected efficiency
0.5π 0.6
0.4
formed for a 60 nm silver particle 关Figs. 3共c兲 and 3共d兲兴 show 0.0π
0.5 0.2
∆Φ
that a similar behavior is obtained but that the opposite-phase 0.0 180 0
0.4 0.2
wavelength, r, is shifted toward shorter wavelengths. These -0.5π
0.3
0.4
0.6 210
graphs evidence that in the 500–600 nm range 共with d -1.0π
0.2
0.8
330
= 30 nm兲, the smaller particles 共60 nm兲 mostly collect elec- 0.4 0.5 0.6 0.7
λ (in µm)
0.8 0.9 1.0 240
270
300
tromagnetic radiation while larger particles 共90 nm兲 act as (b) (c)
reflectors. This property allows the design of Yagi-Uda an-
tennas with a reflector made of slightly larger particles and a FIG. 4. 共Color online兲 共a兲 The nanoantenna is composed of two
collector made of an array of identical smaller particles.27–31 identical silver nanoparticles of diameter 60 nm. The emitter is
More importantly, these calculations show that at a given located at 10 nm from the left particle, and at 40 nm from the right
frequency, a single sphere can act as a reflector or a collector particle. 共b兲 Full line, right scale: reflection efficiency as a function
depending on its distance from the emitter, and that this be- of the emitted wavelength; circles and squares, left scale: dephasing
havior can be controlled inside a very small range of dis- of the emitting and induced dipoles supported by the 60nm sphere
tances 共a few tens of nanometer_S_兲. For example, we can for 40nm 共circles兲 and 10nm 共squares兲 spacings. 共c兲 Emission pat-
observe in Fig. 3共d兲 that at = 550 nm, the nanoparticle be- tern of the oscillating dipole at = 550 nm in the xOz plane.
haves as a collector when it is at a distance of 40 nm from
the emitter while it behaves as a reflector when this distance ences between the emitter and the two induced dipolar
is reduced to 10 nm. Consequently, it is possible to design modes supported by the particles. The wavelength range in
unidirectional antennas by assembling two identical par- which one particle acts as a collector while the other reflects
ticles, i.e., with identical polarizabilities and by tuning the radiation exceeds 100 nm, which is larger than the width of a
distances between the emitter and both particles. However, typical fluorescent emitter. Figure 5共b兲 shows that this an-
Fig. 3 suggests that a stronger directionality can be achieved tenna geometry fulfills these conditions for wavelengths
by assembling two particles of different diameters with mini- ranging from 475 to 600 nm. As expected, the ratio of the
mum and maximum reflection efficiencies at the emission radiated power toward the x ⱖ 0 half space is maximum
wavelength, a property that cannot be achieved with equal D = 90 nm
diameters. We can thus design an ultracompact antenna made 1.0π D = 60 nm
1.0
of 90 and 60 nm particles at an equal 30 nm distance from 0.9
0.5π
Reflected efficiency
the emitter, geometry chosen to optimize the dephasing be- 0.8
tween the dipolar moments of the nanospheres and the emit-
∆φ1, ∆φ2
0.0π 0.7
ter. 30 nm 30 nm 0.6
-0.5π 0.5
x
0.4
-1.0π
0.4 0.5 0.6 0.7 0.8
III. ULTRACOMPACT AND UNIDIRECTIONAL (a) λ (in µm)
NANOANTENNA 90 (b)
120 60
1.0 3.0
Radiative and total decay rates
closely separated by a distance of only 50 nm. The emitter is 0.2 1.0 0.6
0.4
located at 10 nm from the first particle 共which thus acts as 0.6 210 330 0.5 0.5
0.8
the reflector兲 and 40 nm from the second particle 共the collec- 1.0
0.0
0.4 0.5 0.6 0.7 0.8
0.4
240 300
tor兲 关see Fig. 4共a兲兴. Figure 4共b兲 shows the reflection effi- 270 λ (in µm)
(c) (d)
ciency as a function of the wavelength of emission. A good
directivity can thus be achieved with strictly identical par- FIG. 5. 共Color online兲 共a兲 The nanoantenna is composed of sil-
ticles since 70% of the emitted energy is radiated into the ver particles of diameter 60 and 90 nm. The emitter is located at 30
positive x half space. Let us note that both distances, respec- nm from both particles. 共b兲 Full line, right scale: reflection effi-
tively, 10 nm and 40 nm are much smaller than the emitting ciency as a function of the emitted wavelength; circles and squares
wavelength and achievable with biological linkers.7,18 left scale: dephasing of the emitting and induced dipoles supported
Let us now design an asymmetric antenna made of two by spheres of diameter 90 nm 共circles兲 and 60 nm 共squares兲. 共c兲
silver particles with different diameters to optimize their re- Emission pattern of the oscillating dipole at = 550 nm in the xOz
flective and collective properties. The antenna, consisting of plane. 共d兲 Full and circles, left scale: radiative 共dashed lines兲 and
60 and 90 nm diameter silver spheres, was optimized with total 共full line兲 decay rates enhancements as a function of the wave-
respect to the particle sizes while keeping d equal to 30 nm length emission. Full line+ squares, right scale: quantum efficiency
关see Fig. 5共a兲兴. In a first step, we compute the phase differ- 共the intrinsic quantum efficiency is equal to 1兲.
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ULTRACOMPACT AND UNIDIRECTIONAL METALLIC ANTENNAS PHYSICAL REVIEW B 82, 115429 共2010兲
3500
when the phases are of opposite sign, and it can reach more
3000
than 97% at = 520 nm. The emission pattern is recon- x
2500
structed in Fig. 5共c兲 at = 520 nm as a function of the polar 2000
Γtot, Γrad
angle 共in the plane xOz兲. It confirms the high unidirectional- 1500
ity of this antenna since the emitted power toward the left 1000
z
500
half plane is unobservable at this scale. Moreover, this an- 0
tenna narrows the angular redistribution of emitted light 0.4 0.5 0.6 0.7 0.8
λ (µm)
compared to a single nanoparticle since the angular width of
the emission cone is less than ⫾30°. Such angular openings 0.6
(a) (b)
90
1.2 120 60
are easily achievable with commercial microscope 0.5 1.0
Quantum efficiency η
0.8
objectives.33 In practice, this asymmetric nanoantenna, al- 0.4 0.6 150 30
115429-5
BONOD et al. PHYSICAL REVIEW B 82, 115429 共2010兲
*nicolas.bonod@fresnel.fr 19
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