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Introduction
190
Hiroshi Kano
191
SPP
SPP
Metal
Metal
(a)
(b)
Fig. 2. Concept of localized SPPs. (a) Conventional method; (b) Method of localization
a certain point on the metallic surface as shown in Fig. 2b. In this case,
the SPPs interfere with one another and form a localized electric eld. The
dimensions of the localized area are on the order of the wavelength.
In this chapter, we give an overview of the method of exciting localized
SPPs and their properties [11]. Applications of localized SPPs [12,13] are also
described.
Illumination
Reflection
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Hiroshi Kano
Es ( , ) = 0
(otherwise) ,
(1)
where Ei represents the incident amplitude. In this equation, and represent the radial and the azimuthal coordinates, respectively, at the pupil
plane, and the axis is normalized by th wavenumber of the incident light in
vacuum. The light passing any particular position ( , ) of the pupil plane
is converted to a corresponding plane wave by the objective lens and illuminates the KretschmannRaether conguration. Here, Ep and Es correspond
to illumination of the interface by p-polarized and s-polarized light, respectively.
In the KretschmannRaether conguration, multiple reections arise from
each plane wave. To consider this eect, the amplitude transmission coe
z
Vacuum
y
Metal
Glass
(a)
(b)
193
m
tm
01 ( )r12 ( ) exp [ik1z ( )d1 ]
,
m
1 tm
10 ( )r12 ( ) exp [ik1z ( )d1 ]
m = p, s ,
(2)
m
where tm
ab and rab are the Fresnel reection and transmission coecients at
an interface beetween two materials a and b for light that is incident from
material a; they depend on the relative permittivities of the materials on
both sides. In this equation, k1z denotes the z (normal to the interfaces)
component of the wave vector in the silver lm, and d1 denotes the thickness
of the silver lm.
From (1) and (2), the amplitude components produced by light passing the
location ( , ) of the pupil plane are obtainable. Thus, the functions E SPP ,
ESPP and EzSPP are introduced to represent the components which oscillate
in the radial ( ), azimuthal (), and z directions in the sample. With the
coordinates shown in Fig. 4b, these functions can be expressed as
E SPP (x, y, z, , ) =
exp {i [k2x ( , )x + k2y ( , )y + k2z ( )z]}
k2xy ( )
Ep ( , )Tp ( ) ,
k2
ESPP (x, y, z, , ) =
exp {i [k2x ( , )x + k2y ( , )y + k2z ( )z]} Es ( , )Ts ( ) ,
EzSPP (x, y, z, , ) =
exp {i [k2x ( , )x + k2y ( , )y + k2z ( )z]}
k2z ( )
Ep ( , )Tp ( ) , (3)
k2
where
(2 )1/2 ,
c
k2x ( , ) = k2 cos ,
k2y ( , ) = k2 sin ,
k2 =
k2xy ( ) = k2 ,
k2z ( ) = k2 1
2 1/2
(4)
I SPP (x, y, z) =
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Hiroshi Kano
2
EySPP (x, y, z, , )
d d
EzSPP (x, y, z, , )
d d
(6)
Relative permittivity
Glass (BK7)
Silver
( = 488 nm)
( = 632.8 nm)
(1.522)2
(1.515)2
7.901 + 0.7361i
15.87 + 1.073i
Vacuum/Air
(1.000)
(1.000)2
Si Ox
(1.460)2
(1.460)2
(1.485)2
PMMA
(1.495)
0.040
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main peak (in the region x < 0) into account, these main peaks are spread
over a region of size 0.6m 0.4m, which is almost the same as the size of
the diraction-limited spot at this wavelength. One can see that the electric
eld is also conned to the near eld of the metallic surface because the
electric eld accompanying an SPP has an evanescent-decaying nature in the
direction normal to the surface. This is an electric eld produced by localized
SPPs. This calculated result reveals that a microscope utilizing SPPs excited
by this method has a possibility of probing a 0.6m 0.4m region in the
near eld of a metallic surface.
As mentioned above, incident light which passes through a ring of a particular size at the pupil plane can excite SPPs. This means that such light
mainly contributes to the formation of the eld, while the other light does
not. To observe this eect, annular pupil illumination was investigated.
For this annular pupil illumination, linearly polarized light in the region
1.03 < < 1.04 was assumed. Figure 6 presents the result, which shows
a peak at a higher intensity. This means that one can expect further eldenhancement from annular illumination. This is because the eciency of SPP
excitation is higher than for circular pupil illumination, in which most of the
incident light is just reected. The prole of the electric eld exhibits a good
similarity to that in Fig. 5. This behavior can be easily understood by evaluating (2), which describes the contribution of the incident light to the formation
of the electric-eld as a function of . The result shows that p-polarized light
which satises the dispersion-matching dominantly condition contributes to
the eld formation. Thus, a restriction at the pupil plane to annular illumination does not make a great dierence to the result with respect to the prole
of the eld distribution.
z
22.30
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Hiroshi Kano
To appreciate further the nature of SPP excitation, the electric-eldintensity distribution for the same model (circular pupil illumination) but
without the metallic lm was also calculated (Fig. 7). In this image, two
peaks are found in the center again. It is noteworthy that the SPPs enhance
the electric-eld strength by 7.5 times, from a comparison of the maximum
intensities in Figs. 6 and 7.
Other types of incident polarization at the pupil plane were also examined.
Figures 8ac correspond to a radial polarization [14,15], an radial polarization [14,15], and a linear polarization with the phase of the incident light
delayed by in the region x < 0, respectively.
z
2.97
Fig. 7. Calculated electric-field intensity for linearly-polarized light on a glass surface. A glassvacuum configuration and annular illumination were assumed in the
calculation
Fig. 8. Incident polarization at the pupil plane of the objective lens: (a) radial
polarization, (b) azimuthal polarization, and (c) linear polarization but with the
phase in the region < 0 delayed by
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m
m
( ) + r12
( ) exp [i2k1z ( )d1 ]
r01
m ( )rm ( ) exp [i2k ( )d ] ,
1 + r01
1z
1
12
m = p, s .
(7)
(8)
Fig. 9. Calculated results for the electric-field intensity for various types of incident polarization: (a) radial polarization, (b) azimuthal polarization, and (c) linear
polarization but with the phase in the region < 0 delayed by . The Kretschmann
Raether configuration and annular illumination were assumed in the calculations
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Hiroshi Kano
0.75
1.00
of dark arcs, which indicates absorption of the light energy by the th SPP
excitation. This ring appears at = kSPP , which is given by
kSPP =
m n2s
,
m + n2s
(9)
As shown in the previous section, SPPs can be localized around the focal
point of the incident light. In this section, an experiment which conrmed
this localization is described.
First, a KretschmannRaether conguration was fabricated on cover slips,
of the type used in normal microscopes. Silver was chosen as the material
for the metallic lm. By a vacuum evaporation technique, the cover slips
were coated with silver so that the nal thickness of metal was 50 nm. These
substrates were examined for SPP excitation by measuring the relationship
between reectance and incidence angle with a conventional SPP sensor [5].
The substrates were then used for the following SPP experiment.
To conrm the existence of localized SPPs, a microscatterer was introduced onto the silver surface and scanned over the region of the focused spot
of the beam. Figure 11 shows the optical setup of this experiment. An Ar+
laser with a wavelength of 488 nm was used as the primary light source. The
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CCD camera
L4
Pinhole
L3
PMT
+
Ar laser
BS
Objective lens
( NA=0.8 dry )
Substrate
Objective lens
( NA=1.3 oil )
L1
L2
Stage
Fig. 11. Experimental setup used to confirm the existence of localized SPPs
laser beam was focused on the silver surface with an oil immersion objective
lens (NA = 1.3). Latex beads with a size of 1.48 m were used as the microscatterer. The density of the beads was 1 bead per 100m2 . The whole
substrate was scanned with a motorized stage in the lateral directions, instead of the scatterer being scanned over the focus region. To measure the
scattered light, another objective lens (NA = 0.8,dry), which collected the
scattered light towards a 200 m pinhole placed in front of a photomultiplier
tube, was introduced. The purpose of the pinhole was to reduce the amount
of stray light; it hardly provided any spatial resolution in the imaging system.
A CCD camera and white-light illumination were also used to observe the
silver surface. These devices were used for sample alignment.
Figure 12 shows the experimental result. The size of the image is 3.8m
3.8m. In the gure, one can see an image of a latex bead, which conrms the
existence of localized SPPs. The bead image is extended in the polarization
direction (y direction). However, the two peaks are not clear in this image.
In Fig. 13, an image from an area where the beads were more concentrated
is also shown. Many well-separated beads are visible. This result again supports the existence of localized SPPs.
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Hiroshi Kano
1m
Fig. 12. Image obtained when a microscatter was scanned around the beam spot.
The incident light is polarized in the y direction. The silver surface with a single
bead is observed
1m
Fig. 13. Image obtained when a microscatter was scanned around the beam spot.
The incident light is polarized in the y direction. The silver surface with many
beads is observed
is local thickness determination of LBK lms. In this section, thickness measurements of LBK lms [12] are described.
For this experiment, polymethylmethacrylate (PMMA) lms were prepared by using the LangmuirBlodgettKuhn deposition technique. The lms
were multilayer assemblies of 4, 8, and 12 monolayers. These lms were deposited onto substrates that consisted of a glass cover slip, a thin silver lm,
and an SiOx coating. The thin silver lm was prepared by vacuum evaporation again. The thickness of the silver lm was 49 nm. The SiOx layer, with a
thickness of 18.3 nm, was evaporated onto the thin silver lm. The purpose of
the SiOx layer was to protect the silver from chemical contaminations while
the LBK lms were deposited. The SiOx layer was precoated so as to have a
hydrophobic surface property, with HMDS (hexamethyldisilazane).
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1.0
Reflectance
0.8
0.6
0.4
no LBK-film
4 layered LBK-film
8 layered LBK-film
12 layered LBK-film
0.2
0.0
42
44
46
48
Incident angle ( degree )
50
Fig. 14. Measured reflectance of the samples prepared for thickness measurement,
as a function of incidence angle; p-polarized light with = 632.8 nm was used in
the measurement. The experimental data sets were fitted by theoretical curves
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Hiroshi Kano
Laser
ND
Stage
BS
CCD camera
Pupil plane
Sample
Objective lens
Fig. 15. Experimental setup for thickness measurement of LBK films using localized SPPs. ND, P, and BS represent a neutral-density filter, polarizer, and beam
splitter, respectively
monolayer assemblies were found. These results coincide well with the values
obtained by the conventional method. Dierences on the order of a fraction
of a nanometer remain. This is probably because of dierences in the sample
spots observed. These experiments, however, conrm the nanometer-order
resolution in thickness determination.
Reection Fourier spectra were also observed with circularly polarized
light. In this case, complete dark rings were observed. The measured thicknesses were the same as those measured with linearly polarized light.
In this section, the two-dimensional observation of the refractive-index distribution on a metallic surface with localized SPPs is described [13].
For this experiment a scanning SPP microscope was developed which was
based on the optical setup shown in Fig. 10. The dierences were in the
wavelength of the laser ( = 632.8 nm) and the numerical aperture of the
objective lens (NA = 1.4). The sample stage was also dierent from that in
the earlier setup. For sample scanning, a three-dimensional piezo stage with
a feedback system (Melles Griot, Nano-block system) was used. With this
stage, the sample was scanned in two-dimensions and the focus position was
controlled.
For the experiment, microparticles with diameters of 4.0 m and 1.5 m
were used as samples. The material of these particles was silica. These particles were dispersed on silver lms, each of which was evaporated on a cover
(a)
(e)
(b)
(f)
(c)
(g)
(d)
(h)
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Fig. 16. Observed Fourier spectra: (a)(d) for raw data and (e)(h) for data with
fitted rings: (a) and (e) no LBK-film; (b) and (f) 4; (c) and (g) 8; and (d) and (h)
12 monolayers, respectively, of PMMA
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Hiroshi Kano
Fig. 17. Images obtained from (a) a sample with scattered particles (diameter
4.0 m) in a 15 m 15 m area, (b) a sample with particles (diameter 1.5 m)
in a 5 m 5 m area, (c) a sample with a single particle (diameter 1.5 m) in a
2.5 m 2.5 m area
slip of the kind used for optical microscopes. The thickness of each silver lm
was 50 nm.
With these samples, two-dimensional Fourier spectra were obtained with
a CCD camera. In the Fourier spectra, again, the characteristic arcs were
found. With a simplex algorithm, the central position and the radius of the
arcs were estimated by evaluating the cross section between the ring and
the spectrum. The estimated radius corresponds to the propagation constant
of the SPPs. The propagation constant was transformed to a local eective
refractive index by using (9) in reverse. The whole set of Fourier spectra obtained was processed according to this procedure and an image was produced.
Figure 17 shows the images obtained for particles with a diameter of
4.0 m in a 15m15m area, particles with a diameter of 1.5 m in a 5m
5m area, and a single particle with a diameter of 1.5 m in a 2.5m 2.5m
area. In Fig. 17 a one can clearly see the particles as bright spots. The size
of the spots seen in the gure is approximately 1.5 m not 4.0 m, which is
the diameter of the particles. This is because the SPPs probe only the near
eld of the metallic surface and do not probe the whole of the particle. In
Fig. 17 b, one can see four individual particles close to one another. This
image proves that the present microscope can resolve 1.5 m particles. Each
particle occupies an area of about 1.5m 1.0m. Again, this is because
the probe is localized in the near eld of the metal surface. This image suggests that the particles have been scanned by a distorted probe. As shown in
Fig. 17 c, a single particle can be visualized as well. The direction of the distortion shows good coincidence with the direction of the polarization. These
results are supported by the theoretical calculations.
In the theoretical calculations, it was found that the eld distribution of
the localized SPPs excited by linearly polarized light of = 632.8 nm was
spread over a region of size 0.6m 0.4m. However, the spatial resolution
for the microscope did not reach this value. At this moment, a 1.5 m particle
is the smallest particle which gives a proper image. A further increase of the
spatial resolution is expected.
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One of the most interesting possibilities which has not yet been reported on
is the application of the eld enhancement by localized SPPs. Unlike the case
of enhancement by propagating SPPs, one can expect also a focusing eect
of the incident light energy. With this enhancement, the incident light can
interact more eciently with materials. Nonlinear optics, such as multiphoton
absorption phenomena, is one of the elds to which localized SPPs could
be suitably applied [19]. The polarization of incident light will surely play
an important role in achieving the maximum enhancement as shown in the
theoretical calculations.
References
1.
2.
3.
4.
5.
6.
7.
8.
9.
10.
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Hiroshi Kano
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191
12. H. Kano, W. Knoll, Opt. Commun. 153, 235 (1998) 191, 200
13. H. Kano, W. Knoll, Opt. Commun. 182, 11 (2000) 191, 202
14. R. Yamaguchi, T. Nose, S. Sato, Jpn. J. Appl. Phys. 28, 1730 (1989) 196
15. M. Stalder, M. Schadt, Opt. Lett. 21, 1948 (1996) 196
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18. T. Okamoto, I. Yamaguchi, Jpn. J. Appl. Phys. Lett. 36, L166 (1997) 205
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