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Visualization of the complex refractive index of a conductor by frustrated total internal reflection

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A simple imaging geometry in which total internal reflection in a glass prism is frustrated by the proximity of a metal surface is implemented for observation of surface plasmon resonance. At a certain angle of incidence, the total internal reflection is completely suppressed at a certain distance between the metal and the prism surfaces. Using planar metal and spherical prism surfaces, the distance parameter is sampled in a single image. This allows a direct determination of the complex refractive index in bulk samples as well as in thin films. Our experimental data are in good agreement with previously published data.
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Visualization of the complex refractive index of a conductor by frustrated
total internal reflection
Yu. P. Bliokh,
a
R. Vander, S. G. Lipson, and J. Felsteiner
Department of Physics, Technion-Israel Institute of Technology, 32000 Haifa, Israel
Received 12 February 2006; accepted 23 May 2006; published online 11 July 2006
A simple imaging geometry in which total internal reflection in a glass prism is frustrated by the
proximity of a metal surface is implemented for observation of surface plasmon resonance. At a
certain angle of incidence, the total internal reflection is completely suppressed at a certain distance
between the metal and the prism surfaces. Using planar metal and spherical prism surfaces, the
distance parameter is sampled in a single image. This allows a direct determination of the complex
refractive index in bulk samples as well as in thin films. Our experimental data are in good
agreement with previously published data. © 2006 American Institute of Physics.
DOI: 10.1063/1.2220540
Total internal reflection of light at a glass-air interface
can be spoilt by the proximity of a second optical medium
situated within about one wavelength of the interface. This is
a well-known phenomenon and can be described as a process
in which photons tunnel from the glass, through an air bar-
rier, into the second medium. We consider the case where the
second medium is a conductor, having complex refractive
index n
˜
n+ik, which supports surface plasmon resonance
SPR.
1
We use a simple imaging geometry often used to
demonstrate frustrated total internal reflection by a prism in
contact at one point with a convex spherical optical surface.
In contrast to previous investigations, this configuration pro-
vides continuous and accurate control of the thickness of the
barrier. A high contrast interference fringe is observed, which
indicates destructive interference between the totally re-
flected wave and that reflected from the metal. Since two
parameters incidence angle and barrier thickness are re-
quired for maximum frustration, the experiment provides a
simple visual method of determining n
˜
directly, and has the
advantage that it can be carried out on the polished surface of
a bulk sample, as well as on thin films. It may also be appli-
cable to identifying left-handed materials.
2
Surface plasmons
3
are electronic excitations with p po-
larization which propagate on the interface between a con-
ductor and a conventional dielectric. They have many appli-
cations, including electronic devices and biosensors. When
Maxwell’s equations are solved for the interface between a
metal dielectric constant
=
r
+i
i
=n
2
k
2
+2ink and a
conventional dielectric
d
=n
d
2
0, “surface plasmon” solu-
tions are found. These decay exponentially away from the
interface into both media and have component k
x
of the wave
vector parallel to the surface given by
4
k
x
2
= k
0
2
⑀⑀
d
+
d
, 1
where k
0
is the value of the free space wave vector. When
r
d
, Rek
x
k
0
, and so the wave has to be excited ei-
ther by a traveling wave in an optically dense medium
Kretschman configuration Ref. 5, Fig. 1a兲兴 or by a grating
coupler
3
where the grating period provides the necessary
addition to k
0
, Fig. 1b兲兴. In these cases the metal must be in
the form of a thin film, where the coupling is from one side
and the surface plasmon is on the other. Another method
1
couples the plasmon to an evanescent wave in air, produced
by total internal reflection in a glass prism Otto configura-
tion, Fig. 1c兲兴. In this case the surface plasmon is excited on
the air-sample interface, and therefore a bulk conducting
sample can be used. This type of coupling has been em-
ployed in several laboratories for example, Ref. 6, but the
need for accurate control of the separation between the prism
and conductor surfaces makes for complicated mechanics
when used at visible wavelengths. It was also studied by
Bliokh et al.
7
using a dense gas plasma at microwave fre-
quencies, where diffraction by a subwavelength grating pro-
vided the evanescent wave. At optical frequencies, the eva-
nescent wave can be provided by an internally totally
reflecting glass surface, when the angle of incidence in the
glass
inc
is chosen appropriately, so that resonance occurs
when n
glass
k
0
sin
inc
=Rek
x
from 1. The resonance has a
width determined by the damping, i.e., Imk
x
, and so the
phase of the plasmon varies continuously with angle.
8
To
satisfy the boundary conditions between the plasmon and the
evanescent wave in the air gap there has to be a reflected
evanescent wave, which in turn creates an additional travel-
ing wave on its incidence on the glass. This wave interferes
with the totally reflected wave; both of them have phases
determined by
inc
, and for a lossy metal there exists at least
one angle of incidence at which the difference between them
is
.
9
At that angle, for a certain value of the air-gap thick-
ness, the amplitudes of the two waves are equal, and com-
pletely destructive interference occurs. Because the wave
a
Electronic mail: bliokh@physics.technion.ac.il
FIG. 1. Three methods of coupling to surface plasmons. a Prism coupling
Kretschman; b grating coupling; c evanescent wave coupling Otto.SP
indicates the surface on which surface plasmons are excited.
APPLIED PHYSICS LETTERS 89, 021908 2006
0003-6951/2006/892/021908/3/$23.00 © 2006 American Institute of Physics89, 021908-1
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propagation in the gap is evanescent, no further phase differ-
ences are induced there.
The solution of Maxwell’s equations for this problem is
conveniently expressed in terms of two equations.
1,9
The first
expresses the p-wave Fresnel reflection coefficient at the in-
terface between media i and j:
r
ij
=
n
j
cos
i
n
i
cos
j
n
j
cos
i
+ n
i
cos
j
, 2
in which
j
is the complex angle of refraction in the me-
dium, calculated by Snell’s law. The reflectance r
of a
three-layer system glass 1/air gap 2/metal 3兲兴 is given
by the second equation:
r
=
r
12
+ r
23
exp−2dk
z
兩兲
1+r
12
r
23
exp−2dk
z
兩兲
, 3
where k
z
2
=k
0
2
k
x
2
0 and d is the gap thickness. The surface
plasmon energy loss in the metal leads to an appearance of a
deep minimum at the resonant angle of incidence,
res
, when
the plasmon is excited. It was shown in Ref. 9 that the re-
flectance is exactly zero for a certain value d
res
of the gap
thickness. The two experimentally measured values,
res
and
d
res
, allow us to determine the two optical characteristics, n
and k, of the metal under investigation. A useful way of
representing the relationship between n, k and
res
, d
res
is the
series of curves shown in Fig. 2. Any particular conductor
can be identified in the plane of the diagram by means of its
values of n and k. The ordinate and abscissa then show,
respectively, the thickness of the air gap d and the resonance
angle
inc
at which the reflected light has zero intensity.
In order to display these two parameters visually, we use
the proximity of a slightly convex glass-air interface to a
planar air-metal interface or vice versa, the two touching at
one point. The former is made by optically contacting a
0.5 m focal length planoconvex singlet lens to the hypot-
enuse of a right-angled prism. Samples of various metals, in
the form of thick d ⬎␭ evaporated layers on flame-polished
plane glass slides or polished bulk metal plates, were then
lightly pressed onto the convex glass surface using a foam-
rubber plug. The interfaces were illuminated with plane par-
allel p-polarized He–Ne laser light =633 nm through the
prism, at an angle greater than the critical angle, and the
interface was imaged on a charge-coupled device CCD
camera using the reflected light Fig. 3. The imaging lens
had a sufficiently large aperture that the prism could be ro-
tated through about without image vignetting, for deter-
mination of the angle of minimum reflected intensity. The
angles could be accurately measured with respect to the criti-
cal angle, at which Newton’s rings appear in the field of
view. Measurement of the radius of curvature R of the con-
vex surface using an autocollimator determined the relation-
ship between air-gap thickness d and radius r in the image
field, d = r
2
/2R. Since the observation is at an aspect angle
close to 45°, a particular value of d corresponds in the cam-
era plane to an ellipse with axes ratio approximately
2.
Destructive interference occurring at a certain thickness d
min
then gives rise to a dark elliptical fringe Figs. 3 and 4.As
inc
is varied, the contrast of the fringe changes, becoming
close to unity at the abscissa angle
in Fig. 2. The breadth of
the fringe can be related to Imk
x
.
Preliminary experiments to evaluate the technique were
carried out on the metals Cu, Au, Ag, Al, and In, which
satisfy the condition
r
−1 required for support of surface
plasmons, and also on Fe to confirm that the dark fringe is
absent for a metal with
r
−1. The results are indicated in
Fig. 2, together with literature values for these metals at
=633 nm.
10–12
Apart from indium, the results are in good
agreement with the published values. Observed ellipse im-
ages are shown in Fig. 4 for several of the metals; the dif-
FIG. 2. Map of n and k. Contours of n and k on the plane representing the
thickness of the air gap, d /, and the angle
at which minimum ideally
zero reflectance is obtained for thick samples. This map can be used to
derive n
˜
from experimental data. Points representing literature values Refs.
10–12 for several metals are shown, together with our measured values. Al,
Au, Cu, and In samples were prepared by vacuum evaporation thickness
⬎␭, and Cu and Ag samples from bulk 99.99% purity.
FIG. 3. Experimental setup. A typical image is shown on the left, and details
of the tunnelling region are shown on the right.
FIG. 4. Elliptical fringes observed for six samples. Fe does not exhibit SPR.
All films have d ⬎␭. The differences between the radii and the sharpness of
the fringes can be seen clearly. In general, the larger and sharper the ellipse,
the greater the SPR sensitivity of the sample.
021908-2 Bliokh et al. Appl. Phys. Lett. 89, 021908 2006
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ferences between them are very clear. Experiments on Cu
samples, for example, showed considerable dependence on
the method of preparation of the sample evaporated film or
bulk metal. In general, a large sharp ellipse indicates a high
SPR sensitivity. Intensity profiles as a function of air space
thickness were deduced from these images Fig. 5.
The simplicity of the experiment, and the fact that it is
applicable to samples prepared by different methods, makes
it a convenient method to determine n
˜
for conductors satis-
fying n
2
k
2
−1. The experiments showed clearly the dif-
ference between surface treatments chemical, electropolish-
ing, and abrasive polishing, and we believe that the
anomalous behavior of In films is due to surface oxidation,
which may also explain the large variation in published val-
ues for n and k for this metal.
11,12
In addition, the experi-
ments showed that for materials with large k, for which the
angle
is close to critical, the resonance ellipse was visible
below the critical angle, indicating that SPR could be in-
duced by light incident from air. This was also observed by
Cairns et al.
6
Furthermore, the method may be useful in
identifying left-handed negative refractive index materials,
whose SPR properties are discussed by Ruppin
2
and may
include an s-polarized mode. We also used it to compare the
quality of spoons made of nominally pure silver; the convex
shape of a spoon allows contact with a plane prism surface to
be made, since the curvature is provided by the spoons them-
selves. The surface has to be well polished only over a very
small area, and further study should allow a quantitative re-
lationship between the metal quality and its complex refrac-
tive index to be established.
1
A. Otto, Z. Phys. 216, 398 1968.
2
R. Ruppin, J. Phys.: Condens. Matter 13, 1811 2001.
3
H. Raether, in Springer Tracts in Modern Physics, edited by G. Hohler and
E. A. Niekisch Springer, Berlin, 1988, Vol. 111.
4
W. Knoll, Annu. Rev. Phys. Chem. 49, 569 1998.
5
E. Kretschman, Opt. Commun. 6, 185 1972.
6
G. F. Cairns, S. M. O’Prey, and P. Dawson, Rev. Sci. Instrum. 71,4213
2000.
7
Yu. P. Bliokh, J. Felsteiner, and Ya. Z. Slutsker, Phys. Rev. Lett. 95,
165003 2005.
8
A. V. Kabashin and V. I. Nikitin, Opt. Commun. 50,51998.
9
W. Lukosz and H. Wahlen, Opt. Lett. 3,881978.
10
P. B. Johnson and R. W. Christy, Phys. Rev. B 6, 4370 1972.
11
G. J. Kovacs, Thin Solid Films 60,331979.
12
H. E. de Bruijn, R. P. H. Kooyman, and J. Greve, Appl. Opt. 31,440
1992.
FIG. 5. Radial intensity profiles of images as a function of d/. The profiles
are measured at the angle of incidence where highest contrast was obtained.
The minimum intensity is not zero as predicted by the theory, probably
because of surface scattering. For each profile, the intensity shown at a
particular value of d is an average of the values measured around an ellip-
tical ring with the appropriate axis ratio.
021908-3 Bliokh et al. Appl. Phys. Lett. 89, 021908 2006
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An interferometric method for the detection of the phase shifts of reflected light under Surface Plasmon Resonance (SPR) conditions due to refractive index changes is proposed and experimentally realized. The sensitivity threshold of the method to a refractive index variation Δn is estimated to be 4×10−8. The proposed SPR-interferometer provides spatial phase resolution and thus enables to take into account the peculiarities of refractive index distribution over the surface of an SPR-supporting film. It can be successfully applied in bio- and chemical-sensor systems.
Article
We investigated when the reflectance R(p) for p-polarized light becomes exactly zero in an attenuated-total-reflection configuration where surface plasma waves at a metal–dielectric interface are excited. We particularly studied the reflection from coated metal mirrors at infrared wavelengths, where the complex refractive index n2 = n2′ + in2″ of the dielectric coating has a real part smaller than unity. When a certain relation between n2′ and n2″ is satisfied, the reflectance R(p) versus incidence angle has deep broad minima for a large range of coating thicknesses. Such mirrors would be efficient reflection polarizers and would have high hemispherical thermal emissivities.