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NL 9041033
NL 9041033
org/NanoLett
ABSTRACT We experimentally demonstrate a perfect plasmonic absorber at λ ) 1.6 µm. Its polarization-independent absorbance
is 99% at normal incidence and remains very high over a wide angular range of incidence around (80°. We introduce a novel concept
to utilize this perfect absorber as plasmonic sensor for refractive index sensing. This sensing strategy offers great potential to maintain
the performance of localized surface plasmon sensors even in nonlaboratory environments due to its simple and robust measurement
scheme.
KEYWORDS Perfect absorbers, LSPR resonances, infrared sensors, glucose sensing, plasmonics
© 2010 American Chemical Society 2342 DOI: 10.1021/nl9041033 | Nano Lett. 2010, 10, 2342–2348
that different from many plasmonic applications where
losses deteriorate the performance of potential devices for
the realization of perfect absorbers the substantial losses in
the metal are desirable and can be exploited as well. In the
case of five times damping constant of bulk gold, the
reflectance minimum slightly deviates from perfect absor-
bance. The losses in gold with a damping constant equal to
three times that of bulk gold are sufficient to yield a strong
narrow-band resonance. In fact, the structural parameters
described in Figure 1 were particularly optimized for the gold
film (i.e., perfectly impedance matched18 to the air on top
of the sample), which has a damping constant three times
that of bulk gold because it provides the best match to our
experimental gold film.
To better understand the nature of our perfect absorber,
FIGURE 1. Schematic of the perfect absorber structure and the the current distribution at resonance was simulated and is
incident light polarization configuration. The diameter and thickness
of the gold disks are 352 and 20 nm, respectively. The periods in depicted in Figure 2b. It is evident that antiparallel currents
both x and y-directions are 600 nm. The thickness of the MgF2 spacer are excited in the gold disk and the bottom gold layer.36,37
is 30 nm and the thickness of the gold mirror is 200 nm. The whole
structure resides on a glass substrate.
Actually, this is often called a magnetic resonance because
the circulating currents result in a magnetic moment which
sensing methods and is of special interest in numerous can strongly interact with the magnetic field of the incident
applications due to its low-background detection scheme. light.36,37 At resonance, a strong enhancement of the local-
Figure 1 illustrates the geometry of the absorber sensor ized electromagnetic field is established between the two
structure. It consists of two functional layers. The top layer layers. Consequently, electromagnetic energy can be ef-
is a two-dimensional gold disk array and the bottom layer ficiently confined in the intermediate MgF2 spacer and
is a gold mirror. The two layers are separated by an MgF2 therefore no light is reflected back. This gives rise to a
dielectric spacer. Because of the presence of the gold mirror, pronounced reflectance dip in the spectrum with nearly zero
the transmittance of the structure is totally eliminated across intensity, therefore leading to ∼100% absorbance. In fact,
the entire near-infrared frequency regime (i.e., T ) 0). The our device can work as a perfect absorber over a wide range
structure is designed to be polarization independent in x- of incident angles. Figure 2c shows the angular dispersions
and y-directions at normal incidence. To investigate the of the absorbance peak at various angles of incidence for
resonant behavior of the structure, numerical simulations both TE and TM configurations. For the TM polarization, the
were performed by employing a Finite Integration Time absorbance peak is nearly independent of the incident angle
Domain algorithm.32 For excitation of the structure, we use and it is 96% even at 80°. This is because the direction of
normally incident light with its polarization along the x- the magnetic field of the incident light remains unchanged
direction as shown in Figure 1. The permittivity of the MgF2 with various incident angles and it can efficiently drive the
spacer33 is taken as 1.9, and the permittivity of bulk gold in circulating currents at all angles of incidence. Conversely,
the near-infrared34 is described by the Drude model with the for the TE polarization, the magnetic field cannot drive the
plasma frequency ωpl ) 1.37 × 1016 s-1 and the damping circulating currents efficiently at large angles.19 Neverthe-
constant ωc ) 4.08 × 1013 s-1. Owing to the surface less, the absorbance still remains at 50% at 80°.
scattering and grain boundary effects in thin films, the
The designed structure is compatible with nanofabrica-
damping constant of the gold film in the real system is likely tion techniques. The thick gold film and the MgF2 dielectric
higher than that of bulk gold.35 To elucidate the influence of layer were subsequently deposited onto a glass substrate
the damping constant of the gold film on the minimum using electron-gun evaporation. The disk array was defined
reflectance value at resonance, Figure 2a presents the in positive resist (polymethylmethacrylate, PMMA) using
simulated reflectance spectra for damping constants of one, standard electron beam lithography followed by a gold lift-
three, and five times that of bulk gold. As shown in Figure off procedure. The sample has a structure area of 100 µm
2a, reflectance dips with different amplitudes are observ- × 100 µm. The top left picture in Figure 3a shows the normal
able. In particular, a strong resonance with nearly zero view of the sample obtained by a scanning electron micros-
reflectance (R ) 0.28%) is achieved for three times damping copy. To demonstrate the feasibility of our absorber working
constant of bulk gold (see the red curve in Figure 2a). as a LSPR sensor, Figure 3a shows the results of a proof-of-
Consequently, a perfect absorber is obtained (A ) 1 - T - principle experiment, displaying the measured reflectance
R). Nevertheless, for a damping constant equal to one time spectra with air (n ) 1) and water (n ) 1.312),38 on the
that of bulk gold, the reflectance minimum is around 30% sample surface. The measurements were performed by a
and it leads to only 70% absorbance. Notably, this illustrates Fourier-transform infrared spectrometer with electric field
© 2010 American Chemical Society 2343 DOI: 10.1021/nl9041033 | Nano Lett. 2010, 10, 2342-–2348
FIGURE 2. (a) Simulated reflectance spectra in dependence on the damping constant of the gold film. Reflectance with zero intensity is achieved
using a damping constant that is equal to three times that of bulk gold. (b) Calculated current distribution at resonance where perfect absorbance
occurs. Antiparallel currents are excited in the gold disk and the gold film. (c) The simulated angular dispersions of the absorbance peak for
TE and TM configurations.
polarization as illustrated in Figure 1 at normal incidence. characterized by the black curve in Figure 3a, the experi-
The sensing principle relies on the fact that zero reflectance mental reflectance reaches a minimum of 1% at 185.6 THz
(i.e., perfect impedance matching) occurs only for a certain (1.6 µm) in air, which corresponds to an experimental
refractive index of the surrounding medium. The variation absorbance of 99%. When water (red curve) is applied onto
of the refractive index of the surrounding medium gives rise the sample surface, a clear increase of the reflectance
to nonzero reflectance (i.e., nonperfect absorbance) and intensity from 1% to 28.7% at 185.6 THz is visible, resulting
therefore allows for the extremely sensitive detection of the from the refractive index change of the local dielectric
intensity change in reflectance at a fixed frequency. As environment. The correspondingly simulated reflectance
© 2010 American Chemical Society 2344 DOI: 10.1021/nl9041033 | Nano Lett. 2010, 10, 2342-–2348
FIGURE 3. (a) Top: Experimental demonstration of perfect absorbance in air. Experimental tuning of the reflectance and absorbance spectra by changing
the dielectric environment which is adjacent to the gold disks from air to water is shown. The SEM image of the sample is presented in the left column.
Bottom: The correspondingly simulated reflectance and absorbance spectra with different dielectric materials (air and water) on the structure surface. In
simulations, a damping constant equal to three times that of bulk gold was utilized. The agreement between experimental and simulated results is nearly
perfect. (b) Experimental FOM* as a function of frequency. The highest value of FOM* is 87, which is reached at a frequency slightly away from the minimum
reflectance. In the discrete calculation of the experimental FOM*, the reflectance difference between water (Iwater (λ)) and air (Iair (λ)) was taken for the
derivative in eq (1). Iair (λ) was taken for the denominator I (λ) in eq 1. The experimental reflectance spectrum with air on the structure surface is replotted
with a black curve.
© 2010 American Chemical Society 2345 DOI: 10.1021/nl9041033 | Nano Lett. 2010, 10, 2342-–2348
and absorbance spectra characterized by dashed lines are
also shown in Figure 3a. In simulations, a damping constant
equal to three times that of bulk gold for the gold film was
used. The agreement between experimental and simulated
results is nearly perfect.
Subsequently, the FOM* can be calculated according to
© 2010 American Chemical Society 2346 DOI: 10.1021/nl9041033 | Nano Lett. 2010, 10, 2342-–2348
In essence, our sensor scheme suggests potential refrac- (8) Lassiter, J. B.; Aizpurua, J.; Hernandez, L. I.; Brandl, D. W.;
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© 2010 American Chemical Society 2348 DOI: 10.1021/nl9041033 | Nano Lett. 2010, 10, 2342-–2348