Letter

pubs.acs.org/NanoLett

Plasmonic Optical Interference

Dukhyun Choi,*,† Chang Kyun Shin,‡ Daesung Yoon,† Deuk Seok Chung,‡ Yong Wan Jin,*,‡
and Luke P. Lee*,§
†
Department of Mechanical Engineering, School of Engineering, Kyung Hee University, Yongin, 446-701, Republic of Korea
‡
Samsung Advanced Institute of Technology, Yongin, Gyeonggi 446-712, Republic of Korea
§
Biomolecular Nanotechnology Center, Berkeley Sensor and Actuator Center, Department of Bioengineering, University of California
at Berkeley, Berkeley, California 94720, United States
*
S Supporting Information
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ABSTRACT: Understanding optical interference is of great

importance in fundamental and analytical optical design for
Downloaded via SUNGKYUNKWAN UNIV on July 28, 2020 at 09:38:05 (UTC).

next-generation personal, industrial, and military applications.

So far, various researches have been performed for optical
interference phenomena, but there have been no reports on
plasmonic optical interference. Here, we report that optical
interference could be effectively coupled with surface
plasmons, resulting in enhanced optical absorption. We
prepared a three-dimensional (3D) plasmonic nanostructure
that consists of a plasmonic layer at the top, a nanoporous
dielectric layer at the center, and a mirror layer at the bottom.
The plasmonic layer mediates strong plasmonic absorption when the constructive interference pattern is matched with the
plasmonic component. By tailoring the thickness of the dielectric layer, the strong plasmonic absorption can facilely be controlled
and covers the full visible range. The plasmonic interference in the 3D nanostructure thus creates brilliant structural colors. We
develop a design equation to determine the thickness of the dielectric layer in a 3D plasmonic nanostructure that could create the
maximum absorption at a given wavelength. It is further demonstrated that the 3D plasmonic nanostructure can be realized on a
flexible substrate. Our 3D plasmonic nanostructures will have a huge impact on the fields of optoelectronic systems, biochemical
optical sensors, and spectral imaging.
KEYWORDS: Plasmon, optical interference, absorption, structural color, anodic aluminum oxide

W hen two light waves are superimposed, their interaction

leads to constructive and destructive interference,
resulting in interference fringes.1−4 Particularly, interference
characteristics of reflected light. Since optical interference
results from the superimposition of light (i.e., electromagnetic)
waves, constructive interference provides the maximum
fringes on thin structured layers could provide brilliant colors intensity of superimposed light wave and thus could enhance
called structural color, and examples of this can be found in the plasmonic effect. Previously, surface plasmon interference
nature in creatures such as butterflies, hummingbirds, beetles, nanolithography (SPIN)14,15 has been introduced, but this is a
and snakes.5−8 Therefore, thin-film interference could provide a totally different concept with plasmonic optical interference.
great potential for industrial, commercial, and military SPIN uses the interference of surface plasmon waves, but
applications, with biomimetic surfaces that could provide plasmonic optical interference considers coupling between
adaptive camouflage, efficient optical switches, and antire- optical interference from light waves and surface plasmon. In
flection coating. Interference can also greatly enhance Raman this study, we introduce plasmonic optical interference from
scattering by absorbing all of the intensity of an incident beam multilayered 3D plasmonic nanostructures that consist of three
(i.e., leaving no reflected beam), which is known as elements; a plasmonic layer at the top, a dielectric layer at the
interference-enhanced Raman scattering (IERS).9,10 Thus, center, and a mirror layer at the bottom. In our 3D plasmonic
optical interference is a powerful optical tool to effectively nanostructure, the optical behavior of reflected light is
manipulate light at the nanoscale and has many applications in controlled by coupling optical interference with surface
electronics and biophotonics. plasmon. We systematically characterize the functional role of
Optical interference mainly depends on the thickness of the each layer in a 3D plasmonic nanostructure. Maximum
film or the refractive index of the film medium. 2−4 reflection and plasmonic absorption are analyzed by 3D
Furthermore, periodic patterns and photonic lens structures
could change optical interference.11−13 However, there have Received: March 7, 2014
been no reports that optical interference can be effectively Revised: May 5, 2014
coupled by surface plasmon to manipulate the optical Published: May 7, 2014

© 2014 American Chemical Society 3374 dx.doi.org/10.1021/nl5008823 | Nano Lett. 2014, 14, 3374−3381
Nano Letters Letter

Figure 1. Plasmonic optical interference in a multilayered 3D plasmonic nanostructure. (a) SEM image of gold (Au)-coated AAO as the
experimental model and schematic illustration of each layer. The structure consists of a plasmonic layer at the top, a dielectric layer at the center, and
a mirror layer at the bottom. The thickness (t) of a dielectric layer can be tuned. (b) Role of plasmonic and mirror layers. High reflection without a
plasmonic layer occurs due to the mirror layer. Without a mirror layer at the bottom, the structure is semitransparent and creates plasmonic
absorption from the nanoporous gold layer at the top. (c) Coupling of surface plasmons and interference. Strong plasmonic absorption takes places
when constructive interference (red color lines) is matched with the plasmonic layer. On the other hand, reflection occurs when deconstructive
interference is located on the plasmonic layer. (d) Reflection behavior of our 3D plasmonic nanostructure. Due to the strong plasmonic absorption
and high reflection, high peak-to-peak amplitude could be created.

electrodynamic calculations and experiments in terms of the employing the nanoporous plasmonic layer at the top, the
coupling of surface plasmon and interference in the 3D collective excitation of the electron gas is confined near the
plasmonic nanostructure. Depending on the wavelength of an interfaces of the plasmonic nanopores, and the EM field of the
incident beam and the thickness of the dielectric layer, the light at the interface is greatly enhanced. This leads to a
wavelengths of the maximum absorption and reflection are significant enhancement of the incident and reflected radiation
significantly changed. Based on the plasmonic interference,
around the plasmonic nanopores. Without a mirror layer at the
clear structural colors could be observed. We exploit the design
equation to determine the thickness of the dielectric layer that bottom, plasmonic absorption is created from the nanoporous
produces the strong plasmonic absorption at a given wave- gold layer at the top, but the peak-to-peak amplitude (from the
length. The flexible form of the 3D plasmonic nanostructures is reflection to the absorption) is very small due to low reflection
also demonstrated. Finally, we investigate the angle-dependent and interference (Figure 1b). The porous dielectric layer at the
optical behaviors of the 3D nanostructure. middle plays a role to control interference mode matching with
Figure 1a shows a scanning electron microscopy (SEM) the top plasmonic layer by changing its thickness or the
image of our 3D plasmonic nanostructure design using a gold- wavelength of the incident light. Theoretically, the dielectric
coated anodic aluminum oxide (AAO) template. An evaporated layer should not be porous in the 3D layered structure.
gold thin film at the top serves as a plasmonic layer, an AAO However, the porous dielectric layer at the middle in our
layer (i.e., nanoporous alumina) at the center is the dielectric
system provides a great pathway to create a large-area, uniform
layer, and aluminum (Al) at the bottom acts as a reflecting
mirror layer. Incident white light (Iwhite(λ)) results in a reflected nanopore plasmonic layer by simply depositing a metal layer.
wave (Ir(λ)) from the 3D plasmonic nanostructure. The Clear interference patterns (Figure 1c, red lines denote
spectrum of the reflected wave is critically dependent on each constructive interference) were produced by the three-layer 3D
layer of the 3D nanostructure. Without a plasmonic layer, high nanostructure, based on thin-film interference theory. Gen-
reflection from the nanostructure is dominant due to the mirror erally, interference conditions (i.e., constructive or deconstruc-
layer and the transparent dielectric layer (Figure 1b). By tive) for thin films are determined by
3375 dx.doi.org/10.1021/nl5008823 | Nano Lett. 2014, 14, 3374−3381
Nano Letters Letter

Figure 2. Coupling behavior of surface plasmon and interference in the 3D plasmonic nanostructure according to the wavelength of an incident
beam. (a) Local field distribution and interference fringe patterns in the 3D plasmonic nanostructure with the same thickness (tAAO = 300 nm) of a
dielectric layer under different wavelengths. When the constructive interference is positioned on the plasmonic component, plasmonic absorption
(case (i) and (iii)) is created. On the other hand, reflection (case (ii)) occurs when deconstructive interference is located on the plasmonic layer.
Reflection spectra (b) from FDTD simulation and (c) from experiments. The critical role of a plasmonic layer is demonstrated by the reflectance
spectrum of the 3D nanostructure with and without a plasmonic gold (Au) layer at the top. The scale bar of the SEM image is 100 nm. (d) Function
of the Al mirror layer at the bottom. Photographs of regions with and without the Al layer in the 3D plasmonic nanostructure. The corresponding
reflectance spectra for each region are shown.

3376 dx.doi.org/10.1021/nl5008823 | Nano Lett. 2014, 14, 3374−3381

Nano Letters Letter

m based on our experimental model (Figure S1a). As shown in

× λ = 2nd cos θ
2 (1) the SEM image, the top of the AAO template was not flat. We
fabricated AAO by two-step anodization in oxalic acid where
Where m is the interference order as an integer larger than zero, the initial pore size (Dp) of AAO was 32 nm and the unit cell
λ is the incident wavelength, n is the refractive index of a thin size (ρ) was 100 nm.24−26 To maintain the open pores in the
film, d is the film thickness, and θ is the angle of light incident plasmonic layer as well as the AAO, the thickness of evaporated
to the thin film. When reflected light experiences a 180° phase gold was set to 20 nm.26 We monitored the optical coupling
change due to the reflection from a medium of higher refractive behavior of surface plasmon and interference in 3D plasmonic
index based on Fresnel conditions, constructive interference nanostructures by changing the wavelength (λ) of an incident
occurs when m is odd, whereas deconstructive interference beam. Figure 2a shows the local field distribution and
takes place when m is even. In the 3D plasmonic nanostructure, interference fringe patterns in the 3D plasmonic nanostructure
we can imagine two cases: constructive interference is matched with a 300 nm-thick dielectric layer (i.e., tAAO = 300 nm)
with the plasmonic layer (Figure 1c(i)), and destructive according to the wavelength of an incident beam in the visible
interference is positioned with the plasmonic layer (Figure spectrum. Interference patterns occurred at different positions
1c(ii)). The enhanced light wave in constructive interference in the 3D plasmonic nanostructure, depending on the
may generate strong plasmonic absorption at a certain wavelength, with bright fringes indicating constructive interfer-
wavelength, as shown in the yellow color of Figure 1c(i). ence and dark fringes showing destructive interference. The
When the wavelength is changed, destructive interference is enhanced light wave of constructive interference created a
formed at the plasmonic layer and may prevent the plasmonic strong nanoplasmonic local field around the plasmonic
absorption due to minimized light at the plasmonic layer, as nanopore (Figures 2a(i) and 2a(iii)), while no nanoplasmonic
shown in Figure 1c(ii). Thus, a reflected wave Ir(λ) with strong field distribution was detected around the plasmonic nanopore
absorption and high reflection peaks can be produced according with deconstructive interference (Figure 2a(ii)). Figure 2b
to the wavelength (Figure 1d). Finally, we could understand shows the corresponding simulated reflectance spectrum from
that optical behaviors by interference could be controlled by the 3D plasmonic nanostructure. Clear absorption minima were
surface plasmons. generated at λ1 and λ3 (Figure 2a(i) and (iii)), whereas strong
Since an extraordinary transmission from plasmonic nano- reflection occurred at λ2 (Figure 2a(ii)). The same optical
hole arrays16 has been reported, many studies regarding behavior was demonstrated with the gold-coated AAO with tAu
nanopore plasmonic structures have been extensively inves- = 20 nm and tAAO = 300 nm (inset SEM image; Figure 2c).
tigated.17−20 However, most of these studies focused on the The importance of the top plasmonic gold layer was
nanofabrication and the characterization of hole arrays such as demonstrated by reflection spectra with significantly reduced
hole periodicity, hole dimensions, and hole shapes. Our 3D absorption (red lines in Figures 2b and c) in its absence, in
layered nanostructure includes a nanopore plasmonic layer, but both the simulation and the experiment. We also exper-
we focus on the coupling behaviors between the plasmonic imentally examined the role of the mirror layer at the bottom of
layer and the interference modes by adopting a dielectric spacer our 3D nanostructure. Figure 2d shows a photograph of a gold-
and a mirror layer. Of course, a thin plasmonic layer on a coated AAO template with tAAO = 220 nm. Before removing the
dielectric spacer with a back reflector has been also introduced Al mirror layer, a yellow color was observed, but a red color was
and showed color patterns, but the light absorption was displayed after removing the mirror layer, thus clearly
controlled by the environmental dielectric materials deposited demonstrating the change of optical properties of the 3D
on plasmonic layer (i.e., nanocomposite layer on a fixed nanostructure by the mirror layer. The optical behavior was
dielectric spacer) by atomic layer deposition (ALD).21 Our completely different in the presence or absence of the mirror
main control parameter is the thickness of the dielectric spacer layer, as shown by the reflection spectra of the 3D
below the nanopore plasmonic layer, thus controlling nanostructure. Without the mirror layer, the 3D nanostructure
interference modes (i.e., destructive or constructive interfer- showed plasmonic absorption at about 500 nm, which is
ence). Previously, the coupling effects between the plasmonic intrinsically created by a nanoporous gold layer. With the
layer and the dielectric film/cavities have been also investigated mirror layer, the 3D nanostructure formed interference patterns
by considering Fabry−Perot modes, but their structure inside the structure, and the interaction between surface
dimensions and material configurations are different with our plasmon and interference created a different plasmonic
3D layered structure, and the Fabry−Perot modes (i.e., absorption position (here, at about 430 nm) based on the
multiple interference) are different in concept than our thickness of the dielectric layer. Thus, constructive interference
interference modes (i.e., construction and destruction at a wavelength of 430 nm was well matched with the
modes).22,23 Generally, the Fabry−Perot interferometer is plasmonic layer at the top in the 3D plasmonic nanostructure
made of a transparent plate with two reflecting surfaces, but with tAAO = 220 nm. We concluded that the optical coupling of
our interference modes can occur from a dielectric layer (i.e., surface plasmon and interference could indeed determine the
AAO) on one reflecting surface (i.e., Al). By adopting a optical response (i.e., absorption or reflectance) at a specific
plasmonic layer on the dielectric layer with a mirror, we could wavelength in the 3D plasmonic nanostructure.
highly enhance the plasmonic absorption due to the coupling Our experimental model for the 3D plasmonic nanostructure
between the constructive interference and the plasmonic layer. allowed us to easily tailor the thickness of a nanoporous
To determine the optical coupling characteristics of surface dielectric layer (i.e., tAAO). The coupling of surface plasmon and
plasmon and interference in a 3D plasmonic nanostructure, 3D interference could be controlled by changing the thickness of
electrodynamic calculations were performed by employing a the dielectric layer at given wavelengths. When the thickness of
finite difference time domain (FDTD) simulation (see the dielectric layer was 100 nm under the incident beam of 380
Methods and Supporting Information). The geometry of the nm, destructive interference was coupled with the plasmonic
3D plasmonic nanostructure for the 3D FDTD simulation was layer, and no nanoplasmonic local field was produced, thus
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Nano Letters Letter

Figure 3. Tunable optical behavior according to the thickness of the dielectric layer at the middle of the 3D plasmonic nanostructure. (a) Local field
distribution according to the thickness of the dielectric layer at the middle at a wavelength of 380 nm. Reflectance spectra for different thicknesses
(tAAO = 100−300 nm) of a dielectric layer (b) from FDTD simulation and (c) from experiments. (d) Color gamut for structural color display based
on the reflectance spectra for 3D plasmonic nanostructures. The photographs show each color according to the thickness of the dielectric layer. The
structural color covers the full visible range as shown.

leading to no absorption (i.e., strong reflectance) as shown in layer was a critical parameter to control the absorption and
Figure 3a(i). On the other hand, when tAAO was 140 or 260 nm reflectance at a given wavelength.
under the same wavelength of 380 nm, the constructive From the 3D simulations, we could determine the optical
reflectance spectra for different AAO thicknesses (Figure 3b).
interference was matched with the plasmonic layer, so that a
To experimentally verify the optical behavior of our 3D
strong plasmonic local field was produced (Figure 3a(ii) and plasmonic nanostructures, we measured the reflectance of 3D
(iii)). Finally, strong absorption could be created at a specific plasmonic nanostructures fabricated by the deposition of gold
wavelength as shown in positions (ii) and (iii) of Figure 3b. on AAO templates with different thicknesses. The AAO
Thus, we concluded that the thickness (tAAO) of the dielectric thickness (tAAO) increased linearly with anodization time,
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Nano Letters Letter

Figure 4. 3D plasmonic nanostructure applications. (a) Design equation to determine the thickness of a dielectric layer where plasmonic absorption
could be created at a given wavelength. (b) Structural color display of “KHU” capitals for “RGB” colors by tailoring the thickness of the AAO
dielectric layer. The scale bar of the SEM images is 200 nm. (c) Flexible 3D plasmonic nanostructure. Angle dependency of 3D plasmonic
nanostructures for “RGB” colored samples. (d) Color gamut and (e) percent reflectance.

allowing it to be monitored (Figure S2). AAO templates with shifted up to approximately 100 nm due to the lower effective
thicknesses of 100, 120, 140, 260, and 300 nm were created. dielectric constant of the AAO with larger pores.27,28 Our
The evaporated gold thickness was 20 nm in order to produce a findings clearly demonstrated that the optical behavior of 3D
nanoporous plasmonic layer. The thicker gold blocked the plasmonic structures could be controlled by tailoring the
AAO pores, and the thinner gold formed a discontinuous film.
As shown in Figure 3c, the absorption minimum was red- geometry of the AAO dielectric layer.
shifted, and the secondary absorption minimum appeared as We calculated the thickness of the dielectric layer in the 3D
the AAO thickness increased, showing good agreement with plasmonic structure needed to create strong absorption at a
the theoretically simulated spectra (Figure 3b). Interestingly, given wavelength based on eq 1 and the simulation results in
the 3D plasmonic nanostructures produced distinct structural Figure S4. The effective refractive index of the AAO dielectric
colors from red to purple, covering the full visible range (Figure layer can be determined by the Maxwell-Garnett equation29 in
3d). The colors were very well matched with the reflectance which the volume fraction of air and alumina is taken into
spectra of the 3D plasmonic structures and could be tuned by account. For an AAO pore size of 32 nm, the effective refractive
tailoring the AAO thickness (tAAO). Without a plasmonic layer
in the 3D plasmonic structures, such a brilliant color display index was determined to be 1.7 by using the refractive index of
could not be produced. We also explored the effect of pore size alumina of 1.77.30−32 When the Al thickness is 20 nm (tAl) at
of AAO on optical behavior (Figure S3). As the pore size the central position (Figure S2) and the light wave is vertically
increased from 32 to 80 nm, the absorption peak was blue- incident to the structure, eq 1 can be modified as follows:
3379 dx.doi.org/10.1021/nl5008823 | Nano Lett. 2014, 14, 3374−3381
Nano Letters Letter

m ⎛ λ − 400 ⎞ angle of ±20° due to the blue-shift of the reflected light at

× λ = 2 × 1.7 × ⎜tAAO + tAl − ⎟
2 ⎝ 4 ⎠ (2) 700−800 nm. On the other hand, the percent reflectance of the
“G” sample was greatly reduced from the viewing angle of ±10°
The third term in the parentheses is the calibration factor, since the major reflected light at 450−550 nm escaped from the
which may arise from the geometry of our 3D nanostructure as visible range by the blue-shift of the reflection spectrum.
the wavelength increases. The maximum absorption is Therefore, we concluded that the total reflection intensity and
determined when the interference order, m, is odd. Figure 4a color display were critically dependent on the viewing angle.
shows the critical thickness (tAAO)c of the AAO dielectric layer In conclusion, we have theoretically and experimentally
that yields the maximum absorption at a given wavelength. The demonstrated plasmonic optical interference in layered 3D
critical AAO thicknesses determined by eq 2 showed good plasmonic nanostructures. The plasmonic layer at the top
agreement with the experimental results which were played a critical role in creating plasmonic absorption, and the
determined by the absorption positions (Figure 3c). By using mirror layer at the bottom provided a clear interference pattern
eq 2, 3D plasmonic structures could thus be designed where a in the nanostructure. Plasmonic absorption and reflection were
strong nanoplasmonic local field can be obtained at a given controlled by the thickness of the dielectric layer at a given
wavelength, to produce highly tunable nanoplasmonic wavelength. We developed a design equation to determine the
structures. thickness of a dielectric layer which can create strong
Based on the coupling of surface plasmons and interference absorption at a given wavelength. Furthermore, we demon-
from the 3D plasmonic structures, we designed RGB patterns strated that plasmon-enhanced structural colors could be
as shown in Figure 4b. A clear red (R) color was found for the obtained from the 3D plasmonic structures, and we explored
3D plasmonic structure with an AAO thickness of 60 nm, and their flexible design and angle dependency. Such 3D plasmonic
blue (B) and green (G) colors were produced by the 3D nanostructures based on the optical coupling of surface
plasmonic structures with tAAO = 120 and 140 nm, respectively, plasmon and interference offer a promising platform for next-
generation nano/biophotonic devices.

■
as shown in the reflectance spectrum (Figure S5b). Thus, the
capitals “KHU” could be produced with RGB colors. The
detailed fabrication process is described in Figure S5a. To date, ASSOCIATED CONTENT
most color tuning has relied on color filters or sophisticated * Supporting Information
S
methods for controlling the pattern geometry at the micro/ Simulation and fabrication details, pore size effect, theoretical
nanoscale.33−36 In contrast, our 3D plasmonic structure approach for governing equation, and other supporting images.
provides a remarkably simple way of tuning the color display This material is available free of charge via the Internet at
in the full visible range, simply by tailoring the thickness of a http://pubs.acs.org.
dielectric layer.
Nanoporous AAO templates can be formed on a flexible
substrate. After deposition of 200 nm thick Al on a
■ AUTHOR INFORMATION
Corresponding Authors
polyethylene terephthalate (PET) substrate, the first-step *E-mail: [email protected].
anodization of Al provides a nanoporous AAO with an Al *E-mail: [email protected].
layer at the bottom. Since the uniformity of the nanopore array *E-mail: [email protected].
and the pore size of AAO on a flexible PET substrate are Author Contributions
slightly different from the AAO templates fabricated by two- D. Choi and C. K. Shin contributed equally.
step anodization, the resonance wavelengths were different, and
Notes
this is under investigation. However, we were able to find the
The authors declare no competing financial interest.

■
same coupling behaviors of surface plasmon and interference as
well as the brilliant color display from the flexible 3D plasmonic ACKNOWLEDGMENTS
nanostructure. Figure 4c shows a photograph of the gold-
coated AAO on PET that exhibits the flexibility with a This work was financially supported by the Energy Interna-
structural color. The size was 3 × 3 cm2 (Figure S6), but it tional Collaboration Research & Development Program of the
could be easily scaled up to over a 4 in. wafer size. Korea Institute of Energy Technology Evaluation and Planning
We examined the angle dependency of color display of the (KETEP) funded by the Ministry of Knowledge Economy
3D plasmonic structure. Figure 4d shows the color gamut of (MKE) (2011-8520010050), by Basic Science Research
“R”, “G”, and “B” samples according to the viewing angle. To Program through the National Research Foundation of Korea
clearly follow the color change of each sample when the (NRF) funded by the Ministry of Education, Science and
viewing angle was varied, we used the counter color dots (i.e., Technology (2013R1A1A2063798), and by a grant from the
blue for “R” sample, red for “G” sample, and green for “B” Kyung Hee University in 2013 (KHU-20130693).
sample) in Figure 4d. The RGB colors were converged to white
via different color domains. Figure 4e shows the percent
reflectance (defined as the intensity ratio of the reflected light
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