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Broadband and mid-infrared absorber based on

dielectric-thin metal film multilayers


Timothy D. Corrigan,1,2,3,6, Dong Hun Park,2,4,7, H. Dennis Drew,1,2 Shy-Hauh Guo,2,5
Paul W. Kolb,2 Warren N. Herman,2 and Raymond J. Phaneuf1,2,4,5
1

Department of Physics, University of Maryland, College Park, Maryland 20742, USA


2

Laboratory for Physical Sciences, College Park, Maryland 20740, USA

3
4
5

Department of Physical Sciences, Concord University, Athens, West Virginia 24712, USA

Department of Electrical Engineering, University of Maryland, College Park, Maryland 20742, USA

Department of Materials Science and Engineering, University of Maryland, College Park, Maryland 20742, USA
6

e-mail: tdcorrigan@concord.edu
7

e-mail: leomac@umd.edu

Received 28 September 2011; revised 4 January 2012; accepted 4 January 2012;


posted 5 January 2012 (Doc. ID 155325); published 7 March 2012

We propose a periodic multilayer structure of dielectric and metal interlayers to achieve a near-perfect
broadband absorber of mid-infrared radiation. We examine the influence of four factors on its performance: (1) the interlayer metal conductance, (2) the number of dielectric layers, (3) a nanopatterned antireflective layer, and (4) a reflective metallic bottom layer for backreflection. Absorption characteristics
greater than 99% of the 300 K and 500 K blackbody spectra are found for the optimized structures. Incident angle and polarization dependence of the absorption spectra are examined. We also investigate the
possibility of fabricating a nanopatterned antireflective layer to maximize absorption. 2012 Optical
Society of America
OCIS codes: 220.4241, 230.1480, 230.4170, 310.1210, 310.4165, 310.6845.

1. Introduction

For economic and environmental reasons, the prospect of converting waste heat from engines or factories into usable energy is receiving considerable
attention [17]. Other potential heat sources include
infrared (IR) radiation from the Sun [3] or the Earth
that could be exploited, for instance, to provide
electrical power to a satellite in space. A practical,
high-efficiency broadband absorber would find applications in the collection of radiant energy, acting as
the front end of energy harvesting devices from
remote or nearby heat sources.

1559-128X/12/081109-06$15.00/0
2012 Optical Society of America

There has been a long history of design and fabrication of structures for tailoring the reflectance
and absorption of light in various parts of the spectrum, each with their own particular strengths and
weaknesses. Periodic metal gratings tend to be narrow band and produce both directional and polarization dependent absorption [8,9]. Metamaterial
structures are typically bandwidth limited or require multiple layers [1019]. Recently, carbon nanotube forests have been shown to outperform
more traditional, highly porous blacks, but both
of these types of coatings are quite fragile [20].
Quarter-wavelength structures for thermal detectors, based upon the need to minimize the thermal
mass and thus keep the number of layers to a minimum, produce less than optimal performance
[2124].
10 March 2012 / Vol. 51, No. 8 / APPLIED OPTICS

1109

In this paper, we describe a new approach based


upon a multilayer structure consisting of dielectric
layers interspersed with thin metallic layers to
realize broadband mid-infrared absorption [25]. Metallic layers have previously been used for tailoredabsorption devices [2124], but the absorption in
thick metal layers is accompanied by significant reflection and/or transmission, reducing the absorption
efficiency. In our proposed absorber structure, we use
a number of thin metal layers in which each successive layer absorbs a small fraction of the radiant
power over a wide spectral range in the mid-IR while
minimizing the reflection. Such a device should be
relatively easy to fabricate and result in a robust
structure that has excellent thermal transfer properties (relatively high thermal conductivity), making
it attractive for energy harvesting applications.
Our calculations, presented below, predict that it
will absorb over a very broad frequency range, nearly
independent of polarization and over a large range of
angle of incidence, allowing for collection of radiant
heat across a much wider range in the IR than previous methods. In particular, we predict that broadband absorption efficiencies of over 99% should be
attainable in the mid-infrared.
2. Design of Absorber

The proposed blackbody absorber is based on a multilayer geometry consisting of transparent dielectric
layers interspersed with thin metallic layers for
absorption. Each successive metallic layer absorbs
a small fraction of the radiation. For normal incidence, Bragg reflection peaks will occur only near
wavelengths given by ! 2ndm, where n is the index of refraction of the dielectric layers, d is the
thickness of the dielectric layers, and m is a positive
integer. Tuning the absorption to a specific frequency
range can be performed by choosing the dielectric
thickness such that the range of interest (i.e., the
maximum desired absorption) lies in the middle of
the range between Bragg reflection peaks. The reflection peaks can be made narrow by using a large number of layers. In the spectral region between the
narrow reflection peaks, the structure absorbs the
radiant energy by Joule heating in the metal films.
As we show below, overall performance can be
further enhanced by the use of both an antireflective
(AR) coating as the first layer and a backreflective
layer next to the substrate.
The choice of the dielectric is governed by the
requirement that it be transparent over a wide
frequency range. Many materials can serve this
purpose. However, barium fluoride (BaF2 ) is particularly attractive since it is nearly impedance matched
with air, with an index of refraction of about 1.4,
and has a low imaginary component [26], making it
useful to collect radiant energy over a wide range of
frequencies in the IR.
For the absorbing layer, a thin conducting film
with a frequency-independent admittance would be
the ideal choice. The normalized optical admittance
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APPLIED OPTICS / Vol. 51, No. 8 / 10 March 2012

of a metal film of thickness d is y ! Z0 R0 ! Z0 d,


where Z0 is the impedance of free space, R0 is the
sheet resistance, and is the metal resistivity. However, the dispersion in metals limits their useful frequency range to max such that max < 1, where 1
is the carrier relaxation rate. For the low admittance
required to minimize reflection (loss) from the metal
layer, the thickness of the film is less than
the carrier mean free path (l0 ! vF 0 , where vF is
the Fermi velocity of the carriers and 0 is the bulk
relaxation time). Under these conditions, the relaxation rate in the film is controlled by the scattering of
carriers at the interfaces so that 1 10 " vF d
[27]. Assuming F 0 d, the relaxation rate 1 is
approximately vF d. Therefore the increased relaxation rates in thin metal layers extend the useful
frequency range for the absorber. As a result, it
may not be critical to use a high-resistivity metal
for the absorptive layer, thereby increasing the fabrication options. However, as the admittance of such
thin films will depend on the details of fabrication,
we have performed our analysis using the optical
constants n and k of NiCr [28] for the absorbing layer,
which satisfies the condition max 1 in the bulk
for a 500 K blackbody, for example. The calculation
method is described below. We also examined the effects of a reflective silver metal layer between the
substrate and the first BaF2 layer for backreflection
into the multilayer structure.
3. Calculations

To determine the absorption characteristics of the


proposed structure, we have calculated the reflectance and transmittance for s and p polarizations.
We use rigorous expressions that account for multiple reflections inside the film as well as the angle
of incidence, as described briefly here and in more
detail elsewhere [2931]. Assuming that the incident
light is an s (TE)- or p (TM)-polarized plane wave,
both the reflection (r) and transmission (t) coefficients are calculated based on the iteration of the
Airy formula in the one-dimensional multilayered
structure [2931]. The absorbance, A ! 1 T R !
1 jtj2 jrj2 , is then calculated, where T and R are
the transmittance and reflectance, respectively. Note
that, for the calculation of absorbance, only layer
thicknesses and n and k values are necessary. For
the n and k values of NiCr, the HagenRubens relations were used, which was shown to be a good fit for
thin films of NiCr (10100 nm) bypBly
!!! and Cox [28],
and has the form of n ! k ! 3.61 . For the optical
parameters of Ag, we used the LorentzDrude model
with model parameters given in [32].
4. Results and Discussion

For the calculations illustrated in Fig. 1, we assumed


50 layers of BaF2 and NiCr. The figure shows the
absorption for two different thicknesses of dielectric
layers, demonstrating the ability to tune the structure depending on the desired application; these
calculations include the effect of an AR layer

100 30 20

100 30 20

AR
Multilayer
Ag

Sub + Multilayer
Sub + Ag + Multilayer
Sub + Multilayer + AR
Sub + Ag + Multilayer + AR

Fig. 1. (Color online) Calculated absorption versus frequency for


a BaF2 NiCr multilayer device made up of 50 layers of BaF2 whose
thicknesses are varied to optimize absorption of a blackbody radiation heat source at (solid red curve) 500 K and (solid black curve)
300 K. The dashed curves show the intensity of the blackbody spectra at each temperature. For the red curve, the BaF2 layer thicknesses are 1.34 m with an AR layer 1.56 m thick. For the black
curve, the BaF2 layer thicknesses are 1.8 m with an AR layer
2.1 m thick. The NiCr layer thickness is 18 for both cases.

(nAR ! 1.2), as discussed further below. Significantly,


near unity absorption is found for a broad frequency
range in both cases. The black solid curve in Fig. 1 is
for a structure in which the layer thicknesses are
tuned for a blackbody spectrum for a source at
500 K (black dashed curve), a typical ambient temperature of a heat engine. Because of the asymmetry
of the blackbody spectrum, the optimum integrated
absorption is achieved by choosing the peak absorption at 40 THz instead of at the peak of emission
spectrum at 30 THz. In this case, the first reflection
peak is chosen corresponding to 80 THz, and to a
first absorption peak at 40 THz, leading to dielectric
layers of thickness d ! 2n ! 1.34 m. The AR
coatingpthickness
is chosen as d ! 4nAR, where
!!!!!!!!!
nAR ! no n 1.2 (no ! 1, n ! index of refraction
for the dielectric layers) and is the desired peak
absorption wavelength [33,34], in this case dAR !
4nAR ! 1.56 m. In the solid red curve of Fig. 1,
we show the results for an absorber whose parameters are tuned for 300 K radiation (dashed red
curve); this corresponds to the temperature of the
Earth, making it ideal for a satellite harvesting
energy from Earth glow. The peak absorption is
chosen as 30 THz, leading to a dielectric layer of
1.8 m and to an AR layer thickness of 2.1 m.
The NiCr layer thickness for both cases is 18 .
We can also express these results in terms of the
efficiency of the absorber for a given blackbody spectrum, which is given by the integrated absorbed
power/area divided by the total incident intensity.
Integration over the range of 10 to 70 THz yields
an efficiency of 0.9899 for a 500 K blackbody and
of 0.9915 for 300 K.

Fig. 2. (Color online) Calculated absorption versus frequency for


a multilayer structure with 21 BaF2 layers (green, bottom curve)
(d ! 1.34 m, NiCr layer thickness 18 ) with the addition of an
AR layer whose index of refraction is 1.2 and thickness 1.56 m
(black), a Ag layer 5 nm in thickness between the substrate and
first BaF2 layer (blue), and both AR and Ag layers of thicknesses
as in the above cases (red, top curve).

Figure 2 shows the calculated effects of both the


AR layer and of an Ag reflective back layer. The
thickness of the Ag reflective layer was chosen to be
just large enough to reflect 90%, 10 nm. The number of dielectric layers in the structure of Fig. 2 is
N ! 21, and the layer thicknesses are tuned to
produce a first reflection peak at 80 THz and a peak
absorption near 40 THz (d ! 1.34 m, NiCr layer
thickness 18 ). The results predict that an AR coating will provide a significant improvement in the total absorption. The addition of the Ag layer (compare
the green with the blue as well as the black with the
red) is also predicted to improve the absorption efficiency, but the backreflection enhances interference
effects across the device, causing larger oscillations
at frequencies corresponding to the total dielectric
thickness.
In order to probe the dependence of the absorption
spectrum on the number of layers N within the device, we performed calculations for N ! 5, 11, and
21 layers with an AR and Ag layer; layer thicknesses
were optimized for peak absorption at 40 THz in each
case. The results are shown in Fig. 3. The value of the
maximum absorption slightly increases with increasing N; however, there is little improvement from
N ! 11 layers to N ! 21 layers, with both giving over
0.99 absorption at 40 THz. Furthermore, it was found
that the optimal metal admittance varied with the
number of layers. The optimal values of the NiCr
thickness (admittance) required to obtain the highest
absorption corresponded to approximately 30
(0.75), 25 (0.63), and 18 (0.45) for N ! 5, 11,
and 21 layers, respectively [35].
These calculations were for normal incidence of
light. This is adequate for a point source at great
distances compared with the lateral dimensions of
10 March 2012 / Vol. 51, No. 8 / APPLIED OPTICS

1111

100 30 20

N=5
N = 11
N = 21

s- or ppolarized
plane wave

Absorber

Average
p-wave
s-wave

Fig. 3. (Color online) Calculated absorption versus frequency for


a device in which the number of BaF2 layers is N ! 5, 11, and 21
layers. The BaF2 layers are 1.34 m, nAR ! 1.2, dAR ! 1.56 m,
dAg ! 5 nm. The NiCr thickness (admittance) values are 30
(0.75), 25 (0.63), and 18 (0.45), respectively.

the device, but for many applications, the dependence of the absorption on the incident angle is important. Figure 4 shows the calculated absorption
versus incident angle for s and p polarizations as
well as the unpolarized (average of two polarization
cases) as a function of angle for (a) 20 THz, (b) the
peak frequency 40 THz, and (c) 60 THz. The plots
in Fig. 4(b) predict that, at 40 THz, the absorption
will remain greater than 0.95 in each case until the
angle of incidence approaches 60. The drop off of absorption with incident angle is quicker for 20 THz,
dropping to 0.95 for approximately 40 for s polarization and approximately 72 for p polarization. But at
60 THz, it can be seen that, although the absorption
is slightly lower near normal incidence, 0.97, it remains greater than 0.95 for both polarizations until
after 70. The total integrated absorption over all angles is 89%, 92%, and 94% for 20, 40, and 60 THz,
respectively.
From this analysis, we expect that the absorber
should be useful over a wide range of frequencies
and solid angles of the incident radiation. It will
be limited at high frequencies by the metal response
as sd optical interband transitions become important or when is no longer small. Its utility at
low frequencies is limited only because the physical
thickness scales with the wavelength. However, it
should be quite generally useful for center frequencies in the 10100 THz range.
5. Tunable Effective Permittivity Using Nanopatterned
Films

One of the means for optimizing the performance of


the absorber is to include an AR top layer. This requires pa!!!! material with an index of refraction
nAR ! n, where n is the dielectric index of refraction of the insulator used in the multilayer absorber.
This requires a material with an index of approximately 1.2, as mentioned above. Matching this index
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APPLIED OPTICS / Vol. 51, No. 8 / 10 March 2012

Fig. 4. (Color online) Calculated incident angular dependence of


the absorption for a 21 multilayer structure (dBaF2 ! 1.34 m)
with both a 1.56 m AR layer and a 10 nm Ag bottom layer for
s and p polarizations at (a) 20 THz, (b) the peak frequency
40 THz, and (c) 60 THz.

of refraction requirement for a broad frequency range


is difficult from a materials point of view. One seeming option for controlling the index of the AR layer
is a nanoporous material [36] where an effective index of refraction lies between that of the material
and that of the voids. This can be modeled as a
two-phase material described by effective-medium
theory (EMT), where the dielectric serves as the medium and a gas ( ! 1 for vacuum) fills the inclusions
(holes/trenches) [3642]. However, conventional porous films such as nanoporous silica have indices of
refraction that are highly dispersive in the mid-IR
range [36], and other materials such as porous Si
do not match the low index of refraction required
[37,38]. We propose that by, patterning the top dielectric layer using standard lithographic techniques, an
effective permittivity can be achieved, as in the case
of nanoporous materials [40,41]. The effective permittivity is thus tunable because it simply depends
on the volume fraction of inclusions, and using the
same material as the dielectric layers (BaF2 in the
above case) matches the frequency range requirements. As described below, we find that a simple
average of the permittivity of the dielectric and
vacuum yields a good approximation to the effective
permittivity of this layer.
In order to test whether the effective permittivity
eff
r used in the previous simulations for an AR layer
can be fabricated using a single patterned dielectric
layer, we carried out finite element method (FEM)
simulations for a patterned BaF2 AR film 1.56 m
thick. We modeled the effect of the pattern by including a square array of air-filled cylindrical holes, with


20

the use of a patterned AR layer to create a tunable


effective permittivity to optimize the absorption
characteristics. We are currently investigating the
fabrication of these structures, which may enable efficient heat collection for thermal electric devices.

: analytic
30 : analytic

45 : analytic
0 : COMSOL
30 : COMSOL
45 : COMSOL

Fig. 5. (Color online) The filled circles show simulated incident


angular dependence of the absorption spectrum using COMSOL
software for a single layer 1.56 m thick AR film composed
of BaF2 , but containing a square pattern of cylindrical holes
100 nm in diameter, normal to the surface, and separated by a
pitch yielding 50% holes/50% BaF2 , shown for incident angles of
0, 30, and 45. The solid lines show calculated angular incidence
dependence of the absorption spectrum using the Airy formula
based on multilayer structures for an AR film with a permittivity
given by the volume fraction-weighted average of BaF2 and holes
1.56 m thick for the same three incident angles.

axes normal to the surface, 100 nm in diameter and


with a pitch corresponding to an area fraction of
50% over an area of 50 m 50 m with absorbing
boundary conditions. These were done at both normal incidence and at a variety of angles of incidence.
The results for s polarization are shown by solid circles in Fig. 5. For comparison, the solid curves in
Fig. 5 show the results of analytic solutions based
on Fresnel equations and the Airy formula for a
one-dimensional multilayer structure [2931] for s
polarization. The effective permittivity used for the
analytical solutions was obtained by taking the
average of the permittivity of the dielectric material
( ! n2 ! 1.96) and the holes ( ! 1), yielding
eff
r ! 1.48. As shown in Fig. 5, simulated reflectivity
curves show good agreement with those from the
analytic solutions, even at 45, confirming the validity of the EMT. Similar good agreement was obtained
for p polarization (not shown).
6. Conclusion

Our calculations predict that a broadband nearperfect blackbody absorber can be realized by using
a multilayer structure consisting of alternating
layers of BaF2 and NiCr. The absorption for 500 K
blackbody radiation is predicted to be greater than
0.99 for the optimized structure. Optimization includes tailoring four main factors: (1) the interlayer
metal thickness, (2) the number of dielectric layers,
(3) the AR layer, and (4) a thick metal underlayer for
backreflection and second pass. We also investigated

General correspondence and queries for the numerical simulation should be addressed to Corrigan
and Park.
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