Dual-Band Metamaterial Absorbers in the Visible and Near-Infrared

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C: Plasmonics; Optical, Magnetic, and Hybrid Materials

Dual-Band Metamaterial Absorbers in the Visible and Near-Infrared Regions Haixia Xu, Lizhong Hu, Yanxin Lu, Jun Xu, and Yihang Chen J. Phys. Chem. C, Just Accepted Manuscript • DOI: 10.1021/acs.jpcc.9b00434 • Publication Date (Web): 29 Mar 2019 Downloaded from http://pubs.acs.org on March 29, 2019

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The Journal of Physical Chemistry

Dual-Band Metamaterial Absorbers in the Visible and Near-Infrared Regions Haixia Xu, Lizhong Hu, Yanxin Lu, Jun Xu, and Yihang Chen * 1,2

1

1

1

1

1,

Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials, School

of Physics and Telecommunication Engineering, South China Normal University, Guangzhou 510006, China.

2

School of Information Science and Technology, Zhongkai University of Agriculture and

Engineering, Guangzhou 510225, China. *Email: [email protected] ABSTRACT: Metamaterial absorbers have attracted much attention due to their unique ability to achieve nearly perfect absorption in compact structures. Most of the reported metamaterial absorbers exhibit only one absorption band in a specific frequency range, absorbers with two or more absorption bands in the visible and near-infrared regions are desired in many applications. Here, we propose and demonstrate a dual-band metamaterial absorber comprised of an aluminum film, a silica spacer, and a periodic array of aluminum nanodisks. The two absorption bands in the visible and near-infrared range are respectively attributed to the excitation of propagating surface plasmon polariton and localized magnetic polariton in the proposed nanostructure. Large area and high coverage samples of the designed structure were fabricated using a simple and cost-effective colloidal lithography nanofabrication method. We show that the positions of the absorption bands can be separately adjusted by changing the diameter or the lattice constant of the aluminum

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nanodisks on the top of the metamaterial absorbers. Our design of compact and efficient absorbers would find great utility in a variety of applications including filters, sensors, solar cells, thermal emitters, and imaging devices. INTRODUCTION Electromagnetic absorbers have drew much attention since they are crucial for many applications involving thermal emitters , sensors , solar cells , filter , imaging devices , and multiplexing detector 1

2

3

4

5

arrays . Two main types of microstructures were used in the design of artificial absorbing media. 6

One is the Fabry-Perot-type thin film structure, where a wavelength-scale-thick lossy dielectric film backed by a metal or Bragg reflector forms a Fabry-Perot cavity and the absorption gradually accumulates within the lossy dielectric layer. For this type of absorber, the frequencies and the intervals of the absorption bands, determined by the resonance condition of the cavity, are not convenient to adjust, which limits their applications. Another type of absorbing microstructures is metamaterial (MM) , where surface plasmon resonances inside the metallic nanostructures can 7

lead to narrow absorption bands. The MM-based absorbers offer benefits over the thin film absorbers such as further miniaturization, high absorption efficiency, and the tunability of the absorption bands. Recent advances in MM research together with the development of nanofabrication techniques make MM-based absorbers achievable in different frequency ranges from microwave to visible . 8-13

In the past decade, many designs of the MM absorbers have been proposed. One common design is the metal-dielectric-metal triple-layer stack, in which by tailoring the size and the periodicity of the metal nanostructures, the incident light gets absorbed due to the excitation of the plasmonic resonances. However, most of the MM absorbers exhibit only one resonant absorption band , 14-17

absorbers with two or more absorption bands

18-22

are desired in many applications such as chemical


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and biomedical sensing. Recently, several plasmonic MMs with more than one absorption band were demonstrated. For examples, plasmonic absorber metasurfaces were obtained at mid-infrared wavelengths and their absorption bands are originated from the localized surface plasmon resonances , Au-disks/SiO2/Au-film nanostructures were designed to exhibit absorption bands 23

which are due to the excitation of both the localized and propagating surface plasmons , metal24

insulator-metal absorber configuration supporting gap plasmon resonances were proposed and used for plasmonic color printing , dual-band THz MM absorber was realized by means of electric 25

and magnetic dipole resonances . In this paper, we propose a design of dual-band MM absorber 26

where the two absorption bands at visible and near-infrared wavelengths are respectively attributed to the excitation of propagating surface plasmon polariton (SPP) and localized magnetic polariton (MP). Colloidal lithography nanofabrication method was used to fabricate the samples of the dualband MM absorber. Compared with other nanofabrication techniques, our fabrication method is scalable, cost-effective, and allows for wafer-scale production. Our results show that the positions of the two absorption bands can be separately adjusted by changing the structural parameters of the proposed absorbers. SIMULATION MODEL The schematic of the proposed MM absorber is shown in Figure 1(a). The designed structure can be seen as a metal-dielectric-metal stacked system along the z direction. For the top Al nanodisk array, the lattice constant is a, the diameter and height of the nanodisks are D and h, respectively. A silica layer with the thickness of t is embedded between the top Al nanodisks and the bottom Al film. The thickness of the Al film is set as 100 nm to prevent the transmission of light. To evaluate the absorption performance, we perform finite-difference time-domain (FDTD) simulations with



periodic boundary conditions on the trilayer stacked nanostructure. The absorptance (A) of the designed structure is determined by the reflectance (R) as A = 1 ‒ R since the transmittance is zero. Figure 1(b) shows the reflection and absorption spectra of the MM absorber at normal incidence. The geometric parameters are chosen as follows: a = 500 nm, D = 200 nm, h = 24 nm, and t = 50 nm. It is seen that two reflection dips, corresponding to two absorption peaks, appear at 463 and 798 nm, respectively. The reflectance of the first reflection dip at 463 nm is lower than 0.08, accordingly, the absorptance of the first absorption peak is over 0.92. The reflectance of the second reflection dip at 798 nm reaches almost 0, meaning that a nearly perfect absorption peak exists.

Figure 1. (a) Schematic of the MM absorber. (b) Simulated reflectance and absorptance vs wavelengths for the absorber design with a = 500 nm, D = 200 nm, h = 24 nm, and t = 50 nm.

To reveal the physical mechanism of the dual-band absorption, we simulated the field distributions and the current density inside one unit cell of the designed MM structure at the wavelengths of the two absorption peaks, as shown in Figure 2. Figure 2(a), 2(c) and 2(e) show the electric field, current density and magnetic field distributions at the wavelength of 463 nm. It is seen that the electric field is mainly localized at the edge of the upper surface of the Al nanodisk, while the magnetic field is significantly enhanced not only at the upper surface of the Al nanodisk,


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but also in the gaps between the nanodisks. These field patterns are similar to those of the surface plasmon propagating along a metal-dielectric interface, which indicates that the absorption peak at 463 nm originates from the excitation of the SPP. Figure 2(b), 2(d) and 2(f) respectively show the electric field, current density and magnetic field distributions at the resonant wavelength of 798 nm. It is seen that the electric field in the xz-plane is mainly localized on the two sides of the Al nanodisk. The currents in the top Al nanodisk, the SiO2 layer, and the bottom Al film form a loop, generating a strong magnetic field along the y direction, which is the signature of the MP resonance. Therefore, MP resonance should be responsible for the absorption band at longer wavelengths. In addition, as shown in Fig. 1(b), the absorption band corresponding to the MP resonance is fairly broad and its spectral line shape is a bit strange. The reason is that the refractive index of aluminum increases significantly and reaches a maximum at around 800 nm , resulting in 27

the absorption enhancement of the Al-based nanostructure. Such an absorption enhancement effect broadens the absorption band at longer wavelengths.



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Figure 2. Simulated electric field, current density, and magnetic field distributions at the wavelengths of (a, c, e) 463 nm and (b, d, f) 798 nm corresponding to the two absorption peaks in Figure 1(b).

EXPERIMENT SECTION Chemicals and Reagents. Polyacrylic acid (PAA, M = 1800, 2 wt%), Polystyrene (PS, M = v

w

192000, 3 wt%) and Silica spheres of diameter 500 nm were purchased from Sigma-Aldrich. HF


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solution, acetone, chlorobenzene, ethanol absolute, deionized water, concentrated sulfuric acid were used in the experiment processes. Fabrication of the MM absorbers. The proposed MM absorbers were fabricated via an inverted hemispherical colloidal lithography method . The fabrication scheme is shown in Figure 28

3. Firstly, a cleaned silicon substrate was spin coated, in turn, with a sacrificial PAA film at 1000 rpm for 37s, and a PS film at 2500 rpm for 37s. Then, surface modification was made by oxygen plasma treatment for 1 minute to improve the hydrophilicity of the PS surface. Secondly, a self-assembled

29,30

periodic array of silica spheres was obtained by spinning-coating

5 wt% monodisperse silica spheres on the surface of the PS film at 600 rpm for 37 s. Then, the sample was placed on the hotplate with a temperature of 116 °C for 7 min to make the top layer of silica spheres embed into the PS film with a depth equal to the radius of the spheres.

Figure 3. Fabrication scheme of the proposed dual-band MM absorber.



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Thirdly, after being immersed in a 5 wt% HF solution for 2 min to remove the embedded silica spheres, the sample was immersed in the distilled water, making the PAA film dissolved. Then, a PS film with a uniform array of hemispherical dimples floated on the water surface by carefully scratching the edge of the wafer and turning over the sample. Fourthly, a cleaned quartz plate was deposited, in turn, by a 100-nm-thick Al layer and a 40nm-thick SiO layer through magnetron sputtering in the same vacuum chamber. The deposition 2

rate for Al and SiO is R ≈ 0.2 nm/s and R ≈ 0.1 nm/s, respectively. Next, the floating patterned 2

Al

SiO2

PS film was transferred onto the quartz substrate pre-coated with the Al and SiO layers. Then, 2

oxygen plasma etching was employed to gradually etch the surface of the PS film in a downward direction for creating holes with desired sizes at the PS film. The oxygen flow was set at 6 sccm and the applied power was 100 W. The etching rate was about 10 nm/min. After these steps, the air-holes-mask was obtained. Finally, an Al layer was deposited on the mask in a normal direction by magnetron sputtering. Next, the sample was immersed in chlorobenzene at 60 °C for 60 min and then, was sonicated for 20 s to remove the PS film. Because the size of the holes is big at the bottom and small at the top, the mask is particularly suitable for a lift-off process. After that the lift-off process, an array of Al nanodisks was formed on the top of the sample. The scanning electron microscope (SEM) images of the samples are shown in Figure 4. The diameters of the Al nanodisks in the samples corresponding to Figure 4 (a) and 4(b) are about 178 and 395 nm, respectively. For both samples, the lattice constant and the height of the Al nanodisks are 500 nm and 24 nm, respectively. It can be seen from Figure 4 that the patterns on the samples show excellent symmetry. The ring traces on the surface of the sample in Figure 4 (a) are a small


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amount of residual PS film. Due to the nature of colloidal lithography, the pattern has a hexagonal lattice and is short-range ordered in different orientations.

(a)

(b)

Figure 4. SEM images of the fabricated MM absorbers where the diameters of the Al nanodisks are (a) 178 nm and (b) 395 nm, respectively. The lattice constants of the nanodisk arrays in the two samples are the same a = 500 nm.

Compared to another colloidal lithography fabrication method where reactive ion etching is involved , our method is more efficient because it avoids chlorine pollution during the reactive22

ion etching processes. Moreover, our fabrication method is cost-effective, as the air holes mask of different dimensions can be obtained after oxygen plasma etching without changing the diameter of the SiO2 spheres. In addition, the bottom of the holes is much larger in diameter than the top, which makes the mask especially suitable for a standard lift-off process.

RESULTS AND DISCUSSION To characterize the fabricated MM absorbers, we measured the absorptance of the samples by LAMBDA 950 UV/VIS spectrometer. Figure 5 shows the absorption spectra of the dual-band MM absorber with a = 500 nm, h = 24 nm, t = 40 nm, and different diameter D of the Al nanodisks. As shown in Figure 5 (a), two measured absorption peaks appear at 460 and 772 nm, respectively,



with the absorptance of 0.93 and 0.88 for the absorber sample with D = 178 nm. As D increases to 198 nm, the measured absorption peaks shift to 470 and 802 nm, as shown in Figure 5 (b). When D changes to 238 nm, the absorption peak at longer wavelength has a significant shift to 982 nm while the absorption peak at shorter wavelength shifts only a bit to 480 nm, as shown in Figure 5 (c). The FDTD simulated absorption spectra of these absorber samples are also shown in Figure 5. Overall, the measured results agree well with the simulations. Compared to the simulated results, the measured absorption coefficients at the two absorption peaks are lower, which is mainly due to the deviations of the sample structures from the simulation models. As discussed in Section 2, the absorption peak at shorter wavelength results from the excitation of the SPP and thus, should be sensitive to the lattice constant, but not to the nanodisk diameter of the Al nanodisk array. Therefore, as shown in Figure 5, the position of the absorption peak at shorter wavelength remains almost invariant with the changes of D. On the other hand, the absorption peak at longer wavelength originates from the MP resonance, and consequently the peak position shows strong dependency on the diameter of the Al nanodisks.


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Figure 5. Simulated and measured absorption spectra of the dual-band MM absorbers with a = 500 nm, h = 24 nm, t = 40 nm, and different diameter of the Al nanodisks: (a) D = 178 nm, (b) D = 198 nm, (c) D = 238 nm. The insets show the SEM images of the corresponding samples.

Equivalent LC circuit models were successfully used to predict the electromagnetic response inside the metallic constituent elements of MMs

. Here, we use an equivalent LC circuit model

31-34

to acquire a further interpretation for the absorption performance of our designed dual-band absorbers. Figure 6 shows a unit cell of the proposed absorber and its equivalent LC circuit model. In Figure 6, L represents the inductance of the metal structures and can be expressed as m



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Lm = 0.5µ0t , where μ is the vacuum permeability and t is the thickness of the SiO spacer. The 32

0

2

parallel-plate capacitance between the top and bottom metal slabs is, cm = c1e 0e SiO 2 D2t ,where ε

0

and ε are the permittivities of vacuum and SiO , respectively, and c = 0.218 is a numerical factor SiO2

2

1

that takes into account the fringe effect or non-uniform charge distribution at the surfaces of the metal structures . C represents the gap capacitance between the Al nanodisks and can be written 33

g

as cg = e 0tD /(a - D) . In addition, L is the kinetic inductance that originates from the kinetic e

energy of mobile charge carriers, such as free electrons in metals. The value of L can be obtained e

from Le = 1 /(e 0wp 2d ), where ω is the plasma frequency of Al, δ is the effective penetration depth p

of Al and is determined by d = l /(4pk ) , κ is the extinction coefficient . The total impedance of 32

this LC circuit model can be expressed as

32

Ztot (w ) =

Lm + Le 2 - 2 + ( Lm + Le ). 1 - w Cg ( Lm + Le ) w Cm

(1)

2

The MP resonance condition for the MM absorber can be obtained by setting Z = 0, and then, the tot

resonance frequency can be written as

w = 2

C g + Cm ± C g2 + Cm2 ( Le + Lm )C g Cm

.

(2)

Figure 6. The schematic of a unit cell and its equivalent LC circuit model for the proposed MM absorber.


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Table 1 MP resonance wavelengths obtained from the LC circuit model and from the FDTD simulations in Figure 5.

No.

D (nm)

Calculated resonance wavelengths (nm)

Simulated resonance wavelengths (nm)

1

178

738

728

2

198

821

798

3

238

987

993

Table 1 shows the MP resonance wavelengths obtained from Eq. (2) and from the FDTD simulated results in Figure 5, respectively. It is seen that the theoretical predictions agree well with the numerical simulations. Relatively large difference between the calculated and simulated resonance wavelengths exists when D = 198 nm. The reason lies that the error of the value of c1 is larger for this case. Hence, the MP response of the proposed absorber can be well explained by the LC circuit model. In addition, we also investigate the influence of the parameters a (the period of the nanodisk array) and t (the thickness of the SiO layer) on the absorption performance of the proposed MM 2

absorber, as shown in Figure 7. The other structural parameters of the absorbers in Figure 7 are the same as those of the absorber in Figure 1(b). It can be seen from Figure 7(a) that, as a increases from 450 to 550 nm, the absorption peak at shorter wavelength has an obvious red shift while the other absorption peak remains at around 800 nm. As discussed above, the absorption peak at shorter wavelength is originated from the excitation of the SPP, the wave vector of which satisfies

24

k spp =

2p

l0

sin qinc ±

2p m, a

(3)

where λ is the wavelength in free space, θ is the incident angle, and m is an integer. For normal 0

inc

incidence, the increase of the lattice constant a leads to the decrease of k and the increase of spp

lspp = 2p / k spp , resulting in the redshift of the absorption peak at shorter wavelength. It is seen 13 Environment ACS Paragon Plus


from Figure 7(b) that the change of t results in the variations of the absorptance at the two absorption peaks. The absorption peak at shorter wavelength reaches perfect absorption when t = 30 nm and the other absorption peak attains perfect absorption when t = 50 nm. The positions of the two absorption peaks change only a little with the change of t. These phenomena are the results that the impedance of the absorber structure for the two resonance modes, depending on the thickness of the SiO spacer layer, can match with that of the free space at two different t. 2

Figure 7. Absorption spectra of the dual-band MM absorber under different (a) a and (b) t. The other structural parameters are the same as those in Figure 1(b).

In the design of our MM absorbers, the absorption is mainly attributed to the Al nanostructure. If other metals such as Au or Ti are used to replace Al in the absorber design, absorption bands may form in a different wavelength range by optimizing the structural parameters. The fabrication process of the samples is the same except that the deposition of Al film should be replaced by the deposition of other metals.


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CONCOUSIONS In conclusion, we have demonstrated a dual-band MM absorber in the visible and near-infrared region. Colloidal lithography nanofabrication method was used to fabricate the proposed MM absorbers. Our results show that the two absorption bands, originated from the propagating SPP and localized MP, respectively, can be tuned separately by changing the geometrical parameters of the MM absorbers. The presented dual-band absorbers may find applications in the design of high performance filters, sensors, solar cells, thermal emitters, and imaging devices. AUTHOR INFORMATION Corrseponding Author * E-mail :[email protected] Notes The authors declare no competing financial interest ACKNOWLEDGMENTS This work was supported by National Natural Science Foundation of China (Grant No. 11274126) and

Guangdong

Natural

Science

Foundation

(Grant

Nos.

2015A030311018

and

2017A030313035). Y.-H.C. acknowledges financial support from Program for Guangdong Excellent Young Teacher. REFERENCES (1) Liu, X.; Tyler, T.; Starr, T.; Starr, A.F.; Jokerst, N.M.; Padilla,W.J. Taming the Blackbody with Infrared Metamaterials as Selective Thermal Emitters. Phys. Rev. Lett. 2011, 107, 045901. (2) Vlastimil, P.; Petra L.; Hana Š.; Josef S. Testing Gold Nanostructures Fabricated by HoleMask Colloidal Lithography as Potential Substrates for SERS Sensor: Sensitivity, Signal Variability, and the Aspect of Adsorbate Deposition. Phys. Chem. Chem. Phys. 2016, 18, 1961319620.



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Figure 1. (a) Schematic of the MM absorber. (b) Simulated reflectance and absorptance vs wavelengths for the absorber design with a = 500 nm, D = 200 nm, h = 24 nm, and t = 50 nm.

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Figure 3. Fabrication scheme of the proposed dual-band MM absorber.



Figure 4. SEM images of the fabricated MM absorbers where the diameters of the Al nanodisks are (a) 178 nm and (b) 395 nm, respectively. The lattice constants of the nanodisk arrays in the two samples are the same a = 500 nm.


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Figure 5. Simulated and measured absorption spectra of the dual-band MM absorbers with a = 500 nm, h = 24 nm, t = 40 nm, and different diameter of the Al nanodisks: (a) D = 178 nm, (b) D = 198 nm, (c) D = 238 nm. The insets show the SEM images of the corresponding samples.



Figure 6. The schematic of a unit cell and its equivalent LC circuit model for the proposed MM absorber. 881x705mm (72 x 72 DPI)


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Figure 7. Absorption spectra of the dual-band MM absorber under different (a) a and (b) t. The other structural parameters are the same as those in Figure 1(b).


Dual-Band Metamaterial Absorbers in the Visible and Near-Infrared

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