Confined Mie Plasmons in Monolayer Hexagonal-Close-Packed Metallic Nanoshells *

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CHIN. PHYS. LETT. Vol. 29, No. 9 (2012) 097303 Confined Mie Plasmons in Monolayer Hexagonal-Close-Packed Metallic Nanoshells *

CHEN Jing(谌静)1, DONG Wen(董雯)1,2, WANG Qiu-Gu(王秋谷)1, TANG Chao-Jun(唐超军)1, CHEN Zhuo(陈卓)1**, WANG Zhen-Lin(王振林)1 1Department of Physics and National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210093 2School of Physical Science and Technology, Soochow University, Suzhou 215006

(Received 15 June 2012) Using a double templating method by electroless deposition within a templating organic porous mold, we fabricate a monolayer of hexagonal-close-packed metallic nanoshells, each with a small opening. Light transmission spectra of the metallic nanoshell arrays are measured, which show transmission resonances at specific wavelengths whose positions are observed to be independent of the incident angle as well as light polarizations. More interestingly, the resonance wavelengths of Mie plasmon modes are also independent of the surrounding medium. Further numerical simulations confirm these transmission resonances and reveal that they are attributed to the excitations ofhighly localized dipolar, quadrupolar and hexapolar Mie plasmon modes, which are highly confined within metallic nanoshells.

PACS: 73.20.Mf, 81.16.−c DOI: 10.1088/0256-307X/29/9/097303

Surface plasmons (SPs) are the collective oscil- polarization-independent total absorption effect for lations of free electrons, bound by their interaction the metallic nanoporous structures.[18] with light onto the interface between a metal and On the other hand, localized void plasmon modes a dielectric.[1,2] By adopting appropriate nanostruc- excited within metallic nanoshells have not re- tures, plasmons can be locally trapped on a sur- ceived much attention,[19−21] especially experimen- face of nanoparticles[3] or within nano-cavities,[4] pro- tally. More recently, using an electrochemical deposi- ducing significantly enhanced optical fields, which tion method, we have prepared two-dimensional (2D) can be utilized for applications such as plasmonic rigid arrays of cavity-controllable copper colloids and nanolasing,[5,6] sensing,[7,8] surface-enhanced Raman first observed a void plasmon mode confined within scattering (SERS),[9,10] optical antennas,[11] and op- the copper nanocups.[22] However, the void plasmon tical tweezers.[12] Plasmon energy and field distribu- was only limited to a dipolar void plasmon mode and tion are sensitively dependent on nanostructure ge- was weakly excited due to the larger plasmonic loss of ometry, and can be tuned by slight changes in nanos- copper compared to gold or silver, as well as thicker tructure shape or volume.[13] For example, it has been shell thickness and bigger openings for the nanocups. experimentally reported that when an individual gold Although the excitations of a variety of void plasmon nanoshell is reshaped into a symmetry-reduced na- modes within metallic nanoshells have been exten- noegg or nanocup, splitting of plasmon modes at the sively predicted,[19−21] up to now less is known about single nanostructure level is formed.[14] the systematic study on various void plasmon modes Among various nanostructure morphologies, excited within the metallic nanoshells experimentally. metallic nano-cavity structures have received tremen- In this Letter, we present an experimental study dous interest in recent years, due to their distinct on the optical properties of a monolayer of hexagonal- plasmon resonance properties. It is shown that metal close-packing (HCP) gold nanoshells with hollow inte- nano-cavities can efficiently act as plasmon resonators; riors fabricated by a double templating method.[23] It such localized plasmon resonances in the voids (lo- was found that light can transmit through the dense calized void plasmon modes) can be excited, which nanoshell assemblies via the excitations of a variety of have been extensively studied theoretically and exper- localized Mie plasmon modes, of which the positions imentally for metallic nanostructures containing pe- were observed to be independent of the incident angle riodically arranged truncated spherical voids.[4,15−17] and polarization of light. More interestingly, the res- Furthermore, Teperik et al. have shown that the lo- onance wavelengths of Mie plasmon modes were also calized void plasmons can be excited over wide ranges independent of the surrounding medium. Our numer- of incident angles, yielding an omnidirectional and ical simulations further confirmed these transmission

*Supported by the National Basic Research Program of China (No 2012CB921501), the National Natural Science Founda- tion of China (Nos 11174137, 11104136, 11021403, 11004146), the Fundamental Research Funds for the Central Universities (No 1115020403), and the Priority Academic Program Development (PAPD). **Corresponding author. Email: [email protected] © 2012 Chinese Physical Society and IOP Publishing Ltd 097303-1

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CHIN. PHYS. LETT. Vol. 29, No. 9 (2012) 097303

resonances (TRs) and revealed that they are medi- mer membrane is immersed in an electroless plating ated due to the excitations of highly localized dipo- bath. Au is electroless-deposited on the void surface lar, quadrupolar and hexapolar Mie plasmon modes, of the PMMA template.[23] Continuous Au shells can which are highly confined within metallic nanoshells. be formed within the pores of the polymer membrane. After electroless deposition, the whole structure is immersed in a solution of chloroform, wherein the host PMMA membrane is dissolved, and a freestanding or- Sputerring a thin layer gold dered array of metallic nanoshells is left. Figure 2 shows the scanning electron microscopy (SEM) image of the resulting 2D HCP array of hol-

Sealing the template with PMMA low gold nanoshells. It is seen that the replicated gold nanoshells (diameter 1476 nm, thickness 60 ± 5 nm) have a continuous and uniform wall and form a highly ordered structure (period ∼1476 nm). Shown in the Removing SiO2 spheres by HF upper inset of Fig. 2 is the SEM image of the other side of the same sample. From the image, it is seen that each gold nanoshell in fact has a small opening (the inverted cone opening spanning an azimuth an- Electroless plating gold gle of ∼40∘ relative to the shell center), as do the voids in the PMMA matrix. Thus, the hollow gold nanospheres in the 2D metal networks are not com- Removing PMMA by chloroform plete shells but look like nanocups that are intercon- nected at their equator.

2.25

(a) Fig. 1. s-polarization (Color online) Schematic of the fabrication of a 3 gold nanoshell array. 2.00 1

1.75

1.50

1.25

0O 5O

1.00 10O 15O

2 mm 20O 0.75

2.50

(b) p-polarization 3

2.25

2.00 2 mm Transmission (%)Transmission

1.75

Fig. 2. SEM image (top view) of the 2D HCP array of 1.50 hollow gold nanoshells. The upper inset shows the SEM 0O 5O 10O 15O

1.25

image of the bottom-side of the same sample. The gold 20O shell thickness is about 60 ± 5 nm. 1.00 700 800 900 1000 1100 1200 1300 The details of the synthesis process of the samples Wavelength (nm) have been extensively explained elsewhere,[23] which Fig. 3. (Color online) Measured transmission spectra for involves several distinct steps illustrated in Fig. 1. In the 2D HCP hollow nanoshell array for s-polarization (a) and p-polarization ( b) for various incident angles: 휃 = 0∘, brief, a large-area 2D silica colloidal crystal as the pri- 5∘, 10∘, 15∘, and 20∘. mary template was first prepared using our reported method.[24] A thin layer of Au of about 5–8 nm in To characterize the plasmonic properties of these thickness was plasma sputtered onto the surface of 2D ordered structures, the transmission spectra were the silica template. Then, drops of a chlorobenzene measured by using a home-built optical setting sys- solution of polymethyl methacrylate (PMMA) were tem consisting of a 50 W halogen lamp and an optical dripped onto the silica template so that, after evap- spectrum analyzer (ANDO AQ-6315 A) as a function oration of chlorobenzene, the template was embed- of wavelength, for various angles of incidence. Mea- ded within the PMMA film. In the next step, the surements were made using s- and p-polarized light, silica template was dissolved with a 1% HF solu- of which the electromagnetic (EM) wave electric field tion, which left a freestanding PMMA macroporous was perpendicular to and parallel with the plane of membrane with small apertures at the top of each incidence, respectively. pore, where the original silica spheres were in contact For the latter comparison and discussion, we first with the silica substrate.[22,23] Subsequently, the poly- show typical experimental results of the transmission 097303-2 中国科技论文在线 http://www.paper.edu.cn

CHIN. PHYS. LETT. Vol. 29, No. 9 (2012) 097303

for the 2D HCP array in Fig.3, as functions of wave- PMMA at arbitrary incident angle for both s- and p- length for incident angles 휃 = 0∘, 5∘, 10∘, 15∘, and 20∘. polarizations, such as an incident angle of 10∘ [Fig.4]. The transmission spectra for s- and p-polarizations It is distinctly seen that the positions of the TRs indi- are presented separately in Figs.3(a) and 3(b), which cated on Fig. 3 remain unchanged when the surround- show a striking similarity in their optical behavior. ing environment changes from air to PMMA. This im- For s-polarization [Fig. 3(a)], three conspicuous peaks plies that these TRs observed in Fig. 4 are also inde- indicated using the arrows are observed at normal pendent of the surrounding medium. On the basis of incidence, which are located at 712 nm, 946 nm and the above discussion, a conclusion can be made that 1155 nm, respectively. When the angle of incidence these TRs result from localized Mie plasmons trapped was increased from 휃 = 0∘ to 휃 = 20∘, the reso- inside the gold nanoshells. It is noted that due to the nant peaks at the wavelengths of 휆1 and 휆3 only vary openings of the metallic shells, the radiation loss of the in strength, but show no change in position. How- void modes become increased.[6,25] Since a decreasing ever, for the resonance 휆2, there exists a slight po- quality of factor void modes as compared with that of sition shifting with increasing incident angle, which a complete Au shell are supported in the prepared Au most likely arises from the coupling of the plasmon nanoshells, these Mie plasmon modes lead to broad- mode with a delocalized plasmon mode supported ened TR peaks. on this periodic nanoshell array under off-normal

[17] 1000

(b) in incidence. The same effects were observed for p- ( )

2.00 26.00

500 polarization [Fig. 3(b)]. There are also three peaks (a)

TM 22.75

2 in the transmission spectrum under normal incidence, 19.50

16.25 0

13.00 which are located at 712 nm, 946 nm and 1155 nm, (nm)

9.750

1.75 -500 respectively. Moreover, the positions of these reso- 6.500

3.250 TM1 cavity mode

0.000 nant peaks are also almost independent of the incident -1000

2 1000

( )

in TM TM in angle. More importantly, comparing Fig. 3(a) with 1 3 16.00

1.50

500 Fig. 3(b), it is found that the resonant peaks for both 14.00 12.00

10.00 s- and p-polarizations lie approximately at the same 0 8.000 (nm) wavelength. This phenomena suggests that these TRs 6.000 -500 4.000 1.25

2.000

irrespective of the angle and polarization of the inci- TM2 cavity mode 0.000

-1000

Transmission (%)Transmission 1000 2

dent light arise from localized SP excitations of the ( ) in

18.00 in

2D HCP array, which may be confined in the metallic 1.00 500 [21] 15.75 nanoshells or confined in the lattice pores. 13.50

0 11.25 (nm)

9.000

6.750

-500

2.5 4.500 s-polarization 0.75 (a)

800 1000 1200 2.250 TM3 cavity mode

3 -1000 0.000

Wavelength (nm) 2.0

1 -1000-500 0 500 1000

(nm)

1.5

1.0 Fig. 5. Ordered array in air (Color online) (a) Calculated positions for the Mie

Ordered array in PMMA plasmon modes of a single nanoshell, indicated by three 0.5 red markers in the measured transmission spectrum of the Au nanoshell array. (b) Calculated electric field intensity 0.0

2.5 distributions on 푥푧-plane at the resonance wavelengths of p-polarization (b) 3 1 Mie plasmon modes. 2

2.0 Transmission (%)Transmission

1.5 To further reveal the physics of these Mie plasmon

Ordered array in air modes, we performed numerical simulations using the

1.0 Ordered array in PMMA Mie theory.[26] A simple model of a single spherical 0.5 nanoshell with radius 738 nm and Au shell thickness

0.0 60 nm is considered in the calculation since the elec-

700 800 900 1000 1100 1200 1300 tric fields of these Mie plasmon modes are well con- Wavelength (nm) centrated within the cavities of the nanoshells, which Fig. 4. (Color online) Measured transmission spectra for has been verified by our above experiment. In our a comparison between the 2D HCP array in air and in PMMA under s-polarization (a) and p-polarization (b) at simulation, the permittivity of Au is taken from ex- [27] an angle of incidence of 10∘. perimental data. The calculated positions of these Mie plasmon modes for a single nanoshell are indicated In order to make a distinction between those TRs using vertical red lines in the experimental transmis- confined in the metallic nanoshells and confined in sion spectrum in Fig. 5. It can be clearly seen that the lattice pores, we compared the transmission spec- the simulated positions of the Mie plasmon modes co- tra of the 2D HCP array embedded in air and in incide well with the experimental transmission peaks. 097303-3 中国科技论文在线 http://www.paper.edu.cn

CHIN. PHYS. LETT. Vol. 29, No. 9 (2012) 097303

To better understand these TRs, the corresponding [6] Pan J, Chen Z, Chen J, Zhan P, Tang C J and Wang Z L normalized electric field intensity distributions of the 2012 Opt. Lett. 37 1181 Mie plasmon modes are shown in Fig. 5(b). It can be [7] Anker J N, Hall W P, Lyandres O, Shah N C, Zhao J and Van Duyne R P 2008 Nat. Mater. 7 442 seen that these TRs could be attributed to different [8] Li Y Y, Pan J, Zhan P, Zhu S N, Ming N B, Wang Z L, void plasmon modes, and the excitations of dipolar, Han W D, Jiang X Y and Zi J 2010 Opt. Express 18 3526 hexapolar and quadrupolar void plasmon modes ac- [9] Haynes C L and Van Duyne R P 2003 J. Phys. Chem. B 107 count for the TRs at 712 nm, 946 nm and 1155 nm, 7426 [10] Chen L, Liu F X, Zhan P, Pan J and Wang Z L 2011 Chin. respectively. Phys. Lett. 28 057801 In summary, we have fabricated a monolayer of [11] Mühlschlegel P, Eisler H J, Martin O J F, Hecht B and Pohl HCP gold nanoshells, and analyzed the localized plas- D W 2005 Science 308 1607 Nat. Photon. 5 mon modes of the ordered array. A comparison be- [12] Juan M L, Righini M and Quidant R 2011 349 tween the experimental results and the theoretical [13] Halas N J 2005 MRS Bull. 30 362 simulations proves that the light can transmit through [14] Lassiter J B, Knight M W, Mirin N A and Halas N J 2009 the 2D HCP metallic array by the excitations of a Nano Lett. 9 4326 [15] Kelf T A, Sugawara Y, Baumberg J J, Abdelsalam M and variety of Mie plasmon modes, which are highly con- Bartlett P N 2005 Phys. Rev. Lett. 95 116802 fined in metallic nanoshells. These results will fur- [16] Cole R M, Sugawara Y, Baumberg J J, Mahajan S, Abdel- ther stimulate theoretical and experimental interest salam M and Bartlett P N 2006 Phys. Rev. Lett. 97 137401 in controlling the optical properties of the 2D ordered [17] Cole R M, Baumberg J J, Garcia de Abajo F J, Mahajan S, Abdelsalam M and Bartlett P N 2007 Nano lett. 7 2094 microstructure with tunable metallic shells and its po- [18] Teperik T V, García de Abajo F J, Borisov A G, Abdel- tential photonic applications in sensors and plasmonic salam M, Bartlett P N, Sugawara Y and Baumberg J J lasers, as well as SERS and efficient light-emitting de- 2008 Nat. Photon. 2 299 vices. [19] Teperik T V, Popov V V and García de Abajo F J 2004 Phys. Rev. B 69 155402 [20] Penninkhof J J, Sweatlock L A, Moroz A, Atwater H A, van Blaaderen A and Polman A 2008 J. Appl. Phys. 103 References 123105 [21] Tang C J, Wang Z L, Zhang W Y, Zhu S N, Ming N B, Sun [1] Raether H 1988 Surface Plasmons on Smooth and Rough G and Sheng P 2009 Phys. Rev. B 80 165401 Surfaces and on Gratings (Berlin: Springer-Verlag) [22] Chen Z, Dong H, Pan J, Zhan P, Tang C J and Wang Z L [2] Barnes W L, Dereux A and Ebbesen T W 2003 Nature 424 2010 Appl. Phys. Lett. 96 051904 824 [23] Dong W, Dong H, Wang Z L, Zhan P, Yu Z Q, Zhao X N, [3] Kelly K L, Coronado E, Zhao L L and Schatz G C 2003 J. Zhu Y Y and Ming N B 2006 Adv. Mater. 18 755 Phys. Chem. B 107 668 [24] Chen Z, Zhan P, Wang Z L, Zhang J H, Zhang W Y, Ming [4] Coyle S, Netti M C, Baumberg J J, Ghanem M A, Birkin P N B, Chan C T and Sheng P 2004 Adv. Mater. 16 417 R, Bartlett P N and Whittaker D M 2001 Phys. Rev. Lett. [25] Wang Q G, Tang C J, Chen J, Zhan P and Wang Z L 2011 87 176801 Opt. Express. 19 23889 [5] Noginov M A, Zhu G, Belgrave A M, Bakker R, Shalaev [26] Bohren C F and Huffman D R 1983 Absorption and Scat- V M, Narimanov E E, Stout S, Herz E, Suteewong T and tering of Light by Small Particles (New York: Wiley) Wiesner U 2009 Natrue 460 1110 [27] Johnson P B and Christy R W 1972 Phys. Rev. B 6 4370

097303-4 中国科技论文在线 http://www.paper.edu.cn

Chinese Physics Letters Volume 29 Number 9 September 2012

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097802 F4TCNQ-Induced Exciton Quenching Studied by Using in-situ Photoluminescence Measurements ZHU Jian, LU Min, WU Bo, HOU Xiao-Yuan 097803 Preparation and Characterization of Bimodal Magnetoﬂuorescent Nanoprobes for Biomedical Application LEI Jie-Mei, XU Xiao-Liang, LIU Ling, YIN Nai-Qiang, ZHU Li-Xin 097804 A GaN p–i–p–i–n Ultraviolet Avalanche Photodiode ZHENG Ji-Yuan, WANG Lai, HAO Zhi-Biao, LUO Yi, WANG Lan-Xi, CHEN Xue-Kang 中国科技论文在线 http://www.paper.edu.cn

097805 White Hybrid Light-Emitting Devices Based on the Emission of Thermal Annealed Ternary CdSe/ZnS Quantum Dots QU Da-Long, ZHANG Zhen-Song, YUE Shou-Zhen, WU Qing-Yang, YAN Ping-Rui, ZHAO Yi, LIU Shi-Yong

CROSS-DISCIPLINARY PHYSICS AND RELATED AREAS OF SCIENCE AND TECHNOLOGY 098101 A New Grating Fabrication Technique on Metal Films Using UV-Nanoimprint Lithography TANG Min-Jin, XIE Hui-Min, LI Yan-Jie, LI Xiao-Jun, WU Dan 098102 A Self-Aligned Process to Fabricate a Metal Electrode-Quantum Dot/Nanowire-Metal Electrode Structure with 100% Yield FU Ying-Chun, WANG Xiao-Feng, FAN Zhong-Chao, YANG Xiang, BAI Yun-Xia, ZHANG Jia-Yong, MA Hui-Li, JI An, YANG Fu-Hua 098401 A Repairable Linear m-Consecutive-k-Out-of-n:F System TANG Sheng-Dao, HOU Wei-Gen 098402 Effect of Aluminium Nanoparticles on the Performance of Bulk Heterojunction Organic Solar Cells YANG Shao-Peng, YAO Ming, JIANG Tao, LI Na, ZHANG Ye, LI Guang, LI Xiao-Wei, FU Guang-Sheng 098501 Performance Improved by Incorporating of Ru Atoms into Zr-Si Diffusion Barrier for Cu Metallization WANG Ying, SONG Zhong-Xiao, ZHANG Mi-Lin 098502 Enhanced Light Output of InGaN-Based Light Emitting Diodes with Roughed p-Type GaN Surface by Using Ni Nanoporous Template YU Zhi-Guo, CHEN Peng YANG Guo-Feng, LIU Bin, XIE Zi-Li, XIU Xiang-Qian, WU Zhen-Long, XU Feng, XU Zhou, HUA Xue-Mei, HAN Ping, SHI Yi ZHANG Rong, ZHENG You-Dou 098503 Performance Improvement of Ambipolar Organic Field Effect Transistors by Inserting a MoO3 Ultrathin Layer TIAN Hai-Jun, CHENG Xiao-Man, ZHAO Geng, LIANG Xiao-Yu, DU Bo-Qun, WU Feng 098801 Effects of the Molybdenum Oxide/Metal Anode Interfaces on Inverted Polymer Solar Cells WU Jiang, GUO Xiao-Yang, XIE Zhi-Yuan 098901 A New Definition of Modularity for Community Detection in Complex Networks YE Zhen-Qing, ZHANG Ke, HU Song-Nian, YU Jun 098902 Modeling and Simulation of Pedestrian Counter Flow on a Crosswalk LI Xiang, DONG Li-Yun 098903 A Multilane Traffic Flow Model with Lane Width and the Number of Lanes TANG Tie-Qiao, YANG Xiao-Bao, WU Yong-Hong, CACCETTA Lou, HUANG Hai-Jun

GEOPHYSICS, ASTRONOMY, AND ASTROPHYSICS 099401 Field-Aligned Electrons in Polar Region Observed by Cluster on 30 September 2001 ZHANG Zi-Ying, SHI Jian-Kui, CHENG Zheng-Wei, Andrew Fazakerley