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Optics Express

Optics Express

  • Editor: Andrew M. Weiner
  • Vol. 21, Iss. 15 — Jul. 29, 2013
  • pp: 17568–17575
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Dipole plasmon resonance induced large third-order optical nonlinearity of Au triangular nanoprism in infrared region

Ziyu Chen, Hongwei Dai, Jiaming Liu, Hui Xu, Zixuan Li, Zhang-Kai Zhou, and Jun-Bo Han  »View Author Affiliations


Optics Express, Vol. 21, Issue 15, pp. 17568-17575 (2013)
http://dx.doi.org/10.1364/OE.21.017568


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Abstract

Au triangular nanoprisms with strong dipole plasmon absorption peak at 1240 nm were prepared by wet chemical methods. Both numerical calculations and experiments were carried out to investigate the optical properties of the samples. Finite difference time domain (FDTD) and Local Density of States (LDOS) calculations demonstrate that strong electric field enhancement and large LDOS can be obtained at tip areas of the Au triangular nanoprisms. Z scan techniques were used to characterize the nonlinear absorption, nonlinear refraction, as well as one- and two-photon figures of merit (W and T, respectively) of the sample. The results show that maximum nonlinear refractive index can be obtained around the resonance absorption wavelength of 1240 nm, detuning the wavelength from the absorption peak will lead to the decrease of the nonlinear refractive index n2, while the nonlinear absorption coefficient β doesn’t change much with the wavelength. This large wavelength dependence of n2 and small change of β enable the sample to satisfy the all-optical switching demand of W> 1 and T< 1 easily in a large wavelength range of 1200-1300 nm. These significant nonlinear properties of the sample imply that Au triangular nanoprism is a good candidate for future optical switches in infrared optical communication wavelength region.

© 2013 OSA

1. Introduction

Over the past decade, considerable research interests have been apportioned to noble metallic materials for its ability to support surface plasmon modes, which are collective oscillations of electron gas in metal that couple with electromagnetic fields [1

1. S. Lal, S. Link, and N. J. Halas, “Nano-optics from sensing to waveguiding,” Nat. Photonics 1(11), 641–648 (2007). [CrossRef]

5

5. Q. Q. Wang, J. B. Han, D. L. Guo, S. Xiao, Y. B. Han, H. M. Gong, and X. W. Zou, “Highly efficient avalanche multiphoton luminescence from coupled Au nanowires in the visible region,” Nano Lett. 7(3), 723–728 (2007). [CrossRef] [PubMed]

]. With the ability to concentrate and enhance near electric field, plasmonic nanostructures have found numerous promising applications in quantum devices [6

6. M. W. Knight, H. Sobhani, P. Nordlander, and N. J. Halas, “Photodetection with active optical antennas,” Science 332(6030), 702–704 (2011). [CrossRef] [PubMed]

8

8. Z. K. Zhou, M. Li, Z. J. Yang, X. N. Peng, X. R. Su, Z. S. Zhang, J. B. Li, N. C. Kim, X. F. Yu, L. Zhou, Z. H. Hao, and Q. Q. Wang, “Plasmon-mediated radiative energy transfer across a silver nanowire array via resonant transmission and subwavelength imaging,” ACS Nano 4(9), 5003–5010 (2010). [CrossRef] [PubMed]

], plasmon lasers [9

9. V. J. Sorger and X. Zhang, “Physics. Spotlight on plasmon lasers,” Science 333(6043), 709–710 (2011). [CrossRef] [PubMed]

11

11. Z. K. Zhou, X. R. Su, X. N. Peng, and L. Zhou, “Sublinear and superlinear photoluminescence from Nd doped anodic aluminum oxide templates loaded with Ag nanowires,” Opt. Express 16(22), 18028–18033 (2008). [CrossRef] [PubMed]

], and biochemical sensing substrates [12

12. J. A. Fan, C. Wu, K. Bao, J. Bao, R. Bardhan, N. J. Halas, V. N. Manoharan, P. Nordlander, G. Shvets, and F. Capasso, “Self-Assembled plasmonic nanoparticle clusters,” Science 328(5982), 1135–1138 (2010). [CrossRef] [PubMed]

14

14. S. D. Liu, Z. Yang, R. P. Liu, and X. Y. Li, “Multiple Fano resonances in plasmonic heptamer clusters composed of split nanorings,” ACS Nano 6(7), 6260–6271 (2012). [CrossRef] [PubMed]

]. In addition, the growing demand in design and fabrication of photonics and plasmonic devices makes plasmonic material become critical import [15

15. H. M. K. Wong and A. S. Helmy, “Optically defined plasmonic waveguides in crystalline semiconductors at optical frequencies,” J. Opt. Soc. Am. B 30(4), 1000–1007 (2013). [CrossRef]

17

17. B. Lau, M. A. Swillam, and A. S. Helmy, “Hybrid orthogonal junctions: wideband plasmonic slot-silicon waveguide couplers,” Opt. Express 18(26), 27048–27059 (2010). [CrossRef] [PubMed]

].

In this paper, third-order optical nonlinearities including nonlinear absorption coefficient β and refractive index n2 have been investigated, the one- and two-photon figures of merit (FOM) were also evaluated. Furthermore, electric field distribution and local density of state (LDOS) of the Au nanoprism were also simulated. All these remarkable optical properties make the Au triangular nanoprisms have great potential applications in infrared communications and optical switches [32

32. E. Ozbay, “Plasmonics: merging photonics and electronics at nanoscale dimensions,” Science 311(5758), 189–193 (2006). [CrossRef] [PubMed]

35

35. H. W. Ren, S. Xu, Y. F. Liu, and S. T. Wu, “Liquid-based infrared optical switch,” Appl. Phys. Lett. 101(4), 041104 (2012). [CrossRef]

].

2. Experiment

The Au triangular nanoprism is synthesized by seeded growth method [30

30. M. R. Singh, C. Racknor, and D. Schindel, “Controlling the photoluminescence of acceptor and donor quantum dots embedded in a nonlinear photonic crystal,” Appl. Phys. Lett. 101(5), 051115 (2012). [CrossRef]

]. Au nanoparticle seeds were prepared by the reduction reaction with the presence of sodium citrate (0.275mM, 36.33mL), HAuCl4 aqueous solution (15mM, 0.67mL), and NaBH4 (100mM, 1mL). In order to the complete hydrolysis of unreacted NaBH4 adequately, the mixed solution needed to react for a whole night.

Three groups of growth solutions were prepared for the seed-mediated growth steps. Solution A and B were identical which contained NaOH (0.1M, 0.05mL), ascorbic acid (0.1M, 0.05mL), KI (0.1M, 0.075mL), CTAB (0.05M, 9mL) and HAuCl4 (10mM, 0.25mL). While solution C contained NaOH (0.1M, 0.50mL), ascorbic acid (0.1M, 0.50mL), KI (0.1M, 0.075mL), CTAB (0.05M, 90mL) and HAuCl4 (10mM, 2.5mL). All these three groups of solutions were prepared by adding chemicals in the sequence listed above.

Au particle formation started by adding 1mL of seed solution to growth solution A. The mixture was gently shaken, then 1mL of this mixture was added to growth solution B. After a while of gently shaking, the whole mixture was added into solution C. The color of the final mixed solution was changed from clear colorless to purple red in about 20 minutes. The water used in the experiments was purified to 18.2 MΩ cm by using a Millipore Mili-Q water system.

The scanning electron microscopy (SEM) was performed by using a Zeiss Auriga-39-34 electron microscope operated at an accelerating voltage of 20.0 kV. The absorption spectra were recorded by a UV-VIS-NIR spectrophotometer (PerkinElmer Lambda950). The nonlinear optical measurements were performed using a Z-scan setup. For Z-scan measurements, a Ti:Sapphire femtosecond laser (Coherent, Mira 900) pump optical parametric oscillator (OPO, Coherent, APE OPO) was used as a laser sources to obtain the infrared laser emission, the pulse duration of the output laser beam from OPO is about 200 fs and the repetition rate is 76 MHz. Both open- and closed-aperture Z-scan measurements were done to get the third-order optical nonlinear absorption coefficient and refraction index.

3. Results and discussion

Figure 1(b) is the absorption spectra of Au nanoprisms in water solution. Two absorption bands can be easily observed, and the one locates at around 530 nm is due to the dipole plasmon resonance of spherical Au nanoparticle with diameter of about 50 nm [36

36. J. E. Millstone, S. Park, K. L. Shuford, L. D. Qin, G. C. Schatz, and C. A. Mirkin, “Observation of a quadrupole plasmon mode for a colloidal solution of gold nanoprisms,” J. Am. Chem. Soc. 127(15), 5312–5313 (2005). [CrossRef] [PubMed]

]. The stronger absorption peak locates at about 1240 nm is dipole plasmon resonance of Au triangular nanoprisms, and the broad absorption peak is caused by the contribution of the irregular shape prisms. It should note that the absorption intensity at 1240 nm is stronger than that of Au nanoparticles, which implies that the yield of Au nanoprisms is high. Also, there is a small absorption band located at about 800 nm, which is the quadrupole plasmon mode of Au triangular nanoprisms first discovered by J. E. Millstone et al..

To further investigate the near field enhancement property of Au triangular nanoprism, the local density of states (LDOS) along the side-edge of Au nanoprism was calculated. As the LDOS enhancement is proportional to the emission rate of nano-emitters around Au nanoprisms, the LDOS results can directly demonstrate the plasmon-photon interaction property of Au triangular nanoprisms, which is critical for its applications.

The LDOS calculation was performed by using the Green function method with the help of the COMSOL software (version 4.2a). The dielectric constant of the gold was taken from the literature [37

37. P. B. Johnson and R. W. Christy, “Optical Constants of the Noble Metals,” Phys. Rev. B 6(12), 4370–4379 (1972). [CrossRef]

]. An electric point dipole is set 10 nm above the center of side edge of the Au triangular prism [Fig. 3(a)
Fig. 3 The LDOS enhancement along edge-side of Au triangular nanoprism. (a) The simulation mode sketch. (b) The x-position dependence of LDOS along edge-side of Au nanoprism.
], with side-edge length and thickness being 170 nm and 7 nm. To get a good mesh, a sphere with radius 4 nm is set to surround the dipole, furthermore, two blocks with sizes of 272 × 272 × 30 nm3 and 500 × 500 × 100 nm3 are set to separate the nanoprism and the Perfectly Matched Layers (PML). The PML is set to general type with size 1000 × 1000 × 500 nm3. The mesh is predefined as finer. The scattering boundary is set to the outside of the PML.

With the help of the Green function, the LDOS is given as [41

41. L. Novotny and B. Hecht, Principles of Nano-Optics (Cambridge University Press 2006).

]

ρ(r,ω)=2ωπc2Im{tr[G(r,r,ω)]},
(1)

Where Im stands for the imaginary part and tr denotes the trace of the Green tensor matrix in brackets.

From the Maxwell equations, one can getE(r,ω)=iωμ0dr'G(r,r',ω)j(r,ω). By setting a dipole source j(r',ω)=j(ω)δ(r'r0), the Green function can be calculated by the electric field at the position of the dipole as E(r0,ω)=iωμ0G(r0,r0,ω)j(ω).

Also the matrix form of E(r0,ω) can be written as:

E=iωμ0[GxxGxyGxzGyzGyyGyzGzxGzyGzz].[jxjyjz],
(2)

After choosing three j of different directions, all the elements of the Green matrix can be obtained, so as to get the LDOS.

In Fig. 3(b), the dipole source is placed at the centre of the Au nanoprism with 10 nm above the surface (z = 10 nm), and the zero point is set at the centre of edge-side as shown in Fig. 3(a). Define the LDOS enhancement as the ratio between the LDOS of dipole source above Au nanoprism and in vacuum. As shown in Fig. 3(b), the LDOS enhancement increases dramatically as the calculation point moving from the centre to the tip. An LDOS enhancement of 1000 times has been found at the triangular tip, which suggests strong near field enhanced photon-electron interaction [42

42. S. Kéna-Cohen, A. Wiener, Y. Sivan, P. N. Stavrinou, D. D. C. Bradley, A. Horsfield, and S. A. Maier, “Plasmonic sinks for the selective removal of long-lived states,” ACS Nano 5(12), 9958–9965 (2011). [CrossRef] [PubMed]

].

As strong near electric field can induce large optical nonlinearities [43

43. J. B. Han, D. J. Chen, S. Ding, H. J. Zhou, Y. B. Han, G. G. Xiong, and Q. Q. Wang, “Plasmon resonant absorption and third-order optical nonlinearity in Ag-Ti cosputtered composite films,” J. Appl. Phys. 99(2), 023526 (2006). [CrossRef]

], third-order nonlinear absorption and refraction properties as well as one-photon- and two-photon- figures of merit in Au triangular nanoprisms were investigated using z-scan measurements. Figure 4(a)
Fig. 4 Z-scan data of Au triangular nanoprisms in water solution. (a) Schematic of the Z-scan experimental setup: M1 and M2 are reflective mirrors, ND is a neutral density filter, BS is a beam splitter, L is a lens with the focal length of 100 mm, S is sample, A is an aperture, D1 and D2 are detectors. (b) and (c) are open-aperture and closed-aperture Z-scan data with input irradiance intensity I0 = 0.43GW/cm2, respectively. The open symbols are the experiment data and the solid lines are fitting curves. (d) Nonlinear absorption coefficient β and refractive index γ of the sample vs. wavelength. (e) One- and two-photon figures of merit W and T vs. wavelength.
is the schematic of Z-scan setup, a laser source generated from an OPO pumped by a Ti:Sappire femtosecond was used to generate the laser emissions from 1100 nm to 1300 nm. After the attenuation by a neutral density filter, the laser emission with appropriate power was focused onto the sample by a lens with focal length of 100 mm. To minimize the possible heat effect by laser irradiance, the peak irradiance intensity of the laser beam at the focus position I0 was fixed at 0.43GW/cm2. The sample held by a 1 mm thick quartz cell was put onto a moving stage which can sweep along the laser beam directions ( ± Z direction), two power detectors (D1 and D2) were used to monitor the laser powers. The transmission T was extracted from the ratio between power value obtained by detector D2 and the that at the front of the sample calculated from detector D1.

Figure 4(b) presents the normalized open aperture transmittance T as functions of sample position z. The hollow dots are experimental data, and the solid lines are fitting curves using the theoretical expression of T = Σ(-q0)m/(1 + z2/z02)m(1 + m)3/2 (m = 0,1,2,…) [44

44. M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive Measurement of Optical Nonlinearities Using a Single Beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990). [CrossRef]

], where z0 is Rayleigh range and equals to nπω02/λ, ω0 is Gaussian beam spot radius at focus (z = 0), q0 = βI0Leff, Leff is effective thickness of the sample. The nonlinear absorptions between 1100 and 1300 were measured, all the curves are valley types which imply that the third-order nonlinear absorption of the gold triangular prisms here are two-photon induced absorption. Figure 4(b) is the normalized results of the closed-aperture z scan measurements, the hollow dots are experimental data, and the solid lines are fittings. The theoretical relation between T and z is expressed as T = 1 + 4ΔΦ0(z/z0)/{[(z/z0)2 + 9]·[(z/z0)2 + 1]}, where ΔΦ0 = n2kI0Leff, n2 is the nonlinear refraction index, and k is the wave number. All the curves are peak-valley types, which mean that the third-order nonlinear refractive indexes of the sample are negative.

From the data and the fittings in Fig. 4(b) and (c), the third-order optical nonlinear absorption coefficient β and nonlinear refractive index n2 can be extracted. As shown in Fig. 4(d), the wavelength dependent β and n2 values are demonstrated. β doesn’t change much with the change of the wavelength and β is about 0.189 cm/GW at 1240 nm, while n2 increases as the wavelength goes close to the resonance absorption wavelength, and the maxima is 1.87 × 10−4 cm2/GW. The corresponding χ(3) susceptibility of the sample can be calculated using χ(3) = Im{χ(3)} + Re{χ(3)}, where Im{χ(3)} comes from nonlinear absorption of the sample and can be calculated from β (Im{χ(3)} = n02ε0c2β/ω), Re{χ(3)} is contributed by the nonlinear refraction n2 (Re{χ(3)} = 2n02ε0cn2), the imaginary and real part of χ(3) at 1240 nm are calculated to be 1.03 × 10−13 esu and 1.25 × 10−11 esu, respectively. From these calculated results of χ(3), it is clear that third-order nonlinear refraction is dominant effect in the sample. Due to the limiting of our laser sources, the measurements under the wavelength shorter than 1100 nm and longer than 1300 nm can’t be obtained. However, the value of χ(3) at 1240 nm is 20 times larger that obtained at 800 nm (6.48 × 10−13 esu), which means that the large nonlinearities around 1240 nm are due to the local field enhanced plasmon resonance effects. It is important to notice that there are some Au nanoparticles existing in the solution of Au triangular prisms, since the absorption peak of the nanoparticles locates at around 530 nm, which is far away from the measurement wavelength that we used at 1100-1300 nm region, the nonlinear effects attributed from spherical Au nanoparticles can be ignored [45

45. Y. Hamanaka, A. Nakamura, N. Hayashi, and S. Omi, “Dispersion curves of complex third-order optical susceptibilities around the surface plasmon resonance in Ag nanocrystal–glass composites,” J. Opt. Soc. Am. B 20(6), 1227 (2003). [CrossRef]

].

4. Conclusion

We have experimentally and theoretically investigated the nonlinear property of Au triangular nanoprisms synthesized by seeded growth method. The UV-VIS-NIR analysis and FDTD simulation indentify the existence of dipole plasmon resonance at 1240nm. The LDOS calculation shows an enhancement of 1000 times at the triangular tip, which suggests strong near field enhanced photon-electron interaction. The results of Z-scan measurement indicate that third-order susceptibility is 1.25 × 10−11 esu at 1240nm which is about 20 times larger than that obtained at 800nm, and this result confirms the inference of theoretical simulations and calculations. The significant third-order nonlinearity across the range of 1200nm-1300nm satisfy the demands that W>1 and T<1 which suggest Au triangular prisms are good candidate for future of all-optical switching in the 1300 nm telecommunication wavelength band.

Acknowledgment

We greatly thank Prof. Huanjun Chen for helpful discussions. This work was supported in part by NSFC (11204385), National Basic Research Program of China (2010CB923200, 2011TS105), the Fundamental Research Funds for the Central Universities (Grant 12lgpy45), and Fund of Education department of Guangdong Province (2012LYM_0011).

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S. Kéna-Cohen, A. Wiener, Y. Sivan, P. N. Stavrinou, D. D. C. Bradley, A. Horsfield, and S. A. Maier, “Plasmonic sinks for the selective removal of long-lived states,” ACS Nano 5(12), 9958–9965 (2011). [CrossRef] [PubMed]

43.

J. B. Han, D. J. Chen, S. Ding, H. J. Zhou, Y. B. Han, G. G. Xiong, and Q. Q. Wang, “Plasmon resonant absorption and third-order optical nonlinearity in Ag-Ti cosputtered composite films,” J. Appl. Phys. 99(2), 023526 (2006). [CrossRef]

44.

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive Measurement of Optical Nonlinearities Using a Single Beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990). [CrossRef]

45.

Y. Hamanaka, A. Nakamura, N. Hayashi, and S. Omi, “Dispersion curves of complex third-order optical susceptibilities around the surface plasmon resonance in Ag nanocrystal–glass composites,” J. Opt. Soc. Am. B 20(6), 1227 (2003). [CrossRef]

OCIS Codes
(160.4330) Materials : Nonlinear optical materials
(190.4720) Nonlinear optics : Optical nonlinearities of condensed matter
(240.6680) Optics at surfaces : Surface plasmons
(160.4236) Materials : Nanomaterials

ToC Category:
Nonlinear Optics

History
Original Manuscript: April 29, 2013
Revised Manuscript: May 23, 2013
Manuscript Accepted: May 25, 2013
Published: July 16, 2013

Citation
Ziyu Chen, Hongwei Dai, Jiaming Liu, Hui Xu, Zixuan Li, Zhang-Kai Zhou, and Jun-Bo Han, "Dipole plasmon resonance induced large third-order optical nonlinearity of Au triangular nanoprism in infrared region," Opt. Express 21, 17568-17575 (2013)
http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-21-15-17568


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