P123合成的金二氧化硅纳米复合材料的线性和非线性光学特性

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本文主要探讨了在P123(EO20PO70EO20)表面活性剂存在下制备的金/二氧化硅(Au/SiO2)纳米复合材料的线性和非线性光学性质。该研究由湖南国防科技大学科学学院的Jingyue Fang、Shiqiao Qin、Xueao Zhang和Shengli Chang等人进行，他们于2012年3月在《中国光学 letters》上发表了这一成果。首先，通过透射电子显微镜（TEM）图像，研究人员揭示了纳米复合材料的基质结构为有序的多孔结构，呈现出二维六边形相。这种特殊的二维骨架为光的交互提供了独特的平台。此外，宽角X射线衍射(XRD)数据进一步证实了纳米复合物中含有金晶体，这表明金纳米粒子已经成功地嵌入到二氧化硅薄片中。金纳米粒子的存在赋予了这些固体薄膜显著的表面等离子体共振(SPR)效应。这一特性导致纳米复合材料在可见光范围内显示出强烈的吸收峰，这是非线性光学响应的一个关键特征。由于金的光学性质与纳米尺度下的量子尺寸效应，使得其在光-物质相互作用中表现出不同的行为，包括增强光强度依赖的非线性效应，如第二 harmonic generation (SHG)和四波混频(FWM)。线性光学性质，如折射率、吸收系数和透射率，可能受到金颗粒大小、排列方式以及它们与SiO2矩阵的相互作用的影响。而非线性光学效应则涉及光在纳米结构中的高次谐波生成，这在光通信、生物成像和光开关等领域具有潜在的应用价值。这项研究不仅提供了对金/二氧化硅纳米复合材料结构与光学性质之间关系的深入理解，也为设计和优化具有高性能非线性光学功能的新型纳米材料铺平了道路。未来的研究可能集中在优化纳米复合材料的制备方法，以进一步增强其光学性能，或者探索新的应用领域，如光能量转换、光存储和传感等。

COL 10(3), 031601(2012) CHINESE OPTICS LETTERS March 10, 2012

Linear and nonlinear optical properties of Au/SiO

nanocomposite prepared by P123

Jingyue Fang (½½½)

∗

, Shiqiao Qin (zzz), Xueao Zhang (ÜÜÜÆÆÆ¦¦¦), and Shengli Chang (~~~|||)

Scho ol of Science, National University of Defense Technology, Changsha 410073, China

∗

Corresp onding author: fjy nudt@yahoo.com.cn

Received August 11, 2011; accepted September 9, 2011; posted online November 1, 2011

Mesop orous silica thin films loaded with gold nanoparticles are synthesized in the presence of

(P123). Transmission electron microscope images show that the matrix of the nanocom-

p osite is an ordered porous structure with a two-dimensional hexagonal phase. The wide-angle X-ray

diffraction pattern implies that the nanocomposite contains gold crystals. These metallic nanoparticle-

embedded solid thin films show some linear and nonlinear optical properties due to their special structure

and composition. Gold nanoparticles bring about surface plasmon resonance, and an absorption peak

stemming from this effect has been observed. The linear absorption property is analyzed by a quantum

mechanism, and the results show that it is inﬂuenced by the size and volume fraction of gold nanoparticles.

Furthermore, it shows an obviously clear nonlinear optical property measured by the z -scan technique. The

magnitude of the nonlinear refractive index of the nanocomposite is estimated to be about 10

−10

/W.

OCIS codes: 160.4330, 190.4720, 240.6680, 310.6860.

doi: 10.3788/COL201210.031601.

Mesoporous silica thin film (MSTF) has been widely

studied because of its special structure: it has highly or-

dered nanoscale pores and its surface area is much larger

than bulk materials. Furthermore, the pore size of MSTF

can be regulated by adjusting the preparation conditions,

which makes it suitable as a template to assemble other

nanomaterials. Metallic nanoparticle (MNP) possesses

novel optoelectronic properties, and the MSTF pro-

vides one of the means to synthesize MNPs and get the

nanocomposite of MNP-embedded silica thin films. If the

MNPs can be loaded in each pore of the MSTF, MNPs ar-

ray can be obtained in silica thin films. In addition, the

resultant MNPs@MSTF nanocomp osite is compatible

with conventional Si fabrication technology. Moreover,

this technology can fabricate single-electron tunneling de-

vices using the MNPs@MSTF nanocomposite

[1,2]

. They

are expected to surpass the limits of conventional silicon

devices with ultra-low power and scalability down to the

sub-nanometer regime.

We have reported the synthesis of MSTF incorporated

with gold nanoparticles (GNPs)

[3]

; in this letter, we

mainly discuss its optical property. As the surface plasma

resonance (SPR) of GNPs, the nanocomposite displays

some linear optical properties, such that the absorption

peak can be controlled by the MSTF structure, as well

as the size and volume fraction of GNPs

[4−6]

. Within

the framework of the Drude dispersion relation, the SPR

absorption, including that of particles smaller than 10

nm, can be successfully explained with the Maxwell-

Garnett (MG) theory. If the GNPs are so small that the

conduction band breaks into discrete levels, the Drude

expression may no longer be valid and should be replaced

by a quantum mechanical model

[7]

. We use the quantum

mechanical model to analyze how the size and volume

fraction of GNPs inﬂuence the optical property of the

GNPs@MSTF nanocomposite. Nonlinear optical prop-

erty is another important trait of this nanocomposite,

and we get the third nonlinear refractive index by the

z -scan technique

[8]

The synthesis of MSTFs was carried out accord-

ing to the template-assisted evaporation-induced self-

assembly procedure in the presence of surfactant tem-

plate EO

(P123) under acidic conditions.

The final reactant molar ratio was tetraethoxysi-

lane (TEOS): 3-aminopropyltriethoxysilane (APTES):

OH: HCl: H

O: P123 = 0.9: 0.1: 20: 0.15: 5: 0.01.

More details can be found in our previous work

[3]

. Using

HAuCl

as the gold precursor, GNPs were incorporated

in the mesopores of MSTFs by means of neutralization

and reduction reactions. GNPs@MSTF samples with

different reaction time of 2, 6, and 10 h were produced.

Transmission electron microscope (TEM) images were

recorded to observe the surface of MSTFs using FEI

Tecnai G

20 S-Twin apparatus at an accelerating volt-

age of 200 kV. X-ray diffraction (XRD) patterns were

obtained using a Rigaku D/MAX2200 diffractometer

featuring Cu Kα radiation (λ = 0.15418 nm) at 40 kV

and 200 mA. Ultraviolet-visible (UV-VIS) absorption

spectra were recorded on a spectrophotometer (U–4100,

Hitach, Japan) with 2-nm resolution using air as refer-

ence. Moreover, z -scan measurements were performed

using a Ti:sapphire laser (Mai Tai HP, CA, USA) oper-

ated at a repetition rate of 80 MHz in TEM

mode with

an average power of about 2 W.

Figures 1(a) and (b) demonstrate the striped channels

and ringent hexagonal pores, respectively, implying that

MSTF possesses a highly ordered porous structure with

a two-dimensional (2D) hexagonal phase.

The wide-angle XRD pattern of Fig. 2 confirms that

well-crystallized GNPs are incorporated in the matrix

of MSTF since the intensity peak at about 38

◦

can be

indexed to the (111) reﬂections of the face-centered cubic

(FCC) gold. The inset in Fig. 2 shows the high-resolution

TEM (HRTEM) image of a single 8.5-nm-diameter GNP

(the period of the striped channels is about 0.24 nm).

This verifies that the GNP is well crystallized and that

the pore of MSTF confines its size.

1671-7694/2012/031601(4) 031601-1

° 2012 Chinese Optics Letters

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