本文選題：金納米棒 + 局域表面等離激元共振��； 參考：《南京航空航天大學(xué)》2015年博士論文

【摘要】：貴金屬納米材料(尤其金和銀)因其具有良好的物性及其表現(xiàn)出的獨(dú)特光學(xué)特性—局域表面等離激元共振現(xiàn)象(LSPR),成為納米科學(xué)領(lǐng)域中的一個(gè)熱門(mén)課題。在眾多貴金屬納米結(jié)構(gòu)中,金納米棒(GNRs)因其表現(xiàn)出依賴于形貌的各向異性且可調(diào)的SPR特性,在生命科學(xué)、光電技術(shù)等領(lǐng)域受到了廣泛關(guān)注。本論文圍繞金納米棒的合成、自組裝、表面包覆等課題開(kāi)展實(shí)驗(yàn)和理論研究,并借助FDTD數(shù)值計(jì)算分析影響SPR的諸多因素,為基于金納米棒的相關(guān)理論與應(yīng)用研究奠定基礎(chǔ)。本論文的具體研究?jī)?nèi)容和研究成果如下:1.基于晶種生長(zhǎng)法,合成出縱向等離激元共振峰(SPRL)可在近紅外波段可調(diào)的不同長(zhǎng)徑比的金納米棒。研究入射光波長(zhǎng)和環(huán)境溫度對(duì)金納米棒生長(zhǎng)的影響。對(duì)比研究了基于Gan理論和時(shí)域有限差分法(FDTD)下,金納米棒的SPRL峰與其長(zhǎng)徑比和背景介質(zhì)折射率間的關(guān)系。利用FDTD方法研究光源的偏振化方向和金納米棒的端面形貌對(duì)SPRL的影響,結(jié)果表明:偏振化方向主要影響SPRL峰的強(qiáng)度,并與偏振化方向成余弦關(guān)系,而金納米棒端面形貌的變化不但會(huì)引起SPRL峰強(qiáng)度的變化,還會(huì)引起SPRL峰的移動(dòng)。2.利用HS-PEG-SH、CYS和MPA作為連接分子,誘使金納米棒自組裝成端對(duì)端和肩并肩的有序結(jié)構(gòu),并結(jié)合實(shí)驗(yàn)結(jié)果分析了自組裝機(jī)理。FDTD數(shù)值計(jì)算結(jié)果表明:自組裝體中單體的個(gè)數(shù)、棒間的間距和夾角都會(huì)對(duì)SPR耦合產(chǎn)生影響。隨著自組裝體中單體數(shù)目的增多,不同的自組裝形式會(huì)引起SPRL峰發(fā)生紅移或藍(lán)移現(xiàn)象,其相對(duì)移動(dòng)量與單體的數(shù)目均成指數(shù)關(guān)系。隨著間距的增大,棒間的耦合效應(yīng)會(huì)越來(lái)越弱,最終移至單棒的SPRL峰附近。而棒間夾角的變化只是影響了峰的強(qiáng)度,沒(méi)有影響SPR的位置,并且由于對(duì)稱性破缺會(huì)產(chǎn)生的高能峰與低能峰,二者強(qiáng)度間的比值隨夾角的增大成指數(shù)關(guān)系衰減。3.利用溶膠—凝膠法合成出具有不同Si O2殼層厚度的GNR@Si O2核-殼復(fù)合納米結(jié)構(gòu),研究了TEOS在堿性條件下的水解機(jī)理。利用808nm半導(dǎo)體連續(xù)激光器研究了金納米棒和GNR@Si O2的熱穩(wěn)定性,實(shí)驗(yàn)表明:GNR@Si O2的熱穩(wěn)定性明顯要高于金納米棒。對(duì)于金納米棒,隨著輻射激光功率的增大,其表面的CTAB開(kāi)始脫落,裸露的表面發(fā)生熔化,最終形成穩(wěn)定性的球狀結(jié)構(gòu)。而對(duì)于GNR@Si O2核-殼結(jié)構(gòu),隨著輻照功率的增大,金納米棒表面的Si O2殼層會(huì)先發(fā)生斷裂,并使得GNR@Si O2結(jié)構(gòu)遭到破壞。4.實(shí)驗(yàn)上成功制備出具有良好水溶性和熱穩(wěn)定性的金納米棒多聚體核-殼復(fù)合納米結(jié)構(gòu),核是具有端對(duì)端和肩并肩結(jié)構(gòu)的金納米棒組裝體系。結(jié)合FDTD數(shù)值計(jì)算結(jié)果表明:介孔Si O2很好地保持了核顆粒的光學(xué)響應(yīng),且SPRL峰的位置與核內(nèi)金納米棒的個(gè)數(shù)也成指數(shù)遞增或遞減關(guān)系。此外,多聚體核-殼結(jié)構(gòu)也為進(jìn)一步定量研究多聚體間的局域場(chǎng)增強(qiáng)效應(yīng)創(chuàng)造條件。
[Abstract]:Noble metal nanomaterials (especially gold and silver) have become a hot topic in the field of nanoscience because of their good physical properties and their unique optical properties such as local surface isoexciton resonance phenomenon.Among many noble metal nanostructures, gold nanorods have attracted wide attention in life sciences, optoelectronic technology and other fields because of their morphologically dependent anisotropic and adjustable SPR properties.This thesis focuses on the synthesis, self-assembly and surface coating of gold nanorods, and analyzes the factors affecting SPR by FDTD numerical calculation, which lays a foundation for the theoretical and practical research based on gold nanorods.The specific contents and results of this thesis are as follows: 1.Based on the method of seed growth, gold nanorods with different aspect ratios, which can be adjusted in near infrared band, have been synthesized.The effects of incident wavelength and ambient temperature on the growth of gold nanorods were studied.The relationship between the SPRL peak of gold nanorods and the aspect ratio of gold nanorods and the refractive index of background medium under Gan theory and finite-difference time-domain method (FDTD) is studied.The effect of polarization direction of light source and the morphology of gold nanorods on SPRL is studied by FDTD method. The results show that the polarization direction mainly affects the intensity of SPRL peak and has a cosine relationship with the polarization direction.The change of the end morphology of gold nanorods will not only change the intensity of SPRL peak, but also cause the shift of SPRL peak. 2.The self-assembly of gold nanorods was induced by using HS-PEG-SHG CYS and MPA as connecting molecules to form an ordered structure of end-to-end and side-by-side. Combined with the experimental results, the self-assembled mechanism. FDTD numerical calculation results showed that the number of monomers in the self-assembled body was determined.The distance between rods and the angle between rods will affect the SPR coupling.With the increase of the number of monomers in the self-assembly, the red shift or blue shift of the SPRL peak will occur in different self-assembly forms, and the relative mobility is exponentially related to the number of monomers.With the increase of the spacing, the coupling effect between the rods becomes weaker and weaker, and finally moves to the SPRL peak of the single rod.However, the change of the angle between rods only affects the intensity of the peak, but not the position of the SPR, and the ratio of the intensity between the high energy peak and the low energy peak due to symmetry breaking decreases exponentially with the increase of the angle.The GNR@Si O 2 core-shell composite nanostructures with different Sio 2 shell thickness were synthesized by sol-gel method. The hydrolysis mechanism of TEOS under alkaline conditions was studied.The thermal stability of gold nanorods and GNR@Si O 2 have been studied by 808nm semiconductor continuous laser. The experimental results show that the thermal stability of 808nm nanorods is obviously higher than that of gold nanorods.For gold nanorods, with the increase of laser power, the surface CTAB of gold nanorods begins to fall off, the exposed surface melts, and finally a stable spherical structure is formed.However, for the core-shell structure of GNR@Si O 2, with the increase of irradiation power, the Sio 2 shell on the surface of gold nanorods will first break, and the structure of GNR@Si O 2 will be destroyed. 4.The gold nanorods with good water-solubility and thermal stability were successfully prepared. The core is a gold nanorod assembly system with end-to-end and side-by-side structure.The results of FDTD numerical calculation show that mesoporous Sio _ 2 keeps the optical response of nuclear particles very well, and the position of SPRL peak is exponentially increasing or decreasing with the number of gold nanorods in the nucleus.In addition, the core-shell structure of the polymer also creates conditions for further quantitative study of the local field enhancement effect between the polymers.
【學(xué)位授予單位】：南京航空航天大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2015
【分類號(hào)】：O614.123;TB383.1

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