本文選題：銀納米復(fù)合材料　切入點：表面等離激元　出處：《廣東工業(yè)大學(xué)》2017年博士論文　論文類型：學(xué)位論文

【摘要】：納米金屬體系中的耦合效應(yīng)及其誘導(dǎo)的光電物理現(xiàn)象引起研究者的廣泛關(guān)注�；诒砻娴入x激元復(fù)合結(jié)構(gòu)及其增強的熒光效應(yīng)是其中一個重要的研究方向。本論文以銀納米復(fù)合材料體系為單元,提出并設(shè)計了兩種復(fù)合結(jié)構(gòu):Fe3O4@Ag核殼結(jié)構(gòu)(LSP-LSP),銀納米粒子-銀納米線復(fù)合結(jié)構(gòu)(LSP-SPP)。采用紫外-可見分光光度計,拉曼光譜以及FDTD計算模擬,分別研究了核殼結(jié)構(gòu)的尺寸,粒間距對局域表面等離激元特性的影響。重點利用熒光光譜,研究了兩種復(fù)合結(jié)構(gòu)對探針分子熒光增強的影響,并分析其物理機理。本論文在生物分子的熒光成像以及RB分子的檢測方面具有一定的意義。主要研究內(nèi)容如下:運用化學(xué)還原法,成功制備了分散性較好的Fe3O4納米粒子以及Ag納米粒子,通過表面修飾成功制備了 Fe3O4@Ag核殼結(jié)構(gòu)納米顆粒。另外,利用PVP作為表面修飾劑,通過媒介作用將銀納米粒子與銀納米線有機結(jié)合,成功制備了銀納米粒子-銀納米線復(fù)合結(jié)構(gòu)。根據(jù)復(fù)合結(jié)構(gòu)的特點,對于Fe3O4@Ag核殼結(jié)構(gòu),通過納米粒子表面密度的調(diào)控,研究LSP及其耦合的表面等離激元特性;研究手段主要包括:紫外-可見分光光度計測試Fe3O4@Ag核殼結(jié)構(gòu)的吸收光譜;拉曼光譜表征復(fù)合結(jié)構(gòu)的場增強特性,FDTD計算Fe3O4@Ag核殼結(jié)構(gòu)的電磁場分布,結(jié)果表明,對于相鄰的Fe3O4@Ag核殼結(jié)構(gòu),當(dāng)平均距離小于19 nm,形成了表面等離激元耦合,等離激元共振吸收峰紅移,隨著核殼結(jié)構(gòu)平均距離減小,表面等離激元耦合程度增大,表面電磁場增強;對于銀納米粒子-銀納米線復(fù)合結(jié)構(gòu),通過銀納米粒子在銀納米線表面的沉積以及復(fù)合結(jié)構(gòu)表面形貌的蝕刻,研究LSP-SPP耦合的表面等離激元特性。研究手段主要包括:紫外-可見分光光度計測試銀納米粒子-銀納米線復(fù)合結(jié)構(gòu)的吸收光譜;拉曼光譜表征耦合結(jié)構(gòu)的場增強特性,FDTD計算銀納米粒子-銀納米線復(fù)合結(jié)構(gòu)的電磁場分布。結(jié)果表明,銀納米粒子-銀納米線形成復(fù)合結(jié)構(gòu)后,表面形成更多的“熱點”以及LSP-SPP耦合有效增強表面電磁場,表面等離激元共振吸收增大,對探針分子的拉曼光譜具有顯著增強效應(yīng)。實驗研究了這兩種復(fù)合結(jié)構(gòu)表面等離激元耦合增強探針分子的熒光輻射。對于Fe3O4@Ag核殼結(jié)構(gòu),主要運用熒光光譜儀與熒光顯微鏡分析不同尺寸的核殼結(jié)構(gòu)對探針分子熒光輻射的影響,然后研究Fe3O4@Ag核殼結(jié)構(gòu)的LSP-LSP耦合效應(yīng)對探針分子熒光增強的影響,結(jié)果表明,Fe3O4@Ag核殼結(jié)構(gòu)的LSP-LSP耦合可有效增強探針分子的熒光輻射,隨著耦合程度增大,熒光輻射增強越大,對RB分子以及PpIX分子分別具有5.4倍和15.8倍的增強效果;然后通過引入PVA介電層調(diào)控探針分子與核殼結(jié)構(gòu)的平均間距,進一步探究LSP-LSP耦合表面增強熒光的機理,結(jié)果表明,熒光增強與熒光猝滅存在競爭關(guān)系,探針分子與核殼結(jié)構(gòu)的平均間距是影響熒光增強的一個重要因素。對于LSP-SPP復(fù)合結(jié)構(gòu),主要運用熒光光譜儀與熒光顯微鏡分析銀納米粒子在銀納米線表面的沉積對探針分子熒光輻射的影響,然后利用酸刻蝕劑對合結(jié)構(gòu)刻蝕,研究銀納米粒子-銀納米線復(fù)合結(jié)構(gòu)表面形貌對熒光輻射增強的影響,結(jié)果表明,LSP-LSP耦合可有效增強探針分子的熒光輻射,并且復(fù)合結(jié)構(gòu)表面的“熱點”越多,電磁場增強效應(yīng)越大,對RB分子以及PpIX分子分別具有9.6倍和10.6倍的增強效果。最后引入PVA介電層,進一步探究LSP-SPP耦合增強熒光的機理。基于表面等離激元耦合增強熒光的光學(xué)效應(yīng),設(shè)計并優(yōu)化復(fù)合結(jié)構(gòu)應(yīng)用于生物醫(yī)學(xué)上的熒光成像以及RB分子檢測的初步探究。其中Fe3O4@Ag核殼結(jié)構(gòu)應(yīng)用于RB分子環(huán)境污染物的檢測,結(jié)果表明最低可檢測出RB分子的濃度為5×10-8mol/L;銀納米粒子-銀納米線復(fù)合結(jié)構(gòu)應(yīng)用于原卟啉(PpIX)分子的熒光成像,結(jié)果表明LSP-SPP耦合可有效增強原卟啉(PpIX)分子的熒光信號,降低其光漂白性。
[Abstract]:The physical phenomenon of photoelectric coupling effect of nano metal system and its induced caused extensive attention of researchers. The effect of surface plasmon polaritons fluorescence enhancement based on composite structure and is one of the important research direction. In this paper, system of silver nano composites as a unit, proposed and designed two kinds of composite structure: Fe3O4@Ag the core-shell structure (LSP-LSP), silver nanoparticles and silver nanowires composite structure (LSP-SPP) by UV VIS spectrophotometer, Raman spectroscopy and FDTD simulation, the core-shell structure size were studied, effects of particle spacing on the localized surface plasmon characteristics. Using fluorescence spectroscopy, research the effects of two kinds of composite structure on the fluorescence enhancement, and analysis of its physical mechanism. This paper has some significance in the detection of fluorescence imaging of biological molecules and RB molecules. The main research contents Are as follows: using chemical reduction method, successfully prepared better dispersion of Fe3O4 nanoparticles and Ag nanoparticles were successfully prepared by surface modification of Fe3O4@Ag nanoparticles with core-shell structure. In addition, the use of PVP as a surface modifying agent, through the media will be the role of silver nanoparticles and silver nano organic combination of nanowires were successfully prepared silver nanoparticles silver nanowires composite structure. According to the characteristics of the composite structure, the Fe3O4@Ag core-shell structure nanoparticles by regulating the surface density, LSP and the research on coupled surface plasmon properties; research methods mainly include: the absorption spectrum of UV VIS spectrophotometer to test the Fe3O4@Ag core-shell structure; field enhancement properties of Raman Spectra Characterization of the composite structure and calculation of electromagnetic field distribution, Fe3O4@Ag core-shell structure FDTD the results show that for the Fe3O4@Ag core-shell structure adjacent to, when the average distance is less than 19 nm, the formation of Surface plasmon coupled plasmon resonance absorption peak redshifts with core-shell structure average distance decreases, surface plasmon polariton coupling degree increases, the surface field enhancement; for silver nanoparticles and silver nanowires composite structure, nano surface deposition and etching nanowires composite structure surface morphology in silver through silver nanoparticles study of LSP-SPP, the coupling of surface plasmon properties. Main research methods include: UV VIS spectrophotometer test - absorption spectra of silver nanoparticles and silver nanometer composite structure nanowires; field enhancement properties of Raman spectra of coupled structure, calculation of electromagnetic field distribution of silver nanoparticles silver nanowires composite structure. The results showed that FDTD silver nanoparticles, silver nanowires to form a composite structure, formed on the surface of more "hot spots" and LSP-SPP coupling effectively enhance the surface electromagnetic field, surface plasmon resonance absorption In the Raman spectra of the probe molecule has the remarkable enhancement effect. Experimental study of the two kinds of composite structure of surface plasmon coupled fluorescence enhancement of radiation probe molecules. The Fe3O4@Ag core-shell structure, mainly by the analysis of influence of core-shell structure of different size of the fluorescence radiation fluorescence spectrometer and fluorescence microscopy, influence LSP-LSP and Fe3O4@Ag study on the coupling effect of core-shell structure on the fluorescence enhancement results show that LSP-LSP coupling Fe3O4@Ag core-shell structure can effectively enhance the fluorescence of the probe molecules with the coupling degree increases, the greater the enhancement of fluorescence emission, respectively with enhanced effect of 5.4 times and 15.8 times of RB molecules and PpIX molecules; and by introducing the PVA average distance of dielectric layer control probe with core-shell structure, to further explore the mechanism of fluorescence enhancement of LSP-LSP coupling surface. The results show that, There is competition with the fluorescence enhancement of fluorescence quenching, the average distance between probe molecules with core-shell structure is an important factor affecting the fluorescence enhancement. The LSP-SPP composite structure, mainly using fluorescence spectroscopy and fluorescence microscope analysis of silver nanoparticles precipitation effect product radiation on fluorescent probe molecules on the surface of silver nanowires, and then use the acid etching agent the structure of etching, silver nanoparticles of silver nanowires composite structure surface morphology on the fluorescence radiation enhancement effect, the results show that the LSP-LSP coupling can effectively enhance the fluorescence of the probe molecules and the surface of the composite structure more "hot spots", the electromagnetic enhancement effect is greater, respectively, can enhance the effect of 9.6 times and 10.6 times. The RB molecules and PpIX molecules. The PVA dielectric layer, to further explore the mechanism of fluorescence enhancement of LSP-SPP coupled surface plasmon enhancement based on coupling The optical effect of fluorescence detection, a preliminary inquiry design and optimization of composite structure is applied to the biomedical imaging and fluorescence molecular RB. Detection of Fe3O4@Ag core-shell structure is applied to the RB molecule of environmental pollutants which results show that the minimum detectable concentration of RB molecule is 5 * 10-8mol/L; silver nanoparticles and silver nanowires composite structure is applied to protoporphyrin (PpIX) molecular fluorescence imaging, the results show that LSP-SPP can effectively enhance the coupling of protoporphyrin (PpIX) fluorescence signal molecules, reduce the photobleaching.

【學(xué)位授予單位】：廣東工業(yè)大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2017
【分類號】：O657.3

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