客製化理想的粒子尺寸是全面且有效地探究金奈米粒子之各種獨特性質的首要條件。過去，不同的合成方法已成功地被用來製造多功能性的金奈米粒子，然而多數的方法往往在合成後尚必須進行複雜的移除模板之動作。而這些程序更常因受限於動力學本質上的低反應速率而導致大範圍粒子尺寸分布的產生。此論文的研究首先實現了一個完全不同的X-ray輻射合成策略，更強調專注於金奈米粒子的合成以及證實其所伴隨的獨特性質主要源自於卓越的粒子尺寸控制之能力。
在利用同步加速器所產生的高強度X-ray輻照金前驅物下，快速的還原使得粒子的成核反應同時且均勻的展開。這樣的特性使得我們可以在不需要任何的物理模板（例如樹枝狀高分子或微胞）的加入下成功地合成出不同粒徑大小的金奈米粒子，特別是約為1 nm具有相當小範圍粒徑分布且傑出膠體穩定性的金奈米團簇。因此，此方法不僅簡化了合成之程序及增加反應之控制性，更減少了繁雜的純化程序所造成的負面效應之可能性。
在進一步的應用上，我們所合成之金奈米團簇特殊的雙共存性質（即強可見螢光和高癌細胞累積量）為生物醫學研究上提供了一同時可利用X-ray和可見光顯微鏡造影之新型多模態成像技術。這些性質直接源自於尺寸控制之結果，特別僅存於粒徑尺寸小於或接近1.4 nm下。我們也同時證實了該1.4 nm的金奈米團簇具有相當低的癌細胞毒性以及增生之影響性。這些粒子在癌細胞內顯著的累積量使得我們可以利用X-ray造影和螢光顯微技術來追蹤癌細胞在動物體內的位置和轉移之情況。
金奈米粒子同時也允許我們可以對其進行多樣性的表面修飾，使其具備更多不同的物理和生物化學性質。這些成熟的程序不但可以在我們所合成出來的奈米粒子上得以實現，更能有意義地拓展其在生物醫學上具有潛力的應用價值。我們發現特別的表面硫醇基化除了可影響金奈米粒子的尺寸之外，更決定了UV激發出可見螢光的存在與否。藉由分析具有不同碳鏈長度烷基硫醇（從3-巰基丙酸到16-巰基十六烷酸）之金奈米粒子的表面覆蓋來探究了這樣的現象，結果指出：強光致螢光特性僅存在於最小尺寸的金奈米粒子下；隨著烷基硫醇的碳鏈長度增加，其強度也隨之明顯的增加；在最長碳鏈16-巰基十六烷酸的表面覆蓋下可達到28%的量子效率。

The synthesis of gold nanoparticles (Au NPs) with desired size is an important prerequisite for the full exploitation of their properties. Highly functional Au NPs can be synthesized by several means, but these approaches require complex procedures such as template removal. These processes generally are limited by the reaction rate kinetics and result in broad particle size distribution. Our study implemented a completely different synthesis strategy using x-ray irradiation. This thesis focuses specifically on the synthesis of Au NPs and demonstrates the subsequent unique properties make possible due to mainly the exceptional ability to control the particle size.
With very intense X-rays generated by a device such as synchrotron accelerator, the reduction of metal ion in solution completed extremely fast and the nucleation of the reduced metal atoms starts uniformly. These favorable characteristics allow us to successfully synthesize Au NPs in different sizes, especially in very small size ~1 nm, with narrow size distribution and excellent colloidal stability, without access to physical templates such as dendrimers and micelle. The process therefore not only simplifies the synthesis and increases the control on the reaction, but reduces the possible negative effects of more complicated purification process.
Two coexisting properties of these small Au NPs, a strong visible fluorescence and very high accumulation in cancer cells, enable a new type multimodality imaging using X-ray and visible light microscopes in biomedical research. These properties come as a direct consequence of the precise size control; specifically, they exist only when the size is smaller than ~1.4 nm. We also demonstrate that these 1.4 nm Au NPs are non-cytotoxic and do not interfere with cancer cell proliferation. Significant accumulation of these Au NPs in tumor cells allows us to use X-ray imaging and fluorescence microscopy to trace their location in animal and follow their migration.
These nanoparticles, specifically Au NPs, allow versatile modifications of their surface and subsequent physical and biochemical properties. These matured processes can be implemented to our nanoparticles and further expand their potential biomedical applications. We found specifically surface thiolation affects the size of Au NPs and the presence of visible luminescence under UV stimulation. These phenomena were also explored by analyzing alkanethiolate coatings with different carbon chain lengths, from 3-mercaptopropionic acid (3-MPA) to 16-mercaptohexadecanoic acid (16-MHDA). Photoluminescence is present for the smallest NPs, but its intensity becomes more intense as the carbon chain length increases, achieving a quantum efficiency of 28% with a 16-MHDA coating.

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