本論文以線性及非線性光學系統探討鑽石中帶負電荷的「氮原子-空缺」缺陷中心〔記為 (N-V)─〕以及相關缺陷中心「氮原子-空缺-氮原子」缺陷中心〔記為 (NVN 或 H3〕的光譜性質研究。內容分為四大部分。
第一部分以固態Nd-YAG奈秒雷射來進行雙光子掃描顯微影像。利用平板鋪膜方法製造光阻薄膜並旋鍍螢光小球，以及經過R6G染色的洋蔥表皮細胞進行雙光子掃描，可證明此奈米雷射顯微技術可到達0.5微米的解析度。適當使用奈秒雷射來攝取映像，可簡化操作過程，降低成本，對材料的映像顯微有多方面的優點。更因奈秒雷射能輕易製成波長可調，對作選擇性的映像顯微更方便快捷。　
第二部分是利用超快飛秒雷射來進行 type Ib單晶合成鑽石的單光子(532nm)及雙光子(1064nm)激發之螢光光譜研究。合成單晶鑽石晶體經由能量3MeV以及40keV的氫離子束衝擊，接著以高溫攝氏八百度加熱（800℃）退火處理後，在晶格內部會產生很多(N-V)─缺陷中心，而形成紅色螢光鑽石。在以高能量離子束照射前，利用FTIR偵測合成鑽石晶體，藉由1344cm-1 特性峰來推算氮的含量約為100ppm左右，並於液態氮低溫中偵測其UV-VIS光譜，利用吸收光譜中NV的zero-phonon line（ZPL，637nm）強度估算其缺陷濃度約為25ppm。並經由雙光子激發照射，並與其他螢光材料經由相同實驗條件下作比較，估算其雙光子吸收截面積為σNV,TPA = (0.45±0.23) × 10-50 cm4⋅s/photon.
第三部分是說明綠色螢光奈米鑽石（簡稱為gFNDs）的製備與做為生物標記應用的特性。利用473nm連續波藍光雷射來進行type Ia單晶天然鑽石的單光子螢光光譜研究，天然奈米鑽石晶體經由能量40keV的氦離子束或是3MeV的氫離子束衝擊及高溫（800℃）退火處理後，再測其螢光光譜，發現以藍光激發會放出綠色螢光。推論並證實奈米鑽石粉末經過相同的處理程序後，也會有高濃度的H3 center結構產生，而形成綠色螢光奈米鑽石，所發出的綠色螢光不會有光漂白及光閃爍的現象。在以高能量離子束照射前，利用FTIR偵測天然鑽石晶體，藉由1282cm-1 特性峰來推算氮的含量約為900ppm左右。並利用吸收光譜中H3的zero-phonon line（ZPL，503nm）強度計算，可以知道H3 density大約10ppm。我們進一步利用螢光奈米鑽石的化學性穩定、細胞毒性低之特性，利用穿透式白光及廣視野螢光顯微鏡系統，觀察綠色螢光奈米鑽石可以經由細胞吞噬（endocytosis）進入活HeLa細胞中。我們成功地在細胞內看到螢光奈米鑽石，並確認他們的位置是在細胞質而非細胞核。更進一步利用流式細胞儀進行綠色螢光奈米鑽石粒子定性定量及時間相依測量分析，以證明70nm的綠色螢光奈米鑽石可以做為新穎的奈米螢光標記。
第四部分為利用405nm超快飛秒雷射針對 type Ia天然奈米鑽石顆粒作更進一步的光譜性質研究，在這個研究中，我們旋鍍 350nm type Ia 天然奈米鑽石在石英玻片上，經由掃瞄影像、光譜及生命期的測量，顯示其著稱的光學穩定性依舊明顯，且不因不同顆粒而有差別。而我們已知在type Ia 天然奈米鑽石顆粒中，同時存在少許(N-V)─缺陷中心以及H3缺陷中心，於是我們選擇利用拉伸指數數據擬合來分析其螢光生命期且得到很好的擬合曲線。

Abstract
The objective of this research is mainly talking about the linear and nonlinear experimental studies on spectroscopic properties of the nitrogen□vacancy□nitrogen (NVN) and nitrogen□vacancy (N-V)- defect centers in type Ia and Ib diamond, and their related applications in this report are presented in four parts.
The first part, we report the application of a multi-kHz diode-laser-pumped Q-switched Nd:YAG laser operating at 1064 nm to obtain two-photon-excited fluorescence scanning images with photolithography prepared photoresist film, red fluorescent polystyrene beads, R6G-dyed onion skin and also type Ib single crystal diamond. With careful and properly chosen operating parameters, we do not observe damages to the samples after repeated scans. The spatial resolution achieved was about 0.5 micron.
The second part shows experimental results of one-photon (532nm) and two-photon (1064nm) excited fluorescence spectra of the negative charged nitrogen –vacancy (N-V)□□ defect centers in type Ib diamond, and also the deduced results of the corresponding one-photon and two-photon absorption cross sections are reported. Comparing the normalized spectral shapes recorded from one-photon and two-photon excitations, they are very similar except the photoionization effect of neutral (N-V)0 centers which yield 575nm ZPL and the accompanied vibronic band were more obvious under much more intense 1064 nm excitation.
The third part concerns experimental results of one-photon excitation of another related nitrogen vacancy centers, the H3 (NVN) centers, usually can be found in type Ia diamond. This work demonstrate the one-photon (473nm) excited fluorescence spectrum, the estimated corresponding absorption cross sections, and also the alternative use of type Ia diamond nanoparticles in biological applications.
The fourth part is focusing on more detail characterization understanding of H3 centers in type Ia diamond. We chose 405nm as an excitation wavelength to avoid fluorescence sideband contributed from (N-V)-□□ centers. Through stretched-exponential fitting of luminescence lifetime, help us to understand the complex property of type Ia diamond, and also through lifetime measurement correlated with color and polarization dichroism, we found that there is not much correlation between lifetime and the internal polarization property of type Ia diamond. This might because the high concentration of defect centers which produced by the helium beam irradiation and annealing treatment, some distinguishable internal properties of color centers will be washed off, reveals homogeneous optical properties. And the color dichroism result tells us that the major color center properties of type Ia nanodiamond are H3 centers.

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