我們使用鈦藍寶石脈衝雷射(Ti:Al2O3)所輸出波長為800 nm、重複率為82 MHz、時寬為35飛秒(femtosecond)的脈衝為光源，對C6H6、C6H5Br、C6H5Cl、C6H5I、CH3OH、與DMSO等各種透明液體進行Z-scan實驗，結果在這些液體中發現負的非線性折射訊號。另方面，我們使用Nd:YAG雷射所輸出重複率為10Hz、脈衝時寬為19皮秒(picosecond) 的光源在各種透明液體中觀察到正的非線性折射率。兩種不同光源所產生的重大差別可能肇因於脈衝時寬的差別（35 飛秒與19 皮秒）或是脈衝間時距的差別（12.1奈秒(1/82 MHz) 與0.1秒(1/10 Hz)）。在本論文中，我們以電子快門將35飛秒脈衝截成不同時寬(介於1 ms (millisecond)與50 ms間)的脈衝串，並使相鄰兩脈衝串間時距遠大於純熱擴散時間(thermal diffusivity time)，然後以此脈衝串為光源，對透明液體進行Z-scan實驗。結果，我們發現35 飛秒脈衝所引起的負透鏡效應首先率隨著脈衝串時寬的增加而變大，然後當脈衝串時寬超過純熱擴散時間一定程度之後，此一熱透鏡效應趨於穩定。負透鏡效應隨脈衝串時寬增加而改變的趨勢說明跨脈衝累積效應的存在，而當脈衝串時寬超過純熱擴散時間一定程度之後，負透鏡效應有趨於穩定的趨勢。我們則可更進一步指出，跨脈衝累積效應極可能是熱透鏡效應。當我們推論實驗所見的負透鏡效應是一種跨脈衝累積的熱效應之後，我們更進一步注意到，熱透鏡效應隨分子尺寸的增加而增強，以及分子對稱性對於熱透鏡效應的強弱有明顯的影響。

Using the Z-scan technique with 82 MHz 35 fs laser pulses at 800 nm, we observed negative nonlinear refraction in various transparent molecular liquids C6H6, C6H5Br, C6H5Cl, C6H5I, CH3OH, and DMSO. On the other hand, we observed positive nonlinear refraction in these samples with 10 Hz 19 ps laser pulses. This trend imitates that of the previously investigated C2H4Br2, C2H4Br2, CHBr3, CHCl3, CS2, and CBrCl3. Sign flip due to change of the pulse width from 35 fs to 19 ps or that of the pulse-to-pulse separation from 12.1 ns to 0.1 s may be explained in virtue of Raman induced Kerr effect or thermal lensing effect. By conducting the Z-scan technique with the continuously output 35 fs laser pulses sliced into trains of various widths with respect to the thermal diffusivity time constant and by keeping the train-to-train separation considerably longer than that thermal diffusivity time constant, we find the 35 fs pulse-induced negative nonlinear refraction monotonously increases with the pulse width and gradually turns steady on the time scale of thermal diffusivity. This indicates the contribution of thermal lensing effect. In addition, we noticed that the thermal lensing effect increases with the increase of molecular weights or sizes. We found that molecular symmetry plays an important role in thermal lensing effect. Also, we anticipated that thermal lensing effect arises from from resonant and orientational relaxations of the excited molecular skeletal motions.

目錄
第一章 緒論 p.5
第二章 理論基礎 p.7
第1段 吸收和折射巨觀的描述 p.7
第1小節 樣品對光的非線性效應 p.7
第2小節 線性吸收與折射( ) p.13
第3小節 三階非線性吸收與折射( ) p.14
第4小節 總結 p.15
第2段 拉曼感應克爾效應(Raman induced Kerr effect) p.17
第3段 單發脈衝下的克爾運動模型簡述 p.20
第4段 拉曼散射解釋透明液體中的熱效應成因 p.22
第5段 跨脈衝累積熱透鏡效應 p.25
第三章 實驗儀器與架設 p.28
第1節 飛秒雷射架設 p.28
第2節 皮秒雷射架設 p.29
第3節 自相干涉儀 p.30
第4節 Z-scan技術與原理 p.33
第1小節 實驗架設 p.33
第2小節 自散焦現象 p.34
第3小節 自聚焦現象 p.35
第四章 實驗結果與討論 p.37
第1節 飛秒實驗結果與討論 p.37
第1小節 各種不同樣品飛秒Z-Scan p.37
第2小節 調整曝光時間觀察樣品熱效應大小 p.40
第3小節 不同樣品的熱效應比較 p.47
第2節 皮秒實驗結果 p.49
第五章 結論與未來工作 p.52
第1節 苯與苯基的熱效應大小分析 p.54
第2節 不同分子的熱效應大小分析 p.54
第3節 未來工作 p.54
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