液體 / 空氣界面二倍頻現象的超快時間解析光譜研究

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研究生：	黃敞 Huang, Cheng
論文名稱：	液體 / 空氣界面二倍頻現象的超快時間解析光譜研究 Ultrafast Time-Resolved Spectroscopic Studies of SHG at Liquid / Air Interface
指導教授：	鄭博元 Cheng, Po-Yuan
口試委員:
學位類別：	碩士 Master
系所名稱：	理學院 - 化學系 Department of Chemistry
論文出版年：	2008
畢業學年度：	97
語文別：	中文
論文頁數：	100
中文關鍵詞：	二倍頻、瞬態光譜、表面、界面、張量、誤差、SHG 、orientation 、isotherm 、transient spectra
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表面二倍頻現象是二倍頻現象的特例，利用二倍頻現象只可發生在非中心對稱的材料中的特性，來偵測具有中心對稱的材料的表面或界面間的物質特性。本論文的目的是藉由自行架設的表面二倍頻光學系統，觀測染料分子 Coumarin 481 (C481) 在空氣 / 水界面上的熱力學性質 (C481 在界面上的排列情形及吸附自由能 ΔGads)，及動力學性質 (C481 在界面上的 solvation time 及激發態生命期)。
從實驗的結果，在熱力學性質方面，我們可粗略地得知 C481 在界面上的排列情形，以及其表面吸附自由能，並與許多文獻值比較，結果指向 C481 是以 -CF3 及 -C=O 端深入水中，而 -N(C2H5)2 端是暴露在空氣中；在動力學性質方面，我們藉由本實驗室另一套光學系統 -- time-resolved fluorescence by optical Kerr gating (TRF-OKG) 測得 C481 在塊材水溶液中的瞬態光譜，並與表面二倍頻測得的瞬態光譜比較，可知由於 -N(C2H5)2 取代基暴露在空氣中，使得躍遷至 twisted intramolecular charge transfer (TICT) state 的 nonradiative decay process 難以進行，所以界面 C481 的生命期會比水溶液中的 C481 的生命期長，類似處在非極性溶劑的環境中。

第一章、序論...................................................................................................1
   1.0. 前言......................................................................................................1
   1.1. 簡史......................................................................................................1
   1.2. 非線性光學的基本原理及由來...................................................................3
   1.3. 表面二倍頻現象的原理與應用...................................................................8
   1.4. 文獻回顧.............................................................................................10
     1.4.a. 分子在物質表面的排列情形...............................................................10
     1.4.b. 表面分子的吸附熱力學性質...............................................................12
     1.4.c. 界面分子間的電子轉移 (electron transfer，ET)..................................13
     1.4.d. 表面分子的 photoisomerization......................................................15
     1.4.e. 表面分子的 orientational relaxation.................................................16
   1.5. 實驗目的與簡介....................................................................................18
   參考資料....................................................................................................20
第二章、實驗儀器系統....................................................................................24
   2.0. 前言....................................................................................................24
   2.1. Millennia (Nd：YVNO4 cw laser).........................................................24
   2.2. Tsunami (Ti：Sapphire mode locking laser)........................................27
     2.2.a. 聲光調幅鎖模..................................................................................29
     2.2.b. Kerr 效應鎖模 (Kerr lens mode locking，KLM).................................34
     2.2.c. 菱鏡組 (prism pair).........................................................................39
   2.3. Evolution X (Q-switch Nd：YLF laser).................................................41
   2.4. Spitfire (regenerative amplifier for Ti：Sapphire pulsed laser).............46
     2.4.a. stretcher & compressor..................................................................46
     2.4.b. regenerative amplifier...................................................................48
     2.4.c. 同步延遲產生器...............................................................................49
  參考資料.....................................................................................................51
第三章、實驗系統架設....................................................................................53
   3.0. 前言....................................................................................................53
   3.1. 系統簡介.............................................................................................53
第四章、實驗結果與討論.................................................................................57
   4.0. 前言....................................................................................................57
   4.1. 水 / 空氣界面的表面二倍頻測試實驗.......................................................57
     4.1.a. power dependence........................................................................57
     4.1.b. wavelength dependence................................................................58
     4.1.c. polarization dependence...............................................................60
   4.2. C481(aq) / 空氣界面的穩定態光譜.........................................................62
     4.2.a. 分子的在界面上的排列情形...............................................................62
     4.2.b. 分子在界面的吸附自由能..................................................................68
   4.3. C481(aq) / 空氣界面的瞬態光譜............................................................72
  參考資料.....................................................................................................78
第五章、結論.................................................................................................80
附錄.............................................................................................................82
   A.1. 分子在界面上的排列.............................................................................82
      A.1.a. 張量的數學意義及界面 χ(2) 的對稱性................................................82
      A.1.b. I(2ω) 與 χ(2) 之間的關係.................................................................84
      A.1.c. β 的推導及圖形法微擾理論 (diagrammatic perturbation theory)........87
      A.1.d. χ(2) 與 β 之間的關係及 Euler angles................................................89
   A.2. C481(aq) / 空氣界面的瞬態光譜............................................................90
      A.2.a. 瞬態光譜中表面二倍頻訊號的消長.....................................................90
      A.2.b. 瞬態光譜的動力學模型....................................................................92
   A.3. 實驗誤差分析.......................................................................................94
      A.3.a. 適解函數的參數誤差........................................................................94
      A.3.b. 理論數值點的誤差...........................................................................97
      A.3.c. 實驗誤差的運算方法........................................................................98
  參考資料.....................................................................................................98

                                

書籍：
“Classical Dynamics of Particles and Systems” by J. B. Marion and S. T. Thomton, Harcourt Brace Jovanovich, 5th edition.
“渾沌 -- 不測風雲的背後” by James Gleick and 林和 (譯者), 天下文化.
“Introduction to Electrodynamics” by D. J. Griffith, Prentice Hall, 3rd edition.
“Nonlinear Optics” by R. W. Boyd, Elsevier, 2nd edition.
“Quantum Optics” by M. O. Scully and M. S. Zubairy, Cambridge University Press.
“Atom-Photon Interactions : Basic Processes and Applications” by C. Cohen-Tannoudji, J. Dupont-Roc and G. Grynberg, John Wiley and Sons.
“Quantum Chemistry” by I. N. Levine, Prentice Hall, 5th edition.
“Fundamentals of Photonics” by B. E. A. Saleh and M. C. Teich, Wiley-Interscience, 2nd edition.
“Ultrafast Optics” by A. M. Weiner, Wiley (to be published).
“周威銧碩士論文” by 周威銧碩士, 清華大學, 2008.
“丁蕙雯碩士論文” by 丁蕙雯, 清華大學, 2006.
“Chemical Kinetics and Reaction Dynamics” by P. L. Houston, Mc Graw Hill, 1st edition.
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“Modern Quantum Chemistry : introduction to advanced electronic structure theory’ by A. Szabo & N. S. Ostlund, McGraw-Hill, 1996.
“Quantitative Chemical Analysis’ by D. C. Harris, Freeman, 6th edition.

網站：
History of research in nonlinear optics at the institute of optics
http://www.optics.rochester.edu/~stroud/BookHTML/ChapVII_pdf/VII_56.pdf
History of lasers
http://inventors.about.com/od/lstartinventions/a/laser.htm
What is a maser ?
http://einstein.stanford.edu/content/faqs/maser.html
Promote passion with July’s birthstone, Ruby
http://www.a1-birthstone-jewelry.com/july-birthstone-ruby.shtml
Pulsed ruby laser
http://visual.merriam-webster.com/science/physics-optics/pulsed-ruby-laser.php
Calcite photos
http://skywalker.cochise.edu/wellerr/mineral/calcite/calcite6.htm
The mineral calcite
http://mineral.galleries.com/Minerals/Carbonat/calcite/calcite.htm
Langmuir adsorption
http://www.thuisexperimenteren.nl/infopages/langmuir/langmuir.htm
Ti：Sapphire crystal
http://www.redoptronics.com/Ti-Sapphire-crystal.html
Hexagonal crystal system
http://www.minerals.net/glossary/terms/h/hexagona.htm
Gradient index optics technology
http://www.grintech.de/
White light generation
http://www.eecs.umich.edu/USL/NORRIS/WhiteLightSetup.html
Brewster plates
http://www.rp-photonics.com/brewster_plates.html
Irving Langnuir
http://nobelprize.org/nobel_prizes/chemistry/laureates/1932/langmuir-bio.html
Refractive index as a function of wavelength
http://www.philiplaven.com/p20.html
Euler angles
http://mathworld.wolfram.com/EulerAngles.html

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