我們利用一套窄線寬(< 100 kHz)、波長可調(2.66 − 4.77 μm)、高功率(> 3 mW)的中紅外差頻雷射光源，結合光頻梳來進行量測分子與分子離子的轉動振動光譜。本論文的內容分為兩個部分，第一個部分是分子光譜的精密量測−以N2O氣體分子基頻帶光譜(1000 ← 0000)為例;第二個部分是分子離子光譜的精密量測−以𝐻3+離子光譜為例。
N2O氣體分子結構類似於CO2分子，在中紅外波段的高精密光譜量測，期望提供最準確的躍遷頻率作為理論計算驗證的基礎。在4.5 μm 1000 ← 0000實驗，結合頻率調制技術及飽和吸收光譜的實驗架構，觀測了44條躍遷，得到高訊雜比之飽和吸收譜線。頻率測量的方法是將Nd:YAG雷射以碘分子穩頻，Ti:sapphire雷射鎖在N2O飽和吸收譜線的中心，並且以光頻梳(OFC)來校正其頻率，躍遷譜線的頻率準確優於95 kHz。此外，我們與Jet Propulsion Laboratory (JPL) Brian Drouin博士合作數據擬合分析，大幅改進分子常數的準確度，並進一步的修正N2O的理論模型及理論預測的頻率位置。
H3+分子離子是由三個質子及兩個電子所組成的三原子分子，因其簡單結構，對於多原子分子系統它提供一個理論計算的檢驗基礎。到目前為止，大部分𝐻3+躍遷的是利用速度調制光譜方法觀測，以中性氣體之吸收譜線校正頻率，準確度約150~300 MHz。最近，我們實驗室及UIUC McCall研究群分別觀測H3+的飽和光譜，使用光頻梳可以將躍遷頻率的準確度推進至小於1 MHz。這些方法具備非常高的準確度，但系統較複雜、訊號較小，不太適用於弱的吸收譜線。本論文中，我們利用速度調制法來偵測H3+分子離子的振動轉動吸收譜線訊號，並藉由光頻梳系統來測量躍遷頻率，期望能提昇H3+分子離子弱吸收譜線躍遷頻率的準確度。我們量測H3+之R(1,0)譜線，並與飽和吸收光譜量測做比較，發現我們的系統準確度可達4 MHz。未來我們將改進Ti:sapphire OFC和PPLN DFG光譜的鎖頻的準確度，並檢驗弱吸收譜線的測量準確度，最後我們將廣泛地量測H3+譜線。

ABSTRACT
We report the application of a CW mid-infrared difference frequency generation (DFG) source with Optical Frequency Comb (OFC) to molecule and molecular ion spectroscopy. This DFG source has the characteristics of narrow linewidth (< 100 kHz), wide tuning range (2.66 − 4.77 μm) and good power level (> 3 mW). We have accomplished two high precision spectroscopic measurements: molecular spectroscopy of N2O and molecular ion spectroscopy of 𝐻3+.
First, 44 transition lines of sub-Doppler profile of the 1000 ← 0000 N2O fundamental band at 4.5 μm are observed with the frequency modulation spectroscopy. The Nd:YAG laser is stabilized onto the iodine frequency standard line. The Ti:sapphire laser is locked onto the center of N2O transition and then beat with OFC for frequency measurement. The absolute frequencies of those transition lines are derived by fDFG =fTis − fYAG. The measurements of absolute frequencies for transitions up to J = 100 of the 1000 ← 0000 band are accomplished with an accuracy better than 95 kHz. For the molecular constant fitting analysis, we collaborated with Dr. Brian Drouin of Jet Propulsion Laboratory (JPL). With the help of the refined constants, the accuracy has been improved by two orders of magnitude compared with current HITRAN database.
The tri-atomic hydrogen molecular ion 𝐻3+, consisting of three protons and two electrons, is the simplest polyatomic molecule. Due to its simple structure, it is the benchmark of accurate calculation of polyatomic molecule. So far, most of H3+ transitions are observed by the velocity modulation spectroscopy which eliminates the strong absorption line of neutral gas. The transition frequency accuracy is about 150~300 MHz. Recently, our lab and McCall’s group have measured the saturated absorption spectrum of H3+. These two works achieve frequency accuracy better than 1 MHz with the help of optic frequency comb (OFC). Although saturation spectroscopy provides high accuracy, but the spectroscopic systems are more complex and the signal are smaller. In this dissertation, we use the velocity modulation spectroscopy to detect the vibration-rotation absorption transition of H3+ molecular ion, and measure its absolute frequency. For R(1,0) line of H3+, the frequency accuracy of the absorption transition is improved to 4 MHz. In the future, we will improve the stability of the frequency locking of our Ti:sapphire frequency comb and PPLN DFG and test the measurement accuracy of a weak absorption line. Finally, we will extensively measure the weak absorption lines of H3+.

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Chapter 6
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