本論文主要在氮氣、氫氣、氬氣、氦氣與高真空下成長pentacene薄膜，並以此材料為主動層製作有機薄膜電晶體。我們在真空度2×10-5 torr氮氣環境中成長pentacene，其電晶體元件載子遷移率約0.24 cm2/Vs；然而，在氫氣環境中成長pentacene得到的元件載子遷移率約0.008 cm2/Vs，推測在氮氣環境中成長的pentacene薄膜，有較好的分子排列結構。由atomic force microscope (AFM)掃瞄圖發現，其表面形貌出現樹枝狀結構，並且由X-ray diffraction (XRD)的量測結果發現pentacene平均結晶大小與元件載子遷移率有明顯關聯。
接下來分別在表面能以及表面粗糙度類似的高分子材料「聚甲基丙烯酸甲酯(polymethylmethacrylate, PMMA)」與SiO2表面成長pentacene，在這兩種表面成長的pentacene薄膜，都具有良好的結晶品質，然而成長在PMMA表面的pentacene晶粒明顯小很多。以PMMA當修飾層的有機薄膜電晶體，有非常好的電性表現，包括元件載子遷移率超過1.1 cm2/Vs，以及電流開關比大於106，次臨界斜率小於1 V/dec，並進一步利用共振拉曼光譜(Resonance Raman Spectroscope)的量測結果，解釋為何以PMMA當修飾層的有機薄膜電晶體，其電性表現如此優異。
我們藉由XRD、AFM、接觸角量測儀(contact angle meter)、以及拉曼光譜，量測厚度從幾個分子單層到數百奈米的複晶系pentacene薄膜.，分析其隨厚度而變的結晶結構、表面形貌、表面自由能、以及分子微結構；由XRD的數據分析，並定義pentacene分子傾斜角(tilt angle, θtilt)為從分子c軸倒向a軸的角度，發現pentacene薄膜從正交晶相(orthorhombic phase)變化到薄膜相(thin-film phase)，然後再到三斜晶系的塊材相(triclinic bulk phase)。並結合AFM以及薄膜接觸角量測隨著薄膜成長而變化的pentacene表面自由能與晶粒尺寸，來合理解釋隨著pentacene薄膜厚度變化的傾斜角，並提出pentacene初期成長模型。
最後，不同膜厚的pentacene分子振動特性可以藉由拉曼光譜量測得到，再結合XRD與AFM可以讓我們解析pentacene薄膜中的分子微結構；並藉由pentacene薄膜出現在拉曼光譜中的晶場分裂(crystal field splitting)特性以及分析其C-C伸縮振動區的譜線半高寬來決定薄膜內的載子傳輸特性。我們認為初期成長的幾個pentacene分子單層由於其分子間作用力較弱，並且擁有較大的分子緩遲能(molecular relaxation energy)，以及形成較多的晶粒邊界(grain boundary)，以致於有較差的載子傳輸特性。

Pentacene based thin-film transistors (TFTs) have been fabricated using pentacene films grown under various ambiences, such as N2, H2, Ar, He, and high vacuum. The field-effect mobility of 0.24 cm2/Vs was obtained from TFTs fabricated under 210-5 torr nitrogen ambience, however, the pentacene TFTs fabricated in hydrogen ambience under the same pressure yielded very poor mobility of 0.008 cm2/Vs. Pentacene films deposited by thermal evaporation in nitrogen ambience have a high degree of molecular ordering with larger dendritic grains without any surface modification on silicon oxide dielectric. A clean relation between field-effect mobility and X-ray diffraction (XRD) estimated crystallites size was obtained.
Additionally, the pentacene thin films have fabricated on polymethylmethacrylate (PMMA) and on silicon dioxide dielectric surfaces with the similar surface energy and surface roughness. On both surfaces the pentacene films displayed the high crystal quality from XRD scans, although the film on PMMA with significantly smaller grain size. The pentacene-based transistors with PMMA exhibited excellent electrical characteristics, including high mobility of above 1.1 cm2/Vs, on/off ratio above 106, and sharp subthreshold slope below 1 V/dec. The analysis of molecular microstructure of the pentacene films provided a reasonable explanation for the high performance using resonance micro-Raman spectroscopy.
Thickness-dependent crystal structure, surface morphology, surface free energy, and molecular structure and microstructure of a series of polycrystalline pentacene films with different film thickness ranging from several monolayers to the several hundred nanometers have been investigated using XRD, atomic force microscopy (AFM), contact angle meter, and Raman spectroscopy. XRD studies indicate that transformation behaviors of thin film polymorphs are from orthorhombic phase to thin-film phase and then to triclinic bulk phase as measured by the increased tilt angle (θtilt) of the pentacene molecule from the c axis toward the a-b lattice plane. We propose a growth model that rationalizes the θtilt increased with increasing film thickness in terms of grain size and surface free energy which vary with film growth measured by AFM combined with contact angle. The vibrational characterizations of pentacene molecules in different thickness films were investigated by Raman spectroscopy compared to density functional theory calculations of a free molecule. Combining XRD with AFM enables us to distinguish the molecular microstructures in different thin film polymorphs. We proposed a methodology to probe the microscopic parameters determining the carrier transport properties relating to crystal field splitting and half-width of aromatic C-C stretching modes in Raman spectra. The first few monolayer structures located at the dielectric surface could have inferior carrier transport properties due to weak intermolecular interactions, large molecular relaxation energy, and more grain boundaries as compared with triclinic bulk phase at high thickness.

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