本研究對臺北機器局遺址出土之古瓷器，採用非侵入性分析方法，使用顯微拉曼光譜儀、微區X光射線螢光光譜儀 (μ-XRF) 對源自中國與日本兩種不同起源的24件瓷器進行坯體、釉料和顏料的分析，試圖比較兩種不同起源的古瓷器在礦物和化學組成上的異同情形。顯微拉曼分析結果顯示臺北機器局遺址挖掘出土源自中國瓷器坯體的礦物以石英、莫來石為主，日本瓷器則以石英為主，莫來石的存在與否顯示中國與日本來源的瓷器存在著差異。此外由釉料拉曼圖譜分析計算所得到的拉曼聚合指數 (Ip, the Raman Index of Polymerization) ，顯示其燒製溫度大約在1000～1400℃左右，若與顯微拉曼光譜分析礦物種類的結果結合，可進一步推測燒製溫度介於1200℃~1400℃。源自中國瓷器與日本瓷器可能皆含鈣基釉及鉀基釉，此結果與μ-XRF對釉料助溶劑的成分分析結果一致。顏料 (藍色、綠色、紫色及黑色) 的礦物成分拉曼分析結果，大部分僅識別出典型的玻璃結構的 Si-O 拉伸和彎曲包絡圖譜。利用拉曼聚合作用指數 (Ip) 、最大伸長振動峰值波數 (νmax Si-O Stretching) 與前人研究中拉曼圖譜資料比對，本研究的標本點皆落在瓷器區域，與前人研究結果類似。
對古瓷器坯體進行化學成分分析，以坯體中主要氧化物Al2O3與SiO2散點圖顯示，源自日本瓷器除了標本POR24、POR25、POR35及POR38落入中國瓷器的範圍外，其餘標本坯體具有低鋁低矽的特性，原因可能是考古學家錯誤分類的來源或者是仿中國瓷器風格的產品，而源自中國瓷器坯體具有高鋁高矽的特性。顏料分析結果顯示，源自中國瓷器藍色顏料可能以亞鐵離子 (Fe2+) 作為著色劑，而源自日本瓷器藍色顏料可能以氧化鈷作為著色劑且以低量鈷離子 (Co2+) 完全熔融在玻璃網絡中，鐵元素可能是有意添加的，使藍色裝飾呈深藍色。
另外計算 Fe2O3 /CoO 和 MnO/CoO 的比值，源自日本瓷器具有較低的 Fe2O3 /CoO 和 MnO/CoO 比值，因此呈現艷麗深藍，而大多數源自中國瓷器具有較高的 Fe2O3/CoO 和 MnO/CoO 比值，呈現淡藍，僅有源自中國瓷器標本POR-21、POR-22及POR-23具有較低 Fe2O3 /CoO 比值的特殊中國瓷器仍然呈現深藍。綠色顏料部分，源自中國瓷器標本POR17與源自日本瓷器標本POR28、POR33的 μ-XRF 結果顯示皆含有鐵元素，推測其亞鐵離子(Fe2+) 是導致鈣 (鉀) 基釉中觀察到的綠色的原因。源自日本標本POR32、33、35、38和源自中國標本POR34、36、37、39棕色顏料及源自日本標本POR30橘色顏料被鑑定為赤鐵礦。另外，源自日本標本POR31紫色顏料推測其著色劑為亞錳離子 (Mn2+) 。源自日本標本POR31、POR32、POR33黑色顏料推測其著色劑為由氧化鐵 (Fe2O3) 導致的。

In this study, non-invasive methods were employed to analyze antique porcelain excavated from the Taipei Machinery Bureau (TMB) site. Twenty-four porcelain wares of two distinct Chinese and Japanese origins were examined in terms of body, glaze and pigment using a micro-Raman spectrometer and micro X-ray fluorescence (μ-XRF) spectrometer to compare the mineral and chemical composition of the wares of the two different origins. The results of the micro-Raman analysis indicate that the minerals unearthed from the TMB site, which originated from Chinese porcelain bodies, are predominantly quartz and mullite, whereas Japanese porcelain is dominated by quartz. The presence or absence of mullite suggests a difference between porcelain of Chinese and Japanese origins. In addition, the Raman index of polymerization (Ip), calculated from the Raman spectra of the glazes, indicates a firing temperature of around 1000-1400°C. When combined with the results of the micro-Raman spectroscopy of the mineral species, the firing temperature can be further estimated to be in the range of 1200°C-1400°C. Porcelain of Chinese and Japanese origins may both contain calcium- and potassium-based glazes, and this result is concordant with the results of the μ-XRF analysis of the composition of the glaze solubilizers. Raman analytic results of the mineral composition for the pigments (blue, green, purple and black) mostly be identified only Si-O stretching and bending envelope graphs belonging to typical of glass structures. The Ip and the νmax Si-O stretching were compared with the Raman spectra from past research. The samples in this study all fell in the porcelain region, which is similar to the results of previous studies.
Analysis of the chemical composition of the archaic porcelain bodies, using scatter plots of the main oxides in the bodies, Al2O3 and SiO2, shows that, with the exception of the Japanese porcelain specimens POR24, POR25, POR35 and POR38, which fall within the range of Chinese porcelain, the rest of the specimens have low Al and Si characteristics, which may be the result of an archaeological misclassification or an imitation of Chinese porcelain style, whereas the Chinese porcelain bodies have high Al and Si characteristics. The results of the pigment analysis suggest that the blue pigment from Chinese porcelain might have been colored with ferrous ions (Fe2+), whereas the blue pigment from Japanese porcelain might have been colored with cobalt oxide and low levels of cobalt ions (Co2+) completely fused in the glass network, with the iron element possibly added intentionally to give the blue decoration a dark blue hue.
Additionally, when the ratio of Fe2O3/CoO to MnO/CoO was calculated, porcelain of Japanese origin has a lower Fe2O3/CoO and MnO/CoO ratio and therefore appears a brilliant dark blue, while most porcelain of Chinese origin has a higher Fe2O3/CoO and MnO/CoO ratio and exhibits a light shade of blue, except the Chinese porcelain samples POR-21, POR-22 and POR-23, which have a lower Fe2O3/CoO ratio, still appearing dark blue. For the green pigments, μ-XRF results from Chinese porcelain sample POR17 and Japanese porcelain samples POR28 and POR33 both show the presence of iron whose ferrous ions (Fe2+) are presumed to be responsible for the green tint observed in the calcium (potassium) based glazes. The brown pigment from Japanese samples POR32, 33, 35, 38 and the brown pigment from Chinese samples POR34, 36, 37, 39 and the orange pigment from Japanese sample POR30 have been identified as hematite. Further, the coloring agent for the purple pigment from the Japanese sample POR31 is presumed to be manganese ions (Mn2+). The black pigments from the Japanese samples POR31, POR32 and POR33 are presumed to be colored by iron oxide (Fe2O3).

第一章 緒論 1
1.1研究動機與目的 2
1.2研究流程 5
第二章 研究背景 7
2.1陶瓷特性 7
2.2古瓷器的特徵 8
2.3古瓷器的研究方法 10
2.4古瓷器的研究案例 13
2.5臺北機器局遺址背景 18
第三章 實驗原理與分析方法 25
3.1共軛聚焦顯微拉曼光譜儀 25
3.2 X光螢光光譜儀 29
3.3標本基本資料 31
第四章 結果與討論 37
4.1 標本拉曼光譜分析結果 37
4.2 標本μ-XRF分析結果 86
4.3 小結 90
4.4 討論 97
第五章 結論與建議 109
5.1結論 109
5.2建議 111
參考文獻 113
附錄一、顯微拉曼光譜分析圖譜補充 125
附錄二、μ-XRF的分析點位 135

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