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瞬态液相辅助化学溶液沉积法(TLAG-CSD)中氧分压跃升路径生长YBa2Cu3O7–δ的外延取向依赖前驱相中的钡铜比. 为了探究这现象的深层机理, 本文在中高温热处理过程中探究了不同氧分压、不同钡铜比组分对钡铜氧液相([Ba-Cu-O]L)以及反应中间相转变的影响. 研究表明: 液相的形成都具有点到面的特性; 液相出现的温度差异、形态差异, 主要由组分决定, 氧分压只起辅助作用. Y∶Ba∶Cu = 0∶3∶7(记为0-3-7)都先于Y∶Ba∶Cu = 0∶2∶3(记为0-2-3)出现液相, 温差在20 ℃(高氧分压)或40 ℃(低氧分压). 实验发现这两组分的中间相性状存在差异, 高氧分压下中间相BaCuO2在0-3-7组分是单一特征峰, 晶粒大而分散; 0-2-3组分则是多特征峰, 晶粒小而密集. 导致0-3-7组分的液相区表面积小于0-2-3组分, 进而两组分液相中Y3+过饱和度不同, 造成YBCO的取向差异. 最后总结得出无氟液相生成的基本模型, 完全的[Ba-Cu-O]L膜可由0-2-3组分在750 ℃高氧分压下生成.
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关键词:
- TLAG-CSD /
- YBa2Cu3O7–δ外延取向 /
- [Ba-Cu-O]L /
- 钡铜比
The epitaxial orientation of YBa2Cu3O7–δ grown via the oxygen partial pressure jump pathway in transient liquid-phase assisted chemical solution deposition (TLAG-CSD) depends on the barium-to-copper ratio in the precursor phase. To explore the mechanism behind this phenomenon, in this work we investigate the effects of different oxygen partial pressures and barium-to-copper ratio components on the barium-copper-oxygen liquid phase ([Ba-Cu-O]L) and the intermediate phase transition in the medium-high temperature heat treatment process. The research shows that the formation of the liquid phase exhibits a point-to-surface characteristic; the temperature and morphological differences in the liquid phase are mainly determined by the composition, with oxygen partial pressure only playing a supporting role. Y∶Ba∶Cu = 0∶3∶7 (0-3-7) components all appear before Y∶Ba∶Cu = 0∶2∶3 (0-2-3) components in the liquid phase, with a temperature difference of 20 ℃ (high oxygen partial pressure) or 40 ℃ (low oxygen partial pressure). Experimental results indicate that there are differences in the intermediate phase properties between these two components. Under high oxygen partial pressure, the intermediate phase BaCuO2 exhibits a single characteristic peak in the 0-3-7 component, with large and dispersed grains; the 0-2-3 component has multiple characteristic peaks, with small and dense grains. The surface area of the liquid phase region in the 0-3-7 component is smaller than that in the 0-2-3 component, resulting in different supersaturation levels of Y3+ in the liquid phases of the two components and causing orientation differences in YBCO. Finally, the basic model for the formation of fluorine-free liquid phase is summarized, and the complete [Ba-Cu-O]L film can be generated from the 0-2-3 component at high oxygen partial pressure and 750 ℃.-
Keywords:
- TLAG-CSD /
- epitaxial orientation of YBa2Cu3O7–δ /
- [Ba-Cu-O]L /
- barium copper ratio
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图 1 TLAG-CSD的两种路线对应的晶化反应示意图
Fig. 1. Schematic diagram of the crystallization reactions corresponding to the two routes of TLAG-CSD.
图 2 [Ba-Cu-O]L薄膜的热处理过程示意图
Fig. 2. Schematic diagram of heat treatment process of [Ba-Cu-O]L thin film.
图 3 Y∶Ba∶Cu = 1.5∶3∶7和Y∶Ba∶Cu = 1∶2∶3两组分薄膜在相同生长条件下YBCO的外延取向差异, 初始氧分压都为10 ppm
Fig. 3. Different epitaxial orientation of YBCO in Y∶Ba∶Cu = 1.5∶3∶7 and Y∶Ba∶Cu = 1∶2∶3 films grown under the same conditions, the initial oxygen partial pressures are all 10 ppm.
图 4 $ {P_{{{\text{O}}_{2}}}} $ = 1000 ppm, Y∶Ba∶Cu = 0∶3∶7和Y∶Ba∶Cu = 0∶2∶3两组分的液相在中高温热处理过程中的演变, 其中蓝虚线圈为液相痕迹, 红椭圆-蜂窝状为熔融凝固态, 红圆角矩形为大液相区, 橙圆角矩形为液相之间的空隙, 橙虚线标识液相间的分界线, 黄虚线圈为点状液相区
Fig. 4. $ {P_{{{\text{O}}_{2}}}} $ = 1000 ppm, the evolution of the liquid phase of Y∶Ba∶Cu = 0∶3∶7 and Y∶Ba∶Cu = 0∶2∶3 during medium and high temperature heat treatment, where blue dotted circle represents liquid phase trace; red ellipse represents honeycomb molten solid state; red rounded rectangle represents large liquid phase area; orange rounded rectangle represents gap between liquid phases, orange dotted line marks the boundary between liquid phases; yellow dotted circle represents pointed liquid phase area.
图 5 $ {P_{{{\text{O}}_{2}}}} $ = 10 ppm, Y∶Ba∶Cu = 0∶3∶7和Y∶Ba∶Cu = 0∶2∶3两组分的液相在中高温热处理过程中的演变, 其中红虚线圈为液相间的空隙, 蓝虚线框为液相层的阶梯状分布
Fig. 5. Evolution of the liquid phase of two components of $ {P_{{{\text{O}}_{2}}}} $ = 10 ppm, Y∶Ba∶Cu = 0∶3∶7 and Y∶Ba∶Cu = 0∶2∶3 during medium and high temperature heat treatment, where red dotted circle-the gap between the liquid phases, blue dotted frame-the stepped distribution of the liquid phase layer.
图 6 $ {P_{{{\text{O}}_{2}}}} $ = 10 ppm, 640 ℃下Y∶Ba∶Cu = 0∶3∶7组分薄膜表面的EDS元素点扫描, 显示黑色斑块区域富铜元素
Fig. 6. $ {P_{{{\text{O}}_{2}}}} $ = 10 ppm, EDS element point scanning of the surface of the Y∶Ba∶Cu = 0∶3∶7 component film at 640 ℃ shows that the black patch area is rich in copper elements.
图 7 示意不同组分液相形成时期的大小与分布等性状差异
Fig. 7. Indicate the differences in characteristics such as size and distribution during the formation of liquid phases of different components.
图 8 $ {P_{{{\text{O}}_{2}}}} $ = 1000 ppm, Y∶Ba∶Cu = 0∶3∶7和Y∶Ba∶Cu = 0∶2∶3两组分薄膜中高温热处理过程的物相演变, 不同温度是指淬火温度, 由于该实验氧分压属于高氧分压[28](CuO不会被还原), 因此淬火在室温中进行
Fig. 8. Phase evolution during high temperature heat treatment of two-component films with $ {P_{{{\text{O}}_{2}}}} $ = 1000 ppm, Y∶Ba∶Cu = 0∶3∶7 and Y∶Ba∶Cu = 0∶2∶3, the different temperatures refer to the quenching temperatures, the quenching was performed at room temperature because the oxygen partial pressure in this experiment was high[28] (CuO would not be reduced).
图 9 (a), (b) $ {P_{{{\text{O}}_{2}}}} $ = 1000 ppm, 660 ℃下Y∶Ba∶Cu = 0∶3∶7和Y∶Ba∶Cu = 0∶2∶3两组分薄膜表面SEM图以及对应的EDS元素扫描和Ba元素的表面分布图, (c), (d) Y∶Ba∶Cu = 0∶3∶7和Y∶Ba∶Cu = 0∶2∶3两组分薄膜的AFM扫描图像
Fig. 9. (a), (b) $ {P_{{{\text{O}}_{2}}}} $ = 1000 ppm: SEM images of the surface of the two-component films Y∶Ba∶Cu = 0∶3∶7 and Y∶Ba∶Cu = 0∶2∶3 at 660 ℃, and the corresponding EDS element scans and surface distribution of Ba elements; (c), (d) AFM scan images of the corresponding two-component films.
图 10 $ {P_{{{\text{O}}_{2}}}} $ = 10 ppm, Y∶Ba∶Cu = 0∶3∶7和Y∶Ba∶Cu = 0∶2∶3两组分薄膜中高温热处理过程的物相演变, 不同温度是指淬火温度, 由于该实验氧分压属于低氧分压[28](CuO会被还原), 因此淬火是在液氮中进行
Fig. 10. Phase evolution during high temperature heat treatment of two-component films with $ {P_{{{\text{O}}_{2}}}} $ = 10 ppm, Y∶Ba∶Cu = 0∶3∶7 and Y∶Ba∶Cu = 0∶2∶3, the different temperatures refer to the quenching temperatures, the quenching was performed in liquid nitrogen because the oxygen partial pressure in this experiment was low[28] (CuO would be reduced).
图 11 (a)—(c)不同氧分压下, Y∶Ba∶Cu = 0∶3∶7和Y∶Ba∶Cu = 0∶2∶3两组分的BaCO3和BaCuO2特征峰面积随温度的变化, 紫虚线表示两曲线的下降斜率一致, 罗马数字表示不同的温区; (d) Ton是BaCO3的分解温度, TL是形成完全液相的温度
Fig. 11. (a)–(c) Characteristic peak areas of BaCO3 and BaCuO2 of Y∶Ba∶Cu = 0∶3∶7 and Y∶Ba∶Cu = 0∶2∶3 under different oxygen partial pressures vary with temperature, the purple dashed line indicates that the two curves have the same downward slope, and the Roman numerals represent different temperature zones; (d) Ton is the decomposition temperature of BaCO3, and TL is the temperature at which a complete liquid phase is formed.
图 12 (a), (b) Y∶Ba∶Cu = 0∶3∶7和Y∶Ba∶Cu = 0∶2∶3组分的前驱相颗粒均匀分布示意图; (c), (d) 高、低氧分压下完全[Ba-Cu-O]L膜的形成示意图
Fig. 12. (a), (b) Schematic diagrams of uniform distribution of precursor phase particles of Y∶Ba∶Cu = 0∶3∶7 and Y∶Ba∶Cu = 0∶2∶3 components, respectively; (c), (d) schematic diagrams of the formation of complete [Ba-Cu-O]L film under high and low oxygen partial pressures, respectively.
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