掺钼氧化锌透明导电薄膜的制备与特性研究
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摘要
透明导电氧化物(TCOs)薄膜在可见光区具有很高的透过率、在红外区具有很高的反射率、并且具有较低的电阻率。因此在太阳能电池、平板显示和有机发光二极管(OLED)等领域得到了广泛的应用。在各种透明导电氧化物薄膜中，ITO的应用最为广泛，这是因为ITO具有较低的电阻率、较高的功函数、在可见光区具有较高的透过率。但是ITO也存在许多缺点，例如在OLED中，ITO／空穴传输层界面具有较高的势垒，能够影响空穴的传输；铟元素容易向有机层中扩散，降低器件的性能；另外铟在自然界中的含量较少，所以制备ITO薄膜的成本较高。近年来，ZnO及其掺杂体系被广泛研究，有希望成为ITO的替代材料。目前掺Al、Ga、In、Zr、B和稀土等元素的ZnO薄膜已经用各种技术制备出来。尽管如此寻找新型的透明导电氧化物薄膜仍然是非常有意义的。
Mo~(6+)的离子半径为6.2×10~(-11)m，比Zn~(2+)的离子半径(7.4×10~(-11)m)小，因此理论上存在Mo~(6+)替代Zn~(2+)的可能性。并且Mo~(6+)和Zn~(2+)价态差4这一点是非常吸引人的，因为一个掺杂原子可以提供更多的电子。在相同的掺杂浓度下，掺Mo的ZnO薄膜(MZO)具有更高的载流子浓度；另一方面，相同的载流子浓度情况下，MZO薄膜中需要掺入的杂质量更少，从而能够减小薄膜中的缺陷，提高载流子迁移率，降低薄膜的电阻率。
我们采用射频磁控溅射技术，在玻璃衬底上成功制备出了MZO薄膜。利用XRD、SEM、AFM和XPS等分析手段对薄膜的结构、表面形貌和化学性质进行了表征，利用霍耳测试仪和分光光度计分别对薄膜的电学和光学性质进行了测量，总结了大量的数据。详细研究了杂质的掺杂量、薄膜厚度、溅射功率、氩气压和衬底温度对薄膜结构、光学和电学性质的影响。在MZO的应用方面，我们利用MZO薄膜作为阳极、以MZO薄膜作为阳极，制备出具有MZO／TPD／Alq_3／Al结构的有机发光二极管。具体的研究内容和主要结果如下：
Transparent conducting oxide films (TCOs) with high optical transparence in the visible range, high optical reflectance in the infrared range and high electrical conductivity have been widely used in flat panel displays, electronic devices, organic light-emitting diodes and solar cells. Among all the TCOs, indium tin oxide (ITO) has been widely used because of its low resistivity, high transmittance and high work function. However, ITO has some disadvantages such as a high-energy barrier for holes injection at the ITO/hole transport layer interface and the diffusion of indium into the organic layers in organic light-emitting diodes. Recently, ZnO has been actively investigated as an alternate material to ITO because it is nontoxic, inexpensive, and abundant compared with ITO. Moreover, ZnO is chemically stable in hydrogen plasma that is commonly used in the fabrication of TFT-LCDs. Al, Ga, In, Zr, B and rare earth-doped ZnO films have been grown by various deposition techniques. However, looking for new materials still remains interesting and attractive.
The ionic radii of Mo~(6+) is 6.2 × 10~(-11) m, and that of Zn~(2+) is 7.4 × 10~(-11) m, thus it is theoretically possible for Mo~(6+) to substitute Zn~(2+) in the MZO. Moreover, there is a valence difference of 4 between Mo~(6+) and Zn~(2+), which is quite attractive because one dopant atom can contribute more electrons to the electrical conductivity. MZO films should have high carrier mobility because there is fewer dopant in MZO than in other doped oxides at the same carrier concentration.
A new transparent conducting oxide film of molybdenum-doped zinc oxide (MZO) has been prepared by RF magnetron sputtering method on glass substrate. The structural and chemical properties were measured with XRD, SEM, AFM and XPS. The electrical properties were measured with Hall effect measurements using the Van der Pauw
Mo~(6+)的离子半径为6.2×10~(-11)m，比Zn~(2+)的离子半径(7.4×10~(-11)m)小，因此理论上存在Mo~(6+)替代Zn~(2+)的可能性。并且Mo~(6+)和Zn~(2+)价态差4这一点是非常吸引人的，因为一个掺杂原子可以提供更多的电子。在相同的掺杂浓度下，掺Mo的ZnO薄膜(MZO)具有更高的载流子浓度；另一方面，相同的载流子浓度情况下，MZO薄膜中需要掺入的杂质量更少，从而能够减小薄膜中的缺陷，提高载流子迁移率，降低薄膜的电阻率。
我们采用射频磁控溅射技术，在玻璃衬底上成功制备出了MZO薄膜。利用XRD、SEM、AFM和XPS等分析手段对薄膜的结构、表面形貌和化学性质进行了表征，利用霍耳测试仪和分光光度计分别对薄膜的电学和光学性质进行了测量，总结了大量的数据。详细研究了杂质的掺杂量、薄膜厚度、溅射功率、氩气压和衬底温度对薄膜结构、光学和电学性质的影响。在MZO的应用方面，我们利用MZO薄膜作为阳极、以MZO薄膜作为阳极，制备出具有MZO／TPD／Alq_3／Al结构的有机发光二极管。具体的研究内容和主要结果如下：
Transparent conducting oxide films (TCOs) with high optical transparence in the visible range, high optical reflectance in the infrared range and high electrical conductivity have been widely used in flat panel displays, electronic devices, organic light-emitting diodes and solar cells. Among all the TCOs, indium tin oxide (ITO) has been widely used because of its low resistivity, high transmittance and high work function. However, ITO has some disadvantages such as a high-energy barrier for holes injection at the ITO/hole transport layer interface and the diffusion of indium into the organic layers in organic light-emitting diodes. Recently, ZnO has been actively investigated as an alternate material to ITO because it is nontoxic, inexpensive, and abundant compared with ITO. Moreover, ZnO is chemically stable in hydrogen plasma that is commonly used in the fabrication of TFT-LCDs. Al, Ga, In, Zr, B and rare earth-doped ZnO films have been grown by various deposition techniques. However, looking for new materials still remains interesting and attractive.
The ionic radii of Mo~(6+) is 6.2 × 10~(-11) m, and that of Zn~(2+) is 7.4 × 10~(-11) m, thus it is theoretically possible for Mo~(6+) to substitute Zn~(2+) in the MZO. Moreover, there is a valence difference of 4 between Mo~(6+) and Zn~(2+), which is quite attractive because one dopant atom can contribute more electrons to the electrical conductivity. MZO films should have high carrier mobility because there is fewer dopant in MZO than in other doped oxides at the same carrier concentration.
A new transparent conducting oxide film of molybdenum-doped zinc oxide (MZO) has been prepared by RF magnetron sputtering method on glass substrate. The structural and chemical properties were measured with XRD, SEM, AFM and XPS. The electrical properties were measured with Hall effect measurements using the Van der Pauw
引文
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