Co、Sn共掺ZnO薄膜结构及其性能研究
摘要
ZnO是一种直接宽带隙半导体材料,具有六角纤锌矿型晶体结构,在室温下的禁带宽度为3.37eV,激子束缚能约60meV。ZnO具有很好的导热、导电、化学稳定性及良好的紫外吸收性能,广泛应用于表面声波器、UV探测器、传感器、红外反射器和太阳能电池等领域。另外它还具有优越的光电性能,是制造蓝光及紫外光电器件最有应用前景的材料之一。随着光电子技术的迅速发展,对紫光和蓝光等短波长发光材料的需求越来越迫切。由于室温下ZnO的禁带宽度为3.37eV,再加之其较高的激子束缚能,故ZnO理论上不仅具备实现蓝光和紫外光发射的本领,甚至在高于室温的环境中仍具有显著的低阀值激发机制,因此对ZnO发光特性及其发光机制的进一步研究就显得尤为重要。
本文采用溶胶-凝胶旋涂法在玻璃衬底上制备了Co,Sn掺杂ZnO系列薄膜。通过金相显微镜和X射线衍射(XRD)研究了Co与Sn掺杂对薄膜的表面形貌和微结构的影响。XRD结果表明,所有ZnO薄膜样品都存在(002)择优取向,特别Sn单掺ZnO薄膜的c轴择优取向最为显著,而且晶粒尺寸最大。XPS测试表明样品中Co和Sn的价态分别为2+和4+,证实Co~(2+),Sn~(4+)进入了ZnO的晶格。振动样品磁强计(VSM)测量表明Zn_(1-x)Co_xO薄膜具有室温铁磁性。室温光致发光谱(PL)显示在所有的样品中都有较强的蓝光双峰发射和较弱的绿光发射,而在纯ZnO及Co掺杂ZnO薄膜样品中还观察到了较强的紫外发光峰。此外,通过Co,Sn掺杂的控制能够调整薄膜的禁带宽度,进而使得蓝光发光峰发生了位移;同时,掺杂还将影响薄膜中氧位错、锌空位和锌填隙缺陷,因此控制掺杂浓度可以调控薄膜的发光特性。最后,我们还探讨了不同波段光发射的可能机理。
ZnO is a type ofⅡ-Ⅵcompound semiconductor material with a direct wide band gap (Eg~3.37 ev at room temperature) and a high excition binding energy of 60 meV. Its stable crystal structure is hexagonal wurtzite structure. ZnO possesses excellent heat conduction, electric conduction, chemical stability and ultraviolet absorption properties and can be used in many applications, such as surface acoustic wave devices, UV detectors, gas sensors, infra-red reflectors and solar cells and so on. Moreover, it has excellent optoelectronic properties, so ZnO is one of the most promising materials for optoelectronic devices in blue and ultraviolet region. With the rapid development of optoelectronic technology, the demand of the purple and blue short-wavelength light-emitting materials has become more and more imperative. Due to its energy gap of about 3.37eV at RT and high excition binding energy, ZnO can not only achieve blue and UV light emitting in theory, but also has remarkable low threshold value even above room temperature. So the investigations on the optical propertities and luminescence mechanism of ZnO become particularly important.
In this thesis, the Co and/or Sn doped ZnO thin films were deposited on the glass substrate by means of sol-gel method. The influence of Co and/or Sn doping on surface morphologies and mircrostructures of ZnO films has been investigated by metallurgical microscope and X-ray diffraction (XRD). The XRD results indicate that all the ZnO samples show preferential orientation along (002) direction, and the Sn-doped ZnO thin film shows the best c-axis orientation and largest grain size. XPS results reveal that Co and Sn elements exist as Co~(2+) and Sn~(4+), testifying that Co and Sn ions have entered the ZnO crystal lattices successfully. The vibrating sample magnetometer (VSM) measures the ferromagnetic properties of Zn0.95Co0.05O thin films at room temperature. Strong blue double emission and weak green emission were observed in PL spectrum of all the samples. In addition, the ultraviolet peak appeared in the undoped and Co-doped ZnO thin films. Our results reveal that the Co and/or Sn doping can tune the band gap, meanwhile, such doping can also affect oxygen dislocation, zinc vacancy and zinc interstitial defect concentration. Finally, the possible luminescence mechanism of Co and/or Sn doped ZnO films were discussed.
本文采用溶胶-凝胶旋涂法在玻璃衬底上制备了Co,Sn掺杂ZnO系列薄膜。通过金相显微镜和X射线衍射(XRD)研究了Co与Sn掺杂对薄膜的表面形貌和微结构的影响。XRD结果表明,所有ZnO薄膜样品都存在(002)择优取向,特别Sn单掺ZnO薄膜的c轴择优取向最为显著,而且晶粒尺寸最大。XPS测试表明样品中Co和Sn的价态分别为2+和4+,证实Co~(2+),Sn~(4+)进入了ZnO的晶格。振动样品磁强计(VSM)测量表明Zn_(1-x)Co_xO薄膜具有室温铁磁性。室温光致发光谱(PL)显示在所有的样品中都有较强的蓝光双峰发射和较弱的绿光发射,而在纯ZnO及Co掺杂ZnO薄膜样品中还观察到了较强的紫外发光峰。此外,通过Co,Sn掺杂的控制能够调整薄膜的禁带宽度,进而使得蓝光发光峰发生了位移;同时,掺杂还将影响薄膜中氧位错、锌空位和锌填隙缺陷,因此控制掺杂浓度可以调控薄膜的发光特性。最后,我们还探讨了不同波段光发射的可能机理。
ZnO is a type ofⅡ-Ⅵcompound semiconductor material with a direct wide band gap (Eg~3.37 ev at room temperature) and a high excition binding energy of 60 meV. Its stable crystal structure is hexagonal wurtzite structure. ZnO possesses excellent heat conduction, electric conduction, chemical stability and ultraviolet absorption properties and can be used in many applications, such as surface acoustic wave devices, UV detectors, gas sensors, infra-red reflectors and solar cells and so on. Moreover, it has excellent optoelectronic properties, so ZnO is one of the most promising materials for optoelectronic devices in blue and ultraviolet region. With the rapid development of optoelectronic technology, the demand of the purple and blue short-wavelength light-emitting materials has become more and more imperative. Due to its energy gap of about 3.37eV at RT and high excition binding energy, ZnO can not only achieve blue and UV light emitting in theory, but also has remarkable low threshold value even above room temperature. So the investigations on the optical propertities and luminescence mechanism of ZnO become particularly important.
In this thesis, the Co and/or Sn doped ZnO thin films were deposited on the glass substrate by means of sol-gel method. The influence of Co and/or Sn doping on surface morphologies and mircrostructures of ZnO films has been investigated by metallurgical microscope and X-ray diffraction (XRD). The XRD results indicate that all the ZnO samples show preferential orientation along (002) direction, and the Sn-doped ZnO thin film shows the best c-axis orientation and largest grain size. XPS results reveal that Co and Sn elements exist as Co~(2+) and Sn~(4+), testifying that Co and Sn ions have entered the ZnO crystal lattices successfully. The vibrating sample magnetometer (VSM) measures the ferromagnetic properties of Zn0.95Co0.05O thin films at room temperature. Strong blue double emission and weak green emission were observed in PL spectrum of all the samples. In addition, the ultraviolet peak appeared in the undoped and Co-doped ZnO thin films. Our results reveal that the Co and/or Sn doping can tune the band gap, meanwhile, such doping can also affect oxygen dislocation, zinc vacancy and zinc interstitial defect concentration. Finally, the possible luminescence mechanism of Co and/or Sn doped ZnO films were discussed.
引文
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[4]王百齐,夏春辉,富强,王朋伟,单旭东,俞大鹏. Co掺杂ZnO纳米棒的水热法制备及其光致发光性能.物理化学学报, 2008, 24(7): 1165-1168.
[5]张桥保,冯增芳,韩楠楠,林玲玲,周剑章,林仲华.CdS量子点敏化ZnO纳米棒阵列电极的制备和光电化学性能[J].物理化学学报, 2010,26(11): 2927-2934.
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