ⅢA族元素掺杂ZnO透明导电薄膜的研究及在6H-SiC上的电极应用
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摘要
ⅢA族元素掺杂ZnO薄膜具备良好的透明导电性能(透过率>90%,电阻率10-4Ω·cm),且无毒污染、价格低廉,有望取代ITO成为新一代工业应用透明导电薄膜材料。本文研究了磁束缚电感耦合等离子体增强物理气相沉积法(ICP-PVD)制备的ⅢA族元素掺杂ZnO透明导电薄膜,分析了掺杂ZnO薄膜中的半导体性能及光学性能。另外,通过掺杂ZnO薄膜的晶体结构、表面、透明和半导体性能的比较,研究Al、Ga元素掺杂对ZnO透明导电薄膜应用的影响。ZnO与6H-SiC的结构相似,晶格失配度低(c轴～3.3%),因而是6H-SiC基光电器件的良好窗口材料,应用领域及前景非常广泛。因此本文进一步研究了Al、 Ga元素掺杂ZnO/6H-SiC异质结的结构、界面及能带排列,并实现了ZnO:Ga(GZO)透明导电薄膜在6H-SiC光导开关上的电极应用。主要工作内容如下：
1.采用ICP-PVD法制备了一系列ZnO薄膜,确定了该仪器合适的工艺参数范围。在最佳工艺下制备的1mol%Ga掺杂ZnO薄膜结晶质量好,光学可见光平均透过率为93%,电阻率为7.68×10-4Ω.cm。另外研究了沉积氧分压对GZO薄膜的结晶、半导体性能及光学性能的影响。通过GZO薄膜的绿色光致发光分析,提出2.5及2.65eV附近存在两种个相连的施主受主对复合发光,分别对应于跃迁GaZnO+VZn-→GaZn++VZn2-和GaZnO+O1O→GaZn++O1-,并通过薄膜快速退火前后的光致发光全谱给予辅证。
2.研究了ZnO:Al(AZO)及GZO薄膜的透过、半导体性能。在同样的制备工艺及同样的掺杂浓度下,AZO薄膜的导电性能要优于GZO薄膜,这归因于A1的散射半径比Ga小,因此AZO薄膜中的霍尔迁移率更高。而GZO薄膜的透过性能优于AZO薄膜,与掺杂元素的散射无关,归因于Ga元素充当了表面活性剂的作用。GZO薄膜的表面比AZO薄膜光滑,因此漫反射反射更少、透过率更高。提出Ga.Al共掺杂可能会使ZnO材料的电学性能和透过性能得到进一步的提高。Al.Ga掺杂ZnO薄膜材料的禁带宽度均高于本征ZnO,且在同等浓度掺杂下,Ga掺杂ZnO的禁带宽度要比Al掺杂ZnO高0.3eV左右。同步辐射紫外光电子能谱(SRPES)表明两者的能带结构不同,因此AZO与GZO的差别可能归因于Al和Ga的元素掺杂效应不同。Al掺杂能使ZnO价带中2p-3d耦合增强,而Ga掺杂对价带几乎没有影响,因此AZO的价带顶位置相对GZO更高。
3.制备并研究了未退火处理的Al、Ga元素掺杂ZnO/6H-SiC异质结,分析了异质结的结构、界面及能带排列。通过SRPES能谱分析,GZO/6H-SiC异质结的价带能级偏移为1.34±0.04eV,导带的能级偏移为0.93±0.04eV；而AZO/SiC异质结的价带能级偏移为1.78±0.04eV,导带能级偏移为1.4±0.04eV,两者均为ⅡA型异质结结构。同样的制备工艺和掺杂浓度下,GZO/SiC异质结能级偏移与AZO/SiC异质结能级偏移相差约0.4eV,这可能归因于两者界面处晶格失配度变化不同,Ga-O比Al-O更接近Zn-O。另外我们制备了Si面向及C面向的GZO/SiC异质结并获得其能带结构,结果显示Si面向GZO/SiC异质结和C面向GZO/SiC异质结的价带能级偏移相差仅0.05eV。
4.经过快速退火处理后,GZO/SiC异质结界面处的能带结构发生了变化。Si面向GZO/SiC异质结退火后增大0.1eV,而C面向GZO/SiC异质结退火后增大0.25eV。SRPES显示异质结界面出的能谱中出现了类似于SiO2的分量存在。这表明当GZO/SiC异质结经过快速退火处理后,C面向GZO/SiC结构中的氧化程度高于比Si面向GZO/SiC结构,前者类似活性氧化反应,后者类似钝性的氧化反应。该结果也表明快速退火并不适用于ZnO/SiC异质结的制备。
5.电学性能及透过性能测试结果表明SiC衬底上制备的GZO薄膜的透过率约为96%,电阻率约为5.68×10-4Ω.cm,且与SiC之间的接触为欧姆接触,因此能应用为SiC光电器件的透明导电电极。在SiC晶片上沉积GZO薄膜作为SiC光导开关的电极,当外加500V电压,10mJ激光光照时可实现光导开关的导通,导通电阻为13.2Ω。
The ZnO thin film doped with ⅢA group elements is considered as a promising candidate for substituting ITO due to its merits, such as high transmittance (over90%in the visible range), outstanding electric properties (～10-4Ω·cm), innoxiousness and cheapness. In this paper, we prepared Al-and Ga-doped ZnO (AZO and GZO) transparent conductive films (TCF) by Inductively Coupled Plasma Enhanced Physical Vapor Deposition (ICP-PVD). The Structure, surface, transmittance, electrical and electric structure properties were investigated to compare the doping effect on application properties of ZnO TCF. The optical properties of GZO TCF were also studied to confirm the possible emissions and related defects.
At the same time, ZnO TCF is also an attractive candidate electrode for6H-SiC based photoelectric devices due to its similar wurtzite crystal structure and relatively small lattice mismatch (3.3%along the c-axis). In this paper, we prepared Al-and Ga-doped ZnO/6H-SiC heterojunctions, and characterized their structure, interface and band structure. The preliminary application of GZO TCF-electrode on6H-SiC based photoconductive switch was also realized.
The main work included:
1. A serial of ZnO thin films were prepared by ICP-PVD, the suitable process parameters were confirmed. The as deposited1mol%Ga-doped ZnO thin film show a good properties, with transmittance93%and resistivity7.68×10-4Ω·cm. The effect of oxygen partial pressure (PO2) on properties of GZO thin films was also discussed. The photoluminescence of GZO films deposited under different PO2were studied by Gauss fitting. The fitting results suggest two adjacent green emissions located at2.50eV and2.65eV were attributed to donor-acceptor pair combination, corresponding to GaZnO+VZn-→GaZn++VZn2-and GaZnO+OiO→GaZn++O1-transitions, respectively. The conclusion was consistent with the low temperature photoluminescence of GZO films before and after rapid thermal annealing.
2. The2mol%Ga and Al doped ZnO thin films were grown under different deposition atmospheres to discuss the transparence electric and electronic properties. With the same doping concentration and experiment process, the conductivity of AZO films were better than that of GZO, which was due to the higher hall mobility induced by smaller Al scattering radiusl. But the transparence properties was revus, which was due to the smoother surface of GZO films induced by surfactant element Ga. This results suggest the Al and Ga co-doping might be enhanced transparent conductive properties of ZnO thin film. With the same2mol%doping concentration, the doping elements both increased the band gap energy of ZnO, but GZO were0.3eV higher than that of AZO. The Synchrotron radiation photoelectron spectroscopy (SRPES) measurements sugeest the valance band of AZO were different from that of GZO. Al doping effect is different from Ga, which might enhance the2p-3d coupling in ZnO valance band, which induced a higher valance band maximum.
3. Ga doped ZnO (GZO) and Al doped ZnO (AZO) thin films were deposited on n-6H-SiC to form the heteroj unction structure. The band alignments of the doped ZnO/6H-SiC heterojunctions were studied by using the synchrotron radiation photoelectron spectroscopy. Band alignments of GZO/SiC and AZO/SiC heterojunctions were determined by the band offsets calculation. AZO/SiC heterojunction has bigger band offsets than ZnO/SiC and GZO/SiC heterojunction, which is due to the closer doping element covalence radius. Ga-0is more closer to Zn-O than Al-O. The higher mismatch induces higher band offsets on heterojunction interface. The Si-and C-faced GZO/SiC were also prepared and characterized, the valance band offset difference of them was just0.05eV.
4. Band alignments of GZO/SiC heterojunctions were increased after rapid thermal annealing process, be0.1eV and0.25eV for Si-and C-faced, respectively. The SRPES showed a new component was formed on heterojunctions'interface after RTA, which was deduced to be "SiO2" component. This component was deeper and with higher concentration in C-faced GZO/SiC heterojunction than that in Si-faced GZO/SiC heterojunction. The result suggests that the RTA process was not suitable for ZnO/SiC heterojunction.
5. The transmittance and resistivity of2mol%Ga doped ZnO thin films deposited on SiC substrate were96%and5.68×10-4Ω·cm, respectively. The GZO and SiC contact performance as ohmic contact, which suggests that GZO film is a suitable electrode for SiC-based opt-electric device. The SiC Photoconductive switch has been successfully fabricated with GZO thin films as front electrode, which showed an on-state performance while be excitated with lOmJ laser under500V voltage. The on-state resistance was13.2Ohm.
1.采用ICP-PVD法制备了一系列ZnO薄膜,确定了该仪器合适的工艺参数范围。在最佳工艺下制备的1mol%Ga掺杂ZnO薄膜结晶质量好,光学可见光平均透过率为93%,电阻率为7.68×10-4Ω.cm。另外研究了沉积氧分压对GZO薄膜的结晶、半导体性能及光学性能的影响。通过GZO薄膜的绿色光致发光分析,提出2.5及2.65eV附近存在两种个相连的施主受主对复合发光,分别对应于跃迁GaZnO+VZn-→GaZn++VZn2-和GaZnO+O1O→GaZn++O1-,并通过薄膜快速退火前后的光致发光全谱给予辅证。
2.研究了ZnO:Al(AZO)及GZO薄膜的透过、半导体性能。在同样的制备工艺及同样的掺杂浓度下,AZO薄膜的导电性能要优于GZO薄膜,这归因于A1的散射半径比Ga小,因此AZO薄膜中的霍尔迁移率更高。而GZO薄膜的透过性能优于AZO薄膜,与掺杂元素的散射无关,归因于Ga元素充当了表面活性剂的作用。GZO薄膜的表面比AZO薄膜光滑,因此漫反射反射更少、透过率更高。提出Ga.Al共掺杂可能会使ZnO材料的电学性能和透过性能得到进一步的提高。Al.Ga掺杂ZnO薄膜材料的禁带宽度均高于本征ZnO,且在同等浓度掺杂下,Ga掺杂ZnO的禁带宽度要比Al掺杂ZnO高0.3eV左右。同步辐射紫外光电子能谱(SRPES)表明两者的能带结构不同,因此AZO与GZO的差别可能归因于Al和Ga的元素掺杂效应不同。Al掺杂能使ZnO价带中2p-3d耦合增强,而Ga掺杂对价带几乎没有影响,因此AZO的价带顶位置相对GZO更高。
3.制备并研究了未退火处理的Al、Ga元素掺杂ZnO/6H-SiC异质结,分析了异质结的结构、界面及能带排列。通过SRPES能谱分析,GZO/6H-SiC异质结的价带能级偏移为1.34±0.04eV,导带的能级偏移为0.93±0.04eV；而AZO/SiC异质结的价带能级偏移为1.78±0.04eV,导带能级偏移为1.4±0.04eV,两者均为ⅡA型异质结结构。同样的制备工艺和掺杂浓度下,GZO/SiC异质结能级偏移与AZO/SiC异质结能级偏移相差约0.4eV,这可能归因于两者界面处晶格失配度变化不同,Ga-O比Al-O更接近Zn-O。另外我们制备了Si面向及C面向的GZO/SiC异质结并获得其能带结构,结果显示Si面向GZO/SiC异质结和C面向GZO/SiC异质结的价带能级偏移相差仅0.05eV。
4.经过快速退火处理后,GZO/SiC异质结界面处的能带结构发生了变化。Si面向GZO/SiC异质结退火后增大0.1eV,而C面向GZO/SiC异质结退火后增大0.25eV。SRPES显示异质结界面出的能谱中出现了类似于SiO2的分量存在。这表明当GZO/SiC异质结经过快速退火处理后,C面向GZO/SiC结构中的氧化程度高于比Si面向GZO/SiC结构,前者类似活性氧化反应,后者类似钝性的氧化反应。该结果也表明快速退火并不适用于ZnO/SiC异质结的制备。
5.电学性能及透过性能测试结果表明SiC衬底上制备的GZO薄膜的透过率约为96%,电阻率约为5.68×10-4Ω.cm,且与SiC之间的接触为欧姆接触,因此能应用为SiC光电器件的透明导电电极。在SiC晶片上沉积GZO薄膜作为SiC光导开关的电极,当外加500V电压,10mJ激光光照时可实现光导开关的导通,导通电阻为13.2Ω。
The ZnO thin film doped with ⅢA group elements is considered as a promising candidate for substituting ITO due to its merits, such as high transmittance (over90%in the visible range), outstanding electric properties (～10-4Ω·cm), innoxiousness and cheapness. In this paper, we prepared Al-and Ga-doped ZnO (AZO and GZO) transparent conductive films (TCF) by Inductively Coupled Plasma Enhanced Physical Vapor Deposition (ICP-PVD). The Structure, surface, transmittance, electrical and electric structure properties were investigated to compare the doping effect on application properties of ZnO TCF. The optical properties of GZO TCF were also studied to confirm the possible emissions and related defects.
At the same time, ZnO TCF is also an attractive candidate electrode for6H-SiC based photoelectric devices due to its similar wurtzite crystal structure and relatively small lattice mismatch (3.3%along the c-axis). In this paper, we prepared Al-and Ga-doped ZnO/6H-SiC heterojunctions, and characterized their structure, interface and band structure. The preliminary application of GZO TCF-electrode on6H-SiC based photoconductive switch was also realized.
The main work included:
1. A serial of ZnO thin films were prepared by ICP-PVD, the suitable process parameters were confirmed. The as deposited1mol%Ga-doped ZnO thin film show a good properties, with transmittance93%and resistivity7.68×10-4Ω·cm. The effect of oxygen partial pressure (PO2) on properties of GZO thin films was also discussed. The photoluminescence of GZO films deposited under different PO2were studied by Gauss fitting. The fitting results suggest two adjacent green emissions located at2.50eV and2.65eV were attributed to donor-acceptor pair combination, corresponding to GaZnO+VZn-→GaZn++VZn2-and GaZnO+OiO→GaZn++O1-transitions, respectively. The conclusion was consistent with the low temperature photoluminescence of GZO films before and after rapid thermal annealing.
2. The2mol%Ga and Al doped ZnO thin films were grown under different deposition atmospheres to discuss the transparence electric and electronic properties. With the same doping concentration and experiment process, the conductivity of AZO films were better than that of GZO, which was due to the higher hall mobility induced by smaller Al scattering radiusl. But the transparence properties was revus, which was due to the smoother surface of GZO films induced by surfactant element Ga. This results suggest the Al and Ga co-doping might be enhanced transparent conductive properties of ZnO thin film. With the same2mol%doping concentration, the doping elements both increased the band gap energy of ZnO, but GZO were0.3eV higher than that of AZO. The Synchrotron radiation photoelectron spectroscopy (SRPES) measurements sugeest the valance band of AZO were different from that of GZO. Al doping effect is different from Ga, which might enhance the2p-3d coupling in ZnO valance band, which induced a higher valance band maximum.
3. Ga doped ZnO (GZO) and Al doped ZnO (AZO) thin films were deposited on n-6H-SiC to form the heteroj unction structure. The band alignments of the doped ZnO/6H-SiC heterojunctions were studied by using the synchrotron radiation photoelectron spectroscopy. Band alignments of GZO/SiC and AZO/SiC heterojunctions were determined by the band offsets calculation. AZO/SiC heterojunction has bigger band offsets than ZnO/SiC and GZO/SiC heterojunction, which is due to the closer doping element covalence radius. Ga-0is more closer to Zn-O than Al-O. The higher mismatch induces higher band offsets on heterojunction interface. The Si-and C-faced GZO/SiC were also prepared and characterized, the valance band offset difference of them was just0.05eV.
4. Band alignments of GZO/SiC heterojunctions were increased after rapid thermal annealing process, be0.1eV and0.25eV for Si-and C-faced, respectively. The SRPES showed a new component was formed on heterojunctions'interface after RTA, which was deduced to be "SiO2" component. This component was deeper and with higher concentration in C-faced GZO/SiC heterojunction than that in Si-faced GZO/SiC heterojunction. The result suggests that the RTA process was not suitable for ZnO/SiC heterojunction.
5. The transmittance and resistivity of2mol%Ga doped ZnO thin films deposited on SiC substrate were96%and5.68×10-4Ω·cm, respectively. The GZO and SiC contact performance as ohmic contact, which suggests that GZO film is a suitable electrode for SiC-based opt-electric device. The SiC Photoconductive switch has been successfully fabricated with GZO thin films as front electrode, which showed an on-state performance while be excitated with lOmJ laser under500V voltage. The on-state resistance was13.2Ohm.
引文
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