新型硅基SINP异质面蓝紫光电池及SIS异质结光电器件的研究
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摘要
为了不增加电池制造工艺的复杂性,同时又能有效地提高硅光电池在蓝紫光波段(400～600nm)的量子效率。根据半导体能带工程,我们独创性地设计并采用工艺优化的射频磁控溅射ITO减反射/收集电极膜且结合热扩散磷形成浅结、低温热氧化生长超薄SiO2层技术,在p型晶硅衬底上成功制备了高量子效率的蓝紫光增强型SINP异质面光电池(SINP是semiconductor/insulator/np结构的缩写)。另一方面,根据优化的直流磁控溅射、直流反应磁控溅射AZO薄膜工艺条件,并用低温热氧化生长超薄SiO2层在p型晶硅衬底上成功制备了新型SIS异质结光电器件(SIS是semiconductor/insulator/semiconductor结构的缩写)。通过X-光衍射(XRD)、扫描电镜(SEM)、紫外-可见光透射谱(UV-VIS),以及霍尔效应(Hall effect)测量方法,表征了射频磁控溅射ITO薄膜;直流磁控溅射、直流反应磁控溅射AZO薄膜的微结构、光学与电学特性。系统地研究了基片温度对ITO、AZO薄膜微结构、形貌、电学、光学性能的影响及机制。我们对制备得到的SINP硅光电池及SIS异质结器件I-V、C-V及光谱响应特性进行了详细地测试、分析与探讨,获得了以下主要结果:
1.磁控溅射沉积的ITO薄膜结晶度高,并且具有较高的紫外—可见光透过率及优异的电学性能。系统研究了基片温度对射频磁控溅射ITO薄膜微结构、电学及光学性能的影响及机制。结果表明,当基片温度为480℃时,ITO薄膜性能最好,电阻率为9.42×10-5Ω·cm,载流子浓度高达3.461×1021/cm3,霍尔迁移率为19.1 cm2/V·s。ITO薄膜在可见光区域具有高的透射率,在95%以上。ITO薄膜为多晶晶体薄膜,具有高度(222)择优取向,结晶质量好。ITO薄膜在晶硅衬底上具有良好的钝化和减反射效果,尤其是在300～500nm紫外至蓝光区域。
2.用X射线光电子能谱(XPS)对500℃不同氧化时间的超薄氧化硅层及SINP结构光电池样品成分、化学态进行分析。表明表面层中存在非化学态成分。
3. SINP蓝紫光电池具有优异的整流特性及暗电流机制。室温下±1V时,SINP蓝紫光电池整流比为324.7,二极管理想因子n=1.84,AM1.5 100 mW/cm2光照下,光电转换效率η=12.26%。由于在SINP结构中,光电流可以通过高结晶度、高载流子迁移率的ITO薄膜横向输运,避免了高磷浓度n发射区中横向输运的复合,降低了发射区横向电阻影响引起的功率损耗,新型SINP蓝紫光电池短路电流密度高达JSC=38.7 mA/cm2,显示出良好的光伏特性。在500nm波长,蓝紫光增强型SINP光电池外量子效率及响应率高达70%及285 mA/W;在800nm波长,峰值响应率为487 mA/W。最近研制的采用60Ω/□n+—型发射极的浅结SINP光电池进一步提高短波光谱响应,蓝紫光灵敏度极高。器件光谱响应拟和计算结果表明,新型SINP蓝紫光电池的高量子效率得益于浅结,以及高导电率和对蓝紫光具有良好减反射效果的ITO薄膜的应用与结合。具有高蓝紫光以及其它可见光波段的光谱响应和光电转换的增强效果,是该器件的主要特征。其较高的短路电流密度,适合于发展成为新型结构的硅基太阳能电池。
4.以ZnO和Al2O3烧结的陶瓷靶,用直流磁控溅射工艺在玻璃基片上沉积出高质量的AZO薄膜,系统研究了不同基片温度对薄膜微结构、电学和光学性能的影响。当基片温度为480℃时,AZO薄膜性能最好,电阻率为3.483×10-3Ω·cm。AZO薄膜在可见光区域具有高的透射率,在90%左右。AZO薄膜为微晶晶体薄膜,具有高度(002)择优取向,结晶质量好。
5.以高纯度(99.99%)的锌铝合金(wt.98% Zn+wt.2%Al)靶,氩气和氧气为溅射工作气体,用直流反应磁控溅射工艺在玻璃基片上生长出高质量的AZO薄膜。系统研究了基片温度对直流反应磁控溅射AZO薄膜微结构、电学及光学性能的影响及机制。当基片温度为480℃时,AZO薄膜性能最好,电阻率为4.973×10-4Ω·cm,载流子浓度高达1.103×1021/cm3,霍尔迁移率为11.4 cm2/V·s。AZO薄膜在可见光区域具有高的透射率,在90%以上。AZO薄膜为六角纤锌矿结构的微晶晶体薄膜,具有高度(002)择优取向,结晶质量好。
6. SIS异质结器件良好的整流特性表明AZO和p—Si间形成高质量的异质结二极管,在反向偏压下获得明显的光电流。通过对几种磁控溅射方法制备AZO薄膜及SIS异质结器件光电性能的比较可知,由于直流反应磁控溅射高结晶度、高导电率的AZO薄膜作AZO/SiO2/p-Si SIS异质结结构器件的发射极和顶层大面积透明收集电极,大量的光生载流子可以轻易地流过直流反应磁控溅射AZO薄膜进入Cu金属电极而收集到,从而在反向偏压下直流反应磁控溅射AZO/SiO2/p-Si SIS异质结比直流磁控溅射AZO/SiO2/p-Si SIS异质结可获得更高的光电流。通过射频磁控溅射沉积一层高导电率的ITO透明电极薄膜在直流磁控溅射AZO/SiO2/p-Si SIS异质结结构上,将会使异质结光电性能得到很大改进。因为高导电率的ITO薄膜极大地改善了AZO/SiO2/p-Si SIS异质结顶层电流输运结构,可收集到更多的光生载流子,所以在反向偏压下显示了明显的光电转换特性,可获得最高的光电流。SIS异质结不仅具有一定的光生伏特效应,而且在反向偏压下显示出很高的光电流。可以成为低成本的太阳电池及性能优良的紫外—可见—近红外增强型广谱光电探测器。
In order to reduce the technical complexity of the fabrication and simultaneously to improve the quantum efficiency in the range of 400-600 nm, a new type of ITO/SiO2/np-Silicon frame (named as SINP) hetero-interface solar cell has been designed and developed by combining the p-n junction with ITO transparent conductive oxide thin film as top layer of the device, according to the energy band evolution. A series of advanced techniques have been applied to the fabrication process, such as shallow junction, back surface field of aluminum, ultra-thin SiO2 passivation layer, and ITO coating. On the other hand, the novel semiconductor-insulator-semiconductor (SIS) hetero-junction structure has been fabricated by thermally growing an ultrathin silicon dioxide at low temperature and subsequently magnetron sputtering deposition of Al-doped n-ZnO (named as AZO) layer on p-Si (100) wafer. The microstructure, optics and electrical properties of the ITO and AZO films were characterized by XRD, SEM, UV-VIS spectrophotometer and Hall effect measurement, respectively. The influence of the substrate temperatures on the properties of ITO and AZO films were deeply studied. The current-voltage (I-V)、capacitance -voltage (C-V) and spectral response characteristics of SINP hetero-interface solar cell and SIS heterojunctions were analyzed in detail.
1. ITO film possesses high quality in terms of antireflection and electrode functions. The influence of the substrate temperatures on the property of ITO film was deeply studied. The results indicated that ITO film possesses high quality , when the substrate temperature is at 480℃. The resistivity is as low as 9.42×10-5?·cm, the carrier concentration and mobility are as high as 3.46×1021 atom/cm3 and 19.1 cm2/V·s, respectively. The average transmittance of the film is about 95% in the visible region. The film has a bixbyite structure and a preferred growth along the (222) orientation, perpendicular to the substrate surface. The configuration of the ITO layer on the textured Si is suitable for the blue and ultraviolet cells owing to the less loss of the number of photons with a short wavelength, which is more favorable for high efficiency cells.
2. The ultra-thin SiO2 layer and SINP structure samples were analyzed by x-ray photoelectron spectroscopy (XPS). The results showed that the non-stoichiometric matter were present on the surface layers and which resulted in the electronic defects to the minority carrier transportation.
3. The I-V curves of SINP violet photoelectric cell showed the fairly good rectifying behaviors. The values of IF/IR (IF and IR stand for forward and reverse currents, respectively) at 1.0 V for the violet SINP device is as high as 324.7,and the ideality factor of the violet SINP photoelectric cell is 1.84. The conversion efficiencies of the violet SINP cell under illumination of continue light source (AM 1.5 class A) is12.26%. Because the high quality crystallite and the good conductivity of ITO film magnetron-sputtered on SiO2 lead to a great decrease of the lateral resistance, it is possible to decrease the power loss induced by the lateral resistance of emitter region in the new type solar cell with SINP structure. The short-circuit current density of the SINP violet solar cell is as high as JSC = 38.7 mA/cm2. The external quantum efficiencies (EQE) and responsivity of the violet SINP device are 70% and 285mA/W at 500nm, respectively. The spectral responsivity peak of the violet SINP photoelectric cell is 487mA/W at about 800nm.The latest result indicates that the violet SINP photoelectric cell with 60?/□shallow junction can greatly improve the violet response. The calculated results indicates that the high quantum efficiency and responsivity of violet and blue enhanced photovoltaic cell is attributed to the shallow junction and the good conducting, violet and blue antireflection coating of ITO optical film. We found that the main feature of our PV cell is the enhanced violet response and optoelectronic conversion. The improved short-circuit current, open-circuit voltage, and filled factor indicate that the device is promising to be developed into an ultraviolet and blue enhanced photovoltaic device in the future.
4. The AZO films were prepared by direct-current (DC) magnetron sputtering. The target was sintered ceramic disks of ZnO doped with 2 wt% Al2O3 (purity 99.99%). The AZO film possesses high quality in terms of electrode functions, when substrate temperature is at 480℃. The resistivity is as low as 3.483×10-3?·cm. The average transmittance of the film is about 90% in the visible region. The AZO film has a hexagonal wurtzite structure with its dominant orientation along the c-axis perpendicular to the substrate surface.
5. Polycrystalline AZO films were prepared by direct-current (DC) reactive sputtering technique with Zn/Al alloy target. The AZO film possesses high quality in terms of electrode functions, when substrate temperature is 480℃. The resistivity is as low as 4.973×10-4?·cm, the carrier concentration and mobility are as high as 1.103×1021 atom/cm3 and 11.4 cm2/V·s, respectively. The average transmittance of the film is about 90% in the visible region. The AZO film has a hexagonal wurtzite structure with its dominant orientation along the c-axis perpendicular to the substrate surface.
6. The properties of the electronic junctions were investigated by I-V measurement, which reveals that the SIS heterojunction showed a rectifying behavior under a dark condition. It shows fairly good rectifying behavior indicating the formation of a diode between AZO and p-Si. By the comparison of AZO films and SIS heterojunction prepared by different sputtering technique, the conductivity of AZO film prepared by DC reactive sputtering is much higher than that of the AZO film prepared by DC sputtering. Therefore, more photon induced current can easily flow through AZO layer prepared by DC reactive sputtering and enter into the Cu front contact. Thus, higher photocurrent is obtained under a reverse bias. Because the resistivity of ITO film is much lower than that of AZO films, the magnetron- sputtering of the ITO film with the high quality crystallite and the good conductivity on AZO/SiO2/p-Si lead to a great decrease of the lateral resistance. The ITO layer was as the large area surface electrode. Thus, the photon induced current can easily flow through ITO layer entering the Cu front contact, since there is a parallel connection and a high mobility of the top layer of the ITO/AZO/SiO2/p-Si SIS heterojunction. Most high photocurrent can be obtained under a reverse bias. The results indicated that the novel SIS heterojunctions can be not only used for low cost solar cell, but also used for high quantum efficiency of UV and visible lights enhanced photodiode for various applications.
1.磁控溅射沉积的ITO薄膜结晶度高,并且具有较高的紫外—可见光透过率及优异的电学性能。系统研究了基片温度对射频磁控溅射ITO薄膜微结构、电学及光学性能的影响及机制。结果表明,当基片温度为480℃时,ITO薄膜性能最好,电阻率为9.42×10-5Ω·cm,载流子浓度高达3.461×1021/cm3,霍尔迁移率为19.1 cm2/V·s。ITO薄膜在可见光区域具有高的透射率,在95%以上。ITO薄膜为多晶晶体薄膜,具有高度(222)择优取向,结晶质量好。ITO薄膜在晶硅衬底上具有良好的钝化和减反射效果,尤其是在300～500nm紫外至蓝光区域。
2.用X射线光电子能谱(XPS)对500℃不同氧化时间的超薄氧化硅层及SINP结构光电池样品成分、化学态进行分析。表明表面层中存在非化学态成分。
3. SINP蓝紫光电池具有优异的整流特性及暗电流机制。室温下±1V时,SINP蓝紫光电池整流比为324.7,二极管理想因子n=1.84,AM1.5 100 mW/cm2光照下,光电转换效率η=12.26%。由于在SINP结构中,光电流可以通过高结晶度、高载流子迁移率的ITO薄膜横向输运,避免了高磷浓度n发射区中横向输运的复合,降低了发射区横向电阻影响引起的功率损耗,新型SINP蓝紫光电池短路电流密度高达JSC=38.7 mA/cm2,显示出良好的光伏特性。在500nm波长,蓝紫光增强型SINP光电池外量子效率及响应率高达70%及285 mA/W;在800nm波长,峰值响应率为487 mA/W。最近研制的采用60Ω/□n+—型发射极的浅结SINP光电池进一步提高短波光谱响应,蓝紫光灵敏度极高。器件光谱响应拟和计算结果表明,新型SINP蓝紫光电池的高量子效率得益于浅结,以及高导电率和对蓝紫光具有良好减反射效果的ITO薄膜的应用与结合。具有高蓝紫光以及其它可见光波段的光谱响应和光电转换的增强效果,是该器件的主要特征。其较高的短路电流密度,适合于发展成为新型结构的硅基太阳能电池。
4.以ZnO和Al2O3烧结的陶瓷靶,用直流磁控溅射工艺在玻璃基片上沉积出高质量的AZO薄膜,系统研究了不同基片温度对薄膜微结构、电学和光学性能的影响。当基片温度为480℃时,AZO薄膜性能最好,电阻率为3.483×10-3Ω·cm。AZO薄膜在可见光区域具有高的透射率,在90%左右。AZO薄膜为微晶晶体薄膜,具有高度(002)择优取向,结晶质量好。
5.以高纯度(99.99%)的锌铝合金(wt.98% Zn+wt.2%Al)靶,氩气和氧气为溅射工作气体,用直流反应磁控溅射工艺在玻璃基片上生长出高质量的AZO薄膜。系统研究了基片温度对直流反应磁控溅射AZO薄膜微结构、电学及光学性能的影响及机制。当基片温度为480℃时,AZO薄膜性能最好,电阻率为4.973×10-4Ω·cm,载流子浓度高达1.103×1021/cm3,霍尔迁移率为11.4 cm2/V·s。AZO薄膜在可见光区域具有高的透射率,在90%以上。AZO薄膜为六角纤锌矿结构的微晶晶体薄膜,具有高度(002)择优取向,结晶质量好。
6. SIS异质结器件良好的整流特性表明AZO和p—Si间形成高质量的异质结二极管,在反向偏压下获得明显的光电流。通过对几种磁控溅射方法制备AZO薄膜及SIS异质结器件光电性能的比较可知,由于直流反应磁控溅射高结晶度、高导电率的AZO薄膜作AZO/SiO2/p-Si SIS异质结结构器件的发射极和顶层大面积透明收集电极,大量的光生载流子可以轻易地流过直流反应磁控溅射AZO薄膜进入Cu金属电极而收集到,从而在反向偏压下直流反应磁控溅射AZO/SiO2/p-Si SIS异质结比直流磁控溅射AZO/SiO2/p-Si SIS异质结可获得更高的光电流。通过射频磁控溅射沉积一层高导电率的ITO透明电极薄膜在直流磁控溅射AZO/SiO2/p-Si SIS异质结结构上,将会使异质结光电性能得到很大改进。因为高导电率的ITO薄膜极大地改善了AZO/SiO2/p-Si SIS异质结顶层电流输运结构,可收集到更多的光生载流子,所以在反向偏压下显示了明显的光电转换特性,可获得最高的光电流。SIS异质结不仅具有一定的光生伏特效应,而且在反向偏压下显示出很高的光电流。可以成为低成本的太阳电池及性能优良的紫外—可见—近红外增强型广谱光电探测器。
In order to reduce the technical complexity of the fabrication and simultaneously to improve the quantum efficiency in the range of 400-600 nm, a new type of ITO/SiO2/np-Silicon frame (named as SINP) hetero-interface solar cell has been designed and developed by combining the p-n junction with ITO transparent conductive oxide thin film as top layer of the device, according to the energy band evolution. A series of advanced techniques have been applied to the fabrication process, such as shallow junction, back surface field of aluminum, ultra-thin SiO2 passivation layer, and ITO coating. On the other hand, the novel semiconductor-insulator-semiconductor (SIS) hetero-junction structure has been fabricated by thermally growing an ultrathin silicon dioxide at low temperature and subsequently magnetron sputtering deposition of Al-doped n-ZnO (named as AZO) layer on p-Si (100) wafer. The microstructure, optics and electrical properties of the ITO and AZO films were characterized by XRD, SEM, UV-VIS spectrophotometer and Hall effect measurement, respectively. The influence of the substrate temperatures on the properties of ITO and AZO films were deeply studied. The current-voltage (I-V)、capacitance -voltage (C-V) and spectral response characteristics of SINP hetero-interface solar cell and SIS heterojunctions were analyzed in detail.
1. ITO film possesses high quality in terms of antireflection and electrode functions. The influence of the substrate temperatures on the property of ITO film was deeply studied. The results indicated that ITO film possesses high quality , when the substrate temperature is at 480℃. The resistivity is as low as 9.42×10-5?·cm, the carrier concentration and mobility are as high as 3.46×1021 atom/cm3 and 19.1 cm2/V·s, respectively. The average transmittance of the film is about 95% in the visible region. The film has a bixbyite structure and a preferred growth along the (222) orientation, perpendicular to the substrate surface. The configuration of the ITO layer on the textured Si is suitable for the blue and ultraviolet cells owing to the less loss of the number of photons with a short wavelength, which is more favorable for high efficiency cells.
2. The ultra-thin SiO2 layer and SINP structure samples were analyzed by x-ray photoelectron spectroscopy (XPS). The results showed that the non-stoichiometric matter were present on the surface layers and which resulted in the electronic defects to the minority carrier transportation.
3. The I-V curves of SINP violet photoelectric cell showed the fairly good rectifying behaviors. The values of IF/IR (IF and IR stand for forward and reverse currents, respectively) at 1.0 V for the violet SINP device is as high as 324.7,and the ideality factor of the violet SINP photoelectric cell is 1.84. The conversion efficiencies of the violet SINP cell under illumination of continue light source (AM 1.5 class A) is12.26%. Because the high quality crystallite and the good conductivity of ITO film magnetron-sputtered on SiO2 lead to a great decrease of the lateral resistance, it is possible to decrease the power loss induced by the lateral resistance of emitter region in the new type solar cell with SINP structure. The short-circuit current density of the SINP violet solar cell is as high as JSC = 38.7 mA/cm2. The external quantum efficiencies (EQE) and responsivity of the violet SINP device are 70% and 285mA/W at 500nm, respectively. The spectral responsivity peak of the violet SINP photoelectric cell is 487mA/W at about 800nm.The latest result indicates that the violet SINP photoelectric cell with 60?/□shallow junction can greatly improve the violet response. The calculated results indicates that the high quantum efficiency and responsivity of violet and blue enhanced photovoltaic cell is attributed to the shallow junction and the good conducting, violet and blue antireflection coating of ITO optical film. We found that the main feature of our PV cell is the enhanced violet response and optoelectronic conversion. The improved short-circuit current, open-circuit voltage, and filled factor indicate that the device is promising to be developed into an ultraviolet and blue enhanced photovoltaic device in the future.
4. The AZO films were prepared by direct-current (DC) magnetron sputtering. The target was sintered ceramic disks of ZnO doped with 2 wt% Al2O3 (purity 99.99%). The AZO film possesses high quality in terms of electrode functions, when substrate temperature is at 480℃. The resistivity is as low as 3.483×10-3?·cm. The average transmittance of the film is about 90% in the visible region. The AZO film has a hexagonal wurtzite structure with its dominant orientation along the c-axis perpendicular to the substrate surface.
5. Polycrystalline AZO films were prepared by direct-current (DC) reactive sputtering technique with Zn/Al alloy target. The AZO film possesses high quality in terms of electrode functions, when substrate temperature is 480℃. The resistivity is as low as 4.973×10-4?·cm, the carrier concentration and mobility are as high as 1.103×1021 atom/cm3 and 11.4 cm2/V·s, respectively. The average transmittance of the film is about 90% in the visible region. The AZO film has a hexagonal wurtzite structure with its dominant orientation along the c-axis perpendicular to the substrate surface.
6. The properties of the electronic junctions were investigated by I-V measurement, which reveals that the SIS heterojunction showed a rectifying behavior under a dark condition. It shows fairly good rectifying behavior indicating the formation of a diode between AZO and p-Si. By the comparison of AZO films and SIS heterojunction prepared by different sputtering technique, the conductivity of AZO film prepared by DC reactive sputtering is much higher than that of the AZO film prepared by DC sputtering. Therefore, more photon induced current can easily flow through AZO layer prepared by DC reactive sputtering and enter into the Cu front contact. Thus, higher photocurrent is obtained under a reverse bias. Because the resistivity of ITO film is much lower than that of AZO films, the magnetron- sputtering of the ITO film with the high quality crystallite and the good conductivity on AZO/SiO2/p-Si lead to a great decrease of the lateral resistance. The ITO layer was as the large area surface electrode. Thus, the photon induced current can easily flow through ITO layer entering the Cu front contact, since there is a parallel connection and a high mobility of the top layer of the ITO/AZO/SiO2/p-Si SIS heterojunction. Most high photocurrent can be obtained under a reverse bias. The results indicated that the novel SIS heterojunctions can be not only used for low cost solar cell, but also used for high quantum efficiency of UV and visible lights enhanced photodiode for various applications.
引文
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