超薄CIGS太阳电池及组件的研究
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摘要
铜铟镓硒(CIGS)薄膜太阳电池具有高光吸收系数、高转化效率、可调的禁带宽度、高稳定性、较强的抗辐射能力等优点,是一种非常有前途的薄膜太阳电池。随着铜铟镓硒薄膜电池逐渐进入量产阶段,如何降低生产成本成为科研工作者共同追求的目标。发展超薄CIGS吸收层电池不但可以减少In、Ga、Se等稀有元素的用量,降低原料成本,更能减少CIGS薄膜的沉积时间,减少能源消耗与人力成本,提高生产效率。此外,发展超薄电池可以用有限的资源生产更多的产品,对提高资源的利用效率也是非常重要的。因此,超薄吸收层电池己成为目前世界上CIGS电池研究的一个热点。本文在综合国内外研究现状的基础上,对超薄CIGS吸收层电池及组件进行了系统研究,主要取得如下研究成果：
通过理论计算和实验研究了不同CIGS吸收层厚度对材料及电池特性的影响,确定了超薄电池的最佳临界厚度在0.8-1.0μm之间。分别采用恒定衬底温度顺序蒸发法和三步法制备超薄CIGS电池,比较衬底温度对超薄CIGS电池性能的影响。采用恒定衬底温度顺序蒸发法制备CIGS吸收层,发现在衬底温度为350℃时,由于CdS/CIGS (?)自光结构及低含Ga相的存在,电池的短路电流升高明显,进而引起转换效率增加,而在三步法工艺中没有发现此现象。
研究了Ga在超薄电池中的作用：对比研究了Ga含量对超薄及常规厚度CIGS材料及电池性能影响的差异。研究发现Ga/(Ga+In)在0.20-0.36之间变化时,对1μm的CIGS薄膜结晶质量影响不大,而2μm薄膜晶粒尺寸随Ga含量的增加而明显减小；随着Ga含量的增加,1μm薄膜的(112)衍射峰强度降低,而2μm薄膜的(112)衍射峰强度增加,但两种厚度薄膜的择优取向同时逐渐减弱；在相同Ga含量情况下,1μm薄膜的最小带隙值大于的2μm的薄膜,且1gm薄膜的最小带隙值随Ga含量增长的更快,对Ga含量的变化更敏感；随着Ga含量的增加,1μm薄膜电阻率降低,而2μm薄膜电阻率逐渐增加。通过不同厚度的电池器件特性对比,发现Ga含量对超薄电池性能的影响更明显,其增加会导致1μm厚度的电池开路电压快速增加,进而引起电池转化效率较大提升。在Ga／(Ga+In)约为0.37时,1μm的超薄电池的转换效率达到最高。在三步法中第一步采用不同Ga-In间隔时间制备Ga的背梯度,虽然较大的间隔时间可提高Ga的背梯度,但由于影响了薄膜结晶质量,对超薄电池性能改善微弱。第三步采用In/Ga沉积工艺,可以改善薄膜内部Ga的V型分布,增大超薄电池的开路电压和短路电流密度,使电池效率得到提升,1μm厚吸收层电池转换效率达到了13.2%。
在超薄CIGS材料制备工艺优化的基础上,尝试了一些其他改善超薄电池的工艺技术：①提出了在CIGS/Mo界面处添加CIS或CGS界面层的工艺技术,研究发现该工艺可以改善薄膜结晶状况、使薄膜更加致密均匀,有效降低了超薄电池的并联电导值,提高了电池的开路电压和转换效率。②对蒸发法制备CIGS薄膜表面的三角形小岛及孔洞的特性和形成过程进行了研究,认为三角形小岛的形成受薄膜Cu含量影响很大,而三角形孔洞的形成则主要是三角形小岛生长扩展不充分引起的。对含有三角形小岛和没有三角形小岛的薄膜制备的超薄电池进行了比较,发现没有三角形小岛的电池效率有所提高。③采用前掺NaF工艺制备超薄CIGS电池,发现仅靠从苏打玻璃(SLG)衬底扩散来的Na无法满足超薄CIGS电池,需要额外补充Na；由于Na对薄膜缺陷的钝化,以及CIGS/Mo界面处有NaF的残留,使得电池并联电导值降低,长波光生载流子收集增强,超薄电池特性得到改善。通过SMS测试发现CIGS薄膜内Na与Ga的分布形状相同,认为造成这种现象的原因与薄膜生成过程中晶粒尺寸的变化以及Na在不同CIGS相中的固溶度有关。
最后,在CIGS材料及小面积电池的研究基础上研究组件,包括划线工艺、Ga含量、Cu含量、子电池宽度、CdS缓冲层厚度、i-ZnO和ZnO:Al厚度等试验条件对常规厚度和超薄CIGS组件的影响,为发展大面积高效率CIGS组件提供了可靠的数据依据。
Cu(In,Ga)Se2(CIGS) thin film solar cell is considered as the most promising photovoltaic device. This is due to the excellent properties of CIGS thin films, such as high absorption coefficient, suitable and tunable band gap, high stability and strong anti-radiation. At present, CIGS solar cells have been steadily progressing and transfered for mass production. How to reduce the cost of production has became the common goal of researchers around the world.
If the thickness of the CIGS absorber layer is reduced with no, or minor, loss in solar cell performance, the deposition time will be shorter at the same deposition rate, then the labor and power costs will be cut down. In addition, a ultra-thin absorber layer will also reduce the materials usage and thereby materials costs. Furthermore, more CIGS solar cells can be fabricated using the limited In, Ga and Se resources. So it is important to study the ultra-thin CIGS absorber layer and solar cell. So far, the study of the ultra-thin CIGS solar cells has became a hot research topic around the world. In this paper, a series intensive studies on the properties of ultra-thin CIGS absorber layer material and solar cells has been carried based on the previous research results. And then, CIGS modules are also studied based on results of the small area solar cells. The innovative researches are as following.
The impact of CIGS absorber layer thickness on the properties of CIGS material and solar cell is studied by theoretical calculations and actual experiments. It is found that the best critical thickness of the ultra-thin CIGS absorber is between0.8-1.0μm.
CIGS films are prepared respectively by the metal elements sequential evaporation on the constant substrate temperature and three-stage evaporation process, it is comparatively studied the influence of the substrate temperature on the ultra-thin CIGS solar cells performance. It is found that the short-circuit current and conversion efficiency of the solar cell have been improved when the substrate temperature is350℃using metal elements sequential evaporation process. This may could be a reference for the development of high efficiency ultra-thin solar cell prepared on a low substrate temperature. However, it is not found this phenomenon in the three-stage process.
The difference of influence of Ga content on the CIGS material and solar cell performance with ultra-thin and common thickness absorber is studied. When Ga/(Ga+In) changes between the0.20-0.36, little change of the crystal quality of the1μm CIGS film is found, while the grain size of2μm film decreases significantly with increasing Ga content. As Ga content increases, the intensities of (112) peaks of1μm films decrease, while that of2μm films increase, and the preferred orientation of both films decrease. In the case of the same Ga content, the value of the minimum band gap of1μm film is larger than that of2μm film. With increasing Ga content, the minimum band gap value of1μfilm grow faster than2μm film, which denotes that the band gap value of lμm film is more sensitive to the Ga content. As the Ga content increases, the resistivity of1μm film decreases, while2μm film gradually increases. By comparing the characteristics of solar cells with the different thickness absorber, it is found that the performance of ultra-thin solar cell is more strongly influenced by Ga content. The enhancement of Ga content results in the rapidly increase of the open circuit voltage of solar cells with1μabsorber, thereby the efficiency is greatly improved. When Ga/(Ga+In) is about0.37, the highest conversion efficiency of solar cells with1μm absorber is achieved. Ga back gradient are prepared using different Ga-In interval time in the first stage. As the interval time increasing, Ga back gradient is improved. However, the performance of ultra-thin solar cells is improved weakly due to the deterioration of CIGS films crystal quality. In the third stage, the deposition process of In/Ga is used, Ga distribution with V-type of CIGS films can be improved, then the open circuit voltage and short circuit current density of the ultra-thin solar cells increase, and the efficiency is improved, the efficiency of solar cells with1μm absorber has reached13.2%.
Based on the optimization of ultra-thin CIGS materials preparation process, some other processes are tried to improve the performance of ultra-thin solar cells:①The process of deposited a CuInSe2(CIS) or CuGaSe2(CGS) buffer layer in CIGS/Mo interface in ultra-thin solar cells is first proposed. It is found that this process can improve the film crystallization, and the film surface is more compact and uniform. The shunt conductance of ultra-thin solar cells decreases using this process, thereby the open circuit voltage and efficiency are improved.②The characteristics and formation process of triangle island and cavities on the evaporated CIGS thin film surface is studied for the first time. The formation of triangle islands is strongly impacted by Cu content in the CIGS films. The triangle cavities are formed due to the insufficient coalescence of triangle islands. By compareing the performance of ultra-thin solar cells with and without triangle islands, it is found that efficiency of ultra-thin solar cells without triangle islands and cavities is improved.③Before CIGS films is deposited, NaF is evaporated. It is found that Na diffusion from soda line glass (SLG) substrate is insufficient to improve the performance of ultra-thin CIGS solar cells. Due to the passivation of defects by Na and the NaF residual at CIGS/Mo interface, shunt conductance of ultra-thin solar cells decreases and the photo-generated carrier collection in long wavelength increases, therefor, the performance of ultra-thin solar cells is improved. The depth profiles of elements are measured using a secondary ion mass spectroscopy (SIMS). It is found that the distributions of Na show a double grading as the depth profiles of Ga. It is believed that the formation mechanism of Na double grading is related to the growth process of CIGS films.
Finally, the influence of scribing process, width of the cells, Ga and Cu content of CIGS basorber, thickness of CdS buffer layer, i-ZnO and ZnO:Al window layer on the performance of moudles with common thickness and ultra-thin absorber is studied based on the previous research of the CIGS material and small area soalr cells, which could provide a reliable basis data for the development of a large area CIGS modules.
通过理论计算和实验研究了不同CIGS吸收层厚度对材料及电池特性的影响,确定了超薄电池的最佳临界厚度在0.8-1.0μm之间。分别采用恒定衬底温度顺序蒸发法和三步法制备超薄CIGS电池,比较衬底温度对超薄CIGS电池性能的影响。采用恒定衬底温度顺序蒸发法制备CIGS吸收层,发现在衬底温度为350℃时,由于CdS/CIGS (?)自光结构及低含Ga相的存在,电池的短路电流升高明显,进而引起转换效率增加,而在三步法工艺中没有发现此现象。
研究了Ga在超薄电池中的作用：对比研究了Ga含量对超薄及常规厚度CIGS材料及电池性能影响的差异。研究发现Ga/(Ga+In)在0.20-0.36之间变化时,对1μm的CIGS薄膜结晶质量影响不大,而2μm薄膜晶粒尺寸随Ga含量的增加而明显减小；随着Ga含量的增加,1μm薄膜的(112)衍射峰强度降低,而2μm薄膜的(112)衍射峰强度增加,但两种厚度薄膜的择优取向同时逐渐减弱；在相同Ga含量情况下,1μm薄膜的最小带隙值大于的2μm的薄膜,且1gm薄膜的最小带隙值随Ga含量增长的更快,对Ga含量的变化更敏感；随着Ga含量的增加,1μm薄膜电阻率降低,而2μm薄膜电阻率逐渐增加。通过不同厚度的电池器件特性对比,发现Ga含量对超薄电池性能的影响更明显,其增加会导致1μm厚度的电池开路电压快速增加,进而引起电池转化效率较大提升。在Ga／(Ga+In)约为0.37时,1μm的超薄电池的转换效率达到最高。在三步法中第一步采用不同Ga-In间隔时间制备Ga的背梯度,虽然较大的间隔时间可提高Ga的背梯度,但由于影响了薄膜结晶质量,对超薄电池性能改善微弱。第三步采用In/Ga沉积工艺,可以改善薄膜内部Ga的V型分布,增大超薄电池的开路电压和短路电流密度,使电池效率得到提升,1μm厚吸收层电池转换效率达到了13.2%。
在超薄CIGS材料制备工艺优化的基础上,尝试了一些其他改善超薄电池的工艺技术：①提出了在CIGS/Mo界面处添加CIS或CGS界面层的工艺技术,研究发现该工艺可以改善薄膜结晶状况、使薄膜更加致密均匀,有效降低了超薄电池的并联电导值,提高了电池的开路电压和转换效率。②对蒸发法制备CIGS薄膜表面的三角形小岛及孔洞的特性和形成过程进行了研究,认为三角形小岛的形成受薄膜Cu含量影响很大,而三角形孔洞的形成则主要是三角形小岛生长扩展不充分引起的。对含有三角形小岛和没有三角形小岛的薄膜制备的超薄电池进行了比较,发现没有三角形小岛的电池效率有所提高。③采用前掺NaF工艺制备超薄CIGS电池,发现仅靠从苏打玻璃(SLG)衬底扩散来的Na无法满足超薄CIGS电池,需要额外补充Na；由于Na对薄膜缺陷的钝化,以及CIGS/Mo界面处有NaF的残留,使得电池并联电导值降低,长波光生载流子收集增强,超薄电池特性得到改善。通过SMS测试发现CIGS薄膜内Na与Ga的分布形状相同,认为造成这种现象的原因与薄膜生成过程中晶粒尺寸的变化以及Na在不同CIGS相中的固溶度有关。
最后,在CIGS材料及小面积电池的研究基础上研究组件,包括划线工艺、Ga含量、Cu含量、子电池宽度、CdS缓冲层厚度、i-ZnO和ZnO:Al厚度等试验条件对常规厚度和超薄CIGS组件的影响,为发展大面积高效率CIGS组件提供了可靠的数据依据。
Cu(In,Ga)Se2(CIGS) thin film solar cell is considered as the most promising photovoltaic device. This is due to the excellent properties of CIGS thin films, such as high absorption coefficient, suitable and tunable band gap, high stability and strong anti-radiation. At present, CIGS solar cells have been steadily progressing and transfered for mass production. How to reduce the cost of production has became the common goal of researchers around the world.
If the thickness of the CIGS absorber layer is reduced with no, or minor, loss in solar cell performance, the deposition time will be shorter at the same deposition rate, then the labor and power costs will be cut down. In addition, a ultra-thin absorber layer will also reduce the materials usage and thereby materials costs. Furthermore, more CIGS solar cells can be fabricated using the limited In, Ga and Se resources. So it is important to study the ultra-thin CIGS absorber layer and solar cell. So far, the study of the ultra-thin CIGS solar cells has became a hot research topic around the world. In this paper, a series intensive studies on the properties of ultra-thin CIGS absorber layer material and solar cells has been carried based on the previous research results. And then, CIGS modules are also studied based on results of the small area solar cells. The innovative researches are as following.
The impact of CIGS absorber layer thickness on the properties of CIGS material and solar cell is studied by theoretical calculations and actual experiments. It is found that the best critical thickness of the ultra-thin CIGS absorber is between0.8-1.0μm.
CIGS films are prepared respectively by the metal elements sequential evaporation on the constant substrate temperature and three-stage evaporation process, it is comparatively studied the influence of the substrate temperature on the ultra-thin CIGS solar cells performance. It is found that the short-circuit current and conversion efficiency of the solar cell have been improved when the substrate temperature is350℃using metal elements sequential evaporation process. This may could be a reference for the development of high efficiency ultra-thin solar cell prepared on a low substrate temperature. However, it is not found this phenomenon in the three-stage process.
The difference of influence of Ga content on the CIGS material and solar cell performance with ultra-thin and common thickness absorber is studied. When Ga/(Ga+In) changes between the0.20-0.36, little change of the crystal quality of the1μm CIGS film is found, while the grain size of2μm film decreases significantly with increasing Ga content. As Ga content increases, the intensities of (112) peaks of1μm films decrease, while that of2μm films increase, and the preferred orientation of both films decrease. In the case of the same Ga content, the value of the minimum band gap of1μm film is larger than that of2μm film. With increasing Ga content, the minimum band gap value of1μfilm grow faster than2μm film, which denotes that the band gap value of lμm film is more sensitive to the Ga content. As the Ga content increases, the resistivity of1μm film decreases, while2μm film gradually increases. By comparing the characteristics of solar cells with the different thickness absorber, it is found that the performance of ultra-thin solar cell is more strongly influenced by Ga content. The enhancement of Ga content results in the rapidly increase of the open circuit voltage of solar cells with1μabsorber, thereby the efficiency is greatly improved. When Ga/(Ga+In) is about0.37, the highest conversion efficiency of solar cells with1μm absorber is achieved. Ga back gradient are prepared using different Ga-In interval time in the first stage. As the interval time increasing, Ga back gradient is improved. However, the performance of ultra-thin solar cells is improved weakly due to the deterioration of CIGS films crystal quality. In the third stage, the deposition process of In/Ga is used, Ga distribution with V-type of CIGS films can be improved, then the open circuit voltage and short circuit current density of the ultra-thin solar cells increase, and the efficiency is improved, the efficiency of solar cells with1μm absorber has reached13.2%.
Based on the optimization of ultra-thin CIGS materials preparation process, some other processes are tried to improve the performance of ultra-thin solar cells:①The process of deposited a CuInSe2(CIS) or CuGaSe2(CGS) buffer layer in CIGS/Mo interface in ultra-thin solar cells is first proposed. It is found that this process can improve the film crystallization, and the film surface is more compact and uniform. The shunt conductance of ultra-thin solar cells decreases using this process, thereby the open circuit voltage and efficiency are improved.②The characteristics and formation process of triangle island and cavities on the evaporated CIGS thin film surface is studied for the first time. The formation of triangle islands is strongly impacted by Cu content in the CIGS films. The triangle cavities are formed due to the insufficient coalescence of triangle islands. By compareing the performance of ultra-thin solar cells with and without triangle islands, it is found that efficiency of ultra-thin solar cells without triangle islands and cavities is improved.③Before CIGS films is deposited, NaF is evaporated. It is found that Na diffusion from soda line glass (SLG) substrate is insufficient to improve the performance of ultra-thin CIGS solar cells. Due to the passivation of defects by Na and the NaF residual at CIGS/Mo interface, shunt conductance of ultra-thin solar cells decreases and the photo-generated carrier collection in long wavelength increases, therefor, the performance of ultra-thin solar cells is improved. The depth profiles of elements are measured using a secondary ion mass spectroscopy (SIMS). It is found that the distributions of Na show a double grading as the depth profiles of Ga. It is believed that the formation mechanism of Na double grading is related to the growth process of CIGS films.
Finally, the influence of scribing process, width of the cells, Ga and Cu content of CIGS basorber, thickness of CdS buffer layer, i-ZnO and ZnO:Al window layer on the performance of moudles with common thickness and ultra-thin absorber is studied based on the previous research of the CIGS material and small area soalr cells, which could provide a reliable basis data for the development of a large area CIGS modules.
引文
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