掺锗直拉硅中的杂质缺陷及其光伏应用研究
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摘要
太阳能发电被认为是解决能源短缺最有效的途径之一,近10年来,其产业规模正以超过30%的速度增长。为了满足大规模的应用,传统晶体硅太阳电池面临着高转化效率,长使用寿命,低制造成本,尤其是薄片化带来的挑战。由于掺Ge能够增强硅片强度,抑制体内空洞型缺陷,促进直拉硅中氧沉淀以及内吸杂能力,特别是能够减少破片和翘曲,使得掺Ge直拉硅具有薄片太阳电池上有很好的应用前景。
本文在本研究组发明的微量掺锗直拉硅单晶生长的基础上,系统地研究了掺Ge直拉硅基于光伏应用的原生材料特性,以及在电池工艺过程中的杂质缺陷行为,不仅具有较强的理论研究意义,而且对实际电池制备和材料应用具有重要的指导作用。其主要创新成果如下:
系统研究了掺Ge直拉硅原生晶体的少子寿命及电学活性中心的分布规律。实验指出:掺Ge能够改变原生晶体中的电活性缺陷(包括热施主和Ge关复合体)的形成规律,并改变少子寿命沿晶体生长方向的分布。通过热施主的形成实验证实:低浓度和高浓度掺Ge都能抑制热施主的形成,随着Ge浓度升高抑制作用更加明显,高浓度掺Ge还能够改变热施主的电学特性,使热施主对应的红外吸收峰转变为吸收带;高温预处理能够改变热施主的形成速率,在低掺Ge直拉硅中,高温RTA分解原生氧沉淀后,热施主的形成能在短期内增强甚至超过普通直拉硅,在随后的热处理中增强效应迅速消失;另外,Ge关复合体对O_(2i)的俘获对抑制热施主形成起主要作用。
系统研究了掺Ge直拉硅原生晶体中BO复合体相关的光照寿命衰减现象。研究证实:掺Ge能够有效减少BO复合体的饱和密度,对硅片的少子寿命起到了稳定的作用。掺Ge不改变O_(2i)的迁移能,但在略高于室温的条件下,BO复合体的稳定性和分解速率和Ge掺杂有关。研究认为:Ge关复合体对O_(2i)的俘获,以及Ge对BO复合体结构的扰动,是减少光照衰减的主要原因。
研究了Fe和Cu沾污的掺Ge直拉硅单晶的少子寿命特征。掺Ge能够抑制FeB的分解和形成过程。在掺Ge直拉硅中,低温下Cu沾污后硅片的寿命较普通直拉硅样品低,但在高温下Cu沾污后的少子寿命高于普通直拉硅样品,被认为与掺Ge引起的原生空位型缺陷行为等影响有关。
系统研究了直拉单晶硅片的表面金字塔织构的结构转变和光学性质。研究发现:金字塔的长大是通过{111}表面原子的逐层剥离实现的,大的金字塔倾向于占据小金字塔的长大空间,因此会导致金字塔的分化和消失。根据几何光学计算,随机金字塔织构具有较低的反射率下限,800nm对应的反射率仅为0.083。实际金字塔的不规则表面和棱边,以及大量亚微米级的小金字塔都是造成反射率上升的原因。研究表明:硅片的微缺陷(BMD)能够影响金字塔织构的性能,高密度的BMD会促进金字塔的异质形核并抑制其均匀形核,导致金字塔分布稀疏和大小不均,密度达到10~7cm~(-3)以上的BMD能够明显增加织构硅片的反射率,使织构性能下降。研究进一步发现:掺杂浓度(10~(16)～5×10~(19)cm~(-3))的Ge对直拉硅在碱溶液中的腐蚀速率没有影响,当掺Ge原生硅片中的BMD密度小于10~7cm~(-3)时,掺Ge不改变原生直拉硅片的织构特性。
通过对比普通太阳电池,研究了掺Ge对直拉硅太阳电池性能的影响。5×10~(19)cm~(-3)浓度的Ge掺入直拉硅后,能够增加在硅禁带边缘的红外吸收和转化效率,从而提高太阳电池的短路电流,在BSR电池中增幅可达2%。掺Ge对电池的开压和填充引起并没有明显的影响。与此同时,I_(02)的减小和R_(sh)的增加得益于掺Ge对基体内二次缺陷的抑制,总体而言,掺Ge对太阳电池性能的影响不明显。
The photovoltaic(PV)energy market is witnessed by a booming rate beyond 30%per year recently.Silicon(Si)continues to have a prominent place in the PV energy market,with about 90%share of the current PV production.A major factor in the rapid growth in PV energy production is a steady decline of production costs,resulting from increasing solar-cell efficiencies.The cost of the starting wafers has a strong influence on the final cost of＄/W.To cut the cost,thinner wafers are going to be utilized.New materials have been investigated for solar cells.Among them Si-rich SiGe alloys shows some potential to improve the efficiency in comparison to the normal silicon solar cell,but the vast use of germaium(Ge)raises the cost.Ge doped silicon also shows some advantages beyond normal silicon.It can strengthen up the wafers by locking disloactions, inhibit void-type defects and promote the oxygen precipitation etc.Low warpage and breakage can be gained for thin Ge-doped silicon wafers.To understand the properties of Ge-doped silicon from the view of PV application not only makes sense for the knowledges,but also can help to fabricate low-cost and high-efficiency solar cells.Up to now,there is no systematic study reported.
In this thesis,the as-grown Ge-doped Czochralski silicon(CZ Si)character, the effects of Ge on the behavior of grown-in defects and the process induced defects,as well as intentionally induced Fe and Cu metallic impurites,the effect of Ge-doping on the texturisation of wafers and performance of solar cells were systematically studied by means of Microwave photoconductance Decay (MWPCD),Fourier-Transform Infrared(FTIR),Scanning Infrared Microscope (SIRM)and Field-Emitting Scanning Electron Microscope(FE-SEM)techniques.
In as-grown silicon,MWPCD study revealed that the minority carrrier lifetime distribution varied with the ingot position due to the Ge-doping level.The main traps detected were thermal donors and Ge-related defects.The effect of Ge-doping level on the formation of thermal donors with and without pretreatment was also investigated.A short-time enhancement of thermal donors by lightly Go-doping was observed after RTA pretreatment.Based on the experimental results,a reaction that oxygen dimmer(O_(2i))was captured ty Go-related defects was proposed to explain the inhibition of Go on thermal donors.
Under illumination,Go-doping could stabilize the minority carrier lifetime of wafers by reduce light induced degradation(LID)attributed to the BO complex. Go-doping hardly changed the migration barrier of O_(2i),while the stability of BO was slightly reduced at 100℃.The capture of O_(2i)by Go-related defects and the disturbance to BO configuration by Go-doping both contributed to the decrease of LID.
In Go-doped CZ silicon with artificial Fe and Cu contaminations,it was found that the disovation and formation of FeB complex was retarded.At the meantime,the lifetime ratioτ_(GCZ4)/τ_(CZ3)of Cu contaminated wafers was smaller than 1 below critical temperature about 700℃while larger than 1 above 700℃. 1250℃/50 s RTA protreatment can increase the critical temperature to about 900℃.The interaction between Go-Vacancy-related defects and Cu resulted into the lifetime character below critical temperature.At higher temperature,the inhibition of Cu precipitation mostly duo to the locking of dislocations by Go-doping resulted into a higher lifetime in Go-doped silicon.
During the texutrisation of silicon wafers in alkaline aqueous solution, pyramids grew up by peeling atom layers from {111} surfaces of pyramids. Larger ones tended to hold larger space while the smaller ones would decrease or even disappear.Based on the comparison of the experimental reflecting spectra to the calculation results,a dominating reflecting pathway was found out which shew a very low reflectance 0.083.In practice,the reflectance was rised up by nonideal structures of pyramids as well as the very small ones.Texture on wafers with high density of BMD also had higher reflectance.The BMD in wafers beyond 10~7 cm~(-3)could change the nucleation of pyramids further resulted into the non-uniformity of them.Go-doping at 10~(16)～5×10~(19)cm~(-3)level had no obvious effect on the etching rate of silicon in alkaline aqueous solution.And the texturiation character had never been changed when BMD density was smaller than 10~7 cm~(-3)in Ge-doped silicon.
In comparison with conventional CZ Si,Ge doped CZ Si with Ge content 5×10~(19)cm~(-3)was used to fabricate solar cells by the same processes.It was found that the short-circuit current I_(sc)and conversion efficiency of Ge-doped Si solar cells(GSCs)was slightly higher than that of the conventional solar cells(SCs), while the open-circuit voltage and fill factor of both the solar cells was almost the same.The better saturation current I_(02)and shunting resistance R_(sh)for GSCs were gained.
本文在本研究组发明的微量掺锗直拉硅单晶生长的基础上,系统地研究了掺Ge直拉硅基于光伏应用的原生材料特性,以及在电池工艺过程中的杂质缺陷行为,不仅具有较强的理论研究意义,而且对实际电池制备和材料应用具有重要的指导作用。其主要创新成果如下:
系统研究了掺Ge直拉硅原生晶体的少子寿命及电学活性中心的分布规律。实验指出:掺Ge能够改变原生晶体中的电活性缺陷(包括热施主和Ge关复合体)的形成规律,并改变少子寿命沿晶体生长方向的分布。通过热施主的形成实验证实:低浓度和高浓度掺Ge都能抑制热施主的形成,随着Ge浓度升高抑制作用更加明显,高浓度掺Ge还能够改变热施主的电学特性,使热施主对应的红外吸收峰转变为吸收带;高温预处理能够改变热施主的形成速率,在低掺Ge直拉硅中,高温RTA分解原生氧沉淀后,热施主的形成能在短期内增强甚至超过普通直拉硅,在随后的热处理中增强效应迅速消失;另外,Ge关复合体对O_(2i)的俘获对抑制热施主形成起主要作用。
系统研究了掺Ge直拉硅原生晶体中BO复合体相关的光照寿命衰减现象。研究证实:掺Ge能够有效减少BO复合体的饱和密度,对硅片的少子寿命起到了稳定的作用。掺Ge不改变O_(2i)的迁移能,但在略高于室温的条件下,BO复合体的稳定性和分解速率和Ge掺杂有关。研究认为:Ge关复合体对O_(2i)的俘获,以及Ge对BO复合体结构的扰动,是减少光照衰减的主要原因。
研究了Fe和Cu沾污的掺Ge直拉硅单晶的少子寿命特征。掺Ge能够抑制FeB的分解和形成过程。在掺Ge直拉硅中,低温下Cu沾污后硅片的寿命较普通直拉硅样品低,但在高温下Cu沾污后的少子寿命高于普通直拉硅样品,被认为与掺Ge引起的原生空位型缺陷行为等影响有关。
系统研究了直拉单晶硅片的表面金字塔织构的结构转变和光学性质。研究发现:金字塔的长大是通过{111}表面原子的逐层剥离实现的,大的金字塔倾向于占据小金字塔的长大空间,因此会导致金字塔的分化和消失。根据几何光学计算,随机金字塔织构具有较低的反射率下限,800nm对应的反射率仅为0.083。实际金字塔的不规则表面和棱边,以及大量亚微米级的小金字塔都是造成反射率上升的原因。研究表明:硅片的微缺陷(BMD)能够影响金字塔织构的性能,高密度的BMD会促进金字塔的异质形核并抑制其均匀形核,导致金字塔分布稀疏和大小不均,密度达到10~7cm~(-3)以上的BMD能够明显增加织构硅片的反射率,使织构性能下降。研究进一步发现:掺杂浓度(10~(16)～5×10~(19)cm~(-3))的Ge对直拉硅在碱溶液中的腐蚀速率没有影响,当掺Ge原生硅片中的BMD密度小于10~7cm~(-3)时,掺Ge不改变原生直拉硅片的织构特性。
通过对比普通太阳电池,研究了掺Ge对直拉硅太阳电池性能的影响。5×10~(19)cm~(-3)浓度的Ge掺入直拉硅后,能够增加在硅禁带边缘的红外吸收和转化效率,从而提高太阳电池的短路电流,在BSR电池中增幅可达2%。掺Ge对电池的开压和填充引起并没有明显的影响。与此同时,I_(02)的减小和R_(sh)的增加得益于掺Ge对基体内二次缺陷的抑制,总体而言,掺Ge对太阳电池性能的影响不明显。
The photovoltaic(PV)energy market is witnessed by a booming rate beyond 30%per year recently.Silicon(Si)continues to have a prominent place in the PV energy market,with about 90%share of the current PV production.A major factor in the rapid growth in PV energy production is a steady decline of production costs,resulting from increasing solar-cell efficiencies.The cost of the starting wafers has a strong influence on the final cost of＄/W.To cut the cost,thinner wafers are going to be utilized.New materials have been investigated for solar cells.Among them Si-rich SiGe alloys shows some potential to improve the efficiency in comparison to the normal silicon solar cell,but the vast use of germaium(Ge)raises the cost.Ge doped silicon also shows some advantages beyond normal silicon.It can strengthen up the wafers by locking disloactions, inhibit void-type defects and promote the oxygen precipitation etc.Low warpage and breakage can be gained for thin Ge-doped silicon wafers.To understand the properties of Ge-doped silicon from the view of PV application not only makes sense for the knowledges,but also can help to fabricate low-cost and high-efficiency solar cells.Up to now,there is no systematic study reported.
In this thesis,the as-grown Ge-doped Czochralski silicon(CZ Si)character, the effects of Ge on the behavior of grown-in defects and the process induced defects,as well as intentionally induced Fe and Cu metallic impurites,the effect of Ge-doping on the texturisation of wafers and performance of solar cells were systematically studied by means of Microwave photoconductance Decay (MWPCD),Fourier-Transform Infrared(FTIR),Scanning Infrared Microscope (SIRM)and Field-Emitting Scanning Electron Microscope(FE-SEM)techniques.
In as-grown silicon,MWPCD study revealed that the minority carrrier lifetime distribution varied with the ingot position due to the Ge-doping level.The main traps detected were thermal donors and Ge-related defects.The effect of Ge-doping level on the formation of thermal donors with and without pretreatment was also investigated.A short-time enhancement of thermal donors by lightly Go-doping was observed after RTA pretreatment.Based on the experimental results,a reaction that oxygen dimmer(O_(2i))was captured ty Go-related defects was proposed to explain the inhibition of Go on thermal donors.
Under illumination,Go-doping could stabilize the minority carrier lifetime of wafers by reduce light induced degradation(LID)attributed to the BO complex. Go-doping hardly changed the migration barrier of O_(2i),while the stability of BO was slightly reduced at 100℃.The capture of O_(2i)by Go-related defects and the disturbance to BO configuration by Go-doping both contributed to the decrease of LID.
In Go-doped CZ silicon with artificial Fe and Cu contaminations,it was found that the disovation and formation of FeB complex was retarded.At the meantime,the lifetime ratioτ_(GCZ4)/τ_(CZ3)of Cu contaminated wafers was smaller than 1 below critical temperature about 700℃while larger than 1 above 700℃. 1250℃/50 s RTA protreatment can increase the critical temperature to about 900℃.The interaction between Go-Vacancy-related defects and Cu resulted into the lifetime character below critical temperature.At higher temperature,the inhibition of Cu precipitation mostly duo to the locking of dislocations by Go-doping resulted into a higher lifetime in Go-doped silicon.
During the texutrisation of silicon wafers in alkaline aqueous solution, pyramids grew up by peeling atom layers from {111} surfaces of pyramids. Larger ones tended to hold larger space while the smaller ones would decrease or even disappear.Based on the comparison of the experimental reflecting spectra to the calculation results,a dominating reflecting pathway was found out which shew a very low reflectance 0.083.In practice,the reflectance was rised up by nonideal structures of pyramids as well as the very small ones.Texture on wafers with high density of BMD also had higher reflectance.The BMD in wafers beyond 10~7 cm~(-3)could change the nucleation of pyramids further resulted into the non-uniformity of them.Go-doping at 10~(16)～5×10~(19)cm~(-3)level had no obvious effect on the etching rate of silicon in alkaline aqueous solution.And the texturiation character had never been changed when BMD density was smaller than 10~7 cm~(-3)in Ge-doped silicon.
In comparison with conventional CZ Si,Ge doped CZ Si with Ge content 5×10~(19)cm~(-3)was used to fabricate solar cells by the same processes.It was found that the short-circuit current I_(sc)and conversion efficiency of Ge-doped Si solar cells(GSCs)was slightly higher than that of the conventional solar cells(SCs), while the open-circuit voltage and fill factor of both the solar cells was almost the same.The better saturation current I_(02)and shunting resistance R_(sh)for GSCs were gained.
引文
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