CN106972064A - 复合薄膜结构光伏器件及制备方法 - Google Patents

复合薄膜结构光伏器件及制备方法 Download PDF

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CN106972064A
CN106972064A CN201710057584.XA CN201710057584A CN106972064A CN 106972064 A CN106972064 A CN 106972064A CN 201710057584 A CN201710057584 A CN 201710057584A CN 106972064 A CN106972064 A CN 106972064A
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朱俊
周云霞
刘兴鹏
吴智鹏
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University of Electronic Science and Technology of China
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Abstract

复合薄膜结构光伏器件及制备方法，涉及光电转换技术和复合薄膜太阳能技术领域。本发明的复合薄膜结构光伏器件包括铁电功能层、半导体衬底、透明电极和下电极，其特征在于，在铁电层和半导体衬底之间设置有缓冲层，所述缓冲层的材料为钛酸锶或氧化钛，缓冲层厚度为10～30nm。本发明有益效果为：1、将铁电材料和半导体材料相结合，从而拓宽了复合薄膜结构光伏器件的光谱吸收范围，实现了更光谱的吸收波段。2、通过插入钛酸锶(STO)缓冲层，解决了功能层和衬底之间的晶格失配问题，减少了光生载流子在界面缺陷中的复合，显著提高了光电转换效率。

Description

复合薄膜结构光伏器件及制备方法
技术领域
本发明涉及光电转换技术和复合薄膜太阳能技术领域，特别是涉及一种复合薄膜结构光伏器件及制备方法。
背景技术
具有钙钛矿结构的甲胺铅碘类(CH3NH3PbI3)材料目前在与染敏材料复合形成薄膜太阳能电池取得重大突破，电池效率可达10％以上。这些突破为钙钛矿材料与现有太阳能制备技术复合而获得新型高效的太阳能薄膜电池看到了希望。作为同为钙钛矿结构的铁电氧化物因其具有巨大的光生电压，也一直倍受关注。特别是近期在新型的铁电材料BiFeO3(BFO)上观察到高达16伏的光生电压和强紫外光吸收特性，使钙钛矿类材料在清洁能源获取的应用中有了更多的选择。由于两者同为钙钛矿结构，在能带、价键电子结构、电荷输运以及电荷随外场的响应等物理特性有诸多相似之处。相对于甲胺铅碘类材料，钙钛矿铁电氧化物的晶体结构更加稳定，较容易与现有的半导体工艺集成生长在一起，形成高效复合薄膜太阳能电池。以PZT/GaAs外延异质结为例，GaAs本身是一种重要的光伏材料，单结的GaAs能吸收可见光，产生约0.7伏光生电压。若能与钙钛矿铁电材料形成异质结，则两者吸收波段可互补，实现宽波段、更广谱的光能吸收转化，获得具有高开路电压的新型薄膜太阳能电池。
本发明以插入STO缓冲层为例，说明一种新的复合薄膜太阳能电池结构和制备方法。为了得到更大的短路电流，实现宽波段、更光谱的光能吸收转化，获得具有高开路电压的新型复合薄膜太阳能电池，那么获得晶格完美、高光电转化效率的钙钛矿铁电薄膜显得尤为重要。然而，大多数报道中，钙钛矿铁电材料薄膜化后，相对于单晶或者陶瓷材料，光电转化能力偏低。列如溅射制备的多晶BTO薄膜能观察到随极化变化的光伏效应，但是薄膜结构缺陷太多且极化偏小，导致光生载流子在缺陷处复合而不能产生有效的光电转化。即使织构和铁电性良好的掺镧PZT薄膜，由于绝缘性太高，光生载流子无法在薄膜体内形成有效的输运，虽然能产生较大的光伏电压，但光生载流子在纳安量级。那么只有解决钙钛矿铁电薄膜化过程中光电转换效率下降的问题，才能让钙钛矿铁电光伏特性的优势得以发挥。
对于铁电层/缓冲层/半导体衬底结构光伏器件。通常采用镍(Ni)、金(Au)、铝(Al)、银(Ag)的等作为电极材料。电极材料也是影响薄膜光电转化效率的一个重要因素。其中包括电极的透明性等。
发明内容
为了克服上述现有技术的不足，本发明提供了一种铁电层/缓冲层/半导体衬底结构光伏器件及其制备方法，使得光伏器件的光电转换效率大幅度提升，尤其是器件的短路电流得到大幅度的提升。
本发明解决所述技术问题采用的技术方案是，复合薄膜结构光伏器件，包括铁电功能层、半导体衬底、透明电极和下电极，其特征在于，在铁电层和半导体衬底之间设置有缓冲层，所述缓冲层的材料为钛酸锶或氧化钛，缓冲层厚度为10～30nm。
进一步的，所述缓冲层材料为钛酸锶，厚度为20nm。
所述透明电极的材料为氧化铟锡或者掺铝氧化锌，所述铁电功能层的材料为锆钛酸铅或者铁酸铋，半导体衬底的材料为砷化镓。
所述透明电极为面电极，所述下电极为点电极。
本发明还提供一种复合薄膜结构光伏器件的制备方法，其特征在于，包括下述步骤：
1)在半导体衬底上沉积10～30纳米厚度的缓冲层，缓冲层的材料为钛酸锶或氧化钛；
2)在缓冲层上生长铁电功能层；
3)在铁电功能层上沉积上电极，上电极为透明的面电极；
4)在半导体衬底的底面沉积下电极，下电极为点电极。
本发明有益效果为：
1、将铁电材料和半导体材料相结合，从而拓宽了复合薄膜结构光伏器件的光谱吸收范围，实现了更光谱的吸收波段。
2、通过插入钛酸锶(STO)缓冲层，解决了功能层和衬底之间的晶格失配问题，减少了光生载流子在界面缺陷中的复合，显著提高了光电转换效率。
附图说明
图1为本发明具体实施列中复合薄膜光伏器件的结构示意图。
图2所示为本发明具体实施案例中采用PLD生长的异质结的XRD图，插图为摇摆曲线。
图3所示为本发明具体实施案例中采用LMBE生长的缓冲层STO的原位监测(RHEED)高能电子衍射图。
图4所示为本发明具体实施案例中器件的电滞回线图。
图5所示为本发明具体实施案例中器件在一个标准太阳光照射下，短路电流随着电压的变化曲线。图5中，自上向下三条曲线顺次为：Positive Poling,Un-Poling,Negative Poling.
图6所示为本发明具体实施案例中器件的短路电流随着光照强度的变化曲线。
图7所示为本发明具体实施案例中器件的开路电压随着光照强度的变化曲线。
具体实施方式
本发明公开了一种铁电/缓冲层/半导体衬底结构的光伏器件，包括上电极、下电极、铁电功能层和半导体衬底，以及插入的缓冲层。本发明通过插入缓冲层解决了铁电功能层和半导体衬底之间的晶格失配问题。
本实施方式的上电极为透明电极，材质为导电薄膜氧化铟锡(ITO)。下电极为铝(Al)、银(Ag)电极。铁电功能层为锆钛酸铅(PZT)薄膜，厚度为150纳米。
优选的，缓冲层的材料为钛酸锶(STO)，厚度为20纳米。
半导体衬底为砷化镓(AsGa)材料。
本发明还公开了一种复合薄膜光伏器件的制备方法，包括下述步骤：
(1)利用脉冲激光分子束外延(L-MBE)技术，在半导体衬底上沉积20纳米厚度STO缓冲层。
(2)利用脉冲激光沉积技术(PLD)，在缓冲层上生长150纳米厚度的铁电功能层。
(3)在铁电功能层上利用脉冲激光沉积上电极，上电极为面电极。
(4)在半导体衬底上利用电子束蒸发技术沉积下电极，下电极为点电极。
进一步的，所述的步骤(1)中，STO缓冲层生长在AsGa衬底上，采用的是L-MBE技术。本发明利用高能电子衍射仪(RHEED)进行原位监测。
所述铁电功能层材料为Pb(Zr(1-x),Tix)O3，采用PbO、La2O3、TiO2为原料进行配比，其中，x＝0.48。
更进一步的，所述步骤(2)具体包括：
将PZT靶材分别利用无水乙醇和去离子水超声清洗5分钟，高压氮气吹干后放入脉冲激光溅射真空腔体，基片加热至550℃，抽真空至1×10-1Pa以下，然后打开流量计以50sccm的流量向腔体通入氧气，调节腔体至20Pa，待腔体气压稳定后，打开激光器，调节激光频率为3Hz,激光能量为5J/cm-2，溅射30分钟，关闭激光源，调节流量值200sccm的流量，待腔体气压稳定在1×103Pa,原位退火30分钟，之后打开腔体，将样品取出。
制备上电极采用PLD系统，制备下电极采用电子束蒸发法。
实施例
本发明实施例公开了一种复合薄膜结构光伏器件，包括透明电极(上电极)、铁电功能层、缓冲层、半导体衬底和金属下电极。
缓冲层优选钛酸锶(STO)或氧化钛(TiO2)；透明导电电极优选为氧化铟锡(ITO)或者掺铝氧化锌等透明导电材料；金属下电极为铝(Al)或者银(Ag)；铁电功能层为锆钛酸铅(PZT)或者铁酸铋(BFO)；半导体衬底优选为砷化镓(AsGa)。
本实施例提供ITO/PZT/STO/GaAs/Al结构和ITO/PZT/GaAs/Al结构两种器件的对比。ITO为透明导电电极，不会减弱功能层和衬底对光的吸收。缓冲层优选的钛酸锶(STO)，STO的晶格常数为0.392纳米。功能层优选的是PZT，PZT的晶格常数是0.402纳米。半导体衬底优选的是GaAs，GaAs的晶格常数是0.565纳米，实验结果表明缓冲层与衬底是旋转45度匹配生长。缓冲层以及功能生长结构良好。由于晶体结构生长良好，器件的短路电流以及开路电压得到了显著提升。尤其是短路电流提高约10000倍。
下面将结合本发明实例中的附图，对本发明实例中的技术方案进行详细的描述。
如图1所示，本发明的复合薄膜结构光伏器件包括透明导电上电极，PZT功能层，STO缓冲层，GaAs衬底以及金属下电极。器件为5×5cm2的尺寸，透明导电电极厚度为100nm，下电极为金属点电极。
图2为本发明的复合薄膜结构光伏器件的XRD图，以及作为对比的不具备缓冲层现有技术的XRD图。插图为摇摆曲线。
由于缓冲层厚度太薄，生长过程中特采用高能电子衍射仪进行原位监测，衍射图如图3所示。
将样品进行测试电滞回线，如图4。
将样品置于一个模拟太阳光下面得到器件的I-V曲线为图5所示。
分别调整光照的不同强度，测出器件的电流密度随光照强度的不同而发生变化如图6所示，器件的开路电压随光照强度的不同而发生变化如图7所示。

Claims (6)

1.复合薄膜结构光伏器件，包括铁电功能层、半导体衬底、透明电极和下电极，其特征在于，在铁电层和半导体衬底之间设置有缓冲层，所述缓冲层的材料为钛酸锶或氧化钛，缓冲层厚度为10～30nm。
2.如权利要求1所述的复合薄膜结构光伏器件，其特征在于，所述缓冲层材料为钛酸锶，厚度为20nm。
3.如权利要求1所述的复合薄膜结构光伏器件，其特征在于，所述透明电极的材料为氧化铟锡或者掺铝氧化锌，所述铁电功能层的材料为锆钛酸铅或者铁酸铋，半导体衬底的材料为砷化镓。
4.如权利要3所述的复合薄膜结构光伏器件，其特征在于，所述透明电极为面电极，所述下电极为点电极。
5.复合薄膜结构光伏器件的制备方法，其特征在于，包括下述步骤：
1)在半导体衬底上沉积10～30纳米厚度的缓冲层，缓冲层的材料为钛酸锶或氧化钛；
2)在缓冲层上生长铁电功能层；
3)在铁电功能层上沉积上电极，上电极为透明的面电极；
4)在半导体衬底的底面沉积下电极，下电极为点电极。
6.复合薄膜结构光伏器件的制备方法，其特征在于，所述步骤2)为：
将PZT靶材分别利用无水乙醇和去离子水超声清洗5分钟，高压氮气吹干后放入脉冲激光溅射真空腔体，基片加热至550℃，抽真空至1×10-1Pa以下，然后以50sccm的流量向腔体通入氧气，调节腔体至20Pa，待腔体气压稳定后，打开激光器，调节激光频率为3Hz,激光能量为5J/cm-2，溅射30分钟，关闭激光源，调节流量值200sccm的流量，待腔体气压稳定在1×103Pa，原位退火30分钟。
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