作者希望通过该项目PERO-BOOST（EFRE，项目代码NW-1-1-040a），以确认由北莱茵 - 威斯特伐利亚州的财政支持。要感谢阿扎尔Jahanbakhsh和伊内斯·施密特（科隆大学的两个），用于与2步解决方案的制造和表征协助处理钙钛矿层，于尔根博士Schelter（科隆大学）为干扰物质的合成以及教授。里德尔博士和内达Pourdavoud（乌珀塔尔大学都）的X射线衍射测量。

1. ITO基板注:对于一种改进的样本接触，并避免装置的短路，在ITO涂布的玻璃衬底具有使用光刻和蚀刻来图案化。顶部和底部电极的重叠限定了生产太阳能电池的有源区。 <ol><li>切铟锡氧化物（ITO）涂覆的玻璃板上用玻璃刀乘2.5cm基板，得到2.5厘米。 </li><li>在ITO的中心胶的圆形标签（直径= 1.6厘米）覆盖衬底。 </li><li>通过在60℃下放置基板在盐酸的1M的FeCl 3溶液10分钟蚀刻的ITO。 </li><li>清洁基板依次用氯仿，丙酮和在超声浴皂溶液（2％）的。 </li><li>冲洗一次用蒸馏水和干燥N 2下的流动。 </li></ol> 2. ITO基板的臭氧注意:为了除去有机杂质，叔他ITO基板必须臭氧化。这将激活氧化表面，并增加基底上，这对后续层的再生沉积关键的润湿性能。 <ol><li>安装ITO基材上的样品架，并放置在臭氧化室中。 </li><li>照亮下与产生臭氧的紫外线灯（20瓦）（大气压）氧气10分钟。 </li></ol> 3. PEDOT沉积:PSS孔收集联系注:聚（3,4-亚乙基） - 聚（苯乙烯磺酸盐）（PEDOT:PSS）的膜通过旋涂从环境条件（25％至40％相对湿度）下的水悬浮液沉积的。该层用作空穴收集接触，并设有一个高功函数，减少针孔，和导致增加设备的再现性。 <ol><li>放置在PEDOT 150微升:PSS在水悬浮液（1.5％）与基板上的注射器过滤救援人员到场后唉0.45微米的过滤器。 </li><li>用2500rpm的转速的转速为25秒旋涂，随后直接4000与4000转/秒每个的加速度离心5秒。此过程导致40到45纳米厚的PEDOT:PSS薄膜。 </li><li>通过热在热板上在150℃，在空气中10分钟退火该基板从薄膜除去残留的水。 </li></ol> 4.沉积钙钛矿层的注意:碘化铅（PBI 2）对人体有剧毒。即使是少量的对神经，造血，肾脏和肝脏系统极其危险的。手柄含铅与护理解决方案。 注意:在整个本文所研究的钙钛矿薄膜，通过使用碘化铅2和CH 3 的 NH 3我（MAI），为前体材料五种不同的方法来制备。为了避免降解15，膜和设备及其特征的制造具有至b在N 2填充的手套箱（溶液处理）在惰性气氛， 例如下进行e或真空下（蒸镀）。 <ol><li> 处理解决方案 <ol><li>连续沉积<ol><li>放置在旋涂器基板和下降150μL的碘化铅溶解在N，N-二甲基甲酰胺，DMF（400毫克/毫升）与基板上的吸移管。 </li><li>以3000rpm进行30秒，立即旋涂。 </li><li>浸碘化铅2膜中的MAI溶解在异丙醇（10毫克/毫升），在40秒或降MAI溶液到干燥碘化铅2膜和离开那里40秒。 </li><li>旋涂以3000rpm剩余MAI溶液30秒从基材。 </li><li>通过将在基板上的加热板的热量为在100℃下15分钟。 </li></ol></li><li>联合解决方案: <ol><li>在期望的比例溶解既碘化铅和MAI:在DMF（理想1 1摩尔比），以形成具有250毫克浓度的前体溶液/毫升。 </li><li>搅拌在50℃下前体溶液至少5小时。 </li><li>预热基材覆盖有PEDOT:PSS在50℃在热板上5分钟。 </li><li>为了保证在整个一个设备系列增加再现性，通过旋涂机碗内滴下溶剂（200μL）的少量的同时旋涂的钙钛矿层创建甲苯气氛。 </li><li>放置在基板上150μL的前体溶液（从4.1.2.1）。 </li><li>旋转涂布，以从该前体溶液3000转进行30秒的钙钛矿层。旋涂每衬底的钙钛矿材料的一个层。 </li><li>在110℃下加热的热板上30秒所得的钙钛矿层。 </li></ol></li><li>分子添加剂: <ol><li>助溶解氯化铵 （18-20毫克/毫升）在旋涂溶液（如4.1.2.1中所述），以确保更好的膜的形成。作为前进行。 注意:这是在加入的共这样的替代lution从4.1.2。 </li></ol></li></ol></li><li> 真空沉积 <ol><li>一般程序<ol><li>加载清洗基板进入真空系统和撤离。 </li><li>后，达到10 -7毫巴的压力，转移样品至蒸发室和从与快门的蒸发源屏蔽它关闭。 </li><li>加热包含所述前体材料，以约330℃为碘化铅和140℃的MAI的两个来源。注意，在该室中的压力将上升到约10 -4毫巴由于MAI的挥发性质。 </li><li>校准用于使用一个石英晶体监视器天平（QCM），两种材料的蒸发速率位于靠近源，而另一种是在样本位置。该材料加热到蒸发温度，同时写下两个QCMS显示相应厚度。由比率计算工具因子的两个值。对于厚度计算中使用6.16和1.23克/厘米-3分别为碘化铅和MAI。 </li></ol></li><li>共蒸发<ol><li>通过增加或减少的源的温度以达到化学计量正确钙钛矿薄膜2:调整碘化铅的速率到MAI至大约1。 </li><li>打开快门在该样品的前面开始沉积。在达到预期的厚度后，关闭的源加热的快门和转弯。 </li><li>加热1小时的膜在70℃在真空室内以除去挥发性的化合物和完整成膜。 </li></ol></li><li>连续蒸发<ol><li>再次降低MAI源的温度蒸发（约100℃）的点的下方，并升温碘化铅源，直到蒸发启动;沉积的纯碘化铅的50纳米。 </li><li>事后，冷静下来的碘化铅源和蒸发MAI的50纳米亦同。对于较大的厚度重复步骤4.2.3.1 4.2.3.2和交替。 </li><li>加热1小时的膜在70℃在真空室内以除去挥发性的化合物和完整成膜。 </li></ol></li></ol></li></ol> 5。太阳能电池的制备<ol><li>溶解在氯苯受体苯基-C 60 -丁酸甲酯（PC 60 BM）以20mg / mL的浓度，并搅拌至少一天，在50℃的加热板上。 </li><li>准备如前所示的钙钛矿层（协解进程添加剂）（参见4.1.3）。 </li><li>冷却30秒的加热钙钛矿层上的金属板至室温。 </li><li>放置150μL的个人电脑60的基板上的BM溶液</li><li>旋涂的PC 60 BM以2000rpm上造成50纳米厚的层的钙钛矿薄膜的顶部30秒。 </li><li>将充分涂覆基材在为了一个样品保持器和盖用荫罩蒸发在有源层的顶部接触。 </li><li>划伤，以建立接触，以在ITO阳极用手术刀的联系人之一。 </li><li>转移到真空室，用于在阴极顶部接触的沉积。 </li><li>存10纳米的铝在P = 3×10 -6毫巴的最大压力为0.5埃/ s的速率，如由一个石英晶体监控器测定。第一为10nm后的速率可以增加高达2.5埃/ s的，直到达到100nm的层厚度。 </li><li>执行的电流密度与在-0.5至1.5伏（步骤= 0.02 V）的电压范围使用源测量单元中的太阳能电池的电压（JV）的测量。为了确保没有滞后于合营特征出现，测量反向扫描方向，同时，通过扫描从1.5至-0.5伏的偏见也是如此。使用太阳模拟器（100毫瓦平方厘米），使用认证的硅光电二极管校准。 </li></o升&gt;

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作者什么都没有透露。

我们发现，该处理条件对薄膜形态和膜覆盖一个显著影响。这就是为什么很多研究小组发布关于太阳能电池的性能和电离势为相同的钙钛矿材料的不同结果的原因。 为了确保再现性，这是至关重要的，以在惰性气氛（或真空）下进行所有的处理步骤和表征方法由湿度，以避免降解。也离析物的纯度和供应商中发挥重要作用（本文中未研究）。很显然，真空沉积的钙钛矿层的设有高结晶薄膜;然而，在比较，溶液处理的薄膜可以具有更高的吞吐量制造。 在我们的研究中，使用氯化铵作为前体溶液的添加剂，并在旋涂机碗甲苯气氛中提供的最可重复的光滑perovskitË电影。另一方面，浸渍和滴涂覆工艺导致相当粗糙的表面，并且没有进一步考虑设备的应用程序。最后，真空处理图层功能整体较小晶粒尺寸（约100纳米），但通过整部影片和平滑的表面高度覆盖。从不同的前体比样品系列中，我们了解到，该组合物具有在胶片上形成显著的影响力。然而，调查这些层用X射线衍射时（ 图2）的所有薄膜显示出高结晶度，并通过反射表明在14.11°和28.14°的类似四方晶体结构表示（110）和（220）面，而一些层似乎稍微紊乱，这可以通过的弱（002）的外观和（004）反射中看到。然而，XRD衍射峰的无显著扩大观察。有趣的是，在12.63°无碘化铅的不同的阶段的标志是<html>发现，即使是较大的过量纳入碘化铅的。这表明， 碘化铅未并入作为单独相或纳米晶岛屿但稀插页，这使得它无法检测用XRD。因此，使用X射线衍射的是有限的。 另一方面，XPS证实， 碘化铅或MAI（取决于制造方法）的附加量存在于该膜，从在引入氮比的变化为明显。这些插页反过来具有如前面提到的关于该薄膜的电子结构的显著影响。现在，随着在由UPS揭示电离能不同的观察组合从XPS的结果使我们能够这两种现象有关。 图6示出组合图，其中所测量的IE值被绘制为相应的膜的膜组合物（铅氮比）的函数。 图6"SRC ="/文件/ ftp_upload / 55084 / 55084fig6.jpg"/&gt; 图6:提取测量点的全部数据集的40钙钛矿网络LMS。电离能对引线的元素比R EXP至氮含量（如通过XPS确定）依赖;实线是线性音响t键数据和虚线标出±0.12电子伏特的标准偏差。在底部，该网络连接的t残差被示出。从16参考授权转载。版权所有2015年威利 - VCH。 <a href="http://ecsource.jove.com/files/ftp_upload/55084/55084fig6large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> 我们发现这两个值之间的明确的线性关系。我们的研究结果，因此，暗示过量与MAI钙钛矿薄膜具有较低的IE浏览器，而碘化铅富集层增加了IE浏览器。我们发现6.05±0.10电子伏特的IE浏览器对于R EXP = 1，这是比5.4电子伏特的经常发表的IE大得多的最佳摩尔比。这种差异是不太可能是由于加工条件，因为我们发现，适用于各种不同的制备钙钛矿薄膜的此值。它是相当由于在数据评估，其中在这里使用的状态斜率的线性密度导致较高的读出值的差异。这个问题的广泛讨论可以参考17中找到。要注意的是，我们发现在这些薄膜的光学带隙没有变化（ 例如 = 1.60±0.02电子伏特，数据未示出），这意味着它不仅是一种具有不同比率的IE移，但活化能是很重要（EA）同时移动。 最大太阳能电池效率被发现的1.02摩尔比R（PBI 2 MAI）以9.6％的电源转换效率这证实了文献中14稍微结果碘化铅富膜在晶界设有由钙钛矿薄膜的钝化的改进的载体行为由碘化铅。在开路电压的降低了200兆电子伏随着碘化铅含量都可以找到。由于在钙钛矿材料的带隙没有变化发生，V OC的减少不能由的光电间隙并发减少而是由空穴阻挡不足在钙钛矿和PCBM的接口说明（IE PCBM = 6.2电子伏特），由于增加钙钛矿IE中。同时从0.8到0.7的FF为R&gt; 1.05降低支持了这些发现。 总之，我们提出了通过各种制备方法制备的钙钛矿薄膜的广泛研究，发现发生在膜的形成，电子结构和设备性能的强烈变化。特别感兴趣的是由MAI邻故意掺入到调节钙钛矿的IE中的可能性ř碘化铅可用于新型器件结构界面优化2插页。未来的研究将着眼于该向大型设备领域瞄准更先进的制备技术。这些措施包括像刮浆，喷涂技术，以及当前安装在我们的COPT.centre（COPT =中心有机生产技术）设施大规模的印刷方法。

薄膜光伏技术已吸引了的太阳能电池应用的研究的一个显著注意，由于其低的材料消耗和适用性在柔性基板上。最值得注意的是，有机/无机卤化物钙钛矿材料已被证明是在太阳能电池器件上可行的有源层，导致高效率。钙钛矿配有利的性质，如高吸收系数1，高载流子迁移率2，和低的激子结合能3。钙钛矿层可通过各种溶液或使用低成本的前体材料如铅（Ⅱ），碘化（PBI 2）和甲基铵碘化物（MAI）蒸气基于相位的制造方法来制造。这种方式可以容易制备使用低制造温度相比于市售的硅太阳能电池的高结晶膜。 它一直笑WN几个参数对钙钛矿太阳能电池，最显着的薄膜形态的性能有很大的影响，因为它影响激子扩散长度和电荷载体迁移率。聂等人。表明，通过提高钙钛矿薄膜的形态，关于覆盖和平均晶体尺寸，太阳能电池的性能提高4,5。形态已被证明是由前体材料（ⅰ）选择（ 例如 ，使用醋酸铅6），（ⅱ）分子添加剂（如NH 4 Cl）的7，（ⅲ）的溶剂的选择，（ⅳ）的热影响溶剂气氛（如甲苯或氯苯8），特别是（v）的制备方法9的选择下退火。基于溶液的过程一样，效率超过17％4中的太阳能电池的一步或两步旋涂结果&lt;/ SUP&gt;，10，11，12，而真空沉积钙钛矿型太阳能电池产量的15.4％，13的效率。 已经表明，过量的碘化铅钙钛矿层为太阳能电池的性能有利由于由钙钛矿薄膜的钝化在晶界14的改进的载流子平衡通过碘化铅。然而，很少的工作已经完成，以理解的化学计量上的钙钛矿薄膜材料的影响的作用。 在本文中，我们在广泛不同的准备钙钛矿的电影呈现了广泛的研究，并展示如何制备方法和前体化学计量的影响形态，结晶度，态密度，薄膜成分和太阳能电池的性能。一个全面的概述介绍，从制造到电影characterization一路器件性能。

<table><tbody><tr><td>ITO</td><td>Rose</td><td></td><td>&amp;lt; 15 &amp;Omega;/sq</td></tr><tr><td>PEDOT:PSS</td><td>Heraeus Clevios</td><td>P VP .Al&amp;nbsp; 4083</td><td></td></tr><tr><td>MAI</td><td></td><td></td><td>Synthesized as found in literature</td></tr><tr><td>PbI&lt;sub&gt;2&lt;/sub&gt;</td><td>Alfa Aesar</td><td>44314</td><td>99.999% trace metals basis, -10 mesh beads</td></tr><tr><td>NH&lt;sub&gt;4&lt;/sub&gt;Cl</td><td>Suprapure</td><td>101143</td><td>99.995%</td></tr><tr><td>PCBM</td><td>Nano C</td><td></td><td>99.9%</td></tr><tr><td>Chlorobenzene</td><td>Sigma Aldrich</td><td>270644</td><td>Chromasolv for HPLC (99.9%)</td></tr><tr><td>&lt;em&gt;N,N&lt;/em&gt;-Dimethylformamide</td><td>Acros Chemicals</td><td>&amp;nbsp;348430010</td><td>Extra dry, stored over molecular sieves (99.8%)</td></tr><tr><td>Toluene</td><td>Sigma Aldrich</td><td>244511</td><td>anhydrous</td></tr></tbody></table>

influence of hybrid perovskite fabrication methods on film formation, electronic structure, and solar cell performance

杂化有机/无机卤化物钙钛矿近来一直在太阳能电池应用领域的极大兴趣的话题，有潜力实现设备效率超过其他的薄膜器件的技术。然而，据报道在器件效率和基本物理性能的大变化。这是由于薄膜在加工过程中非故意的变化，这些都没有得到充分的迄今研究。因此，我们进行了大量的CH 3 NH 3碘化铅3钙钛矿，其中我们显示的形态和电子结构的广泛的研究如何制备方法以及离析物甲基铵碘化物和铅（II），碘化冲击性能等的混合比膜的形成，晶体结构，态密度，能量水平，最终太阳能电池的性能。

为了获得在不同的制造方法钙钛矿电影的整体视图，它的结构，电子和器件特性结合在一起是非常重要的。扫描电子显微镜（SEM）给出形态良好的印象。因此，由不同的制造方法制造的所有膜的影响。钙钛矿薄膜的代表性子集示于图1，其可视化的薄膜形态的制备方法的显著影响。 理想情况下，平滑的和无针孔膜需要的设备。如可以看到的，这是从与添加剂的 NH 4 Cl和甲苯气氛共溶液中制备的气相沉积膜（F，G），该浸涂那些（D，E），以及膜的情况下（A1至a5）中与碘化铅的变化的比R为0.6 MAI至1.4。与此相反，薄膜无覆盖<html> UT添加剂（h）中，以及浸涂（D，E）和下拉式涂布那些（B，C）示出了大的空隙，针状结构，或表面粗糙度大，因此不为设备应用是有用的。 <img alt="图1" src="/files/ftp_upload/55084/55084fig1.jpg" /> 图1:通过不同的处理方法制备的钙钛矿薄膜的SEM图像。 （A1 - A5）与添加剂和甲苯气氛对PBI 2到MAI（R），（ 二 ）落涂料具有40秒的加载时间，（C）不同比例共同的解决方案落涂料，具有120秒的加载时间，（ D）浸涂（10秒加载时间），（ 五 ）浸涂（3 600■装载时间），（F）共蒸发，（G）连续蒸发（H）共同解决方案，无需添加剂。刻度条表示1微米的长度。tp_upload / 55084 / 55084fig1large.jpg"目标="_空白"&gt;点击此处查看该图的放大版本。 最后， 图1为A1-A5显示使用具有添加剂和甲苯的氛围共同液配制0.6 碘化铅的比R混合MAI到1.4的变化。在表面覆盖和晶体尺寸显示的是，这里还有不同的电影形态出现的变化。 虽然SEM是可视化薄膜的形态和覆盖面，并获得电影粗糙的印象的好工具，但没有结构信息中给出。 因此，为了进一步表征钙钛矿薄膜，使用X射线衍射（XRD）。与使用Cu的Kα这种技术α阳极（λ= 1.54056埃）在2θ为10之间的范围内的晶相<html> 6;和40°（的0.00836°步长）进行了监测和表征。在许多出版物XRD被用来确定钙钛矿薄膜的质量。 图2示出了具有碘化铅2的六个不同的混合比到MAI样本的子集的XRD测量，并且因此对应于SEM图像在图1A1-A5。此外，纯碘化铅的光谱被示出。由此看来，在所述钙钛矿层的质量的前体溶液的化学计量的影响，因为诸如不同相的外观， 即 碘化铅和MAI的附加的阶段掺入，进行了研究。光谱显示出四方晶体结构，并反射与它们对应的晶面索引。出人意料的是，在非化学计量膜中观察到的MAI或碘化铅的无附加的阶段。 NT"&gt; <img alt="图2" src="/files/ftp_upload/55084/55084fig2.jpg" /> 图2:纯碘化铅2的XRD图形，以及使用前体（由数字右侧给定比率）的各个摩尔比通过共溶液法（用NH 4 Cl和甲苯气氛）制备钙钛矿的样品。为比较，所述曲线标准化，以峰值在14.11°和垂直移动。从16参考授权转载。版权所有2015年威利 - VCH。 <a href="http://ecsource.jove.com/files/ftp_upload/55084/55084fig2large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> 作为X射线衍射没有提供关于该膜的组合物的信息，X射线光电子能谱（XPS）使用，这是能够直接测量膜的化学计量。对于这个测量，镁，钾α激励源（hν= 1252.6电子伏特）与10 EV（能量分辨率= 800兆电子伏）的通能使用。的相对灵敏度因子（RSF）必须考虑到对每个单独测量元件。因此，它校准为我们的测量系统的RSFS（镁，钾α源，X射线源和分析器50.0°之间的角度）是重要的。我们使用了大量的小分子的校准碘峰与三- （4- iodphenyl） -胺（C 18 H 12 I 3 N）和经由碘化铅校准铅。碳被用作基准，因为这样与RSF（的C1s）= 1，因此，RSF因素的个体元件; RSF（N1s的）= 1.8，RSF（I3D 5/2）= 32.8，和RSF（Pb4f 7/2）= 16.5。 图3示出的蒸气沉积膜的有代表性的XPS能谱，以在上部子图表示的特性核心电平峰值。在较低的子图I3D 5/2（619.6 eV）的，N1s的（402.7电子伏特），的C1s（286.6eV）和Pb4f 7/2（138.6 eV）的峰被示出。所有的信号可以由单个混合高斯/洛伦兹峰被装配，仅在碘在较高的结合能的小功能通常观察到的情况下，但是这是一个摇上行峰，因此不涉及实际的额外的接合状态。我们可以通过在信号强度整合和由它们各自的无国界记者组织16正常化它提取所有准备钙钛矿层的相对膜组成。 N::铅:在一些薄膜，从该理想薄膜化学计量Ç发现大偏差I的1:1:1:3; 如导致0.4ð1.5之间变化氮的比例。这是为蒸气沉积膜，其中，共蒸发是难以控制和再现，尤其如此。用于溶液处理的样品，在另一方面，实际的和预期的前体的混合比与最终膜组成一致非常以及确定从XPS。 <img alt="图3" src="/files/ftp_upload/55084/55084fig3.jpg" /> 图3:代表XPS谱。以上示出了完整的XPS扫描，下面的特写XPS积分峰的测量显示。 <a href="http://ecsource.jove.com/files/ftp_upload/55084/55084fig3large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> 为了研究在膜组合物的这些变化是如何影响状态密度，我们转向紫外线光电子能谱（UPS）。要执行的UPS测量，氦放电灯（在21.22 eV的他我，样品偏差-8 V）时，用2 eV的通能和110兆电子伏的能量分辨率（从费米边缘宽度确定）。对于所有样品，全谱首先测定，然后使用较高分析器光圈以增加信噪比，一个详细的更高分辨率的扫描<html>进行VB的区域。在UPS谱，特别是VB区域扫描，从多色他我的辐射导致卫星峰为数字数据分析过程中修正。 图4示出的所有研究样品的完整数据集的UPS曲线，涵盖共和顺序蒸发（淡红色），以及不同的溶液处理（暗红色）的方法。我们仅想强调的是在电离能（IE）的显著变化观察，从图4的左手情节的高结合能切断位置的变化显着。这些变化在加工和薄膜成分所带来的变化，并导致IE 5.67和6.4电子伏特之间的可调性。有关更详细的讨论，请参阅附图16。 JPG"/&gt; 图4:所研究样品的代表子集的UPS的扫描。左侧面板显示了较高的结合能量截止（HBEC）和价带区域，而右侧示出了高分辨率特写VB的发病为蒸气沉积（淡红色线）和溶液加工（暗红色线）钙钛矿型薄膜。所有的曲线一直以沿x轴转移到大约3 EV对齐功能。从16参考授权转载。版权所有2015年威利 - VCH。 <a href="http://ecsource.jove.com/files/ftp_upload/55084/55084fig4large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> 如我们从我们以前该钙钛矿从不同前体的混合比制备的膜导致在电子结构的变化，而不破坏该膜的晶体结构的实验得知，我们希望调查的前体比对太阳能电池性能的影响。因此，ITO / PEDOT:用共溶液处理钙钛矿层（与添加剂和甲苯气氛），使用碘化铅的比例到MAI从0.7至1.2制备的PSS /钙钛矿/ PC 60 BM /铝的太阳能电池。 图5示出薄膜的化学计量（意比率R）上的太阳能电池特性的功率转换效率（PCE），短路电流（J SC），开路电压（V OC）和填充因子（FF）的影响。的9.6％的最高效率被发现为1.02的预期的摩尔比， 即接近理想的钙钛矿组合物。 <img alt="图5" src="/files/ftp_upload/55084/55084fig5.jpg" /> 图5:PCE，J SC，V OC和FF的特性值。这些值是从太阳能电池装置INDEP的测量提取碘化铅的预期混合比R INT为MAI的endent用于薄膜制备。从16参考授权转载。版权所有2015年威利 - VCH。 <a href="http://ecsource.jove.com/files/ftp_upload/55084/55084fig5large.jpg" target="_blank">请点击此处查看该图的放大版本。</a>

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Influence of Hybrid Perovskite Fabrication Methods on Film Formation, Electronic Structure, and Solar Cell Performance

我们通过比较晶体结构，状态，能级密度，最终的太阳能电池的性能提出对不同的制造方法的有机/无机钙钛矿薄膜的影响的广泛的研究。

上成膜钙钛矿型混合制造方法，电子结构和太阳能电池性能的影响

Hybrid organic/inorganic halide perovskites have lately been a topic of great interest in the field of solar cell applications, with the potential to ...

influence-hybrid-perovskite-fabrication-methods-on-film-formation

Universidad de Cartagena UDEC

Research

JoVE Journal

Chemistry

18.4K 次观看.  University of Cologne. 我们通过比较晶体结构，状态，能级密度，最终的太阳能电池的性能提出对不同的制造方法的有机/无机钙钛矿薄膜的影响的广泛的研究。 

视频: Influence of Hybrid Perovskite Fabrication Methods on Film Formation, Electronic Structure, and Solar Cell Performance

Printing Fabrication of Bulk Heterojunction Solar Cells and In Situ Morphology Characterization

Polymer-based materials hold promise as low-cost, flexible efficient photovoltaic devices. Most laboratory efforts to achieve high performance devices have used devices prepared by spin coating, a process that is not amenable to large-scale fabrication. This mismatch in device fabrication makes it difficult to translate quantitative results obtained in the laboratory to the commercial level, making optimization difficult. Using a mini-slot die coater, this mismatch can be resolved by translating the commercial process to the laboratory and characterizing the structure formation in the active layer of the device in real time and in situ as films are coated onto a substrate. The evolution of the morphology was characterized under different conditions, allowing us to propose a mechanism by which the structures form and grow. This mini-slot die coater offers a simple, convenient, material efficient route by which the morphology in the active layer can be optimized under industrially relevant conditions. The goal of this protocol is to show experimental details of how a solar cell device is fabricated using a mini-slot die coater and technical details of running in situ structure characterization using the mini-slot die coater.

Printing Fabrication of Bulk Heterojunction Solar Cells and In Situ Morphology Characterization

Here, we present a protocol to fabricate organic thin film solar cells using a mini-slot die coater and related in-line structure characterizations using synchrotron scattering techniques.

散装异质结太阳能电池的印刷和制作<em&gt;原位</em&gt;形态特征

Polymer-based materials hold promise as low-cost, flexible efficient photovoltaic devices. Most laboratory efforts to achieve high performance devices ...

科研

工程学

Fabrication of Fully Solution Processed Inorganic Nanocrystal Photovoltaic Devices

We demonstrate a method for the preparation of fully solution processed inorganic solar cells from a spin and spray coating deposition of nanocrystal inks. For the photoactive absorber layer, colloidal CdTe and CdSe nanocrystals (3-5 nm) are synthesized using an inert hot injection technique and cleaned with precipitations to remove excess starting reagents. Similarly, gold nanocrystals (3-5 nm) are synthesized under ambient conditions and dissolved in organic solvents. In addition, precursor solutions for transparent conductive indium tin oxide (ITO) films are prepared from solutions of indium and tin salts paired with a reactive oxidizer. Layer-by-layer, these solutions are deposited onto a glass substrate following annealing (200-400 &#176;C) to build the nanocrystal solar cell (glass/ITO/CdSe/CdTe/Au). Pre-annealing ligand exchange is required for CdSe and CdTe nanocrystals where films are dipped in NH4Cl:methanol to replace long-chain native ligands with small inorganic Cl- anions. NH4Cl(s) was found to act as a catalyst for the sintering reaction (as a non-toxic alternative to the conventional CdCl2(s) treatment) leading to grain growth (136&#177;39 nm) during heating. The thickness and roughness of the prepared films are characterized with SEM and optical profilometry. FTIR is used to determine the degree of ligand exchange prior to sintering, and XRD is used to verify the crystallinity and phase of each material. UV/Vis spectra show high visible light transmission through the ITO layer and a red shift in the absorbance of the cadmium chalcogenide nanocrystals after thermal annealing. Current-voltage curves of completed devices are measured under simulated one sun illumination. Small differences in deposition techniques and reagents employed during ligand exchange have been shown to have a profound influence on the device properties. Here, we examine the effects of chemical (sintering and ligand exchange agents) and physical treatments (solution concentration, spray-pressure, annealing time and annealing temperature) on photovoltaic device performance.

This protocol describes the synthesis and solution deposition of inorganic nanocrystals layer by layer to produce thin film electronics on non-conductive surfaces. Solvent-stabilized inks can produce complete photovoltaic devices on glass substrates via spin and spray coating following post-deposition ligand exchange and sintering.

全面解决方案处理的无机纳米晶体光伏器件的制造

We demonstrate a method for the preparation of fully solution processed inorganic solar cells from a spin and spray coating deposition of nanocrystal ...

Morphology Control for Fully Printable Organic&#8211;Inorganic Bulk-heterojunction Solar Cells Based on a Ti-alkoxide and Semiconducting Polymer

The photoactive layer of a typical organic thin-film bulk-heterojunction (BHJ) solar cell commonly uses fullerene derivatives as the electron-accepting material. However, fullerene derivatives are air-sensitive; therefore, air-stable material is needed as an alternative. In the present study, we propose and describe the properties of Ti-alkoxide as an alternative electron-accepting material to fullerene derivatives to create highly air-stable BHJ solar cells. It is well-known that controlling the morphology in the photoactive layer, which is constructed with fullerene derivatives as the electron acceptor, is important for obtaining a high overall efficiency through the solvent method. The conventional solvent method is useful for high-solubility materials, such as fullerene derivatives. However, for Ti-alkoxides, the conventional solvent method is insufficient, because they only dissolve in specific solvents. Here, we demonstrate a new approach to morphology control that uses the molecular bulkiness of Ti-alkoxides without the conventional solvent method. That is, this method is one approach to obtain highly efficient, air-stable, organic-inorganic bulk-heterojunction solar cells.

A method for fully printable, fullerene-free, highly air-stable, bulk-heterojunction solar cells based on Ti alkoxides as the electron acceptor and the electron-donating polymer fabrication is described here. Moreover, a method for controlling the morphology of the photoactive layer through the molecular bulkiness of the Ti-alkoxide units is reported.

基于一个钛醇盐和半导体聚合物为全可印刷有机 - 无机批量异质结太阳能电池形貌控制

The photoactive layer of a typical organic thin-film bulk-heterojunction (BHJ) solar cell commonly uses fullerene derivatives as the electron-accepting ...

Low Pressure Vapor-assisted Solution Process for Tunable Band Gap Pinhole-free Methylammonium Lead Halide Perovskite Films

Organo-lead halide perovskites have recently attracted great interest for potential applications in thin-film photovoltaics and optoelectronics. Herein, we present a protocol for the fabrication of this material via the low-pressure vapor assisted solution process (LP-VASP) method, which yields ~19% power conversion efficiency in planar heterojunction perovskite solar cells. First, we report the synthesis of methylammonium iodide (CH3NH3I) and methylammonium bromide (CH3NH3Br) from methylamine and the corresponding halide acid (HI or HBr). Then, we describe the fabrication of pinhole-free, continuous methylammonium-lead halide perovskite (CH3NH3PbX3 with X = I, Br, Cl and their mixture) films with the LP-VASP. This process is based on two steps: i) spin-coating of a homogenous layer of lead halide precursor onto a substrate, and ii) conversion of this layer to CH3NH3PbI3-xBrx by exposing the substrate to vapors of a mixture of CH3NH3I and CH3NH3Br at reduced pressure and 120 &#176;C. Through slow diffusion of the methylammonium halide vapor into the lead halide precursor, we achieve slow and controlled growth of a continuous, pinhole-free perovskite film. The LP-VASP allows synthetic access to the full halide composition space in CH3NH3PbI3-xBrx with 0&#160;&#8804; x&#160;&#8804; 3. Depending on the composition of the vapor phase, the bandgap can be tuned between 1.6 eV&#160;&#8804; Eg&#160;&#8804; 2.3 eV. In addition, by varying the composition of the halide precursor and of the vapor phase, we can also obtain CH3NH3PbI3-xClx. Films obtained from the LP-VASP are reproducible, phase pure as confirmed by X-ray diffraction measurements, and show high photoluminescence quantum yield. The process does not require the use of a glovebox.

Here, we present a protocol for the synthesis of CH3NH3I and CH3NH3Br precursors and the subsequent formation of pinhole-free, continuous CH3NH3PbI3-xBrx thin films for the application in high efficiency solar cells and other optoelectronic devices.

可调谐带隙无针孔 Methylammonium 铅卤化物钙钛矿薄膜的低压蒸气辅助解决工艺

Organo-lead halide perovskites have recently attracted great interest for potential applications in thin-film photovoltaics and optoelectronics. Herein, ...

化学

Monovalent Cation Doping of CH3NH3PbI3 for Efficient Perovskite Solar Cells

Here, we demonstrate the incorporation of monovalent cation additives into CH3NH3PbI3 perovskite in order to adjust the optical, excitonic, and electrical properties. The possibility of doping was investigated by adding monovalent cation halides with similar ionic radii to Pb2+, including Cu+, Na+, and Ag+. A shift in the Fermi level and a remarkable decrease of sub-bandgap optical absorption, along with a lower energetic disorder in the perovskite, was achieved. An order-of-magnitude enhancement in the bulk hole mobility and a significant reduction of transport activation energy within an additive-based perovskite device was attained. The confluence of the aforementioned improved properties in the presence of these cations led to an enhancement in the photovoltaic parameters of the perovskite solar cell. An increase of 70 mV in open circuit voltage for AgI and a 2 mA/cm2 improvement in photocurrent density for NaI- and CuBr-based solar cells were achieved compared to the pristine device. Our work paves the way for further improvements in the optoelectronic quality of CH3NH3PbI3 perovskite and subsequent devices. It highlights a new avenue for investigations on the role of dopant impurities in crystallization and controls the electronic defect density in perovskite structures.

Monovalent Cation Doping of CH3NH3PbI3 for Efficient Perovskite Solar Cells

Here, we present a protocol to adjust the properties of solution-processed CH3NH3PbI3 through the incorporation of monovalent cation additives in order to achieve highly efficient perovskite solar cells.

CH的单价阳离子兴奋剂<sub&gt; 3</sub&gt; NH<sub&gt; 3</sub&gt;碘化铅<sub&gt; 3</sub&gt;对钙钛矿型高效太阳能电池

Here, we demonstrate the incorporation of monovalent cation additives into CH3NH3PbI3 perovskite in order to adjust the optical, excitonic, and electrical ...

Flash Infrared Annealing for Perovskite Solar Cell Processing

Organic&#8211;inorganic perovskites have an impressive potential for the design of next generation solar cells and are currently considered for upscaling and commercialization. Currently, perovskite solar cells rely on spin-coating which is neither practical for large areas nor environmentally friendly. Indeed, one of the conventional and most effective lab-scale methods to induce perovskite crystallization, the antisolvent method, requires an amount of toxic solvent that is difficult to apply on larger surfaces. To solve this problem, an antisolvent-free and rapid thermal annealing process called flash infrared annealing (FIRA) can be used to produce highly crystalline perovskite films. The FIRA oven is composed of an array of near-infrared halogen lamps with an illumination power of 3,000 kW/m2. A hollow aluminum body enables an effective water-cooling system. The FIRA method allows the synthesis of perovskite films in less than 2 s, achieving efficiencies &#62;20%. FIRA has a unique potential for the industry because it can be adapted to continuous processing, is antisolvent-free, and does not require lengthy, hour-long annealing steps.

We describe a flash infrared annealing method used for the synthesis of perovskite and mesoscopic-TiO2 films. Annealing parameters are varied and optimized for processing on fluorine-doped tin oxide (FTO) glass and indium tin oxide-coated polyethylene terephthalate (ITO PET), subsequently giving devices power conversion efficiencies &#62;20%.

用于佩罗夫斯基特太阳能电池处理的闪光红外退火

Organic&#8211;inorganic perovskites have an impressive potential for the design of next generation solar cells and are currently considered for upscaling ...

环境科学

Key Factors Affecting the Performance of Sb2S3-sensitized Solar Cells During an Sb2S3 Deposition via SbCl3-thiourea Complex Solution-processing

Sb2S3 is considered as one of the emerging light absorbers that can be applied to next-generation solar cells because of its unique optical and electrical properties. Recently, we demonstrated its potential as next-generation solar cells by achieving a high photovoltaic efficiency of &#62; 6% in Sb2S3-sensitized solar cells using a simple thiourea (TU)-based complex solution method. Here, we describe the key experimental procedures for the deposition of Sb2S3 on a mesoporous TiO2 (mp-TiO2) layer using a SbCl3-TU complex solution in the fabrication of solar cells. First, the SbCl3-TU solution is synthesized by dissolving SbCl3 and TU in N,N-dimethylformamide at different molar ratios of SbCl3:TU. Then, the solution is deposited on as-prepared substrates consisting of mp-TiO2/TiO2-blocking layer/F-doped SnO2 glass by spin coating. Finally, to form crystalline Sb2S3, the samples are annealed in an N2-filled glove box at 300 &#176;C. The effects of the experimental parameters on the photovoltaic device performance are also discussed.

Key Factors Affecting the Performance of Sb2S3-sensitized Solar Cells During an Sb2S3 Deposition via SbCl3-thiourea Complex Solution-processing

This work provides a detailed experimental procedure for the deposition of Sb2S3 on a mesoporous TiO2 layer using a SbCl3-thiourea complex solution for applications in Sb2S3-sensitized solar cells. This article also determines key factors governing the deposition process.

利用SbCl3-硫脲复合溶液处理锑23沉积物对锑2S3敏化太阳能电池性能影响的关键因素

Sb2S3 is considered as one of the emerging light absorbers that can be applied to next-generation solar cells because of its unique optical and electrical ...

Solution-Processed "Silver-Bismuth-Iodine" Ternary Thin Films for Lead-Free Photovoltaic Absorbers

Bismuth-based hybrid perovskites are regarded as promising photo-active semiconductors for environment-friendly and air-stable solar cell applications. However, poor surface morphologies and relatively high bandgap energies have limited their potential. Silver-bismuth-iodine (Ag-Bi-I) is a promising semiconductor for optoelectronic devices. Therefore, we demonstrate the fabrication of Ag-Bi-I ternary thin films using material solution processing. The resulting thin films exhibit controlled surface morphologies and optical bandgaps according to their thermal annealing temperatures. In addition, it has been reported that Ag-Bi-I ternary systems crystallize to AgBi2I7, Ag2BiI5, etc. according to the ratio of the precursor chemicals. The solution-processed AgBi2I7 thin films exhibit a cubic-phase crystal structure, dense, pinhole-free surface morphologies with grains ranging in size from 200 to 800 nm, and an indirect bandgap of 1.87 eV. The resultant AgBi2I7 thin films show good air stability and energy band diagrams, as well as surface morphologies and optical bandgaps suitable for lead-free and air-stable single-junction solar cells. Very recently, a solar cell with 4.3% power conversion efficiency was obtained by optimizing the Ag-Bi-I crystal compositions and solar cell device architectures.

Herein, we present detailed protocols for solution-processed silver-bismuth-iodine (Ag-Bi-I) ternary semiconductor thin films fabricated on TiO2-coated transparent electrodes and their potential application as air-stable and lead-free optoelectronic devices.

无铅光伏吸收剂的溶液处理 "银铋碘" 三元薄膜

Bismuth-based hybrid perovskites are regarded as promising photo-active semiconductors for environment-friendly and air-stable solar cell applications. ...

Inkjet Printing All Inorganic Halide Perovskite Inks for Photovoltaic Applications

A method for synthesizing photoactive inorganic&#160;perovskite quantum dot inks and an inkjet printer deposition method, using the synthesized inks, are demonstrated. The ink synthesis is based on a simple wet chemical reaction and the inkjet printing protocol is a facile step by step method. The inkjet printed thin films have been characterized by X-ray diffraction, optical absorption spectroscopy, photoluminescent spectroscopy, and electronic transport measurements. X-ray diffraction of the printed quantum dot films indicates a crystal structure consistent with an orthorhombic room temperature phase with (001) orientation. In conjunction with other characterization methods, the X-ray diffraction&#160;measurements show high quality films can be obtained through the inkjet printing method.

A protocol for synthesizing inorganic-lead-halide hybrid perovskite quantum dot inks for inkjet printing and the protocol for preparing and printing the quantum dot inks in an inkjet printer with post characterization techniques are presented.

用于光伏应用的喷墨打印所有无机舱齐德 perovskite 油墨

A method for synthesizing photoactive inorganic&#160;perovskite quantum dot inks and an inkjet printer deposition method, using the synthesized inks, are ...

Facile Synthesis of Colloidal Lead Halide Perovskite Nanoplatelets via Ligand-Assisted Reprecipitation

In this work, we demonstrate a facile method for colloidal lead halide perovskite nanoplatelet synthesis (Chemical formula: L2[ABX3]n-1BX4, L: butylammonium and octylammonium, A: methylammonium or formamidinium, B: lead, X: bromide and iodide, n: number of [BX6]4- octahedral layers in the direction of nanoplatelet thickness) via ligand-assisted reprecipitation. Individual perovskite precursor solutions are prepared by dissolving each nanoplatelet constituent salt in N,N-dimethylformamide (DMF), which is a polar organic solvent, and then mixing in specific ratios for targeted nanoplatelet thickness and composition. Once the mixed precursor solution is dropped into nonpolar toluene, the abrupt change in the solubility induces the instantaneous crystallization of nanoplatelets with surface-bound alkylammonium halide ligands providing colloidal stability. Photoluminescence and absorption spectra reveal emissive and strongly quantum-confined features. X-ray diffraction and transmission electron microscopy confirm the two-dimensional structure of the nanoplatelets. Furthermore, we demonstrate that the band gap of perovskite nanoplatelets can be continuously tuned in the visible range by varying the stoichiometry of the halide ion(s). Lastly, we demonstrate the flexibility of the ligand-assisted reprecipitation method by introducing multiple species as surface-capping ligands. This methodology represents a simple procedure for preparing dispersions of emissive 2D colloidal semiconductors.

This work demonstrates facile room-temperature synthesis of colloidal quantum-confined lead halide perovskite nanoplatelets by ligand-assisted reprecipitation method. Synthesized nanoplatelets show spectrally narrow optical features and continuous spectral tunability throughout the visible range by varying the composition and thicknesses.

上成膜钙钛矿型混合制造方法，电子结构和太阳能电池性能的影响

摘要

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