M.阿卜迪 - Jalebi感谢纳瓦技术有限公司为博士奖学金。 MI达累斯萨拉姆和M.Grätzel感谢阿卜杜勒阿齐兹国王城科学和技术（KACST）和瑞士国家科学基金会（SNSF）的资金支持。笔者想感谢皮埃尔Mettraux博士在分子和混合材料表征中心，洛桑联邦理工学院为进行XPS测量。 A.Sadhanala十分感谢印度 - 英国APEX项目的资金支持。 SP Senanayak承认皇家学会伦敦牛顿奖学金。 RH朋友，M.阿卜迪 - Jalebi和A. Sadhanala要感谢来自EPSRC的支持。

1.合成和质朴和基于添加剂CH 3的沉积NH 3碘化铅3 注:防潮和氧在受控条件下在氩气手套箱内制备所有溶液（H 2 O级:&lt;1ppm的和O 2水平:&lt;10ppm的）。 <ol><li>在80℃下溶解碘化铅2的553毫克（1.2 M），在1毫升的N，N-二甲基甲酰胺（DMF）中不断搅拌下。 </li><li>添加0.02M的一价阳离子的卤化物的碘化铅溶液。 </li><li>旋涂在6,500 rpm时得到的黄色透明溶液到衬底（ 例如，介孔-TiO 2的）30秒以4,000rpm的坡道。 </li><li>烘烤在电炉上的膜在80℃下进行30分钟。 </li><li>在5毫升异丙醇中溶解40毫克碘甲基铵（MAI）的。 </li><li>旋涂的MAI溶液足量到使用两步骤protoc所得碘化铅膜其次是20秒旋转在4000转醇，其中包括45秒的加载时间。 </li><li>退火在电炉上的旋涂钙钛矿薄膜在100℃下45分钟。 </li></ol> 2.太阳能电池的制造<ol><li> 基板制备 <ol><li>图案氟掺杂的氧化锡（FTO）包被的玻璃。 <ol><li>覆盖在FTO玻璃半透明粘合带的活动区域。 </li><li>倒在FTO基板的未覆盖区域的锌（Zn）的粉末。 </li><li>在蒸馏水中制备的2M盐酸（HCl）的。 </li><li>倒入HCl溶液到该覆盖用Zn粉在FTO玻璃的一部分。 </li><li>用清水洗净FTO并取出磁带。 </li></ol></li><li>清洁基片<ol><li>洗，用2％（重量/体积）的洗涤剂在FTO玻璃上。 </li><li>超声处理在丙酮和异丙醇（IPA）在蚀刻FTO基板10分钟。 </li><li>对待FTO基板与ultraviolet / O 3清洗剂15分钟。 </li></ol></li></ol></li><li> 空穴阻挡层的沉积 <ol><li>在7毫升IPA中添加钛二异丙醇二（乙酰丙酮）（TAA）的0.6毫升。 </li><li>穿上在450℃的加热板上的清洁和图案化的FTO基板和覆盖加热前的接触面积。 </li><li>喷雾热分解的TAA溶液到使用O 2作为载气的未覆盖区域。 </li><li>离开样品在450℃下30分钟。 </li></ol></li><li> 电子传输层的沉积 <ol><li>稀释商用的 TiO 2浆料（30纳米粒径）用乙醇（2:7，重量比）。 </li><li>通过超声处理30分钟均质化的 TiO 2稀释。 </li><li>旋涂二氧化钛稀释到制备的样品紧凑型二氧化钛层30秒以5,000rpm 2,000 rpm的坡道。 </li><li>退火二氧化钛膜在500℃下进行30分钟。 </li><li>治疗在蒸馏水的 TiCl 4的40mM溶液所得介孔TiO 2的薄膜在70℃20分钟。 </li><li>在退火450 四氯化钛-处理电影 °下进行30分钟。 </li></ol></li><li> 钙钛矿层的沉积 注意:用二氧化钛层中的FTO基板转移到干燥空气箱与&lt;1％用于制造工艺的其余部分的湿度。 <ol><li>旋涂的准备碘化铅解决方案（有和没有掺杂剂）到介孔二氧化钛30秒在6,500 rpm转速下拥有4000 rpm的坡道。 </li><li>烘烤在电炉上的膜在80℃下进行30分钟。 </li><li>旋涂足够量的MAI溶液成使用两步骤的协议，其中包括45秒的加载时间接着在4000 rpm的转速2000转的斜坡纺纱20秒所得碘化铅膜。 </li><li>退火在hotpla旋涂钙钛矿薄膜德在100℃下45分钟。 </li></ol></li><li> 空穴输送层的沉积 <ol><li> 72.3毫克螺OMeTAD添加到1毫升氯苯和摇动直到溶液变得透明。 </li><li>通过在乙腈中加入520毫克的LiTFSI的使双（三氟甲基磺酰基）酰亚胺（的LiTFSI）的贮备溶液。 </li><li>加入的LiTFSI原液17.5微升和4- 叔丁基吡啶（TBP）的螺OMeTAD溶液28.8μL。 </li><li>旋涂层30秒以上溶液以4000rpm 2,000 rpm的坡道。 </li></ol></li><li> 顶部接触的热蒸发 <ol><li>面膜样本，并把它们在蒸发器的真空室。 </li><li>蒸发80纳米的金为0.01纳米/秒的速率。 </li></ol></li></ol>

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The authors declare that they have no competing financial interests.

介观钙钛矿的太阳能电池的典型架构是在这项工作中，其中系列的材料是旋涂在导电基底和热蒸发金属接触（ 图1）之间使用。介孔TiO 2的层用的TiCl 4，其被报告给钝化表面陷阱和提高电子传输层和吸收体材料21，22之间的接口处理。然后在钙钛矿层使用顺序两步沉积技术沉积。在完全转化卤化铅进入钙钛矿在第二步骤是必不可少的，以实现最高的光吸收16，图 17，我们表明，一价阳离子的卤化物添加剂（ 如，碘化钠和溴化亚铜）导致完全转化。另外，介孔二氧化钛层的完全覆盖瓦特第i个钙钛矿过度层是至关重要的，以消除在空穴传输层（ 例如，螺OMETAD）和电子传输层（ 例如，介孔二氧化钛）23之间的潜在重组。我们示出，加入一价阳离子的卤化物（ 例如，碘化亚铜和碘化银）可提高钙钛矿覆盖层，这导致了装置的高开路电压的表面覆盖。 我们的方法的主要优点是掺杂步骤，在那里我们引入一价阳离子入CH 3 NH 3碘化铅3结构来提高电荷的密度，电荷传输，和吸收体层的导电性。正如上一节中所述，上述的掺杂剂显著增强两个电子和空穴迁移率。此外，显着降低在电荷输送活化能，以及在perovski的高能紊乱德膜，是由单价阳离子掺杂实现。 在这项工作中，我们已经证明掺杂CH 3 NH 3碘化铅3如在介观钙钛矿太阳能电池结构的吸收体层的方法。价阳离子的卤化物被用于调谐CH 3 NH 3碘化铅3钙钛矿薄膜的形态，光学，和电性能，以提高光电性能。因此，我们的CH 3的连续的两步沉积掺入三种不同的一价阳离子（即钠离子 ，铜+和Ag +），它们具有相似的离子半径的Pb 2+，在引入源的 NH 3碘化铅3 。其结果是，在CH 3 NH 3碘化铅3的结构和光电特性的显着的改善发生在这些添加剂的存在，导致对所制造的太阳能电池更高的PCE。因此，我们的工作喜ghlights掺杂CH 3 NH 3碘化铅3作为吸收层，它可以在钙钛矿太阳能电池（ 例如，平面结构）的所有其它构造，以进一步提高钙钛矿薄膜的电子质量被使用的便利途径。 本文的基本数据，请访问:https://www.repository.cam.ac.uk/handle/1810/260187。

目前，世界上能量需求（ 即，85％）的主要部分是由石油，煤和天然气的燃烧，这有助于全球变暖和对我们的环境1的有害作用提供。因此，能源的CO 2 -零排放能源的发展是至关重要的利益。光伏（PV）是一种理想的能量转换的过程，可以达到这个要求。然而，成本和效率，对于广泛采用光伏技术的主要障碍，必须提高。新兴基于新的材料，如钙钛矿太阳能电池（PSC）光伏技术，有降低成本和提高效率的组合。这是通过廉价的材料是容易得到的，以及通过快速，简便，低能量处理路由的利用率达到相比硅基同行2,34。一个显着的提高电源转换效率（PCE），从3.8％到超过22％，有报道以来光伏建筑5，6，7，8日首次亮相的混合有机-无机铅卤化物钙钛矿。这种卓越的性能从强的光吸收源自具有非常尖锐的能带边缘，在非常低的高能紊乱，弱束缚的激子，很容易离解成具有大的扩散长度自由载流子，以及杂化有机 - 无机的光子循环能力铅卤化物钙钛矿9，10，11，12。这些材料被归类在钙钛矿系列，它是由有机卤化物和金属卤化物盐结晶，形成在ABX 3结晶</sub&gt;结构，其中X是阴离子，A和B是不同尺寸的阳离子（A为大于B）。对于A网站报道阳离子包括甲基铵（MA），formamidinium（FA）和铯（Cs）;这些阳离子的组合示出了最高性能13,14。此外，在B位的二价阳离子的主要候选是铅，其可通过锡取代;带隙可以成功红移在混合钙钛矿15铅锡超过1000纳米。同样，在X站点乘员已被广泛研究，其中，碘（I）和溴（Br）之间的混合物被引入作为主要候选16,17。因此，它是非常合理的，通过改变它们的化学组成来操纵的钙钛矿的结构，形态和光电特性。 尽管增强CRYSTAlline质量和钙钛矿薄膜的宏观均匀性是实现高效的装置18的关键参数，边界的多晶结构域，原点并在钙钛矿吸收剂电子缺陷的作用，且电荷收集层中时的作用之间的冲击在钙钛矿太阳能电池损失过程尚未很好地理解。关于在钙钛矿结构的电子缺陷的性质，它已经报道了许多缺陷，如I或Pb空位的，导致状态是非常接近或状态中的导带和价带中的连续体中，这可能对光伏器件19的负电子的影响。此外，铅阳离子和在所述钙钛矿平面碘化物阴离子之间的强共价键合相互作用可能导致本征缺陷的存在（ 例如，下协调铅二聚体和三聚体我），这可能创造带边缘，该装置20的操作期间充当电荷复合中心内ë站点。 在这里，我们研究了掺杂CH 3的影响NH 3碘化铅钙钛矿与单价阳离子卤化物，包括钠 ，铜+和Ag +，降低价金属离子比铅离子 。因此，我们通过增加他们的基于卤化物的盐的用量合理（ 例如，碘化钠，溴化亚铜，崔和AGI）进入钙钛矿原料液把这些阳离子。这些阳离子具有类似于铅离子的离子半径，所以置换掺杂内的晶体是可能的。我们已经表明，这些阳离子的存在强烈影响既形态和钙钛矿层的覆盖。此外，这些阳离子（ 如，Na +和Ag +）会的存在已被证实通过X射线光电子能谱（XPS），以及一个significan在钙钛矿的费米能级T改变由Kelvin探针力显微镜（KPFM）进行测定。通过将这些阳离子成依次沉积钙钛矿的太阳能电池中，我们在PSC的发电效率达到的改善（15.6％比较14％）。因此，为提高太阳能电池结构的吸收体层（ 例如，钙钛矿）的结构和光电特性以最大化电荷输送和钝化表面的陷阱，以达到最高的光伏性能是十分必要的。

<table><tbody><tr><td>Fluorine doped Tin Oxide (FTO)-coated glass</td><td>Sigma-Aldrich&amp;nbsp;</td><td>735264-1EA</td><td>Resistivity&amp;asymp;13 &amp;Omega;/sq</td></tr><tr><td>Zinc powder</td><td>Sigma-Aldrich&amp;nbsp;</td><td>96454</td><td>Molecular Weight 65.39&amp;nbsp;</td></tr><tr><td>Hydrochloric acid&amp;nbsp;</td><td>Sigma-Aldrich&amp;nbsp;</td><td>84415</td><td>&amp;ge;37 wt. %</td></tr><tr><td>Hellmanex detergent&amp;nbsp;</td><td>Sigma-Aldrich&amp;nbsp;</td><td>Z805939-1EA</td><td>pkg of 1 L&amp;nbsp;</td></tr><tr><td>Titanium diisopropoxide bis(acetylacetonate)&amp;nbsp;</td><td>Sigma-Aldrich&amp;nbsp;</td><td>325252</td><td>75&amp;nbsp;wt. % in isopropanol</td></tr><tr><td>Titania Paste</td><td>DYESOL</td><td>MS002300</td><td>30 NR-D Transparent Titania Paste</td></tr><tr><td>Lead(II) iodide</td><td>Sigma-Aldrich</td><td>211168</td><td>99 wt. %</td></tr><tr><td>&lt;em&gt;N,N&lt;/em&gt;-Dimethylformamide&amp;nbsp;</td><td>Sigma-Aldrich&amp;nbsp;</td><td>437573</td><td>ACS reagent, &amp;ge;99.8%</td></tr><tr><td>Methylammonium iodide</td><td>DYESOL</td><td>MS101000</td><td>Powder&amp;nbsp;</td></tr><tr><td>SpiroMeOTAD</td><td>Sigma-Aldrich&amp;nbsp;</td><td>792071</td><td>99% (HPLC)</td></tr><tr><td>Bis(trifluoromethane)sulfonimide lithium salt</td><td>Sigma-Aldrich&amp;nbsp;</td><td>544094</td><td>99.95% trace metals basis&amp;nbsp;</td></tr><tr><td>4-&lt;em&gt;tert&lt;/em&gt;-Butylpyridine</td><td>Sigma-Aldrich&amp;nbsp;</td><td>142379</td><td>Purity: 96%</td></tr><tr><td>Chlorobenzene</td><td>Sigma-Aldrich</td><td>284513</td><td>anhydrous, 99.8%</td></tr><tr><td>2-Propanol (IPA)</td><td>Sigma-Aldrich&amp;nbsp;</td><td>278475</td><td>anhydrous, 99.5%&amp;nbsp;</td></tr><tr><td>Ethanol</td><td>Sigma-Aldrich</td><td>2860</td><td>absolute alcohol, without additive, &amp;ge;99.8%</td></tr></tbody></table>

monovalent cation doping of ch3nh3pbi3 for efficient perovskite solar cells

在这里，我们证明，为了调整光学，激子，和电性能的一价阳离子的添加剂掺入CH 3 NH 3碘化铅3钙钛矿。掺杂的可能性通过加入单价阳离子卤化物与类似的离子半径的Pb 2+，包含Cu +，Na +和银离子的影响。在费米能级的转变和子带隙光吸收的显着降低，与钙钛矿低级高能紊乱一起被实现。顺序的数量级的增强在本体空穴迁移率和基于添加剂的钙钛矿装置内的显著减少运输活化能的混合物实现。在这些阳离子的存在下在上述改进的性质的合流导致的钙钛矿太阳能电池的光电参数的增强。在碘化银开路电压和70 mV的增加2毫安/厘米2小鬼rovement在基于溴化亚铜，NaI-和太阳能电池的光电流密度均达到较原始设备。我们的工作铺平了在CH 3 NH 3碘化铅3钙钛矿和随后的器件的光电质量进一步改善的方式。它强调了对结晶掺杂杂质的作用，调查了新的途径，并控制在钙钛矿结构中的电子缺陷密度。

场发射扫描电子显微镜（FESEM）来记录所制造的钙钛矿太阳能电池的两个横截面图像（ 图1）和沉积的碘化铅和CH 3 NH 3碘化铅3薄膜的顶视图图像（ 图2）。 X射线衍射（XRD）和X射线光电子能谱（XPS）进行了表征钙钛矿薄膜的结构特性（ 图3和4）。光热偏转谱（PDS）和开尔文探针力显微镜（KPFM）分别用来探测钙钛矿薄膜，光学和电学性能（ 图5和6）。此外，基于空间电荷限制电流（SCLC）随温度的散装运输测量于钙钛矿设备（ 图7）进行的。最后，一个标准photovolta进行的制造的装置的集成电路的测量（ 图8和表1）。 基于该顶视图中的碘化铅和CH 3 NH 3碘化铅3沉积在图2所示的介孔TiO 2的层（MP-TiO 2的）上，被示出在钙钛矿形态的添加剂的作用，其中的SEM图像碘化铅的大枝形水晶基于乃样品中得以实现。这导致了钙钛矿的较大的非对称晶体的形成。此外，我们得到基于AGI-CuI-和样品的均匀和无针孔的钙钛矿封盖层（ 图2c和2e）。调查价阳离子的卤化物添加剂对CH 3 NH 3碘化铅3和碘化铅转化成CH 3 NH 3碘化铅的晶体结构的效果进行3，X射线衍射（ 图3）。虽然最终钙钛矿的晶体结构保持不变所有样品，显而易见的是，在2θ衍射峰= 12.6，其对应于未转化的碘化铅，在碘化钠和溴化亚铜添加剂的存在被淘汰了。为了确认对CH 3内的这些单价阳离子的存在的NH 3碘化铅3钙钛矿薄膜，我们进行了XPS分析， 如图4。对XPS数据的基础上，我们展示了钙钛矿薄膜内的Na和Ag离子的存在，而Cu的浓度无法估计，可能是由于碘（I 3P1 / 2）和铜的贴近（铜2P1 / 2）的峰。 示于图5a，其通过PDS测量了钙钛矿的吸收光谱的一价阳离子的添加剂的效果。显而易见的是，相对于原始样品的添加剂基于CH 3 NH 3碘化铅3有较低的子带隙的吸收。此外，观察到Cu基样本，其中来自卤化铜（ 图5b）的特性吸收的吸收尾巴。尽管吸收尾部证实铜阳离子在最终钙钛矿薄膜的存在，这是显而易见的，基于所述PDS之间的比较的CuI基于碘化铅2和CH 3 的 NH 3碘化铅3中 ，它们的掺入是不完整的。此外，Urbach能（铕），这是一种材料的充满活力的病症的程度的量度，估计为原始基础的AgI-NaI-，CuBr-，CuI-，和钙钛矿，和的值是15.6， 11.8，12.8，13.5，和15.2毫电子伏特，分别为（ 图5a的插图）。 为了探讨在ELECTR上述添加剂的影响CH 3 NH 3碘化铅3 ONIC结构，我们进行KPFM，其中测量线轮廓的接触电位差（CPD）。这对应于图6所示的钙钛矿的表面功函数（Φ）。在的CPD（ 即 0.1 V）的明确转变添加剂为基础的钙钛矿相对于原始的一所示的钙钛矿费米能级向价带移动。这种变化在钙钛矿的费米能级可以归因于任一取代对-掺杂（ 例如，更换铅2+与一价阳离子X +）或表面钝化在钙钛矿的晶体表面。 调查上的电荷的密度和在CH 3 NH 3其传输性碘化铅3掺杂的效果，我们进行了温度依赖散装运输测量（ 图7a </str翁&gt;）。然后，我们基于完整电子和基于添加剂空穴只有原始和钙钛矿设备的空间电荷限制电流（SCLC）所估计的散装载流子迁移（μSCL）。在导电性和在电子和空穴的迁移率都显着增加了实现的，特别是用于相对于原始的钙钛矿（ 表1）的碘化钠和溴化亚铜样品。值得注意的是，在电荷迁移率和电导率的改善是在短路电流（J SC）的增强一致和填图7b示出的装配式太阳能电池的因子（FF）。此外，我们估计用于电子和利用温度依赖性散装运输测量，其中，一个清晰的下降是基于添加剂的钙钛矿所取得的孔既电荷传输（E A）的活化能。这种改善是由于因为掺杂和填充个的载流子的高密度Ë运输陷阱，从而导致在运输屏障显著下跌。 我们制造根据上述的一价阳离子的卤化物，相应的合营曲线，并且总结在图8a和表1的光电参数的钙钛矿的太阳能电池。在开路电压的显著改善是两种CuI-（0.99 V）和AgI-基于由于提供了理想的表面覆盖的太阳能电池（1.02Ⅴ）（ 图2c和2e）来实现的。此外，被实现在短路电流（≈2毫安厘米-2）为CuBr-和基于碘化钠基太阳能电池的显着增加，这可以归因于碘化铅的完全转化成CH 3 NH 3碘化铅3。这种改善是通过在图8b中示出的入射光子-电流转换效率（IPCE）谱证实。最后，Higher电源转换效率（PCE）的15.2％，15.6％和15.3％水平为NaI-，CuBr-实现，基于翠设备，分别比较了原始的钙钛矿太阳能电池14.0％的价值。 <img alt="图1" src="/files/ftp_upload/55307/55307fig1.jpg" /> 图1:钙钛矿介观太阳能电池架构。具有以下结构的完整设备的SEM横截面显微照片:FTO /紧凑的 TiO 2 /孔-的TiO 2 / CH 3 NH 3碘化铅3 /螺OMeTAD / Au等。 <img alt="图2" src="/files/ftp_upload/55307/55307fig2.jpg" /> 图2:碘化铅钙钛矿结构的形态分析。 碘化铅（左侧）和CH 3 NH 3碘化铅3的顶视图的SEM图像（右侧）的结构:（1）原始，（ <st<html>荣&gt;二）CuBr-，（C）CuI-，（D）NaI-，和沉积在介孔TiO 2的（E）基于碘化银基钙钛矿样包被的FTO。这个数字已经从18引用转载。 <a href="http://ecsource.jove.com/files/ftp_upload/55307/55307fig2large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> <img alt="图3" src="/files/ftp_upload/55307/55307fig3.jpg" /> 图3:单价阳离子卤化物添加剂对钙钛矿结晶的影响。原始和添加剂基于CH 3的X射线衍射光谱的 NH 3碘化铅3钙钛矿是生长在介孔二氧化钛膜，其沉积在FTO涂覆玻璃。这个数字已经从18引用转载。T ="_空白"&gt;点击此处查看该图的放大版本。 <img alt="图4" src="/files/ftp_upload/55307/55307fig4.jpg" /> 图4:在CH 3 NH 3碘化铅3钙钛矿结构的一价阳离子的轨迹。质朴，基于AGI-CuBr-，CuI-，NaI-和钙钛矿薄膜XPS分析。这个数字已经从18引用转载。 <a href="http://ecsource.jove.com/files/ftp_upload/55307/55307fig4large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> <img alt="图5" src="/files/ftp_upload/55307/55307fig5.jpg" /> 图5:钙钛矿薄膜的光学性能。 （a）由原始和添加剂的铅来源钙钛矿薄膜的吸收光谱使用PDS技术测量。该插图示出所有样品相应的Urbach能量。误差棒是由SD在拟合Urbach末尾定义。 （ 二 ）的原始和基于溴化亚铜-碘化铅和钙钛矿薄膜，以及的CuBr的PDS吸收光谱的比较淀积在MS-TiO 2和加入CuBr-仅膜。这个数字已经从18引用转载。 <a href="http://ecsource.jove.com/files/ftp_upload/55307/55307fig5large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> <img alt="图6" src="/files/ftp_upload/55307/55307fig6.jpg" /> 图6:关于钙钛矿薄膜的表面电位的一价阳离子的添加剂的影响。使用KPFM原始和添加剂为基础的钙钛矿电影记录CPD线轮廓。 AFM的地形影像显示在顶部。这个数字已经从18引用转载<html> 。 <a href="http://ecsource.jove.com/files/ftp_upload/55307/55307fig6large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> <img alt="图7" src="/files/ftp_upload/55307/55307fig7.jpg" /> 图7:钙钛矿薄膜的电荷传输特性。 （a）仅空穴设备（ITO / PEDOT:PSS /钙钛矿/金）的合资公司特征，用于估计SCLC空穴迁移率利用。注意，电流密度（J），按比例与钙钛矿层的厚度。 （ 二 ）在J SC的趋势，μ 小时 ，μe表示原始和添加剂为基础的钙钛矿。这个数字已经从18引用转载。 <a href="http://ecsource.jove.com/files/ftp_upload/55307/55307fig7large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> T"FO:保together.within页="1"&gt; <img alt="图8" src="/files/ftp_upload/55307/55307fig8.jpg" /> 图8:光伏性能特性。 （ 一 ）为100毫瓦/厘米2的照射下的设备的电流-电压特性，获得使用不同类型添加到引线源溶液的一价阳离子的卤化物。 （ 二 ）事件光子-电流效率（IPCE）谱作为单色光的波长为原始基础的AgI-CuBr-，CuI-，NaI-，和钙钛矿的太阳能电池的功能。这个数字已经从18引用转载。 <a href="http://ecsource.jove.com/files/ftp_upload/55307/55307fig8large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> <table border="1" fo:keep-together.within-page="1" fo:keep-with-next.within-page="always"><tbody><tr><td> 样品类型 </td><td>ĴSC </td><td> 开路电压 </td><td> FF </td><td> PCE </td><td> Ëμ </td><td> μH＆ </td><td> êA E </td><td> êA h 对 </td></tr><tr><td></td><td> （毫安厘米-2） </td><td> （V）的 </td><td></td><td> （％） </td><td> （ 平方厘米/ VS） </td><td> （ 平方厘米/ VS） </td><td> （兆电子伏） </td><td> （兆电子伏） </td></tr><tr><td> 精粹 </td><td> 21.03 </td><td> 0.95 </td><td> 0.70 </td><td> 14.01 </td><td> 0.02 </td><td> 0.008 </td><td> 135 </td><td> 198 </td></tr><tr><td> 溴化亚铜 </td><td> 22.92 </td><td> 0.95 </td><td> 0.72 </td><td> 15.61 </td><td> 0.05 </td><tD&gt; 0.04 </td><td> 88 </td><td> 132 </td></tr><tr><td> 碘化亚铜 </td><td> 21.81 </td><td> 0.99 </td><td> 0.71 </td><td> 15.25 </td><td> 0.02 </td><td> 0.036 </td><td> 94 </td><td> 157 </td></tr><tr><td> 碘化钠 </td><td> 22.97 </td><td> 0.9 </td><td> 0.73 </td><td> 15.14 </td><td> 0.04 </td><td> 0.07 </td><td> 77 </td><td> 137 </td></tr><tr><td> 碘化银 </td><td> 19.24 </td><td> 1.02 </td><td> 0.72 </td><td> 14.18 </td><td> 0.005 </td><td> 0.006 </td><td> 105 </td><td> 177 </td></tr></tbody></table> 表1:PSC 的光伏和电荷传输参数。从JV测量和电荷迁移率与该显示最佳性能和原始和添加剂的基于钙钛矿太阳能电池的活化能衍生，沿着光电参数的总结分别˚F使用两步淀积法abricated。值得注意的是，光伏参数的统计遵循同样的趋势，表现最好的设备。此表已从参考18再现。

Watch this Scientific Journal Video about Monovalent Cation Doping of CH3NH3PbI3 for Efficient Perovskite Solar Cells at JoVE.com

Monovalent Cation Doping of CH3NH3PbI3 for Efficient Perovskite Solar Cells

在这里，我们提出了一个协议，以实现高效率的钙钛矿的太阳能电池以调节溶液处理的CH 3 NH 3碘化铅3的通过一价阳离子添加剂的掺入的属性。

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 ...

monovalent-cation-doping-ch3nh3pbi3-for-efficient-perovskite-solar

Universidad de Cartagena UDEC

Research

JoVE Journal

Engineering

Monovalent Cation Doping of CH3NH3PbI3 for Efficient Perovskite Solar Cells

16.5K 次观看.  University of Cambridge. 在这里，我们提出了一个协议，以实现高效率的钙钛矿的太阳能电池以调节溶液处理的CH 3 NH 3碘化铅3的通过一价阳离子添加剂的掺入的属性。 

视频: Monovalent Cation Doping of CH3NH3PbI3 for Efficient Perovskite Solar Cells

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 ...

科研

工程学

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

Hybrid organic/inorganic halide perovskites have lately been a topic of great interest in the field of solar cell applications, with the potential to achieve device efficiencies exceeding other thin film device technologies. Yet, large variations in device efficiency and basic physical properties are reported. This is due to unintentional variations during film processing, which have not been sufficiently investigated so far. We therefore conducted an extensive study of the morphology and electronic structure of a large number of CH3NH3PbI3 perovskite where we show how the preparation method as well as the mixing ratio of educts methylammonium iodide and lead(II) iodide impact properties like film formation, crystal structure, density of states, energy levels, and ultimately the solar cell performance.

We present an extensive study on the effects of different fabrication methods for organic/inorganic perovskite thin films by comparing crystal structures, density of states, energy levels, and ultimately the solar cell performance.

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 ...

化学

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, ...

Recombination Dynamics in Thin-film Photovoltaic Materials via Time-resolved Microwave Conductivity

A method for investigating recombination dynamics of photo-induced charge carriers in thin film semiconductors, specifically in photovoltaic materials such as organo-lead halide perovskites is presented. The perovskite film thickness and absorption coefficient are initially characterized by profilometry and UV-VIS absorption spectroscopy. Calibration of both laser power and cavity sensitivity is described in detail. A protocol for performing Flash-photolysis Time Resolved Microwave Conductivity (TRMC) experiments, a non-contact method of determining the conductivity of a material, is presented. A process for identifying the real and imaginary components of the complex conductivity by performing TRMC as a function of microwave frequency is given. Charge carrier dynamics are determined under different excitation regimes (including both power and wavelength). Techniques for distinguishing between direct and trap-mediated decay processes are presented and discussed. Results are modelled and interpreted with reference to a general kinetic model of photoinduced charge carriers in a semiconductor. The techniques described are applicable to a wide range of optoelectronic materials, including organic and inorganic photovoltaic materials, nanoparticles, and conducting/semiconducting thin films.

A Time Resolved Microwave Conductivity technique for investigating direct and trap-mediated recombination dynamics and determining carrier mobilities of thin film semiconductors is presented here.

通过时间分辨微波电导率重组动力学薄膜光伏材料

A method for investigating recombination dynamics of photo-induced charge carriers in thin film semiconductors, specifically in photovoltaic materials ...

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 ...

A Modular Microfluidic Technology for Systematic Studies of Colloidal Semiconductor Nanocrystals

Colloidal semiconductor nanocrystals, known as quantum dots (QDs), are a rapidly growing class of materials in commercial electronics, such as light emitting diodes (LEDs) and photovoltaics (PVs). Among this material group, inorganic/organic perovskites have demonstrated significant improvement and potential towards high-efficiency, low-cost PV fabrication due to their high charge carrier mobilities and lifetimes. Despite the opportunities for perovskite QDs in large-scale PV and LED applications, the lack of fundamental and comprehensive understanding of their growth pathways has inhibited their adaptation within continuous nanomanufacturing strategies. Traditional flask-based screening approaches are generally expensive, labor-intensive, and imprecise for effectively characterizing the broad parameter space and synthesis variety relevant to colloidal QD reactions. In this work, a fully autonomous microfluidic platform is developed to systematically study the large parameter space associated with the colloidal synthesis of nanocrystals in a continuous flow format. Through the application of a novel translating three-port flow cell and modular reactor extension units, the system may rapidly collect fluorescence and absorption spectra across reactor lengths ranging 3 - 196 cm. The adjustable reactor length not only decouples the residence time from the velocity-dependent mass transfer, it also substantially improves the sampling rates and chemical consumption due to the characterization of 40 unique spectra within a single equilibrated system. Sample rates may reach up to 30,000 unique spectra per day, and the conditions cover 4 orders of magnitude in residence times ranging 100 ms - 17 min. Further applications of this system would substantially improve the rate and precision of the material discovery and screening in future studies. Detailed within this report are the system materials and assembly protocols with a general description of the automated sampling software and offline data processing.

Detailed herein are the operation and assembly protocols of a modular microfluidic screening platform for the systematic characterization of colloidal semiconductor nanocrystal syntheses. Through fully adjustable system arrangements, highly efficient spectra collection may be carried out across 4 orders of magnitude reaction time scales within a mass transfer-controlled sampling space.

胶体半导体纳米晶系统研究的模块化微流控技术

Colloidal semiconductor nanocrystals, known as quantum dots (QDs), are a rapidly growing class of materials in commercial electronics, such as light ...

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.

CH的单价阳离子兴奋剂

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