The authors acknowledge the support of the Cambridge Overseas and Commonwealth Trust, the Rutherford Foundation of New Zealand, Girton College Cambridge. This work has been funded by ERC Advanced Investigator Grant, Novox, ERC-2009-adG247276 and by the EPSRC (under RGS3717).

1.氧化亚铜预处理。 <ol><li> 铜箔的氧化 <ol><li>切0.127毫米厚铜箔到13毫米×13平方毫米和清洁，丙酮超声处理。 </li><li>升温铜箔至1000℃，同时连续通过炉子流入Ar气。监测在整个氧化的气体分析器炉内的气体气氛。当达到1000℃的温度下，引入氧气到炉中，在一个流率以得到10,000ppm的氧气分压，并保持该至少2小时。 2小时后，关闭氧气，但保留氩气的流动。 </li><li>冷却炉至500℃（保持Ar气体流动）。通过从炉中的坩埚的迅速撤离淬灭氧化样品。浸基板去离子水中更快地冷却它们。 </li></ol></li><li> 铜2 O的蚀刻 <ol><li>通过反复施加蚀刻基片的一侧的稀硝酸滴（1:H 2 O和70％的HNO 3 1:1混合物），以从表面除去任何氧化铜。继续蚀刻直到没有灰膜是在Cu 2 O表面上是可见的。注意:此过程在一个通风柜进行。 </li><li>蚀刻后立即冲洗用去离子水各基板和异丙醇超声处理。干燥用空气枪。 </li><li>存款80纳米的黄金到铜2 O基板蚀刻的一侧通过蒸发1g的金颗粒置于钨舟的电阻蒸发器内部。使用基础压力8×10 -6毫巴和4所述的电流达到0.8埃/秒的蒸发速率。 </li><li>通过施加酸一滴到表面蚀刻在稀硝酸基板的另一侧。确保酸不蚀刻在另一侧的金膜。如第1.2.2描述冲洗，超声。 </li><li>封面用黑色绝缘漆底物（使用高温Ëngine搪瓷）使用油漆刷，留下大约为0.1 cm 2的作为太阳能电池的有源区的未掩蔽区域。覆盖上用记号笔完全背面的金电极。 </li></ol></li></ol> 2.存入锌1-X镁×○使用AP-SALD反应堆注意:存款锌1-X镁X在铜的一面暴露无遗2 O基板13在这项工作中，使用了定制的AP-SALD反应器，改编自柯达开发的原始设计O透明导电膜11,12详情在反应器的定制在参考文献中给出。 12。 <ol><li>设置对AP-SALD系统如下: <ol><li>使用二乙基锌（DEZ）作为锌前体和二（乙基环戊二烯基）镁作为镁前体。这些都是在各自的玻璃起泡每个包含液体前体。前体是自燃的，应该永远不会与空气或水接触。沉积系统是气密。 </li><li>氧化锌沉积，通过二乙基锌到25毫升/分钟，载在RT（20℃）调整氮气的鼓泡速率。锌氧化镁沉积，通过经由二乙基锌通过双（乙基环戊二烯基）镁（其被加热到55℃）6-毫升/分钟和200毫升/分钟设定鼓泡速率调整每个前体的气体馏分以控制到锌与Mg的比例在锌1-X镁点¯xO. </li><li>设置氮气载气的流速为金属前体混合物到100毫升/分钟。在通过去离子水，其中使用作为氧化剂为100ml /分钟气泡氮气。此蒸汽与氮气载气以200ml /分流动稀释。 </li><li>在500毫升/分钟到气体歧管流动氮气。在AP-SALD气体歧管，该氮气被分割至四个独立的通道。每个通道用于在空间上两个氧化剂通道从它们之间的金属前驱物混合通道中分离出来。 </li></o升&gt; </li><li>保持气体歧管在通过循环水的40℃的温度。升温阶段（移动压板），以期望的温度（50 - 150℃）。 </li><li>设置所需的样品与头部的距离，样本大小，压板速度（50毫米/秒），并振荡数（周期）与软件控制压板。该ZnO蒸镀速率为1.1纳米/秒（或每个周期）及锌1-X镁×○淀积速率是在150℃下大约0.54纳米/秒。沉积循环的典型数量是200。 </li><li>沉积在400振荡或直到一个明确的厚的均质薄膜可以看出载玻片所需的氧化物。 </li><li>放置在玻璃掩模基板，如果需要，然后将其放置在气歧管下。头部（气歧管）的高度调整至50μm的衬底的上方。 </li><li>存款锌1-X镁×○首先打开阀门的镁前体起泡，那么锌前体起泡片，然后开始MOVI通过点击在软件"开始沉积"纳克的气体歧管下压板上。只为了避免氧化亚铜表面接触而加热的氧化剂与金属前体5振荡扫描衬底之后打开轰2 O鼓泡器。 </li><li>当沉积完成时，从加热压板尽快除去所述Cu 2 O基板和关闭金属前体的起泡器阀门。清洗在歧管中的气体流路用刀片以除去任何沉积的氧化物粉末。如在2.6节开始下一个沉积周期。 </li><li>完成后，清洗系统30分钟关闭阀门氮之前。 </li></ol> 3. ITO溅射<ol><li>通过直流磁控管在下列条件下溅射20溅射氧化铟锡（ITO）的175纳米:功率20瓦，基础压力&lt;10 -9毫巴中，Ar压力为2.5帕在为35nm的溅射速率/分，溅射ITØ5分钟的175纳米厚的ITO膜。所得ITO /氧化锌/铜2 O异质结示于图3。 </li></ol> 4.整理设备的<ol><li>清洗从用丙酮金电极的标记笔，以暴露金电极。 </li><li>通过坚持2 Ag膏细线到ITO和Au电极应用电子触点。 </li></ol>

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The authors declare that they have no competing financial interests.

该协议中的关键步骤是由铜2 O与CuO基材表面氧化的规定。这些包括在稀硝酸衬底蚀刻氧化之后以及金电极的蒸发后，以除去任何的CuO，最小化时基板在露天耗费锌1-X镁×○沉积之前，最后的沉积锌1-X镁×○对Cu 2 O基板由AP-SALD。 相比于常规的ALD AP-SALD的优点是膜可以与生长速率是幅度较高的一个到两个数量真空外生长。然而，这意味着，在Cu 2 O底物具有在温度至少刚刚沉积，这足以对一个薄的CuO层形成在表面上之前，升高被暴露于氧化剂中的空气。这看似限制对AP-SALD方法的某些氧化敏感本草应用LS。然而，通过优化的AP-SALD条件如温度和时间，以及减少的Cu 2 O暴露于空气和水分，用AP-SALD以ZnO /铜2 O设备的转换效率的六倍制成达到。改善来自于理解的Cu 2 O与CuO氧化为氧化铜作为异质结太阳能电池的材料，并相应地修改制造协议的主要限制因素。 为了完全避免氧化亚铜的氧化，基板必须保持在惰性气氛或真空中所有的时间，采用露天沉积技术如AP-SALD时它可以是具有挑战性的。而避免在基于真空的技术3,18，用于大规模生产的Cu 2 O的氧化，它是重要的，这个问题可以在大气制造工艺被最小化。在AP-SALD，衬底表面可以暴露于还原剂之前异质的形成，并通过由n型氧化物的沉积过程中使用成型气体与CuO的还原平衡的Cu 2 O的氧化。25还原剂在AP-SALD使用可能是一个与还原气体（ 例如，N 2 + 5％的H 2 25），或一个周期数与之前沉积的还原前体， 即，不含水的循环，以减少的CuO回的惰性气体的混合物铜2 O之前的氧化锌氧化物开始在其表面上生长。 在这项工作中，一个标准的协议已经开发出来，最大限度地减少形成氧化铜由AP-SALD露天优化制造步骤从铜2 O处理和蚀刻PN结的形成。这项工作的成功表明AP-SALD的作为在廉价和可扩展的光电器件应用一种很有前途的方法的潜力。可用于快速depos的技术的各种n型和p型半导体金属氧化物的银行足球比赛以及阻断，缓冲液和在热敏基材包括塑料太阳能电池的阻挡层。

氧化亚铜（铜2 O）是一个地球丰富无毒p型半导体材料1。与2电子伏特的带隙，氧化亚铜可以实现光吸收剂在异质结或串联型太阳能电池的作用。在异质结太阳能电池，铜2 O已知与多种n型大的带隙的半导体，例如ZnO 2和其掺杂变体3,4， 的 Ga 2 O 3 5,6和TiO 2 7配对（对于更对Cu 2 O光伏详细概述见参考文献8）。的Cu 2 O的异质结太阳能电池的开发是示于图1，其中，靠近每个数据点被指示合成该异质结的方法。可以注意的是基于真空的方法，如脉冲激光沉积（PLD）或允许更高的功率转换效率的原子层沉积（ALD）来实现（高达6.1％9）。在合作ntrast，对于非真空合成方法如电化学沉积（ECD）的效率仍然很低。然而，对于低成本光伏最好是合成的真空外异质结。而异质结形成一个自由真空，可扩展的技术是更合适的选择，它仍然具有挑战性由这种方法生产的高品质的接口。在这项工作中，我们利用一个露天，称为大气压力的空间的原子层沉积（AP-SALD）可伸缩的薄膜沉积工艺生长的n型氧化物对Cu 2 O类太阳能电池。 AP-SALD比传统的ALD的进步是，在前者中，前体在空间，而不是在时间10分离。在沉积过程中，衬底振荡上来回含有由惰性气体通道分开，前体气体通道， 如图2中的气体歧管下一个加热压板。携带precurs氮气ORS通过气体歧管向下朝横向移动压板垂直流动。由于压板的振荡，在基片上的每个点被顺序地暴露于氧化剂和金属前体，如在图2中示出。这使得金属氧化物膜由层成长层。 AP-SALD反应器的设计和操作的详细说明，可以在其他地方被发现。11,12这种方法允许沉积比传统的ALD和外部真空，这与卷对卷工艺兼容更快的发生数量级一到两个数量。通过AP-SALD生产高质量保形氧化物膜可以在低温下在各种基底上，包括塑料，这使得AP-SALD薄膜被应用到低成本功能器件如太阳能电池13被沉积（&lt;150℃） ，发光二极管14和薄膜晶体管15。 该定制的AP-SALD气歧管在这项工作中使用的是机械性地保持放置在原稿台上的基片上。这使得基板 - 歧管间距独立于气体流量的控​​制。为50微米的大的间隔被使用，这导致在气相中的金属前体与氧化剂之间的混合。因此，AP-SALD反应器中的化学汽相沉积（CVD）模式下操作。这被认为是超过在ALD模式操作有利的，因为膜在更高的速率高的厚度均匀性增加，但仍和当在相同的温度下ALD薄膜沉积是结晶的。12在这里，我们仍然参阅反应器中作为的AP-SALD反应器，因为它具有相同的基本设计原理的其它的AP-SALD反应器。11 我们使用我们的反应器中，为我们的太阳能电池沉积在n型层，特别是氧化锌和氧化锌镁（锌1-X镁×○16,17）。结合镁INTÒ的ZnO允许待调整的导带，这是用于减少由于带尾热化13和界面重组损失重要的。18,19 这里，我们显示如何调整为要获得关于允许改进的界面质量的热氧化的氧化亚铜衬底并因此更好的太阳能电池的性能上沉积的氧化锌和锌镁氧化物膜的条件。重组在异质结界面由于氧化亚铜表面上形成的过度氧化铜（CuO的）的:这个改善是通过铜2 O基础的太阳能电池识别的主要限制因素成为可能。

<table><tbody><tr><td>Copper foil</td><td>Avocado Research Chemicals LTD T/A Alfa Aesar</td><td>13380</td><td>0.127 mm thick, 99.9% (metals basis), annealed</td></tr><tr><td>Rapidox Oxygen analyzer</td><td>Rapidox</td><td>Model 2100</td><td></td></tr><tr><td>Alumina boat</td><td>Almath Crucibles LTD</td><td>6121203</td><td>Dimensions 20 mm x 50&amp;nbsp;mm x 5&amp;nbsp;mm</td></tr><tr><td>Gold pellets</td><td>KJLC</td><td>EVMAUXX40G</td><td>99.99% pure, 1/8&quot; x 1/8&quot;, sold by the gram</td></tr><tr><td>Diethylzinc</td><td>Aldrich</td><td>256781</td><td>&amp;ge;52 wt. % Zn basis</td></tr><tr><td>Bis(ethylcyclopentadienyl)magnesium</td><td>Strem Chemicals UK</td><td>12-0510</td><td>5 g</td></tr><tr><td>ITO target</td><td>GoodFellow Cambridge Limited</td><td>LS 427438</td><td>Indium Oxide/Tin Oxide target (In&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;3&lt;/sub&gt; 90 / SnO&lt;sub&gt;2&lt;/sub&gt; 10). Condition: Hot-pressed. Thickness: 2.0&amp;nbsp;mm &amp;#177; 0.5&amp;nbsp;mm. Size: 35.5&amp;nbsp;mm x 55.5&amp;nbsp;mm &amp;#177; 0.5&amp;nbsp;mm</td></tr><tr><td>VHT engine enamel paint</td><td>Halfords</td><td>325019</td><td>very high temperature engine enamel black paint</td></tr><tr><td>Nitric acid HNO&lt;sub&gt;3, &lt;/sub&gt;ACS reagent 70%&amp;nbsp;</td><td>Sigma-Aldrich Co Ltd</td><td>438073-2.5L</td><td>Harmful, irritant</td></tr><tr><td>2% Oxygen/Argon 200 bar</td><td>BOC Limited</td><td>225757-L</td><td>gas mixture for Cu foil oxidation, to be diluted with Ar</td></tr></tbody></table>

improved heterojunction quality in cu2o-based solar cells through the optimization of atmospheric pressure spatial atomic layer deposited zn1-xmgxo

Atmospheric pressure spatial atomic layer deposition (AP-SALD) was used to deposit n-type ZnO and Zn1-xMgxO thin films onto p-type thermally oxidized Cu2O substrates outside vacuum at low temperature. The performance of photovoltaic devices featuring atmospherically fabricated ZnO/Cu2O heterojunction was dependent on the conditions of AP-SALD film deposition, namely, the substrate temperature and deposition time, as well as on the Cu2O substrate exposure to oxidizing agents prior to and during the ZnO deposition. Superficial Cu2O to CuO oxidation was identified as a limiting factor to heterojunction quality due to recombination at the ZnO/Cu2O interface. Optimization of AP-SALD conditions as well as keeping Cu2O away from air and moisture in order to minimize Cu2O surface oxidation led to improved device performance. A three-fold increase in the open-circuit voltage (up to 0.65 V) and a two-fold increase in the short-circuit current density produced solar cells with a record 2.2% power conversion efficiency (PCE). This PCE is the highest reported for a Zn1-xMgxO/Cu2O heterojunction formed outside vacuum, which highlights atmospheric pressure spatial ALD as a promising technique for inexpensive and scalable fabrication of Cu2O-based photovoltaics.

热力学，氧化铜是在RT在空气中氧化铜的唯一稳定的阶段，由于在Cu-O系的相稳定性图揭示21 - 23。为了验证CuO的存在的Cu 2 O的蚀刻的吸收光谱的表面上和未腐蚀热氧化铜2 O基材采取光热偏转谱（PDS） -一个高度敏感的技术，它允许用于子带隙吸收测量24（ 图4）。两个谱表明吸收上述1.4电子伏特，这与CuO的带隙重合，在2电子伏特（ 氧化亚铜带隙）饱和之前。未蚀刻衬底具有低于2电子伏特一个较高的吸收，未腐蚀的Cu 2 O比蚀刻基板上的表面上暗示CuO的较厚的层。 图4中的插图显示CuO的作为氧化（未蚀刻）的Cu 2 O基板上的灰层。而无灰膜可以直​​观地蚀刻基板上被检测到，一些氧化铜仍存在其表面上，作为PDS测量表明。的非常薄的氧化铜薄膜的铜2 O基板的表面上存在还证实用X射线光电子能谱（XPS）19,25。本在Cu 2 O的表面上的氧化铜在异质结界面，可以作为复合中心，因此，氧化铜存在下，在pn结是不希望的引入深能级陷阱态（铜离子 ）18。 加热的Cu 2 O底物中的氧化剂（ 例如 ，空气和水分）的存在有利于的Cu 2 O和CuO的氧化。为了通过AP-SALD以获得多晶氧化锌，基片被加热到150℃。当衬底在升高的温度在露天或氧化剂气体下的沉积期间保持，CuO的迅速形成在Cu <suB&gt; 2 O的表面上。 图5显示了之前和在150℃的氮气的气流下在AP-SALD压板花费3分钟后扫描的蚀刻铜2 O基片的电子显微镜（SEM）图像。多个的CuO副产物可以看出退火基板上，与他们的组合物是接近的CuO如通过能量色散X射线光谱（EDX）验证。 光电器件，用在150℃下由AP-SALD沉积为400秒的蚀刻热氧化铜2 O基板的顶部的ZnO制成。 图6A示出该标准设备的表面上。可以注意到许多棒状和花状的副产物存在于设备。如先前使用EDX和PDS证实，这些副产物是氧化铜和发生由于铜2 O暴露于空气和氧化剂。 表1和图7（&#39;的ZnO /铜2 O标准&#39;Curve）证明该设备的性能相对较差。 为了避免在Cu 2 O的表面上的CuO的形成，用于通过在蚀刻热氧化铜2 O底物AP-SALD沉积的ZnO的条件进行了优化。采取了以下措施，以最小化的CuO生长:还原沉积温度（ 图8A）;减少的沉积时间（ 图8B）;扫描衬底表面的几个振荡不暴露于氧化剂气体， 即只用金属前体和惰性通道开放（ 图8C）;最后，在空气中裸铜2 O基板的不必要的加热避免刚沉积的开始之前。发现在Cu 2 O ZnO蒸镀的最优参数为100℃，100秒和5不含水的循环。优化的装置的表面是自由的CuO outgrowt的HS，如展示于图6B。优化的ZnO /铜2 O装置的电流密度-电压（JV）特性与图7中的标准设备进行比较。这两个标准和优化的ZnO /铜2 O设备的光伏性能在表1中提出，它可以可以看出，由以下四个上述措施，在器件的功率转换效率的六倍达到了。 为了进一步阐明的AP-SALD条件的优化对CuO的还原和异质结质量的影响，外部量子效率（EQE）测量在沉积在150℃和100℃（ 图9）与氧化锌设备执行。两个设备的EQE谱，而在高于475纳米的波长相近，在波长显著差异低于475纳米，这是波长的范围<html>小号吸收附近的接口。对于较短波长辐射，使用ZnO器件在更高的温度下进行的EQE为小于一半，与氧化锌器件在较低温度下进行的。这表明，更多的氧化铜存在于在较高温度下进行的氧化锌/铜2 O接口，从而减少了电荷收集从接近异质由于增加重组的区域。 毫克被并入的AP-SALD ZnO薄膜为了提高氧化锌的导带和以减少重组进一步15。锌1-X镁×○/铜2 O太阳能电池用优化锌0.8镁0.2 O薄膜制成，造成2.2％的设备PCE -基于O型最高迄今为止对Cu 2太阳能电池的露天制作异质结（参见图7和表1中的设备的性能）。 内容"FO:保together.within页="1"&gt; <img alt="图1" src="/files/ftp_upload/53501/53501fig1.jpg" /> 图1 的Cu 2-O基太阳电池出版年份效率（该图已被从价修饰8）。标记表明是否在真空或大气（非真空）形成界面和标签指示的方法异质结的形成。 MSP -磁控溅射，IBS -离子束溅射，VAPE -真空电弧等离子体蒸发。 <a href="https://www.jove.com/files/ftp_upload/53501/53501fig1large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> <img alt="图2" src="/files/ftp_upload/53501/53501fig2.jpg" /> 图2 AP-SALD沉积工艺的示意图（与常规的ALD相比），设置用于产生多组分金属牛集成开发环境（ 一 ）传统ALD（Δ-掺杂）各前体和净化步骤的顺序曝光（这个数字已经从文献再现。11）。在本手稿的上下文中，M1为二乙基锌蒸气，M2双（乙基环戊二烯基）镁蒸气，并O1和O2的水蒸汽。 （B）的在AP-SALD金属前体的混合物（共注入），惰性气体通道（等同于"吹洗"工序）和氧化剂顺序曝光（该图已被从参考再现11）。 （C）的一般AP-SALD反应器，示出了由惰性气体通道空间分离的前体，与振荡的不同信道下方的衬底的示意图（此图是从参考文献11，这是从一个在参考文献的变形再现。 26）。 （D）与原子力显微镜的AP-SALD体系的重要组成部分的原理概述（AFM）图像显示的形态基板前后锌1-X镁×○沉积（这个数字已经从文献再现。13）。 <a href="https://www.jove.com/files/ftp_upload/53501/53501fig2large.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/53501/53501fig3.jpg" /> 铜2 O与ZnO和ITO薄膜基板可观察到的ITO的图3.截面SEM图像/氧化锌/铜2 O异质结（这个数字已经从8参考转载）。保形涂料。 <a href="https://www.jove.com/files/ftp_upload/53501/53501fig3large.jpg" target="_blank">请点击这里查看一个更大的版本这个数字。</a> <img alt="图4" src="/files/ftp_upload/53501/53501fig4.jpg" /> 图4. PDS蚀刻和未腐蚀（如-OXI的光谱<html> dized）的Cu 2 O基板（这个数字已经从参考修改。8）。该插图显示蚀刻和未蚀刻氧化亚铜基板的照片。 <a href="https://www.jove.com/files/ftp_upload/53501/53501fig4large.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/53501/53501fig5.jpg" /> 图5.为3分钟新鲜蚀刻退火后，在150℃的空气中的Cu 2 O基板时（A）和（B）的表面的SEM图像（该图已被从参考再现8）。插图显示面与EDX获取的构图。 <a href="https://www.jove.com/files/ftp_upload/53501/53501fig5large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> <html> 501 / 53501fig6.jpg"/&gt; 图6.氧化锌/铜2 O太阳能电池的使用（A）的标准条件和（B）的AP-SALD的ZnO优化条件下（此图是从参考再现。8）方面的表面的SEM图像，各种副产物可在标准的设备看到。 <a href="https://www.jove.com/files/ftp_upload/53501/53501fig6large.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/53501/53501fig7.jpg" /> 图7.光JV特性锌1-X镁×○/铜2 O的标准和优化的AP-SALD条件（这个数字已经从参考修改。8）。该合资公司的曲线展示太阳能电池性能的改善，当制造太阳能电池锌的组合物和AP-SALD条件1-X镁×○膜被优化。小号://www.jove.com/files/ftp_upload/53501/53501fig7large.jpg"目标="_空白"&gt;点击此处查看该图的放大版本。 <img alt="图8" src="/files/ftp_upload/53501/53501fig8.jpg" /> 图8的AP-SALD参数对ZnO /铜2 O太阳能电池的性能的影响。水的（A）和（B）的AP-SALD ZnO蒸镀时间和温度上的装置的开路电压（V OC）的影响（该图已被从参考再现。8），（C）的相关与器件的开路电压空闲周期。 <a href="https://www.jove.com/files/ftp_upload/53501/53501fig8large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> <img alt="图9" src="/files/ftp_upload/53501/53501fig9.jpg" /> 图9. EQE SPECTR的ZnO /铜2 O太阳能电池的ZnO沉积在100℃和150℃。 （这个数字已经从文献转载8）。该器件的开路电压在图例中表示。 <a href="https://www.jove.com/files/ftp_upload/53501/53501fig9large.jpg" target="_blank">请点击此处查看该图的放大版本。</a> <table fo:keep-together.within-page="1"><tbody><tr><td> 太阳能电池 </td><td> 沉积温度，℃， </td><td> 沉积时间，秒 </td><td> ĴSC， 毫安 /平方厘米 </td><td> 开路电压，V </td><td> FF，％ </td><td> PCE，％ </td></tr><tr><td>氧化锌/铜2 O标准</td><td> 150 </td><td> 400 </td><td> 3.7 </td><td> 0.18 </td><td> 35 </td><td> 0.23 </td></tr><tr><td>氧化锌/铜2 O优化</td><td> 100 </td><td> 100 &lt;/ TD&gt; <td> 7.5 </td><td> 0.49 </td><td> 40 </td><td> 1.46 </td></tr><tr><td>锌镁0.8 0.2 /铜2 O优化</td><td> 150 </td><td> 100 </td><td> 6.9 </td><td> 0.65 </td><td> 49 </td><td> 2.20 </td></tr></tbody></table> 表1. 标准和优化的AP-SALD锌 1-X 镁 ×○沉积参数和最佳相应的ITO的性能/锌 1-X 镁 ×○/铜 2 O太阳能电池（该表已被修改的参考8） 。ĴSC -短路电流密度，FF -填充因子。

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Improved Heterojunction Quality in Cu2O-based Solar Cells Through the Optimization of Atmospheric Pressure Spatial Atomic Layer Deposited Zn1-xMgxO

在这里，我们提出了一个协议，用于合成锌1-X镁×○/铜2 O异质结在露天时，透过大气压力的空间原子层沉积（AP-SALD）锌1-X镁×○对氧化亚铜的低温。这样的高品质的共形金属氧化物可以在各种基材上，包括由这种廉价和可扩展的方法塑料的生长。

在铜改善异质结质量<sub&gt; 2</sub&gt; O型的太阳能电池通过大气压力的空间原子层沉积的优化<br /&gt;锌<sub&gt; 1-X</sub&gt;镁<sub系列&gt; X</sub&gt; 0

Atmospheric pressure spatial atomic layer deposition (AP-SALD) was used to deposit n-type ZnO and Zn1-xMgxO thin films onto p-type thermally oxidized Cu2O ...

improved-heterojunction-quality-cu2o-based-solar-cells-through

Research

JoVE Journal

Chemistry

Improved Heterojunction Quality in Cu2O-based Solar Cells Through the Optimization of Atmospheric Pressure Spatial Atomic Layer Deposited Zn1-xMgxO

12.1K 次观看.  University of Cambridge. 在这里，我们提出了一个协议，用于合成锌1-X镁×○/铜2 O异质结在露天时，透过大气压力的空间原子层沉积（AP-SALD）锌1-X镁×○对氧化亚铜的低温。这样的高品质的共形金属氧化物可以在各种基材上，包括由这种廉价和可扩展的方法塑料的生长。 

视频: Improved Heterojunction Quality in Cu2O-based Solar Cells Through the Optimization of Atmospheric Pressure Spatial Atomic Layer Deposited Zn1-xMgxO

Harvesting Solar Energy by Means of Charge-Separating Nanocrystals and Their Solids

Conjoining different semiconductor materials in a single nano-composite provides synthetic means for the development of novel optoelectronic materials offering a superior control over the spatial distribution of charge carriers across material interfaces. As this study demonstrates, a combination of donor-acceptor nanocrystal (NC) domains in a single nanoparticle can lead to the realization of efficient photocatalytic1-5 materials, while a layered assembly of donor- and acceptor-like nanocrystals films gives rise to photovoltaic materials.
Initially the paper focuses on the synthesis of composite inorganic nanocrystals, comprising linearly stacked ZnSe, CdS, and Pt domains, which jointly promote photoinduced charge separation. These structures are used in aqueous solutions for the photocatalysis of water under solar radiation, resulting in the production of H2 gas. To enhance the photoinduced separation of charges, a nanorod morphology with a linear gradient originating from an intrinsic electric field is used5. The inter-domain energetics are then optimized to drive photogenerated electrons toward the Pt catalytic site while expelling the holes to the surface of ZnSe domains for sacrificial regeneration (via methanol). Here we show that the only efficient way to produce hydrogen is to use electron-donating ligands to passivate the surface states by tuning the energy level alignment at the semiconductor-ligand interface. Stable and efficient reduction of water is allowed by these ligands due to the fact that they fill vacancies in the valence band of the semiconductor domain, preventing energetic holes from degrading it. Specifically, we show that the energy of the hole is transferred to the ligand moiety, leaving the semiconductor domain functional. This enables us to return the entire nanocrystal-ligand system to a functional state, when the ligands are degraded, by simply adding fresh ligands to the system4.
To promote a photovoltaic charge separation, we use a composite two-layer solid of PbS and TiO2 films. In this configuration, photoinduced electrons are injected into TiO2 and are subsequently picked up by an FTO electrode, while holes are channeled to a Au electrode via PbS layer6. To develop the latter we introduce a Semiconductor Matrix Encapsulated Nanocrystal Arrays (SMENA) strategy, which allows bonding PbS NCs into the surrounding matrix of CdS semiconductor. As a result, fabricated solids exhibit excellent thermal stability, attributed to the heteroepitaxial structure of nanocrystal-matrix interfaces, and show compelling light-harvesting performance in prototype solar cells7.

A general strategy for the development of charge-separating semiconductor nanocrystal composites deployable for solar energy production is presented. We show that assembly of donor-acceptor nanocrystal domains in a single nanoparticle geometry gives rise to a photocatalytic function, while bulk-heterojunctions of donor-acceptor nanocrystal films can be used for photovoltaic energy conversion.

通过电荷分离纳米晶及其固体收获太阳能

Conjoining different semiconductor materials in a single nano-composite provides synthetic means for the development of novel optoelectronic materials ...

科研

工程学

Making Record-efficiency SnS Solar Cells by Thermal Evaporation and Atomic Layer Deposition

Tin sulfide (SnS) is a candidate absorber material for Earth-abundant, non-toxic solar cells. SnS offers easy phase control and rapid growth by congruent thermal evaporation, and it absorbs visible light strongly. However, for a long time the record power conversion efficiency of SnS solar cells remained below 2%. Recently we demonstrated new certified record efficiencies of 4.36% using SnS deposited by atomic layer deposition, and 3.88% using thermal evaporation. Here the fabrication procedure for these record solar cells is described, and the statistical distribution of the fabrication process is reported. The standard deviation of efficiency measured on a single substrate is typically over 0.5%. All steps including substrate selection and cleaning, Mo sputtering for the rear contact (cathode), SnS deposition, annealing, surface passivation, Zn(O,S) buffer layer selection and deposition, transparent conductor (anode) deposition, and metallization are described. On each substrate we fabricate 11 individual devices, each with active area 0.25 cm2. Further, a system for high throughput measurements of current-voltage curves under simulated solar light, and external quantum efficiency measurement with variable light bias is described. With this system we are able to measure full data sets on all 11 devices in an automated manner and in minimal time. These results illustrate the value of studying large sample sets, rather than focusing narrowly on the highest performing devices. Large data sets help us to distinguish and remedy individual loss mechanisms affecting our devices.

Tin sulfide (SnS) is a candidate material for Earth-abundant, non-toxic solar cells. Here, we demonstrate the fabrication procedure of the SnS solar cells employing atomic layer deposition, which yields 4.36% certified power conversion efficiency, and thermal evaporation which yields 3.88%.

通过热蒸发和原子层沉积使记录效率的SnS太阳能电池

Tin sulfide (SnS) is a candidate absorber material for Earth-abundant, non-toxic solar cells. SnS offers easy phase control and rapid growth by congruent ...

Synthesis and Characterization of High c-axis ZnO Thin Film by Plasma Enhanced Chemical Vapor Deposition System and its UV Photodetector Application

In this study, zinc oxide (ZnO) thin films with high c-axis (0002) preferential orientation have been successfully and effectively synthesized onto silicon (Si) substrates via different synthesized temperatures by using plasma enhanced chemical vapor deposition (PECVD) system. The effects of different synthesized temperatures on the crystal structure, surface morphologies and optical properties have been investigated. The X-ray diffraction (XRD) patterns indicated that the intensity of (0002) diffraction peak became stronger with increasing synthesized temperature until 400 oC. The diffraction intensity of (0002) peak gradually became weaker accompanying with appearance of (10-10) diffraction peak as the synthesized temperature up to excess of 400 oC. The RT photoluminescence (PL) spectra exhibited a strong near-band-edge (NBE) emission observed at around 375 nm and a negligible deep-level (DL) emission located at around 575 nm under high c-axis ZnO thin films. Field emission scanning electron microscopy (FE-SEM) images revealed the homogeneous surface and with small grain size distribution. The ZnO thin films have also been synthesized onto glass substrates under the same parameters for measuring the transmittance.
For the purpose of ultraviolet (UV) photodetector application, the interdigitated platinum (Pt) thin film (thickness ~100 nm) fabricated via conventional optical lithography process and radio frequency (RF) magnetron sputtering. In order to reach Ohmic contact, the device was annealed in argon circumstances at 450 oC by rapid thermal annealing (RTA) system for 10 min. After the systematic measurements, the current-voltage (I-V) curve of photo and dark current and time-dependent photocurrent response results exhibited a good responsivity and reliability, indicating that the high c-axis ZnO thin film is a suitable sensing layer for UV photodetector application.

We offered a method to directly synthesize high c-axis (0002) ZnO thin film by plasma enhanced chemical vapor deposition. The as-synthesized ZnO thin film combined with Pt interdigitated electrode was used as sensing layer for ultraviolet photodetector, showing a high performance through a combination of its good responsivity and reliability.

合成和高c轴ZnO薄膜等离子体的特性增强化学气相沉积系统及其紫外探测器的应用

In this study, zinc oxide (ZnO) thin films with high c-axis (0002) preferential orientation have been successfully and effectively synthesized onto ...

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

In Situ Monitoring of the Accelerated Performance Degradation of Solar Cells and Modules: A Case Study for Cu(In,Ga)Se2 Solar Cells

The levelized cost of electricity (LCOE) of photovoltaic (PV) systems is determined by, among other factors, the PV module reliability. Better prediction of degradation mechanisms and prevention of module field failure can consequently decrease investment risks as well as increase the electricity yield. An improved knowledge level can for these reasons significantly decrease the total costs of PV electricity. 
In order to better understand and minimize the degradation of PV modules, the occurring degradation mechanisms and conditions should be identified. This should preferably happen under combined stresses, since modules in the field are also simultaneously exposed to multiple stress factors. Therefore, two 'Combined Stress test with in situ measurement' setups have been designed and constructed. These setups allow the simultaneous use of humidity, temperature, illumination, and electrical biases as independently controlled stress factors on solar cells and minimodules. The setups also allow real-time monitoring of the electrical properties of these samples. This protocol presents these setups and describes the experimental possibilities. Moreover, results obtained with these setups are also presented: various examples about the influence of both deposition and degradation conditions on the stability of thin film Cu(In,Ga)Se2 (CIGS) as well as Cu2ZnSnSe4 (CZTS) solar cells are described. Results on the temperature dependency of CIGS solar cells are also presented.

In Situ Monitoring of the Accelerated Performance Degradation of Solar Cells and Modules: A Case Study for CuIn,GaSe2 Solar Cells

Two &#39;Combined Stress test with in situ measurement&#39; setups, which allow real-time monitoring of accelerated degradation of solar cells and modules, were designed and constructed. These setups allow the simultaneous use of humidity, temperature, electrical biases, and illumination as independently controlled stress factors. The setups and various experiments executed are presented.

就地太阳能电池和模块加速性能退化的监测: 铜 (in, Ga) Se2太阳能电池的实例研究

The levelized cost of electricity (LCOE) of photovoltaic (PV) systems is determined by, among other factors, the PV module reliability. Better prediction ...

Well-aligned Vertically Oriented ZnO Nanorod Arrays and their Application in Inverted Small Molecule Solar Cells

This manuscript describes how to design and fabricate efficient inverted solar cells, which are based on a two-dimensional conjugated small molecule (SMPV1) and [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM), by utilizing ZnO nanorods (NRs) grown on a high quality Al-doped ZnO (AZO) seed layer. The inverted SMPV1:PC71BM solar cells with ZnO NRs that grew on both a sputtered and sol-gel processed AZO seed layer are fabricated. Compared with the AZO thin film prepared by the sol-gel method, the sputtered AZO thin film exhibits better crystallization and lower surface roughness, according to X-ray diffraction (XRD) and atomic force microscope (AFM) measurements. The orientation of the ZnO NRs grown on a sputtered AZO seed layer shows better vertical alignment, which is beneficial for the deposition of the subsequent active layer, forming better surface morphologies. Generally, the surface morphology of the active layer mainly dominates the fill factor (FF) of the devices. Consequently, the well-aligned ZnO NRs can be used to improve the carrier collection of the active layer and to increase the FF of the solar cells. Moreover, as an anti-reflection structure, it can also be utilized to enhance the light harvesting of the absorption layer, with the power conversion efficiency (PCE) of solar cells reaching 6.01%, higher than the sol-gel based solar cells with an efficiency of 4.74%.

This manuscript describes how to design and fabricate efficient inverted SMPV1:PC71BM solar cells with ZnO nanorods (NRs) grown on a high quality Al-doped ZnO (AZO) seed layer. The well-aligned vertically oriented ZnO NRs exhibit high crystalline properties. The power conversion efficiency of solar cells can reach 6.01%.

定向定向 ZnO 纳米阵列及其在倒小分子太阳电池中的应用

This manuscript describes how to design and fabricate efficient inverted solar cells, which are based on a two-dimensional conjugated small molecule ...

Fabrication of Schottky Diodes on Zn-polar BeMgZnO/ZnO Heterostructure Grown by Plasma-assisted Molecular Beam Epitaxy

Heterostructure field effect transistors (HFETs) utilizing a two dimensional electron gas (2DEG) channel have a great potential for high speed device applications. Zinc oxide (ZnO), a semiconductor with a wide bandgap (3.4 eV) and high electron saturation velocity has gained a great deal of attention as an attractive material for high speed devices. Efficient gate modulation, however, requires high-quality Schottky contacts on the barrier layer. In this article, we present our Schottky diode fabrication procedure on Zn-polar BeMgZnO/ZnO heterostructure with high density 2DEG which is achieved through strain modulation and incorporation of a few percent Be into the MgZnO-based barrier during growth by molecular beam epitaxy (MBE). To achieve high crystalline quality, nearly lattice-matched high-resistivity GaN templates grown by metal-organic chemical vapor deposition (MOCVD) are used as the substrate for the subsequent MBE growth of the oxide layers. To obtain the requisite Zn-polarity, careful surface treatment of GaN templates and control over the VI/II ratio during the growth of low temperature ZnO nucleation layer are utilized. Ti/Au electrodes serve as Ohmic contacts, and Ag electrodes deposited on the O2 plasma pretreated BeMgZnO surface are used for Schottky contacts.

Attainment of high-quality Schottky contacts is imperative for achieving efficient gate modulation in heterostructure field effect transistors (HFETs). We present the fabrication methodology and characteristics of Schottky diodes on Zn-polar BeMgZnO/ZnO heterostructures with high-density two dimensional electron gas (2DEG), grown by plasma-assisted molecular beam epitaxy on GaN templates.

等离子体辅助分子束外延法制备的锌极性 BeMgZnO/氧化锌异质结构肖特基二极管的制备

Heterostructure field effect transistors (HFETs) utilizing a two dimensional electron gas (2DEG) channel have a great potential for high speed device ...

Developing High Performance GaP/Si Heterojunction Solar Cells

To improve the efficiency of Si-based solar cells beyond their Shockley-Queisser limit, the optimal path is to integrate them with III-V-based solar cells. In this work, we present high performance GaP/Si heterojunction solar cells with a high Si minority-carrier lifetime and high crystal quality of epitaxial GaP layers. It is shown that by applying phosphorus (P)-diffusion layers into the Si substrate and a SiNx layer, the Si minority-carrier lifetime can be well-maintained during the GaP growth in the molecular beam epitaxy (MBE). By controlling the growth conditions, the high crystal quality of GaP was grown on the P-rich Si surface. The film quality is characterized by atomic force microscopy and high-resolution x-ray diffraction. In addition, MoOx was implemented as a hole-selective contact that led to a significant increase in the short-circuit current density. The achieved high device performance of the GaP/Si heterojunction solar cells establishes a path for further enhancement of the performance of Si-based photovoltaic devices.

Here, we present a protocol to develop high-performance GaP/Si heterojunction solar cells with a high Si minority-carrier lifetime.

研制高性能的 gap-硅异构太阳能电池

To improve the efficiency of Si-based solar cells beyond their Shockley-Queisser limit, the optimal path is to integrate them with III-V-based solar ...

Fabrication of Robust Nanoscale Contact between a Silver Nanowire Electrode and CdS Buffer Layer in Cu(In,Ga)Se2 Thin-film Solar Cells

Silver nanowire transparent electrodes have been employed as window layers for Cu(In,Ga)Se2 thin-film solar cells. Bare silver nanowire electrodes normally result in very poor cell performance. Embedding or sandwiching silver nanowires using moderately conductive transparent materials, such as indium tin oxide or zinc oxide, can improve cell performance. However, the solution-processed matrix layers can cause a significant number of interfacial defects between transparent electrodes and the CdS buffer, which can eventually result in low cell performance. This manuscript describes how to fabricate robust electrical contact between a silver nanowire electrode and the underlying CdS buffer layer in a Cu(In,Ga)Se2 solar cell, enabling high cell performance using matrix-free silver nanowire transparent electrodes. The matrix-free silver nanowire electrode fabricated by our method proves that the charge-carrier collection capability of silver nanowire electrode-based cells is as good as that of standard cells with sputtered ZnO:Al/i-ZnO as long as the silver nanowires and CdS have high-quality electrical contact. The high-quality electrical contact was achieved by depositing an additional CdS layer as thin as 10 nm onto the silver nanowire surface.

Fabrication of Robust Nanoscale Contact between a Silver Nanowire Electrode and CdS Buffer Layer in CuIn,GaSe2 Thin-film Solar Cells

In this protocol, we describe the detailed experimental procedure for the fabrication of a robust nanoscale contact between a silver nanowire network and CdS buffer layer in a CIGS thin-film solar cell.

在 Cu(In、Ga)Se2薄膜太阳能电池中制造银纳米线电极与 CdS 缓冲层之间的强健纳米级接触

Silver nanowire transparent electrodes have been employed as window layers for Cu(In,Ga)Se2 thin-film solar cells. Bare silver nanowire electrodes ...

Close-Space Sublimation-Deposited Ultra-Thin CdSeTe/CdTe Solar Cells for Enhanced Short-Circuit Current Density and Photoluminescence

Developments in photovoltaic device architectures are necessary to make solar energy a cost-effective and reliable source of renewable energy amidst growing global energy demands and climate change. Thin film CdTe technology has demonstrated cost-competitiveness and increasing efficiencies due partially to rapid fabrication times, minimal material usage, and introduction of a CdSeTe alloy into a ~3 &#956;m absorber layer. This work presents the close-space sublimation fabrication of thin, 1.5 &#181;m CdSeTe/CdTe bilayer devices using an automated in-line vacuum deposition system. The thin bilayer structure and fabrication technique minimize deposition time, increase device efficiency, and facilitate future thin absorber-based device architecture development. Three fabrication parameters appear to be the most impactful for optimizing thin CdSeTe/CdTe absorber devices: substrate preheat temperature, CdSeTe:CdTe thickness ratio, and CdCl2 passivation. For proper sublimation of the CdSeTe, the substrate temperature prior to deposition must be ~540 &#176;C (higher than that for CdTe) as controlled by dwell time in a preheat source. Variation in the CdSeTe:CdTe thickness ratio reveals a strong dependence of device performance on this ratio. The optimal absorber thicknesses are 0.5 &#956;m CdSeTe/1.0 &#956;m CdTe, and non-optimized thickness ratios reduce efficiency through back-barrier effects. Thin absorbers are sensitive to CdCl2 passivation variation; a much less aggressive CdCl2 treatment (compared to thicker absorbers) regarding both temperature and time yields optimal device performance. With optimized fabrication conditions, CdSeTe/CdTe increases device short-circuit current density and photoluminescence intensity compared to single-absorber CdTe. Additionally, an in-line close-space sublimation vacuum deposition system offers material and time reduction, scalability, and attainability of future ultra-thin absorber architectures.

This work describes the complete fabrication process of thin absorber cadmium selenium telluride/cadmium telluride photovoltaic devices for enhanced efficiency. The process utilizes an automated in-line vacuum system for close-space sublimation deposition that is scalable, from fabrication of small area research devices as well as large-scale modules.

近空间升升-沉积超薄CDSeTe/CdTe太阳能电池，增强短路电流密度和光致发光

Developments in photovoltaic device architectures are necessary to make solar energy a cost-effective and reliable source of renewable energy amidst ...

在铜改善异质结质量

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