CN1641483A - 形成具有低电阻率金属图案的方法 - Google Patents

形成具有低电阻率金属图案的方法 Download PDF

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CN1641483A
CN1641483A CNA200410081932XA CN200410081932A CN1641483A CN 1641483 A CN1641483 A CN 1641483A CN A200410081932X A CNA200410081932X A CN A200410081932XA CN 200410081932 A CN200410081932 A CN 200410081932A CN 1641483 A CN1641483 A CN 1641483A
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metal
pattern
described method
metal pattern
water
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CN100461000C (zh
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卢昌镐
宋基镕
金珍詠
塔玛拉·拜克
G·A·布兰尼茨基
T·V·盖夫斯卡娅
V·G·索科洛夫
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Samsung Electronics Co Ltd
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Abstract

本发明公开了一种用于形成低电阻率金属图案的方法。该方法包含以下步骤：(i)将光催化化合物涂布到衬底上以形成光催化薄膜层；(ii)将水溶性聚合物涂布到光催化薄膜层上以形成水溶性聚合物层；(iii)将该两层选择性曝光以形成用作晶体生长的核的潜图案；以及(iv)将潜图案镀以金属以在其上生长金属晶体。根据该方法，可以以低成本、较简单的方式形成包含低电阻率金属的多层电路图案，并且可以根据预定用途自由选择构成各层的金属。该低电阻率金属图案可有利地应用于平板显示器件如LCDs、PDPs和ELDs。

Description

形成具有低电阻率金属图案的方法
根据35U.S.C.§119(a)本非临时申请要求2003年12月16日提交的韩国专利申请No.2003-92112的优先权，该申请在此引入作为参考。
技术领域
本发明涉及用于形成具有低电阻率的金属图案的方法。更具体地，本发明涉及用于通过以下方式形成金属图案的方法，即顺序地在衬底上形成由光催化化合物(即其反应性可被光改变的化合物)组成的光催化层和水溶性聚合物层，将该两层选择性曝光以形成用于通过光反应进行晶体生长的潜像中心(latent image centers)，将该潜图案(latent pattern)镀以所需的金属以在潜图案上生长金属晶体。
背景技术
随着对大显示面和高分辨率的平板显示器(flat panel displays)(如液晶显示器(LCDs)、等离子显示屏(PDPs)和无机和有机发光显示器(ELDs))的需要增加，金属线路(metal wiring)的长度被大大延长。而且，可增加孔径比(aperture ratio)的设计比例尺也在下降。这就产生了一些问题，例如线路电阻和电容，以及信号延迟和失真急剧增大。在这些情况下，发展用于形成低电阻率金属线路的方法对于开发高分辨率和大面积平板显示器件至关重要。
已经积极探讨了在大尺寸LCDs中采用低电阻率铝(Al)作为线路材料。此时，采用铝合金AlNd来防止线路的不均匀问题(如使用纯铝时由于物质迁移所出现的小丘(hillock))。然而，由于加入合金会引起电阻率增加，以及α-Si或ITO的高反应性导致接触电阻增加，因此当铝合金用作源极/漏极材料时需要采用多层结构(如Cr/AlNd/Cr)。但是，形成多层金属图案需要复杂的工艺，其使得生产力受到限制。
下表1的周期表中列出了可用于形成平板显示器件的金属线路的各种金属。
尽管目前使用铝合金，但铜(Cu)和银(Ag)已成为极感兴趣的研究热点。这是因为它们在无定形硅层上具有低的电阻率和良好的接触性质。然而，当铜或银用作栅电极时，其与下部衬底的附着性差，从而在下续步骤中金属线路易于剥落。另外，当铜或银用作源极或漏极时，原子在200℃下扩散进入无定形硅层或者由于电驱动发生电迁移。这使得线路和器件的性能劣化。因此，为了将铜或银用作具有低电阻率的线路材料，需要形成另外的金属层。该层要具有良好的衬底附着性并且在线路材料的较低部份和/或较高部份具有低的接触电阻。这导致多层金属图案。
为了满足以较低成本形成大显示面的需要，需要发展能够用新材料代替常规线路材料的技术，从而可以用相对简单的方式形成多层金属线路。
目前，采用光致抗蚀剂形成金属图案。然而，该方法含有许多复杂的步骤，包括金属溅射、光致抗蚀剂图案化和显影，及蚀刻。因此它不适合用于形成多层金属图案。另外，对于在尺寸增大的玻璃衬底上形成大面积图案，还存在与发展真空薄膜沉积设备有关的实质性技术难度和制造成本增加。
美国专利No.5,534,312报道了一种用于形成金属图案而无需蚀刻工艺的方法。该方法包括以下步骤：将对光敏感的有机化合物和金属配位结合在一起从而生成有机金属化合物；将该有机金属化合物涂布在衬底上，然后，不采用感光树脂用光照射该有机金属化合物。在这一方法中，当涂布的衬底通过带图案的掩膜曝光时，光与有机金属化合物直接反应导致与金属配位结合的有机配体发生降解。该降解使得配体和金属分开。金属原子和邻近的金属原子或周围的氧反应最终形成金属氧化物膜图案。然而，由于配体污染，该方法是存在问题的。为了形成金属或金属氧化物膜，大多数配体通过光反应而分开。另外，与提高氧化物膜的电导性有关的是，该方法不利地包含还原和表面退火，其在200℃或更高温度、氮氢混合气流下进行30分钟至数小时。
在日本专利特开平No.2002-169486中描述了另一种通过喷墨过程形成金属线路的方法。但是，该方法存在分辨率低和难以形成高电导线路的问题。另外，美国专利No.6,521,285论述了通过微接触印刷(pringint)和无电镀(electroless plating)形成金属线路。然而，此方法具有的缺点是：很难形成在大面积平板显示器件中使用的均匀金属线路。
因此本领域需要能形成包括高电导金属的多层金属图案的简单方法。
发明内容
本发明的发明人发现可以用简单的方式形成包括高电导金属的单层或多层金属图案。其通过下列步骤完成：顺序地在衬底上形成由其反应性可被光改变的化合物(即光催化(photocatalytic)化合物)组成的光催化薄膜层和水溶性聚合物层，将两层选择性曝光以形成用于晶体生长的潜像中心(通过光反应)，并将潜图案镀以所需的金属以在潜图案上生长金属晶体。另外，本发明的发明人还发现该金属图案具有优异的金属线路性质。
因此，本发明的特征是提供一种用于以快速、有效和简单的方式形成单层或多层金属图案的方法。进行该方法无需要求高真空或高温条件的金属薄膜形成过程。而且，该方法对于精细图案的形成或下续蚀刻过程不涉及光致抗蚀工艺。
本发明的另一特征是提供了采用本方法形成的金属图案制造的平板显示器件。
根据本发明的特征，提供用于形成金属图案的方法，包括以下步骤：(i)将光催化化合物涂布到衬底上以形成光催化薄膜层；(ii)将水溶性聚合物涂布到光催化薄膜层上以形成水溶性聚合物层；(iii)将该两层选择性曝光以形成用于晶体生长的潜像中心；和(iv)将潜图案镀以金属以在其上生长金属晶体。
根据本发明，还提供了用本发明的方法形成的金属图案。
根据本发明，还提供了包含作为金属线路的金属图案的平板显示器件。
根据本发明，还提供了包含作为电磁干扰过滤器(electromagneticinterference filter)的金属图案的平板显示器件。
附图说明
从结合附图的下文的详细描述中将会更清楚地理解本发明的上述和其它目的、特征和其它优点，其中：
图1是根据本发明的实施例1形成的金属图案的光学显微镜图；
图2是根据本发明的实施例2形成的金属图案的电子显微镜图；和
图3是根据本发明的实施例3形成的金属图案的光学显微镜图。
具体实施方式
在下文中，将基于各个步骤更详细地解释本发明。
步骤(i)：
在该步骤中，将光催化化合物涂布到衬底上以在衬底上形成透明的无定形的光催化薄膜层。
此处所用的术语“光催化化合物”指其特性能被光显著改变的化合物，特别是在未曝光时是惰性的而在曝光(如紫外光)下能被激活的化合物。在紫外光的照射下，光催化化合物曝光部分的电子被激发，因而能够表现出活性如还原能力。因此，曝光部分的金属离子被还原，从而在曝光部分上可形成负型潜图案。
光催化化合物的优选例子包括能通过退火形成透明的无定形TiO2的任意含钛(Ti)有机金属化合物，如钛酸四异丙基酯、钛酸四正丁基酯、钛酸四(2-乙基-己基)酯、聚钛酸丁基酯(polybutyltitanate)等。
在将光催化化合物溶解在适当的溶剂如异丙醇中之后，可以在衬底上采用旋涂、喷涂、丝网印刷(screen printing)等进行该溶液的涂布。
可用于本发明的衬底的例子包括但不特别限定为透明塑料和玻璃材料。透明塑料衬底的例子，可提及如丙烯酸类树脂、聚酯、聚碳酸酯、聚乙烯、聚醚砜、烯烃马来酰亚胺共聚物、降冰片烯基树脂等。在需要极好的耐热性的情况中，优选烯烃马来酰亚胺共聚物和降冰片烯基树脂。否则，优选采用聚酯膜、丙烯酸类树脂等。
通过涂布光催化化合物形成30-1,000nm厚的涂层。涂布之后，在热板上或对流炉中在不高于200℃的温度下加热涂层20分钟以形成所需的光催化薄膜层。在高于200℃的温度下加热会导致结晶TiO2层的形成，从而使得光学性质和图案化分布(patterning profile)变差。
步骤(ii)：
在该步骤中，将水溶性聚合物涂布在光催化薄膜层以在其上形成水溶性聚合物层。此处所用的水溶性聚合物的例子包括均聚物，如聚乙烯醇、聚乙烯酚(polyvinylphenols)、聚乙烯吡咯烷酮、聚丙烯酸、聚丙烯酰胺、明胶，及其共聚物。
首先，将1-30％重量的水溶性聚合物溶解在水中。之后，将所得的溶液涂布在光催化薄膜层上，然后加热以形成水溶性聚合物层。
这样形成的水溶性聚合物层在促进紫外光照下的光还原反应和用于提高光催化活性中发挥着作用。
为了进一步提高其光敏性，优选将光敏剂加入水溶性聚合物层中。可以采用选自着色剂、有机酸、有机酸盐和有机胺的水溶性化合物作为光敏剂。光敏剂的具体例子包括焦油着色剂(tar colorants)、叶绿酸的钾盐和钠盐、核黄素(riboflavine)及其衍生物、水溶性胭脂树橙、CuSO4、焦糖(caramels)、姜黄素、胭脂虫红(cochinal)、柠檬酸、柠檬酸铵、柠檬酸钠、草酸、酒石酸钾、酒石酸钠、抗坏血酸、甲酸、三乙醇胺、一乙醇胺、苹果酸等。
基于100重量份的水溶性聚合物，加入的光敏剂的量为0.01-50重量份。
之后，在不高于100℃的温度下加热水溶性聚合物层5分钟或少于5分钟以蒸发水。控制最终水溶性聚合物层的厚度为0.1～1μm。
步骤(iii)：
在该步骤中，将光催化薄膜层和水溶性聚合物层有选择地曝光以形成用于在其上生长晶体的潜像中心。曝光气氛和曝光量没有特别限制，可以根据所用的光催化化合物的种类进行适当选择。在后续的镀金属步骤中活化的光催化图案用作金属晶体生长的核。
为了在下续步骤(iv)中有效形成金属图案，将潜图案用金属盐溶液处理以在其上形成催化剂图案。优选使用银(Ag)盐溶液、钯(Pd)盐溶液或其混合溶液作为该金属盐溶液。
步骤(iv)：
在该步骤中，对在步骤(iii)中形成的用于晶体生长的潜像中心，或根据需要的催化剂图案，进行金属镀覆(metal-plating)以在用于金属生长的带图案的核上生长金属晶体，从而形成金属图案。采用电镀或无电镀方法进行金属镀覆。由于通过用金属盐溶液处理潜图案而形成的催化剂图案在无电镀时具有足够的活性，因此加速了晶体生长，从而有利于形成更加致密堆积(densely packed)的金属图案。
在形成金属图案上可以理解，通过连续镀覆在用于晶体生长的潜像中心上至少可以生长两层金属晶体以形成多层金属图案。例如，将用于晶体生长的潜像中心镀以所需的金属以形成第一金属层，然后将第一金属层镀以另一种所需的金属以只在形成了第一金属层的部份形成第二金属层，从而可有利地地形成多层金属图案。
可以根据预定的用途适当选择所用镀覆金属的种类和镀覆次序。组成各金属层的金属可以彼此相同或不同。可适当控制金属层的厚度。
为了形成具有低电阻率的金属图案，需要考虑与衬底的附着性和衬底和绝缘膜之间的接触性质。在本发明中，优选使用金属如Ni、Pd、Sn或Cr，或其合金来形成第一金属层，以及高电导金属如Cu、Ag或Au，或其合金来形成第二金属层。此时，优选形成的金属层具有的厚度分别为0.1-1μm和0.3-20μm。就低价格和易于形成而言，优选采用镍来形成第一金属层，及优选采用银或铜形成第二金属层。
当高电导的第二金属层接触ITO(氧化铟锡)或半导体组分时，为了改善第二金属层和ITO或半导体组分之间的接触电阻，可镀以Ni、Pd、Sn、Cr，或其合金以形成第三金属层。在采用铜来形成高电导第二金属层的情况中，为了防止因表面上氧化物膜的形成而引起第二金属层物理性质的劣化，可以采用贵金属如Ag或Au来形成第三金属层。
或者，为了改善接触电阻，可以通过以用于形成第一金属层的金属镀覆第二金属层形成第三金属层。
可适当结合各种镀覆方法以形成多层金属层。例如，当在绝缘膜上形成第一金属层时，采用无电镀工艺。另一方面，当Cu或Ag用于形成第二金属层时，采用无电镀或电镀工艺。
采用公知的方法完成无电镀或电镀，并可使用购买的镀覆组合物用于镀覆。在无电镀工艺中，将其上形成了用于晶体生长的Pd或Ag核催化剂的衬底浸入镀覆溶液中，该溶液包含：1)金属盐、2)还原剂、3)络合剂、4)pH调节剂、5)pH缓冲剂和6)改性剂。金属盐1)用作提供金属离子的来源。金属盐的例子包括相应金属的氯化物、硝酸盐和醋酸盐。还原剂2)还原存在于衬底上的金属离子。还原剂的具体例子包括NaBH4、KBH4、NaH2PO2、肼、formaline和多糖(如葡萄糖)。优选NaH2PO2用于镍镀溶液，formaline和多糖用于Cu或Ag镀溶液。络合剂3)用于防止在碱性溶液中氢氧化物的沉淀，以及控制自由金属离子的浓度，从而防止金属盐的分解并调节镀覆速度。络合剂的具体例子包括氨水溶液、乙酸、鸟嘌呤酸(guanine acid)、酒石酸、螯合剂(如EDTA)和有机胺化合物。优选螯合剂(如EDTA)。pH调节剂4)在调节镀覆溶液的pH中起作用，并选自酸性或碱性化合物。pH缓冲剂5)抑制镀覆溶液的pH发生突变，并选自有机酸和弱酸性无机化合物。改性剂6)是能提高涂布和平面化(planarization)性能的化合物。改性剂的具体例子包括普通的表面活性剂和能吸附干扰晶体生长的化合物的吸附剂。
在电镀方法中，采用具有包含1)金属盐、2)络合剂、3)pH调节剂、4)pH缓冲剂和5)改性剂的组合物的镀覆溶液。在镀覆溶液组合物中包含的组分的功能和具体例子如同上述在无电镀方法中所说明的。
这样形成的低电阻率金属图案可以用作平板显示器件如LCDs、PDPs和ELDs的金属线路或电磁干扰过滤器。
现在参考下面的优选实施例详细描述本发明。然而，所给出的这些例子是为了进行说明而不应解释为对本发明范围的限制。
用于晶体生长的潜像中心的形成
将聚钛酸丁基酯的异丙醇溶液(2.5wt％)通过旋涂涂布到作为衬底的透明聚酯膜上之后，将所得的涂层在150℃下干燥5分钟，以使其具有约100nm的厚度。将1重量份的三乙醇胺(基于100重量份的聚合物)作为光敏剂独立地加入聚乙烯醇聚合物(Polyscience)(分子量为25000)的水溶液(5wt％)中，然后进行搅拌。在聚钛酸丁基酯涂层上涂布所得的混合物并在60℃下干燥两分钟以制备光催化膜层。采用UV曝光系统(Oriel，U.S.A)通过其上形成有微小图案的光掩膜用具有宽波长范围的紫外光照射光催化薄膜层。曝光之后，将该衬底浸入在1升水中含0.6g PdCl2和1ml HCl的溶液中以在曝光部分的表面上沉积Pd颗粒。结果，形成了沉积Pd的负性图案作为晶体生长的核。
实施例1：采用无电镍镀和无电铜镀形成负型铜线路
将上述制备的衬底浸入无电镍镀溶液中以进行带图案的镍线路的晶体生长。将镍线路图案浸入无电铜镀溶液中以形成负型双层镍-铜线路图案。在此制备无电镍镀溶液和无电铜镀溶液使其分别具有下表2所示的组成(a)和(b)。在下表3中显示了该金属图案的基本物理性质。使用α-step(由Dektak制造)测量图案的厚度，4-点探针(4-point probe)测量电阻率。使用光学显微镜测量分辨率，及通过斯柯奇胶带剥离测试(scotch tape peeling test)确定附着力。图1显示了该金属图案的光学显微镜图。
实施例2：采用无电镍镀和电铜镀形成负型铜线路
将通过其上形成了网孔图案的光掩膜照射而制备的衬底浸入无电镍镀溶液中以选择性生长镍线路的晶体。将镍线路图案浸入电铜镀溶液，然后对该镀覆溶液施加电流(0.15A)以形成负型双层镍-铜线路图案。制备无电镍镀溶液和电铜镀溶液使其分别具有下表2所示的组成(a)和(c)。在下表3中显示了该金属图案的基本物理性质。图2显示了该金属图案的电子显微镜图。
实施例3采用无电镍镀和无电银镀形成负型银线路
将上述制备的衬底浸入无电镍镀溶液中以选择性生长镍线路的晶体。在此制备无电镍镀溶液使其具有下表2所示的组成(a)。将镍线路图案浸入无电银镀溶液(S-700，Kojundo，chemical，Co.，Ltd.，Japan)中以形成负型双层镍-银线路图案。在下表3中显示了该金属图案的基本物理性质。图3显示了该金属图案的光学显微镜图。
表2
  (a)无电镍镀溶液   (b)无电铜镀溶液   (c)电铜镀溶液
  NiCl2·6H2O 10gNaH2PO2·2H2O 30gNaCH3COO 10gNH4Cl 40g水1l5～10分钟50μmNi厚度＞0.1μm   CuSO4·5H2O 12gKNaC4H4O6·6H2O 55gNaOH 18gNa2CO3 10gNa2S2O3·5H2O 0.0002gCH2O(40％)20ml水1l5～10分钟50μmCu厚度＞0.1μm   CuSO4·5H2O 72gH2SO4 230gHCl 0.125gOKUNO Lucina10g水1l
表3
  实施例序号     金属厚度(μm)     电阻率(μohm-cm)     分辨率(μm)     附着力
  实施例1     0.4     2.7     ＜8     好
  实施例2     1.5     2.0     ＜10     好
  实施例3     0.3     2.5     ＜8     好
根据本发明的方法，采用简单的涂布方法(而不是常规物理沉积)和之后的曝光和简单镀覆处理、通过形成光催化薄膜可以形成单层和多层金属图案。因此，本发明可提供用于以快速、有效和简单的方式形成单层或多层低电阻率的金属图案的方法，而无需要求高真空条件的溅射过程及采用感光树脂和蚀刻方法的光图案化(photopatterning)过程。由本发明的方法形成的低电阻率金属图案可有利地应用于平板显示器件。
尽管为了说明已公开了本发明的优选实施方式，但本领域的技术人员会理解到：在不偏离如所附的权利要求书所公开的本发明的范围和实质下可以进行各种改变、添加和替代。

Claims (14)

1.一种形成金属图案的方法，其包含以下步骤：
(i)将光催化化合物涂布到衬底上以形成光催化薄膜层；
(ii)将水溶性聚合物涂布到光催化薄膜层上以形成水溶性聚合物层；
(iii)将该两层选择性曝光以形成用于晶体生长的潜像中心；和
(iv)将潜图案镀以金属以在其上生长金属晶体。
2.权利要求1所述的方法，其中在曝光下激发所述光催化化合物的电子，使得光催化化合物具有活性。
3.权利要求2所述的方法，其中所述光催化化合物是通过退火形成无定形TiO2的含钛有机金属化合物。
4.权利要求3所述的方法，其中所述含钛有机金属化合物是钛酸四异丙基酯、钛酸四正丁基酯、钛酸四(2-乙基-己基)酯或聚钛酸丁基酯。
5.权利要求1所述的方法，其中所述水溶性聚合物是至少一种选自聚乙烯醇、聚乙烯酚、聚乙烯吡咯烷酮、聚丙烯酸、聚丙烯酰胺、明胶，及其共聚物的聚合物。
6.权利要求1所述的方法，其中所述水溶性聚合物层还包括光敏剂。
7.权利要求6所述的方法，其中所述光敏剂选自着色剂、有机酸、有机酸盐和有机胺。
8.权利要求7所述的方法，其中所述光敏剂选自焦油着色剂、叶绿酸的钾盐和钠盐、核黄素及其衍生物、水溶性胭脂树橙、CuSO4、焦糖、姜黄素、胭脂虫红、柠檬酸、柠檬酸铵、柠檬酸钠、草酸、酒石酸钾、酒石酸钠、抗坏血酸、甲酸、三乙醇胺、一乙醇胺和苹果酸。
9.权利要求1所述的方法，其还包含用金属盐溶液处理在步骤(iii)中形成的用于晶体生长的潜像中心的步骤，以在该潜图案上形成催化剂图案。
10.权利要求9所述的方法，其中所述金属盐溶液是钯(Pd)盐溶液、银(Ag)盐溶液，或其混合溶液。
11.权利要求9所述的方法，其中将所述催化剂图案用Ni、Pd、Sn、Cr，或其合金进行无电镀以形成第一金属图案，然后将第一金属图案用Cu、Ag、Au，或其合金进行电镀或无电镀以形成第二金属图案。
12.一种金属图案，其通过权利要求1所述的方法形成。
13.一种平板显示器件，其包含权利要求12所述的金属图案作为金属线路。
14.一种平板显示器件，其包含权利要求12所述的金属图案作为电磁干扰过滤器。
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