CN1123034C - 发光器件及其制造方法和有机发光器件结构 - Google Patents

发光器件及其制造方法和有机发光器件结构 Download PDF

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CN1123034C
CN1123034C CN97193731A CN97193731A CN1123034C CN 1123034 C CN1123034 C CN 1123034C CN 97193731 A CN97193731 A CN 97193731A CN 97193731 A CN97193731 A CN 97193731A CN 1123034 C CN1123034 C CN 1123034C
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斯蒂芬·R·弗雷斯特
鲍尔·E·布罗斯
马克·E·汤姆森
弗拉基米尔·布罗维奇
顾功
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Abstract

使用由有机化合物制作的双异质结构器件构成的垂直叠层(308，310，312)的彩色有机发光器件。垂直叠层结构(300)形成在具有ITO(304)或类似金属的透明涂层的玻璃基底(302)上以提供衬底。在衬底上淀积的是垂直叠层分布的三个双异质结构器件(308，310，312)，各由适当的有机材料形成。使具有最长波长的双异质结构位于叠层的顶部来实现堆叠。

Description

发光器件及其制造方法和有机发光器件结构
本申请是1994年12月13日提出的名为“彩色有机发光器件”的美国专利No.08/354674的部分后继申请。
本发明涉及到彩色有机发光器件，更确切地说是涉及到用于平板电子显示器、平视显示器等等之中的器件。
电子显示是现代社会中传递信息的必不可少的方法，并已被用于电视机、计算机终端和其它大量应用中。其它的介质都提供不了这样的速度、多功能性和交互性。已知的显示技术包括等离子体显示器、发光二极管(LED)、薄膜电致发光显示器等等。
主要的非发射技术利用所知的一种液晶(LC)或液晶显示器(LCD)的有机分子的电光性质。LCD的工作相当可靠，但其对比度和分辨率低，且需要高功率的后照光。有源矩阵显示器采用各能激话一个LC象素的晶体管的阵列。无疑，有关平板显示器的技术是关系重大的，并不断地取得了进展。S.W.Depp和W.E.Howard的文章“平板显示器”(ScientificAmerican，1993年3月，p90-97)指出，至1995年，平板显示器可望单独形成40-50亿美元的市场。对任何一种显示技术所希望的因素，是在光水平良好和价格有竞争性的情况下提供高分辨率全色显示的能力。
彩色显示以红(R)、绿(G)、蓝(B)三原色进行工作。在使用有机薄膜材料的显示红、绿、蓝的发光器件(LED)中，已取得了明显的进展。这些薄膜材料是在高真空条件下淀积的。这种技术已在全世界许多地方被开发，并在许多研究机构中被采用。
目前最好的高效有机发射结构被称为双异质结构LED，示于图1A并指定为现有技术。这种结构非常相似于采用GaAs或InP材料的常规无机LED。
在图1A所示的器件中，玻璃支持层10涂覆有氧化铟锡(ITO)薄层11，由层10和11组成衬底。接着，在ITO层11上淀积一个主要是输运空穴的有机薄层(HTL，100-500埃)12。淀积在HTL层12表面上的是薄的(通常为50-100埃)发射层(EL)13。如果各层太薄，则薄膜的连续性可能不好，而较厚的薄膜内阻高，要求在更高的功率下工作。发射层(EL)为从100-500埃厚的电子输运层14(ETL)注入的电子，提供与来自HTL层12的空穴进行复合的位置。ETL材料的特征是其电子迁移率明显地高于空穴迁移率。在1994年3月15日授与Tang等人的题为“有机电致发光彩色图象显示器”的美国专利No.5294870中，公开了现有技术ETL、EL和HTL的例子。
EL层13常常掺以高荧光染料，以便调节颜色并提高LED的电致发光效率。借助于淀积金属接触15、16和顶电极17，就完成了图1A所示的器件。接触15和16通常由铟或Ti/Pt/Au制成。电极17常常是一种双层结构，由诸如直接接触有机ETL层14的Mg/Ag合金17’和Mg/Ag上的诸如金(Au)或银(Ag)的高功函数金属厚层17”组成。厚层17”是不透明的。当在顶电极17和接触15与16之间施加恰当的偏置电压时，就通过玻璃衬底10发生光发射。图1A的LED器件根据其发射的颜色和结构，通常具有0.05％-4％的发光外量子效率。
另一种称为单异质结构的已知的发射结构示于图1B，并被指定为现有技术。此结构与图1A结构的差别在于EL层13也用作ETL层，取消了图1A的ETL层14。但为了有效地工作，图1B的器件必须组合一个电子输运能力良好的EL层13，否则如图1A器件那样必须包含一个分立的ETL层14。
目前，在绿色LED中已观察到最高的效率。而且已达到3-10V的驱动电压。这些早期的非常有前景的演示已采用了非晶或高度多晶的有机层。这种结构无疑限制了载流子穿越薄膜的迁移率，反过来又限制了电流并提高了驱动电压。这种器件的明显的失效模式是多晶状态引起的晶粒迁移和生长。电极接触退化也是一个明显的失效机制。
图1C示出了又一种已知的LED器件，示出了一种单层(聚合物)LED的典型剖面图。如所示，此器件包含涂覆有ITO薄层3的玻璃支持层1，用来形成基底衬底。旋涂的聚合物有机薄层5制作在例如ITO层3上，并提供前述器件的HTL、ETL和EL层的所有功能。金属电极层6制作在有机层5上。此金属通常是Mg、Ca或其它常规使用的金属。
在Tang等人的美国专利No.5294870中，公开了采用有机化合物作为发光象素的彩色电致发光图象显示器的一个例子。此专利公开了多个发光象素，它含有用来在蓝色发射子象素区发射蓝光的有机介质。荧光介质被横向分隔于蓝色发射子象素区。荧光介质吸收有机介质发射的光，并在不同的子象素区发射红光和绿光。采用掺有荧光染料的材料来在吸收来自蓝色子象素区的蓝光时发射绿光或红光，其效率低于直接由绿色或红色LED来形成绿光或红光。其理由是，效率为EL的量子效率、荧光的量子效率与(1-透射率)的乘积。于是，这种显示器的缺点就是每一个发射的颜色都要求不同的横向分隔的子象素区。
本发明的一个目的是提供一种采用各用来发射一种不同颜色的几种有机电致发光介质的彩色有机发光器件。
本发明的又一目的是在高清晰度彩色显示器中提供这样一种器件，其中的有机介质排列在叠层结构中，使从显示器的一个公共区能够发射任何一种颜色。
本发明的再一目的是提供一种极为可靠的、断电时基本透明的且生产成本比较低的三色有机发光器件。
本发明的另一目的是提供一种借助于生长相似于电致发光二极管中所用的那些材料的有机材料而实现的器件，以获得高度可靠、高度密集、效率高的且要求低的驱动电压的用于RGB显示器的有机LED。
根据本发明的一个方面，提供了一种至少包含一个在不带电时透明的有机发光器件的发光器件，它包含：具有顶表面和底表面的透明衬底；涂于所述衬底顶表面的透明的第一氧化铟锡薄膜涂层；涂于所述第一氧化铟锡层上的透明的空穴导电材料涂层；覆盖所述空穴导电材料的透明的电子导电且高度电致发光的有机材料层；涂于所述有机材料层上的透明的较薄的金属电极膜；覆盖所述金属电极膜的透明的第二氧化铟锡薄膜涂层；以及用来接收偏压以激发所述器件并使其从其顶表面和底表面发射给定颜色的光的键合于所述第一和第二氧化铟锡层的第一和第二电接触。
根据本发明的另一方面，提供了一种制造不带电时透明的彩色发光器件结构的方法，它包含下列步骤：在透明衬底上制作第一透明导电层；在所述第一透明导电层上淀积透明的第一空穴输运层；在所述第一空穴输运层上淀积透明的第一有机发射层，以提供第一发射颜色；在所述第一有机发射层上，用汽相淀积方法淀积透明的第一电子输运层；在所述第一电子输运层上，用溅射方法淀积第二透明导电层，所述第二透明导电层用来接收第一偏置电位；在所述第二透明导电层上淀积透明的第二空穴输运层；在所述第二空穴输运层上淀积透明的第二有机发射层，以提供第二发射颜色；在所述第二发射层上，用汽相淀积方法淀积透明的第二电子输运层；以及在所述第二电子输运层上，用溅射方法淀积第三透明导电层，所述第三透明导电层用来接收第二偏置电位。
根据本发明的再一方面，还提供了一种有机发光器件结构，包括：在衬底上形成的第一导电层；在第一导电层上形成的有机透明发光器件；在有机透明发光器件上形成的厚度为50-400埃的透明导电金属层；以及在透明导电金属层上形成的第二导电层，其中，所述第二导电层包括氧化铟锡以外的透明导电氧化物。
图1A是根据现有技术的典型有机双异质结构发光器件(LED)的剖面图。
图1B是根据现有技术的典型有机单异质结构发光器件(LED)的剖面图。
图1C是根据现有技术的已知的单层聚合物LED结构的剖面图。
图2A、2B和2C分别是根据本发明各实施例，分别利用结晶有机发光器件(LED)集成的三色象素的剖面图。
图3-11示出了可用来组成产生各种颜色的有源发射层的各种有机化合物。
图12(A-E)说明了用来制造根据本发明的彩色LED的掩模工序。
图13(A-F)说明了用来制造根据本发明的彩色LED的干法腐蚀工序。
图14A示出了为简化其封装而设计的根据本发明一个实施例的彩色LED。
图14B示出了本发明另一实施例的气密封装件的剖面图。
图14C是沿图14B中的14C-14C的剖面图。
图15方框图示出了采用根据本发明的LED并具有显示驱动电路的RGB显示器。
图16示出了其堆叠的LED的数目增大到N(N为整数1、2、3、……、N)的本发明另一实施例的LED器件。
图17示出了本发明另一实施例的基本上透明的有机发光器件(TOLED)。
图18示出了图17的本发明实施例的从100埃厚的Mg-Ag接触发射的TOLED光谱输出(虚线)和从有关衬底发射的TOLED光谱输出(实线)，以EL强度(任意单位a.u.)对波长(nm)的形式绘出。
图19是透射率(％)对波长(nm)的曲线，示出了具有100埃厚的Mg-Ag电极的图17的TOLED的透射光谱与波长的关系的一个例子。
图20示出了图17的TOLED顶接触的工艺原型在波长为530nm时的透射率(％)对Mg-Ag接触厚度的曲线。
图21示出了用来在有机层上局部制作透明接触的本发明一个实施例的在衬底有机层上淀积Mg∶Ag膜的系统。
图22方框图一般地示出了本发明一个实施例的在有机层上制作透明接触必须进行的三个连续操作。
图23示出了本发明一个实施例的用来在预先淀积于有机层上的Mg∶Ag金属合金膜顶部淀积氧化铟锡(ITO)膜的溅射系统。
已描述了图1A，这是一种现有技术的双异质结构有机发光器件。如将要描述的那样，在本发明中采用了图1A的器件基本结构。
参照图2A，其中示出了本发明一个实施例中的高密度的集成RGB象素结构的示意剖面图，此结构是用生长即真空淀积的有机层来实现的。由于能够在各种材料(包括金属和ITO)上生长有机材料，故可组成本发明实施例中示为20、21和22的LED双异质结构(DH)的叠层。为了说明起见，在图2A的例子中，认为LED 20在叠层的底部，LED 21在叠层中部，而LED 22在叠层的顶部。还有，此叠层在图2A中示为垂直取向，但LED也可以是其它取向。在其它的实施例中，在SH器件可与DH器件一样用作发光器的情况下，单异质结构(SH)LED(见图1B)叠层或聚合物基LED器件(见图1C)叠层都可用作DH LED的替代。而且，含有真空淀积的和聚合物发光材料的组合的SH和DH器件，都被认为是在本发明的构思与范围之中。
像器件20这样的各个器件结构，包含真空淀积即生长在或淀积在ITO层35表面上的HTL层20H。例如在图2A的器件结构中示出了，在顶部ETL层20T和HTL层20H之间夹有一个EL层20E。待要描述的ETL层20T和其它ETL层由M(8-羟基喹啉)n(M为金属离子；n＝2-4)之类的有机材料组成。在Tang等人的美国专利No.5294870中可找到其它适当的有机ETL材料的例子。制作在顶部ETL层20T上的是厚度通常在50-400埃范围内的薄的半透明的低功函数(最好是＜4eV)金属层26M。适当的可选用者包括Mg、Mg/Ag和As。淀积在金属层26M顶部上的是另一个透明的薄的ITO导电层26I。(此处为方便起见，将金属层26M和ITO层26I的双层结构称为ITO/金属层26)。像20、21和22这样的各个双异质结构器件，都具有一个制作在ITO透明导电层26I或35上的底部HTL层。然后淀积EL层和另一个ETL层。HTL、ETL、ITO、金属和有机EL层中的每一个，由于其组分和很小的厚度而都是透明的。各个HTL层的厚度可以是50埃至大于1000埃；各个EL层的厚度可以是50埃至大于200埃；各个ETL层的厚度可以是50埃至1000埃；各个金属层26M的厚度可以是50埃至大于100埃；而各个ITO层26I和35的厚度可以是1000埃至大于4000埃。为了得到最佳的性能，各层的厚度最好维持在上述范围的下端，但这些范围并不意味着要受到限制。于是，各个LED20、21和22(不包括ITO/金属层)的厚度最好是靠近200埃。
若SH LED器件而不是DH LED器件被用来提供LED 20、21、22，则如先前图1B的SH所述的那样，ETL层和EL层由层13之类的单层来提供。层13通常是铝喹啉(Al-quinolate)。图2B示出了这一点，其中EL层20E、21E和22E分别提供EL和ETL层二种功能。但图2A的DHLED叠层相对于图2B的SH LED叠层的优点是，DH LED可得到具有高效率的更薄的总体结构。
在图2A和2B中，即使各个LED的中心彼此偏离，从LED 20、21和22各个器件出来的总光束也基本上重合。虽然各光束在同心结构中是重合的，但更靠近玻璃衬底的发射器件或非发射器件，对发射器件即更远离玻璃衬底的器件来说是透明的。但二极管20、21和22不必彼此偏离，而是可以彼此同心地堆叠，其上来自各个器件的光束彼此整个重合。图12E示出了一种同心结构，下面将根据器件制造工艺来加以描述。注意在偏离和同心结构之间的功能中不存在差别。各个器件以基本上全方向的方式通过玻璃衬底发射光。跨越叠层29中的三个LED的电压被控制来提供任何时刻从特定象素得到的所希望的发射颜色和亮度。于是，如图2A和2B示意地示出的那样，每个LED 22、21和20可以分别用R、G和B束同时激发，通过并经由透明层而可见。各个DH结构20、21和22，在施加适当的偏置电压时，能够发射不同颜色的光。双异质结构LED 20发射蓝光。双异质结构LED 21发射绿光，而双异质结构(DH)LED 22发射红光。可以激活单个LED 20、21和22或其不同的组合，以便部分地根据各个LED 20、21和22中电流的幅度来选择性地获得各个象素的所希望的光的颜色。
在图2A和2B的例子中，LED 20、21和22分别用电池32、31和30进行正向偏置。电流从各个电池32、31和30的正极，分别通过各个器件的各层，分别流入其相关LED 20、21和22的阳极端子40、41、42，并从用作阴极端子的端子41、42和43，分别流到各个电池32、31和30的负极。结果，光就从各个LED 20、21和22发射。LED器件20、21和22被做成能够分别由所包含的用来选择性地使电池32、31和30在进入和退出与其各个LED的连接状态之间进行转换的装置(未示出)使其选择性地激发。
在图2A和2B的本发明的实施例中，LED 22的顶部ITO接触26I是透明的，使三色器件可用于平视显示。但在本发明的另一实施例中，顶部接触26I由诸如Mg/Ag、In、Ag或Au之类的厚的金属制成，用来通过衬底13向上反射发射的光，从而大大提高器件的效率。借助于在玻璃衬底37和ITO层35之间制作多层介电薄膜涂层以提供抗反射表面，也能够提高整个器件的效率。需要三组抗反射层，逐一在各层发射的各个波长处形成一个抗反射层。
在另一个实施例中，图2A的器件以相反的方式构成，用以提供从叠层顶部而不是前者那样从底部出来的光发射。参照图2C，反结构的例子是用厚的反射金属层38来代替ITO层35。蓝色LED 20则用互换HTL层20H与ETL层20T而保持EL层20E仍然夹在其间的方法来提供。而且，金属接触层26M现在被淀积在ITO层26I的顶部。如反转蓝色LED 20所述的那样，叠层的绿色LED 21和红色LED 22各由互换层构成(各个HTL层和ETL层互换，随之以互换金属层和ITO层)。注意在反结构中，蓝色器件20必须在顶部而红色器件22在底部。电池30、31和32的极性也要反过来。结果，在正向偏置发光时，分别流过器件20、21和22的电流方向与图2A实施例的相同。
在此例子中，器件的剖面图内有一个台阶状分布。透明接触区(ITO)26I使得能够分隔叠层中各个象素元件的偏压，而且此材料可用作工艺步骤中的腐蚀停止层。各个DH LED结构20、21和22的分立的偏压，使象素输出的波长能够调节到CIE(国际发光委员会)色度标准所定义的可见光谱的任何所希望的颜色。蓝光LED 20被置于叠层的底部，而且是三个器件中最大的一个。由于蓝光对红光和绿色是透明的，故蓝色在底部。最后，如将要描述的那样，采用透明ITO/金属层26对材料进行“分隔”，简化了器件的制造。这是使图2A、2B和2C所示的象素LED器件成为可能的与有机化合物有关的真空生长和制造工艺的非常独特的情况。图2A、2B和2C所示的垂直分层使得有可能以最小的面积来制造三色象素，因此，使其对高清晰度显示器来说很理想。
如图2A、2B和2C所示，各个DH结构器件20、21和22分别能够同时或分别地发射箭头B、G和R所表示的光。注意光是从各个LED 20、21和22的整个横向部分发射的，R、G、B箭头不分别代表实际发射光的宽度。以这种方式，R、G、B颜色的添减由眼睛来组合，导致感觉到不同的颜色和灰度。在彩色观测和显示色度学领域中，这是众所周知的。在所示的偏移结构中，红、绿、蓝光束大体上是重合的。从叠层可产生各种颜色中的任何一种颜色，而且看起来好象是来自一个单一象素的颜色。
DH结构中所用的各有机材料逐层垂直堆叠生长，表示红光的波长最长的器件22位于顶部，而表示蓝光的波长最短的元件20位于底部。以这种方式，可将象素即器件中的光吸收减到最小。各个DH LED器件用ITO/金属层26(具体地说是半透明金属层26M和氧化铟锡层26I)分隔。还可以利用金属淀积的方法来处理ITO层26I，以便在暴露的ITO表面上提供不同的接触区40、41、42和43。这些接触40、41、42和43由诸如Ti/Pt/Au、Cr/Au或Mg/Ag的铟、铂、金、银或合金制成。用常规金属淀积或汽相淀积来淀积接触的方法是众所周知的。像40、41、42和43这样的接触使叠层中的各个LED能够分别地偏置。有机LED材料与透明电极26I之间的化学性质的重大差异，使电极能够用作腐蚀停止层。这使各个象素元件在器件工艺过程中能够被选择性地腐蚀和曝光。
各个LED 20、21、22有其自己的偏压电位源(在本例子中分别示意地示为电池32、31和30)，使各个LED能够发光。当然，可用适当的信号来分别代替电池30、31、32。如所知，LED为了发光(各个DHLED)而要求最小阈值电压，因此用电池符号来示意地表示此激发电压。
EL层20E、21E、22E可以用根据其产生所有原色及其中间色的能力而选定的有机化合物来制造。如以下描述的那样，此有机化合物通常选自三价金属喹啉络合物、三价金属桥式喹啉络合物、席夫碱二价金属络合物、锡(四价)金属络合物、金属的乙酰丙酮化合物的络合物、金属二配位配合基络合物、二磷酸酯、二价金属马来腈二硫醇络合物、分子电荷转移络合物、芳香和杂环聚合物、以及稀土混合螯合物。
三价金属喹啉络合物由图3所示结构式表示，其中M是选自周期表3-13族和镧系的三价金属离子。Al+3、Ga+3和In+3是最佳的三价金属离子。
图3的R包括氢、置换和未置换的烷基、芳基以及杂环原子团。烷基原子团可以是直链或支链，且最好是具有1-8个碳原子。甲烷和乙烷是烷基原子团的恰当例子。最佳的芳基原子团是苯基，而R的杂环原子团的例子包括吡啶基、咪唑、呋喃和噻吩。
R的烷基、芳基和杂环原子团可以用至少一个选自芳基、卤素、氰和烷氧基的最好有1-8个碳原子的替代物来代替。最佳的卤素是氯基。
图3的L原子团表示一种含有吡啶甲基酮、置换与未置换的水杨酰醛(例如用巴比土酸置换的水杨酰醛)的配合基、R(O)CO-结构式(其中R如上定义)的原子团、卤素、RO-结构式(其中R如上定义)的原子团和喹啉(例如8-羟基喹啉)及其衍生物(例如巴比土酸置换的喹啉)。图3所示结构式覆盖的最佳络合物是M为Ga+3而L为氯基的络合物。这种化合物产生蓝色发光。当M为Ga+3而L为甲基碳化物时，则产生在蓝色至蓝绿色区域发光的络合物。利用巴比土酸置换的水杨酰醛或巴比土酸置换的8-羟基喹啉作为L原子团，可望得到黄色或红色发光。利用喹啉作为L原子团，可望产生绿色发光。
图4A和4B示出了可用于本发明的三价金属桥式喹啉络合物。比起现有技术器件中使用的3-喹啉(图3的络合物，其中L为喹啉)，这些络合物产生绿色发光并表现极好的环境稳定性。如上所述，这些络合物中所用的三价金属离子M以Al+3、Ga+3或In+3最好。图4A所示的Z原子团具有SiR结构式，其中R如上定义。Z也可以是形成磷酸盐的P＝O结构式的原子团。
席夫碱二价金属络合物包括图5A和5B中所示的那些，其中M1是选自周期表2-12族的二价金属，最好是Zn(见Y.Hanada等人的论文“Axomethin-Zn络合物薄膜中的蓝色电致发光”，Japanese JAP，Vol.32，pp.L511-L513(1993))。R1原子团选自图5A和5B所示的结构式。R1原子团最好通过吡啶基原子团的胺或氮配位于络合物的金属。X选自氢、各带有1-8个碳原子的烷基、烷氧基、芳基、杂环原子团、磷化氢、卤化物和胺。最佳的芳基原子团是苯基，而最佳的杂环原子团选自吡啶基、咪唑、呋喃和噻吩。X原子团影响席夫碱二价金属络合物在有机溶剂中的溶解度。图5B所示的特定席夫碱二价金属络合物的发光波长为520nm。
本发明EL层中所用的锡(四族)金属络合物产生绿光。这些络合物中包括具有SnL1 2L2 2结构式的那些络合物，其中L1选自水杨酰醛、水杨酸或喹啉(例如8-羟基喹啉)。L2包括除氢之外的前述所有的R原子团。例如，锡(四族)金属络合物(其中L1为喹啉，而L2为苯基)的发光波长(λem)为504nm，这是从固态光荧光测量得到的波长。
锡(四价)金属络合物还包括具有图6结构式的那些络合物，其中Y是硫或NR2(其中R2选自氢和置换的或未置换的烷基和芳基)。烷基原子团可以是直链或支链，且最好有1-8个碳原子。最佳的芳基原子团是苯基。烷基和芳基的替代物包括具有1-8个碳原子的烷基和烷氧基、氰和卤素。L3可选自烷基、芳基、卤化物、喹啉(例如8-喹啉)、水杨酰醛、水杨酸和马来腈二硫醇(”mnt”)。当A是S，Y是CN，而L3是”mnt”时，可望得到红色到橙色之间的发光。
图7所示的M(乙酰丙酮化物)3络合物产生蓝色发射。金属离子M选自周期表3-13族的三价金属和镧系。最佳的金属离子是Al+3、Ga+3和In+3。图7中的R原子团与图3中定义的R相同。例如，当R是甲基，而M分别选自Al+3、Ga+3和In+3时，从固态光荧光测量得到的波长分别是415nm、445nm和457nm(见J.Kido等人的论文“采用镧系络合物的有机电致发光器件”，Journal of Alloys and Compounds，Vol.92，pp.30-33(1993))。
本发明所使用的金属二配位基络合物通常发蓝色光。
这种络合物的结构式为MDL4 2，其中M选自周期表的3-13族的三价金属和镧系。最佳的金属离子是Al+3、Ga+3、In+3和Sc+3。D是图8A所示的二配位基配合基的例子。更确切地说，二配位配合基D包括2-吡啶甲基酮、2-喹啉酮和2-(o-苯氧基)吡啶酮，其中图8A中的R原子团如上定义。
最佳的L4原子团包括乙酰丙酮化物；结构式为OR3R的化合物(其中R3选自Si、C，而R选自与上述相同的原子团)；3，5-二叔丁基苯酚；2，6-二叔丁基苯酚；2，6-二叔丁基甲酚；以及分别示于图8B-8E的H2Bpz2。
作为例子，由铝(吡啶甲基酮)二(2，6-二叔丁基苯氧化物)得到的固态光荧光测量的波长(λem)为420nm。上述化合物的甲酚衍生物也测得为420nm。铝(吡啶甲基酮)二(OSiPh3)以及钪(4-甲氧基-吡啶甲基酮)二(乙酰丙酮化物)各测得为433nm，而铝(2-(o-苯氧基)吡啶)二(2，6-二叔丁基苯氧化物)测得为450nm。
二磷酸酯化合物是另一类可用于根据本发明的EL层的化合物。此二磷酸酯由下面的通用结构式表示：
M2 x(O3P-有机-PO3)y
M2是金属离子。这是一种四价金属离子(例如，当x和y都等于1时，为Zr+4、Ti+4和Hf+4。当x为3而y为2时，此金属离子M2处于二价状态，并包括例如Zn+2、Cu+2和Cd+2)。上述结构式中所用的“有机”意味着任何一种能够用磷酸酯原子团实现二官能化的芳基或杂环荧光化合物。
作为图9A和9B所示的例子，最佳的二磷酸酯化合物包括苯基亚乙烯基二磷酸酯。具体地说，图9A示出了β-苯乙烯基二苯乙烯二磷酸酯，而图9B示出了4，4’-二苯基二(乙烯基磷酸酯)，其中R如前所述，而R4选自最好带有1-8个碳原子的置换的和未被置换的烷基原子团以及芳基。最佳的烷基原子团是甲基和乙基。最佳的芳基原子团是苯基。烷基和芳基的最佳替代物至少包括选自芳基、卤素、氰、烷氧基的最好带有1-8个碳原子的一种替代物。
二价金属马来腈二硫醇(”mnt”)络合物具有如图10所示的结构式。二价金属离子M3包括带有+2电荷的所有金属离子，最好是Pt+2、Zn+2和Pd+2之类的过渡族金属离子。Y’选自氰和置换或未被置换的苯基。苯基的最佳替代物选自烷基、氰、氯基和1，2，2-三氰乙烯基。
L5表示不带电荷的原子团。最佳的L5原子团包括P(OR)3和P(R)3，其中R如上述，即L5可以是螯合配合基，例如2，2’-二吡啶基；菲咯啉；1，5-环辛二烯；或二(二苯磷)甲烷。
如从C.E.Johnson等人的论文“发光的铱(I)、铑(I)和铂(II)二硫酚络合物”(见Journal of the American Chemical Society，Vol.105，p.1795(1983))推导的那样，表1示出了这些化合物的各种组合的发光波长的例子。
                              表1
络合物                                 波长*(nm)
铂(1，5-环辛二烯)(mnt)                  560
铂(P(OET)3)2(mnt)                    566
铂(P(OPh)3)2(mnt)                    605
铂(二(二苯磷)甲烷)(mnt)                 610
铂(PPh3)2(mnt)                       652
*波长得自固态光荧光测量。
用于本发明EL层的分子电荷转移络合物，是含有与电子施主结构相络合的电子受主结构的那些络合物。图11A-11E示出了可以与图11F-11J所示的电子施主结构形成电荷转移络合物的各种适当的电子受主。图11A和11H所示的原子团R与上述的相同。
这些电荷转移材料膜用从分立料池将施主和受主分子蒸发到衬底上的方法，或用直接蒸发预制好的电荷转移络合物的方法来制备。根据何种受主被耦合于何种施主，发光波长范围可从红色到蓝色。
处于固态时有荧光的芳族和杂环族化合物的聚合物，可在本发明中用作EL层。这种聚合物可用来产生各种不同颜色的发射。表2提供了适合的聚合物及其相关发射颜色的例子。
                               表2
聚合物                               发射颜色
聚(对苯撑乙撑)                       蓝到绿
聚(二烷氧基苯撑乙撑)                 红/橙
聚(噻吩)                             红
聚(苯撑)                             蓝
聚(苯基乙炔)                         黄到红
聚(乙烯基咔唑)                       蓝
本发明中所使用的稀土混合螯合物包括键合于二配位基芳族或杂环族配合基的任何镧系元素(例如La、Pr、Nd、Sm、Eu和Tb)。此二配位配合基用来输运载流子(例如电子)，但不吸收发射能量。于是，二配位配合基用来将能量输运到金属。稀土混合螯合物中的配合基的例子包括水杨酰醛及其衍生物、水杨酸、喹啉化物、席夫碱配合基、乙酰丙酮化物、菲咯啉、二吡啶、喹啉和吡啶。
空穴输运层20H、21H和22H可由卟啉化合物组成。此外，空穴输运层20H、21H和22H可至少有一个空穴输运芳族三元胺，这是一种至少含有一个只键合于碳原子(其中至少一个是芳基环的成员)的三价氮原子的化合物。例如，芳族三元胺可以是诸如单芳基胺、二芳基胺、三芳基胺或聚芳基胺之类的芳基胺。在Tang等人的美国专利No.5294870中，公开了其它适合的芳族三元胺以及所有的卟啉化合物，此处将其全部列为参考，只要不相互冲突即可。
根据本发明的叠层有机LED三色象素的制造可用下列二种工艺之一来实现：掩模工艺或干法腐蚀工艺。为了说明的目的，二种待要描述的工艺都假定是双异质结构LED，亦即，对各个有源发射层只用一个有机化合物层，光从底部玻璃衬底表面进入。应该指出的是，每个有源发射层具有多个有机化合物层的多异质结有机LED和/或反转结构(光从叠层的顶表面进入)，也可以由本技术领域熟练人员对所述的工艺稍作修改而加以制造。
图12(A-E)说明了根据本发明的掩模工艺。首先，借助于将衬底50浸入沸腾的三氯乙烯或相似的氯化了的碳氢化合物中大约5分钟，对待要涂覆ITO层52的玻璃衬底50进行清洗。接着在丙酮中冲洗约5分钟，再在甲醇中冲洗约5分钟。然后用超高纯(UHP)氮吹干衬底50。使用的所有清洗溶剂最好都是“电子级”的。在清洗之后，在真空中用常规溅射或电子束方法，在衬底50上制作ITO层52。
然后如下在ITO层52上制作蓝色发光的LED 55(见图12B)。掩模73被置于ITO层52的预定的外部。掩模73和掩模工序中所用的其它掩模，在工艺步骤之间引入和取出时，必须使器件不暴露于潮气、氧和其它可能降低器件使用寿命的沾污物。借助于在充满氮气或惰性气体的环境中替换掩模，或借助于用遥控处理技术在真空环境中将掩模遥控置于器件表面上，可以实现这一点。通过掩模73的窗口，在真空中不暴露于空气而相继淀积了厚度为50-100埃的空穴输运层(HTL)54和厚度为50-200埃的蓝色发射层(EL)56(示于图12B)。然后在EL 56上淀积厚度最好为50-1000埃的电子输运层(ETL)58。然后用例如最好由10％的Ag和90％的Mg或其它低功函数金属或金属合金组成的半透明金属层60M覆盖ETL 58。层60M很薄，最好是小于100埃。可以用诸如汽相淀积、离子束淀积、电子束淀积、溅射和激光烧蚀之类的大量常规定向淀积技术中的任何一种来淀积层54、56、58和60M。
然后，用常规溅射或电子束方法，在金属层60M上制作厚度约为1000-4000埃的ITO接触层60I。此处为方便起见，夹层60M和60I被视为一个单层60，与图2的层26基本上相同。各个层60的低功函数金属部分60M直接与其下的ETL层接触，而ITO层60I与紧靠其上的HTL层接触。注意整个器件制造工艺最好在一直保持真空而不要在各个步骤之间影响真空的情况下完成。
图12C示出了用与制造蓝色发光LED 55所采用的基本上相同的掩模和淀积技术在层60顶部制造的绿色发光LED 65。LED 65包含HTL 62、绿色发射层64和ETL 66。第二金属薄层60M(厚度小于100埃，薄得足以半透明，但不致损失电学连续性。)被淀积在ETL层66上，接着用另一个厚度为1000-4000埃的ITO层60I来形成第二夹层60。
图12D示出的是用相似的掩模和金属淀积方法制作在层60上(具体在60I上)的红色发光LED 75。红色发光LED 75由HTL 70、红色发光EL72和ETL 74组成。然后在LED 75上制作由层60I和60M组成的顶部夹层60。同样，如上述图2实施例所述，在变通实施例中，顶部透明ITO层60I可用也起通过衬底50反射向上的光的平面镜作用的恰当的金属电极来代替，从而降低了从器件顶部出来的光的损失。各个ETL层74、66和58的厚度为50-200埃；各个HTL层54、62和70的厚度为100-500埃；而各个EL层56、64和72的厚度为50-1000埃。为了得到最佳的亮度和效率，含有ITO/金属层的各个层应保持尽可能接近于上述范围的下端，但这些范围不意味着限制。
然后，最好在一个步骤中完成ITO层52上的电接触51和59以及ITO/金属层60的ITO部分60I上的电接触88、89、92、94和96的制作。这些电接触可以是铟、铂、金、银或诸如Ti/Pt/Au、Cr/Au或Mg/Ag之类的组合。可以在器件其它部分被掩模之后，用汽相淀积或其它适当的金属淀积技术来淀积。
掩模工艺的最后步骤是如图12E所示，用绝缘层97覆盖除被掩蔽的所有金属接触51、59、88、89、92、94和96之外的整个器件。绝缘层97是不透潮气、氧气和其它沾污物的，从而防止了LED被沾污。绝缘层97可以是SiO2、Si2N3之类的氮化硅或由电子束、溅射或者热解增强或等离子增强CVD淀积的其它绝缘体。所用的淀积技术应当不使器件的温度升高到120℃以上，因为这样的高温可能使LED的特性变坏。注意120℃是可变的，而且代表了本发明所用的典型有机材料的软化点。
图13(A-F)示出了制造根据本发明的LED叠层的干法腐蚀工艺。参照图13A，首先以相同于上述掩模工艺的方法清洗玻璃衬底102。然后在真空中用常规溅射或电子束方法，在玻璃衬底102上淀积ITO层101。再用常规真空淀积技术，或在聚合物情况下用旋涂或喷涂技术，在ITO层101的整个表面上淀积厚度一般与掩模工艺中相同的HTL 104、蓝色EL105、ETL 106以及含有金属层107M和ITO层107I的夹层。ITO/金属夹层107由直接淀积在ETL层106上的厚度小于100埃的低功函数金属层107M以及金属层107M上的厚度为1000-4000埃的ITO层107I组成。在ITO层107I的整个顶表面上，用低温等离子体CVD方法，淀积厚度为1000-2000埃的氮化硅或二氧化硅掩蔽材料层108。然后在氮化硅层108上旋涂诸如HPR 1400J之类的正光刻胶层109。如图13B所示，光刻胶层109的外沿110(见图13A)被暴露出来并用标准光刻工艺清除掉。暴露的外沿部分110对应于底部ITO层101待要暴露和电连接的区域。参照图13C，用CF4∶O2等离子体清除掉对应于清除光刻胶区域的氮化硅层108的外沿区域111(图13B中规定的)。然后用离子研磨方法或其它等离子体腐蚀，清除ITO/金属层107I和107M的暴露的外沿部分。再用O2等离子体分别相继清除ETL层106、EL层105和HTL层104的相应的暴露的外沿部分，并清除图13D所示的残留光刻胶层109。最后，再次用CF4∶O2等离子体清除掉氮化硅掩模108，得到图13D所示的蓝色LED结构。
除了SiNx 150如所示覆盖之外，同样顺序的干法腐蚀工艺步骤被用来制造蓝色LED顶部的绿色LED，接着如图13E所示，用光刻胶掩模113掩蔽ITO层101的外沿部分。然后进行HTL层114、绿色EL层116等等的淀积(见图13F)。再用相同于制造蓝色LED的光刻和腐蚀方法来完成绿色LED 115的制作。然后用基本上相同的干法腐蚀工艺来制造绿色LED顶部的红色LED 117。再如掩模工艺所述的那样，在带有暴露电接触的适当的图形的LED叠层上，淀积相似于图12E的层97的钝化层119。光刻胶掩模被用来使钝化层119中能够干法腐蚀出一些孔。接着，在孔中淀积金属152。用“剥离”工艺清除最后的光刻胶层和过量的金属。
不管采用掩模方法还是干法腐蚀方法或其它方法，在制造LED叠层之后，都必须恰当地将叠层封装起来，以便获得可接受的器件性能和可靠性。图14(A-C)说明了本发明的用来简化封装并为例如多达4个本发明彩色LED器件提供气密性封装的本发明的实施例。图14(A-B)中所用的与图12E相同的参考号表示完全相同的部分。封装也可以使用几乎完全相同的图13F的结构。参照图14A，在本例子中，在用例如诸如SiNx之类的绝缘层97涂覆整个器件之后，利用熟知的腐蚀/光掩蔽方法分别制作通道孔120、122和124以暴露蓝色、绿色和红色LED(有机发光二极管)的最顶部的金属层60M’、60M”和60M。然后，用常规工艺步骤，在从暴露的金属层60M’、60M”和60M分别到边沿处铟焊块132、133和134的路径中，淀积适当的金属电路126、128和130(通常是金材料)。同样，通过制作的金属(例如金)电路135，阳极端子被制成带有内端接触ITO层52和边沿铟焊块136处的外端，这些都是用常规工艺制作的。然后用诸如SiNx的额外绝缘材料涂覆器件以形成绝缘覆盖，使焊块132、133、134和136沿一边暴露出来。以这种方式，可用常规方法，亦即下述的本发明的封装实施例，容易地封装有机LED器件。
以下分别参照图14A、14B和14C来描述本发明另一实施例的将一个公共衬底50上的4个彩色LED器件做在一个封装结构中的方法。原材料包括涂覆有氧化铟锡(ITO)覆盖层52的玻璃衬底50。下列步骤被用来得到封装的彩色有机LED阵列：
1.用常规方法掩蔽ITO层52，以便在ITO层52顶部的同心正方形带环图形(在此例子中可使用其它一些图形)中淀积SiO2层138。
2.用上述的方法在ITO层52上的区域140中，制作4个共用公共层的三色LED叠层，用以得到例如图12E或13F和14A中的一种结构。
3.借助于掩蔽，淀积金属接触170-181；各终止于SiO2层138上的外端处，分别用来提供外部电连接或键合焊点170’-181’。注意图14A中的接触126、128和130分别与接触170-181中的每相连的三个是同样的。每三个接触一组，亦即170-172、173-175、176-178和179-181，终止于其内端即另一端，以分别提供4个有机LED器件中的每一个分别与金属层60M’、60M”、60M的电连接。本例子中，在所有4个LED器件共用的ITO层52的边沿上，借助于掩模，淀积了另一个金属接触182，用来提供公共阳极连接。注意，若通过恰当的掩蔽和腐蚀，4个LED器件被制作在完全独立的层中，则为以后的阵列必须分别提供4个阳极接触，以便能够以多路复用方式运行。本例子所述的彩色LED阵列是一种非多路复用阵列。
4.借助于在二个步骤中采用“L”形掩模进行掩蔽，或借助于光刻，用例如溅射、或等离子体增强CVD、或电子束淀积方法中的一种方法，在暴露键合焊点170’-181’的连续带或环中，淀积例如第二SiO2层184。
5.在第二SiO2层或带184顶部上的连续带或环186中，淀积Pb-Sn或其它低熔点焊料。
6.在覆盖玻璃188的底部上，淀积待要与焊料密封环186重合的金属环190。
7.将此装备件置于诸如干燥氮气之类的惰性气氛中，加热以熔化焊料环186，从而得到气密密封，使惰性气体陷于内部区域192中。
8.如图14B所示，在装备件上安置盖板玻璃188，使金属环190紧靠焊料环186。
参照图15，其中示出了一种RGB有机LED显示器。点195是省略符号。194的完整显示器包含多个像196的象素。象素排列成XY矩阵以覆盖涂覆有ITO的玻璃片的整个表面区。每个象素包含图2所示的一个堆叠的LED结构。图2中指定为蓝(B)、绿(G)和红(R)的各个端子线，不具有如电池30、31和32那样的固定的偏置装置，而是被拉出并分别连接到适当的水平和垂直扫描处理器197和198，所有这些都在显示发生器199(可能是一台电视机)的控制下。因此，每个LED矩阵至少有二个轴(x，y)，且每个LED至少与二个轴相交。而且，x轴可代表水平轴，而y轴代表垂直轴。如何将诸如NTSC信号之类的电视信号转换成彩色显示用的R、G和B颜色分量，是众所周知的。采用红、绿和蓝作为原色的计算机监视器，也是众所周知的。用垂直和水平扫描方法来驱动和控制这种器件，同样是众所周知的。淀积在显示器表面上的整个象素结构的阵列，用典型的XY扫描方法(如使用XY寻址)来扫描。这些方法被用于有源矩阵显示器中。
人们可以根据所需的信号内容，用脉冲宽度调制来选择性地激活各个DH LED象素的红、绿和蓝输入。以这种方式，显示器各线中的各个LED被选择性地访问和寻址，并被用许多方法(例如借助于脉冲宽度调制或借助于台阶形发生的电压)来进行偏置，以使这些器件发射单一颜色或彩色，致使从所述结构发射的光产生一个具有预定形状和颜色的图象。人们也可以串联扫描各个xy轴，且串联激活矩阵中选定的LED以发光，用以形成具有串联垂直产生的颜色的图象。选定的LED可以被同时激活。
如上所指出，图2所示的垂直分层方法使得能够在极小的区域中制造三色DH LED象素。这就使人们有可能提供诸如具有每英寸300-600线或更高分辨率的显示器之类的高清晰度显示器。用现有技术(其中产生不同颜色的有机发射层或荧光物质是彼此横向分隔的)来获得这样高的分辨率要更困难得多。
基于现代标准，人们能够提供图2所示的LED器件，其有效面积小得足以将数百个象素二极管垂直和水平地堆叠在1平方英寸的面积之内。因此，此制造方法使人们能够得到具有高光强度的极高的分辨率。
图16示出了包含高达N(其中N是整数1、2、3、…N)个LED的叠层的彩色LED器件的本发明的另一实施例。根据将来工艺的水平，N有一个实际限度。例如，用前面图12(A-E)所述的掩模工艺或图13A-13F所述的干法腐蚀工艺，能够提供N层LED的叠层。图16的叠层阵列的基底即底部是例如图13F所示的衬底102上制作有ITO层101的玻璃衬底102。本例子中的覆盖第一LED器件和后面LED各相继包含在ITO层101、HTL层154、EL层156、ETL层158、金属层160和ITO层162上。第N层的LED器件164还包含制作在其最顶部ITO层162上的最顶部金属层(见图13F的层152)。如在图13F的彩色叠层中那样，在叠层上淀积了钝化层119。各个LED器件的EL层156的材料被选来提供相关LED的特定颜色。如在三色器件中那样，波长较短的(蓝色)器件在叠层中必须位于波长较长的(红色)器件的下面，以避免由红色发光层造成的光吸收。为各个LED选择的颜色和叠层LED的实际数目依赖于特定的应用以及所需的颜色和待要提供的灰度容量。这种彩色器件也可用于光通信网络，其中用叠层中给定器件发射的不同的波长来传输不同的光信道。发射的光的固有的同心性质使得有可能将几个波长耦合于一个光纤。在实际的这种叠层阵列中，以例如相似于图14A、14B和14C的叠层彩色LED器件所述的方法，进入孔被制作成达及各个器件的ITO层162，接着淀积恰当的金属化，用以简化封装和叠层内各LED器件的电连接。
此器件可用来提供任何尺寸的低损耗、高分辨率、高亮度的全色平板显示器。这使得本发明的范围扩展到尺寸小至数毫米的显示器，这只是一个实用的限制。显示器上产生的图象可以是分辨率依赖单个LED尺寸的文本或全色图表。
本发明人认为，如上面图1A-16所述，若彩色有机LED要改进成当OLED未激活时对用户基本上全透明，则这种透明的有机发光器件(以下称为TOLED)可直接用于平视显示器和其它应用。为此描述的目的，平视显示器在未激活时，对用户是基本上透明的，从而为用户提供了透视能力。在本例子中，当给定的一个或更多个器件被激活发光时，显示器的受影响部分将借助于上述结合本发明下述实施例的有机LED而照亮单个或彩色显示器。为了实现这一点，本发明人想出了用以克服现有技术在诸如用于有机发光器件(OLED)中的软材料上淀积透明电接触时所涉及的困难而不像使用所知的现有技术通常发生的那样损伤下方各层的方法和设备。本发明人认为，在克服这些问题时，OLED器件可用于采用各种其它显示技术的平视显示器中，这本身将受益于用来制作对用户基本上透明的接触的本发明的下述实施例。例如，可受益于本发明的应用是用于摩托驾驶员头盔上或喷气战斗机驾驶员头盔上的护目镜中的平视显示器，各用OLED来形成图形用以提供仪表、地图、目的地等等的直接图象显示。采用这种OLED平视显示器的其它应用还可包括防风罩、遥控警报器等上的显示器。视频游戏显示器和其它类型显示器也可以包含本发明的OLED。因此，下述的本发明实施例被相信代表了尖端技术中的一个重大进步。
在硬质材料或诸如例如用于无机太阳能电池中的硅(Si)之类的不受50℃以上温度影响的材料上淀积透明接触的方法是已知的。应该指出的是，虽然本发明的下述实施例的预计好处是用来在诸如有机层之类的软材料上制作透明接触，但此方法和设备也可用来在硬质材料上淀积透明接触。
应该指出的是，有关美国专利申请No.08/354674的上述的提供OLED的本发明的实施例，提供了具有从吸收带红移高达0.5eV(电子伏特)的发光带的器件。结果，本OLED在其本身的发射谱上以及整个大部分可见光谱上是高度透明的，从而提供了在无机半导体光发射器中找不到的性能。通过如下所述将本发明的实施例用来提供基本上透明的接触，本发明发现了一类新的真空淀积的有机发光器件，其未激活时的透明度大于71％，并在激活时能够高效率地从二极管顶表面和底表面发射光(量子效率接近或超过1％)。
为了实现上述的结果，本发明人要克服的第一个问题是发现一种能够与下方有机层形成良好的化学键的金属以提供机械稳定性。通过采用镁(Mg)和银(Ag)的金属合金膜，肯定能够提供这样一种金属。但除Mg∶Ag金属合金膜之外，其它金属和/或诸如掺氟的氧化锡、Ca、In、Al、Sm、Y、Yb、MgAl和各种含有这些材料的合金，也可以采用(见Tang等人的美国专利No.5294870)。现今认为Mg∶Ag膜代表了本发明的最佳实施例。若接触由单一金属组成，则此金属必须具有低的功函数。当接触由金属合金组成时，至少一种金属必须具有低的功函数。在使用Mg∶Ag时，Mg具有低的功函数。所选择的金属还必须确保通过用各种材料进行的实验所确定的与有机层的良好的电连接。良好的电连接确保了金属接触即电极能够把足够数量的载流子注入到有机层中。
在解决了确定一种金属或金属合金来提供与下方有机层的良好化学键合和电接触的第一问题之后，本发明人的下一个问题是，在保留诸如低的电阻之类的其它性质的同时，确定如何使接触透明。已知借助于使金属层非常薄，可以获得层的所希望的透明度。但本发明人认为，在本例子中，层必须足够厚，以便在金属层顶部淀积氧化铟锡(ITO)层的所要求的后续工序中保护下方的有机层。而且，薄的Mg层氧化迅速，因此在制作之后必须尽可能快地涂覆ITO，以便保护Mg层。完成这些工作的现有工艺是在高温和高功率淀积中进行的，这可能损伤下方的有机层。因此，本发明人想出了一种用来在非常低的功率和室温(通常为22℃(72F))下，于金属层上淀积ITO层的工艺。
ITO层除了透明外，还是导电的，因此降低了与Mg∶Ag形成的多层接触的电阻。ITO由于通常不提供与有机材料的良好键合(亦即对有机材料的粘附性不好)，而且通常不是使电子进入有机电致发光材料的良好注入体，故不能单独使用。在本例子中，Mg∶Ag层确实提供了对有机层和对ITO层的良好键合，而且是一种良好的电子注入体。
图17示出了本发明人制造的用来提供透明有机发光器件(TOLED)的设计样板。在此例子中，器件300生长在预先涂覆有根据ITO膜的厚度而具有一般为20Ω/口的薄层电阻的透明氧化铟锡(ITO)薄膜304的玻璃衬底302上。注意，虽然衬底302在此例子中由透明玻璃组成，但也可以由诸如例如塑料材料之类的其上能够涂覆ITO的任何其它透明坚固的支持物提供。ITO膜也可用任何适当的导电氧化物或导电透明聚合物来代替。在淀积有机膜之前，用常规方法预先清洗衬底302。用升华方法在低于10-4乇的真空中淀积厚度为200埃的空穴导电化合物N，N’-二苯基-N，N’二(3-甲苯基)1-1’二苯基-4，4’双胺(TPD)，接着淀积厚度为400埃的电子导电的高度电致发光的Alq3(三羟基喹啉铝)层308。为器件300提供电子注入接触的顶层310借助于例如通过50-400埃厚的半透明Mg-Ag合金(大约的原子比为Mg∶Ag＝40∶1)薄电极的掩模(未示出)进行淀积而制成。根据应用，可以采用诸如Mg∶Ag＝50∶1之类的其它原子比，但注意，本发明不意味着要限制为任何特定的比率即接触金属的组分。最后，用溅射淀积在层310 Mg-Ag表面上的厚度为400埃的第二ITO层312来覆盖TOLED器件300。此第二ITO层312在能够生长第二TOLED的顶部，提供了连续的透明导电表面(见上面图12、13和16的描述)。ITO层312被做成尽可能厚，以便降低电阻同时保持可接受的透明度。用常规工艺将电接触314(负极)和316(正极)分别键合于ITO层312和304。
图18示出了本例子中从具有厚度为100埃的Mg-Ag电极310的TOLED的顶部和衬底器件表面测量得到的器件300的输出。这种直径为1mm的TOLED器件的典型工作条件是10-4A和10V驱动电压(加于端子314和316之间)。虽然从顶部接触的光发射相对于从背接触的光发射有稍许红移，但从二个表面的发射谱相似于前述的常规Alq3基器件(C.W.Tang和S.A.VanSlyke，Appl.Phys.Lett.，Vol.51，913(1987)；P.E.Burrows和S.R.Forrest，Appl.Phys.Lett.，Vol.64，2285(1993))。这可能是由Mg-Ag与ITO膜的吸收谱的差别和/或Mg-Ag/ITO电极中界面态造成的吸收所引起的。此例子器件300的发光总内量子效率为0.75％，这与常规Alq3基OLED的效率是可比拟的。通过衬底302的发射强度比从顶部接触312的发射强度高大约10％。
图19详细地示出了具有厚度为100埃的膜310的TOLED 300的透明度与波长的函数关系。在曲线的短波端，由于ITO吸收、Mg-Ag吸收以及Alq3向L2和Bb态的很强的分子跃迁的联合作用，器件变为不透射。但注意，器件在Alq3的峰值发射波长(530nm)处是63％透明的，且这一透明度延伸于可见红色波段。还由于Mg-Ag顶部接触的吸收，红外区中显然有一些损耗。图20示出了具有厚度范围为50-400埃的Mg-Ag膜310的Mg-Ag接触310在波长530nm处的透射。对于最薄的Mg-Ag膜，观察到了92％的透明度。本发明人迄今得到的最薄的可工作的TOLED器件具有厚度为75埃的Mg-Ag接触310，对应于81％的接触透明度和71％的总器件透明度。拟合于图20数据的直线的斜率，给出Mg-Ag的光吸收系数为1.1×106cm-1，这是与计算得到的180埃的趋肤深度一致的。
注意，当上述样板TOLED器件在绿色光谱区发射时，由于从吸收到发射的很大的弗兰克-康登红移是许多有机材料的特性，故所示的在可见光谱的任何波段发射的有机器件的结构应该工作得同样好。因此采用简单的制造工艺，有可能制成可独立寻址的彩色发射元件叠层。而且，如前所述，此结构也应当可用于聚合物基的OLED。例如，具有覆盖ITO层的Mg∶Ag合金薄膜同样地被描述分别用作图2A、2B和2C的OLED器件的层26M和26I，用以提供改进的透明接触26；并用作图12B、12C、12D和12E的层60M和60I，以及图13A、13B、13C、13D、13E和13F的层107M和107I，用以提供改进的透明接触60和107。同样，具有覆盖ITO层312的Mg∶Ag层310可用来代替图14A的OLED器件的金属层60M’、60M”和60M的金属，以及图16的OLED器件的金属层160。以这种方式可得到实用的TOLED彩色器件。
下面描述对于有机发光器件或其它器件，将透明接触置于有机材料层上的方法和设备。在本例子中，第一步骤是用从电阻加热的钼舟同时热蒸发各组分金属原子的方法，在靶有机层上分别淀积例如40∶1的Mg∶Ag合金薄膜。如前面参照图20所示，在决定得到的接触的透明度时，金属合金膜的厚度是主要的。图21示意地示出了实现这一点的系统即设备。注意在本发明的蒸发系统和其它系统的下列描述中，本发明人在此例子中所用的实际元件，与供应这些元件的厂家的名称和地址的索引一起，列于下面的表中。
下面详细描述图21所示的在有机衬底上淀积Mg∶Ag膜的蒸发系统。
在由Alcatel 150l/s的涡轮泵(E2)与Alcatel初级泵(E3)和冷阱(E4)一起保持的大约10-7乇的背景压力的真空室(E1)中，进行Mg∶Ag膜蒸发。在本例子中，Ag和Mg金属源被装于用10kW(E6)和1kW(E7)电源电阻加热的钼(Mo)舟(E5)中，以便蒸发或汽化Mg∶Ag。衬底(E8)被置于Mo舟(E5)之上30cm(d1)，并用水冷的不旋转的衬底夹具(E9)固定。位于Mo舟(E5)和衬底(E8)之间路径中的快门(E10)可遥控选择性地操作成开启或关闭的位置，以便分别使启动或阻挡衬底(E8)上的Mg∶Ag蒸发膜淀积。注意在最佳淀积系统中，用二个快门(E10A，E10B，未示出)来代替单个快门(E10)，用以分别独立地阻挡或开启来自相关舟(E5)的Mg和Ag蒸汽流向衬底(E8)。用位于衬底下的膜厚监测器(E11)来测量淀积膜的厚度。为了提供对二个舟的蒸发速率的独立测量，还有二个监测器(E12，E13)分别位于各个Mo舟(E5)之上。
如所述，图21的系统按下列步骤运行，以便在衬底(E8)上淀积本例子的Mg∶Ag膜：
将快门(E10)置于关闭位置。
将蒸发室(E1)抽空到1×10-6乇(但最好是10-3-10-10乇)。
接通10kW电源(E6)并缓慢提高其功率输出直至Ag开始熔化。
在衬底-膜厚度监测器(E11)上设定Ag的密度和声学阻抗参数。
设定10kW电源(E6)的输出，使此例子中由衬底厚度监测器(E11)记录的Ag的淀积速率为每秒0.1埃，但可以高达每秒5埃。注意Ag厚度监测器(E12)记录的速率(R1)。
借助于按需要调节10kW电源(E6)的输出，在整个淀积过程中保持R1恒定。
在衬底-膜厚度监测器(E11)上设定Mg参数。
设定1kW电源(E7)的输出，使由衬底厚度监测器(E11)记录的Mg的淀积速率为每秒5埃，但此例子中最好是每秒0.1-10埃。注意Mg厚度监测器(E13)记录的速率(R2)。
借助于按需要调节1kW电源(E7)的输出，在整个淀积过程中保持R2恒定。
将衬底(E8)安装在衬底夹具(E9)上。
将快门(E10)置于开启位置。
淀积100埃的Mg∶Ag合金，但在本例子中也可以是50-500埃。
在衬底(E8)上淀积Mg∶Ag合金膜之后，将衬底从热蒸发室(E1)经由装料密封室(S4)传送到RF溅射系统的溅射室(S1)(见图22)。在此例子的这一传送过程中，通过使用装料密封室(S4)，样品保持在真空或诸如氮气或氩气之类的惰性气氛中。
接着，在室(S1)中，用RF溅射方法在Mg∶Ag金属合金膜顶部淀积氧化铟锡(ITO)膜。此ITO膜的电阻率为1.5×10-3Ωcm。在本例子中，ITO膜的厚度为400埃。
本例子中图23所示的溅射系统被安置在高真空室(S1)中，高真空室的背景压力用CTI-Cryogenics Cryo-Torr 8低温深冷泵(S2)保持在1×10-3-1×10-10乇的范围(背景压力最好较低，以便降低与环境气体的相互作用)。通过闸阀(S3)固定于此室的是背景压力由Leybold Turbovac 50涡轮泵(S5)保持在大气压到1×10-10乇范围(最好是较低的背景压力)的装料密封室(S4)。样品通过装料密封室(S4)被引入溅射系统并在完成淀积时被取出。在本例子中，Pure Tech.，Inc制造的溅射靶(S6)是SnO2∶In2O3＝10∶90(重量比)的纯度为99％的材料。靶(S6)的直径为2英寸，厚度为八分之一英寸。八分之一英寸厚的铜背板(S17)用真空环氧树脂固定于靶(S6)的背面，以防止靶(S6)过热和破裂。靶(S6)与Advanced Energy自动可调阻抗匹配网络(S9)一起，装在由Advanced Energy RF电源(S8)(最大RF功率输出为600W，工作频率为13.56MHz)供电的AJA International磁控溅射枪(S7)中。至少提供20W RF功率的RF电源是足够的。位于溅射枪(S7)和靶(S6)上的快门(S10)可以选择性地置于开启或关闭位置，以分别启动或防止衬底(S11)上的溅射膜淀积。衬底(S11)被置于装有快门的靶(S6)的上方15cm(d2)，并用水冷的不旋转的衬底夹具(S12)固定。注意d2可以是5-30cm，但也可以更大。用位于衬底(S11)下的校准的膜厚监测器(S13)来测量淀积膜的厚度。溅射气体是纯度为99.9999％的氩气(Ar)和纯度为99.998％的氧气(O2)的混合物。进入溅射室(S1)的气体流用单个MKS质量流量控制器(S14)来控制。溅射室(S1)内部的气体压力用MKS Baratron 121A型绝对压力传感器(S15)监测，并用位于低温深冷泵(S2)前的蝶形阀(S16)控制。
图23的溅射系统按下列步骤运行，以便在Mg∶Ag膜顶部淀积ITO层：
从真空室(E1)移出样品。
将样品引入装料密封室(S4)。
将装料密封室抽空到其背景压力。
将样品传送到溅射室(S1)中，并置于溅射靶(S6)上。
将靶快门(S10)置于关闭位置。
将流入溅射室的氩气(Ar)流设定于200sccm的最佳流速(根据系统抽速可为20-1000sccm)，氧气(O2)流最好设定于0.1sccm(根据氩气流速和溅射功率，可以设定于0.0-100sccm，其中较高的溅射功率要求较高的氧气流速)。
设定蝶形阀(S16)以保持20毫乇的室内压力，在本例子中最好低达1毫乇，但必须足以点燃等离子体并维持等离子体。
将RF电源(S8)的输出功率设定于15W-30W并启动电源。当自动调节阻抗匹配网络(S9)发现最佳设定时，等离子体应该点燃。
借助于设定蝶形阀(S16)，将溅射室(S1)内部的压力降低到5毫乇，以便在下一步骤中当功率降低时维持等离子体。
缓慢地将RF电源(S8)的输出功率降低到等于或小于5W，确保阻抗匹配网络(S9)有足够的时间来响应这一变化。
将靶快门(S10)置于开启位置。
根据ITO层透明度与其电导率之间所需的平衡，淀积50-600埃的ITO。
注意本发明的重要实施例是在溅射ITO时采用低的RF功率(5W或更低)来淀积Mg∶Ag层上的ITO薄膜，以避免损伤下方的有机层。在溅射室中使用诸如Xe∶Ar＝1∶10或CH3∶Ar＝1∶20之类的不同的气体混合物，RF功率可降低到5W以下，在保持ITO膜生长速率的情况下，进一步避免了对有机层的损伤。溅射室中的RF功率最好缓慢地降低到维持等离子体点燃所需的最小瓦数。
下面表1给出的参考号为(E1)-(E13)的图21淀积系统的以及参考号为(S1)-(S17)的图23溅射系统的零件表，列出了零件或型号以及有关制造厂家。表1后面是厂家索引，提供了验证过的厂家全名及其最新地址和电话号码。应该指出的是，本发明不意味着要限制使用所示的元件和零件以及厂家，此处提出来只是为了充分说明本发明人在进行其发明到实验性设计样板过程中所使用的设备。
表1项目    品名                    型号               制造厂家E1      真空室                  DV-502A            DentonE2      150l/s涡轮泵            CFF-450 Turbo      AlcatelE3      初级机械泵              20008A             AlcatelE4      液氮冷阱                standard           DentonE5      钼源舟                  standard           MathisE6      10kW电源                standard           DentonE7      1kW电源                 standard           DentonE8      用户提供的衬底E9      水冷衬底夹具            custom             DentonE10     快门                    standard           DentonE11     膜厚监测器                      STM-100/MF       SyconE12     膜厚监测器                      STM-100/MF       SyconE13     膜厚监测器                      STM-100/MF       SyconS1      真空室                                           DCA Inst.S2      低温深冷泵                      Cryo-Torr 8      CTIS3      闸阀(直径6英寸)                 GC-4000M         MDCS4      装料密封室(6英寸，6             custom           MDC
    路交叉)S5      涡轮泵                          Turbovac 50      LeyboldS6      SnO2∶In2O3＝10∶90靶(直    带Cu背板(S17)    Pure Tech
    径2英寸)S7      RF磁控溅射枪                                     AJA Intern.S8      600W 13.56MHz RF电源            RFX-600          Adv.EnergyS9      阻抗匹配网络                    ATX-600          Adv.EnergyS10     S7的组成零件                                     AJA Intern.S11     用户提供的衬底                  customS12     水冷衬底夹具                    custom           DCA Inst.S13     膜厚监测器                      STM-100/MF       SyconS14     质量流量控制器                  1259C            MKSS15     绝对压力传感器                  Baratron#121A    MKSS16     蝶形阀                          L6691-301        VarianS17     Cu背板                          Epoxied to(S6)   Pure Tech
制造厂家索引
Adv.Energy：
Advanced Energy Industries，Inc.
1600 Prospect Parkway，Fort Collins，CO 80525
(303)221-4670
AJA Intern.：
AJA International
North Scituate，MA 02060
(800)767-3698
Alcatel：
Alcatel Vacuum Products，Inc.
Hingham，MA 02043
(617)331-4200
CTI：
CTI-Cryogenics
Mansfield，MA 02048
(508)337-5000
DCA Inst.
DCA Instruments，Inc.
400 West Cummings Park，Suite 3900，Woburn，MA 01801
(617)937-6550
Denton：
Denton Vacuum，Inc.
Moorestown，NJ 08057
(609)439-9100
Leybold：
Leybold Vacuum Products，Inc.
Export，PA 15632
(800)443-4021
Mathis：
R.D.Mathis Co.
2840 Gundry Ave.，P.O.Box 6187，Long Beach，CA 90806
(310)426-7049
MDC：
MDC Vacuum Products Corp.
Hayward，CA 94545
(510)887-6100
MKS：
MKS
6 Shattuck Rd.，Andover，MA 01810
(508)975-2350
Pure Tech：
Pure Tech，Inc.
Carmel，NJ 10512
(914)878-4499
Sycon：
Sycon Instruments
6757 Kinne St.，East Syracuse，NY 13057
(315)463-5297
Varian：
Varian Vacuum Products
Lexington，MA 02173
(800)8-VARIAN.
在Mg∶Ag膜310上生长ITO层312的本发明另一实施例中(见图17)，最近发现，借助于用上面给出的非破坏性(慢速)方法生长第一个50-100埃，接着用较高的RF电源(E8)的功率设定(例如20-40W)增加生长速率使接触312更厚，可以提高ITO的生长速率。由于已经有了在(S8)功率设定较低(例如1-7W)时生长的厚度为50-100埃的保护顶盖，故这一快速生长的第二ITO层没有能力渗透慢速生长的第一ITO接触而破坏下方的Mg∶Ag层和有机层310与308。还发现，有机层的Alq3及其有关化合物完全可免于这种损伤，而蓝光化合物是易受损伤的。结果，本发明人现在是在“双异质结构”(见图1A)中例如首先置入TPD 306，然后置入厚度为50-1000埃的蓝色发光材料层，接着置入厚度为300-1000埃的Alq3层。得到的TOLED器件仍然发蓝光。
本技术领域的熟练人员可以理解对此处所述的本发明的各个实施例的各种修正。这些修正意味着要被所附权利要求的构思与范围覆盖。例如，在本发明的另一实施例中，借助于从图1C所示的有机器件，或从淀积的金属磷化物膜来制作LED 20，而不是所有三层都置于真空中，也可以提供诸如上述图2的三色器件之类的彩色叠层LED器件。二个其余的叠层LED可以用真空淀积或其它方法来制作。Mg∶Ag合金的组分也可以是从Mg∶Ag＝1∶1到40∶1直到具有恰当化学性的100％的Mg。在又一实施例中，可以用预溅射、喷涂或浸入方法来制作TOLED器件的ITO层。

Claims (62)

1.一种至少包含一个在不带电时透明的有机发光器件的发光器件，它包含：
具有顶表面和底表面的透明衬底；
涂于所述衬底顶表面的透明的第一氧化铟锡薄膜涂层；
涂于所述第一氧化铟锡层上的透明的空穴导电材料涂层；
覆盖所述空穴导电材料的透明的电子导电且高度电致发光的有机材料层；
涂于所述有机材料层上的透明的较薄的金属电极膜；
覆盖所述金属电极膜的透明的第二氧化铟锡薄膜涂层；以及
用来接收偏压以激发所述器件并使其从其顶表面和底表面发射给定颜色的光的键合于所述第一和第二氧化铟锡层的第一和第二电接触。
2.权利要求1的发光器件，其中所述的金属电极膜由镁和银的合金组成。
3.权利要求2的发光器件，其中所述的合金的原子比镁∶银的范围为1∶1-40∶1-100∶0。
4.权利要求1的发光器件，其中所述的有机材料层包含三羟基喹啉铝。
5.权利要求2的发光器件，其中所述的有机材料层包含三羟基喹啉铝。
6.权利要求1的发光器件，其中所述的衬底由玻璃组成。
7.权利要求1的发光器件，其中所述的空穴导电材料由N，N’-二苯基-N，N’二(3-甲苯基)1-1’二苯基-4，4’双胺组成。
8.权利要求1的发光器件，其中所述的空穴导电材料层的厚度为200埃。
9.权利要求1的发光器件，其中所述的空穴导电材料层的厚度为400埃。
10.权利要求1的发光器件，其中所述的金属电极膜的厚度范围为50埃-400埃。
11.权利要求1的发光器件，其中所述的第一和第二氧化铟锡层的厚度分别是1000埃和400埃。
12.一种发光器件，它包含：
在层状结构中彼此层叠的多个权利要求1所述的发光器件；
将所述多个发光器件分隔开的多个透明的导电层；以及
多个第三电接触，它们各自分别键合于所述多个导电层中的一个，用以启动各个发光器件在其相关的第一和第三接触之间接收分立的偏置电位以激发它通过其相关的叠层发射光。
13.权利要求12的发光器件，其中叠层中的各个所述发光器件在被激发时，通过叠层发射不同波长即颜色的光。
14.一种制造不带电时透明的彩色发光器件结构的方法，它包含下列步骤：
在透明衬底上制作第一透明导电层；
在所述第一透明导电层上淀积透明的第一空穴输运层；
在所述第一空穴输运层上淀积透明的第一有机发射层，以提供第一发射颜色；
在所述第一有机发射层上，用汽相淀积方法淀积透明的第一电子输运层；
在所述第一电子输运层上，用溅射方法淀积第二透明导电层，所述第二透明导电层用来接收第一偏置电位；
在所述第二透明导电层上淀积透明的第二空穴输运层；
在所述第二空穴输运层上淀积透明的第二有机发射层，以提供第二发射颜色；
在所述第二发射层上，用汽相淀积方法淀积透明的第二电子输运层；以及
在所述第二电子输运层上，用溅射方法淀积第三透明导电层，所述第三透明导电层用来接收第二偏置电位。
15.权利要求14的方法，还包含下述步骤：在淀积所述第一空穴输运层之前，掩蔽所述第一透明导电层的一个区域，以便暴露所述第一透明导电层的所述区域，从而使所述第一偏置电位能够施加于所述第二透明导电层与所述第一透明导电层的所述区域之间。
16.权利要求14的方法，在淀积第一空穴输运层之后还包含下述步骤：将所述第一空穴输运层的一个区域腐蚀掉，以暴露所述第一透明导电层的一部分，从而使所述第一偏置电位能够加于所述第二透明导电层和所述第一透明导电层的所述暴露部分之间。
17.权利要求14的方法，其中所述的用来在所述第一有机发射层上淀积第一电子输运层以及在所述第二有机发射层上淀积第二电子输运层的汽相淀积步骤，各包括：
将所述衬底置入真空室，使所述衬底上的待要涂覆的第一和第二有机发射层中的一个暴露出来；
选择置于所述真空室的待要淀积在所述第一和第二有机发射层中的一个上作为电子输运层的金属或金属合金；
将所述真空室中的压力降低到为1×10-6乇；
熔化金属或金属合金组分以产生所希望的淀积速率，以便在所述第一和第二有机层中的暴露的一个上进行汽相淀积；
监测正在淀积的所述金属的厚度；以及
当达到所希望的厚度时，阻挡通向所述第一和第二有机发射层中的一个的汽相金属流。
18.权利要求17的方法，其中所述的以在所述第一电子输运层上溅射第二透明导电层和在所述第二电子输运层上溅射第三透明导电层的方法而进行的淀积步骤，各包含下列步骤：
将所述衬底置入装料密封室，使接纳第二或第三导电层的第一和第二电子输运层中的一个暴露；
将所述装料密封室中的压力降低到1×10-7乇；
在真空下将衬底从所述装料密封室传送到所述溅射室；
将所述衬底置于溅射靶上；
将氩气流通入所述溅射室；
将氧气流通入所述溅射室；
将所述溅射室中的压力保持在20毫乇；
形成点燃等离子体的射频功率和阻抗匹配，以便借助于打开靶快门而开始将所述靶材料溅射到所述第一和第二电子输运层中暴露的一个；
缓慢地将射频功率电平降低到维持所述等离子体点火的最低电平；以及
在有关的透明导电材料溅射淀积到所要求的厚度之后，关闭所述靶快门。
19.权利要求17的方法，其中所述的第一和第二电子输运层各由镁∶银金属的合金制成。
20.权利要求18的方法，其中所述的氩气的流速为200sccm。
21.权利要求18的方法，其中所述的氧气的流速为0.1sccm。
22.权利要求19的方法，其中所述的熔化步骤包括下列步骤：
将银的淀积速率定为每秒0.1埃；以及
将镁的淀积速率定为每秒5埃。
23.一种至少包含一个在不带电时透明的有机发光器件的发光器件，它包含：
具有顶表面和底表面的透明的衬底；
涂于所述衬底顶表面的透明的第一导电材料薄膜涂层；
至少一个包含覆盖所述第一导电材料层的高度电致发光的有机材料的透明的层；
覆盖所述有机材料层的透明的第二导电材料薄膜涂层；以及
用来接收偏压以激发所述器件并使其从其顶表面和底表面发射给定颜色的光的键合于所述第一和第二导电涂层的第一和第二电接触。
24.权利要求23的发光器件，其中所述的第一导电层由氧化铟锡薄膜涂层组成。
25.权利要求23的发光器件，其中所述的第二导电材料涂层包含：
覆盖所述有机材料层的低功函数金属层；和
覆盖所述低功函数金属层的氧化铟锡层。
26.权利要求25的发光器件，其中所述的低功函数金属由低功函数镁和银的合金组成。
27.权利要求23的发光器件，还包含提供夹在所述第一导电材料涂层和所述电致发光有机材料层之间的空穴输运层的透明的空穴导电材料层。
28.权利要求27的发光器件，还包含提供夹在所述第二导电材料涂层和所述电致发光有机材料层之间的电子输运层的透明的电子导电材料层。
29.权利要求26的发光器件，其中所述的合金的原子比镁∶银的范围为1∶1-40∶1-100∶0。
30.权利要求23的发光器件，其中所述的有机材料层包含三羟基喹啉铝。
31.权利要求26的发光器件，其中所述的有机材料层包含三羟基喹啉铝。
32.权利要求23的发光器件，其中所述的衬底由玻璃或塑料材料中的一种组成。
33.权利要求27的发光器件，其中所述的空穴导电材料由N，N’-二苯基-N，N’二(3-甲苯基)1-1’二苯基-4，4’双胺组成。
34.权利要求27的发光器件，其中的空穴导电材料层的厚度为200埃。
35.权利要求25的发光器件，其中所述的低功函数金属层的厚度范围为50埃-400埃。
36.权利要求24的发光器件，其中所述的第一和第二氧化铟锡层的厚度分别是1000埃和400埃。
37.一种发光器件，它包含：
在层状结构中彼此层叠的多个权利要求23所述的发光器件；
将所述多个发光器件分隔开的多个透明的导电层；以及
多个第三电接触，它们各自分别键合于所述多个导电层中的一个，用以启动各个发光器件在其相关的第一和第三接触之间接收分立的偏置电位以激发它通过其相关的叠层发射光。
38.权利要求37的发光器件，其中叠层中的各个所述发光器件在被激发时，通过叠层发射不同波长即颜色的光。
39.一种有机发光器件结构，包括：
在衬底上形成的第一导电层；
在第一导电层上形成的有机透明发光器件；
在有机透明发光器件上形成的厚度为50-400埃的透明导电金属层；以及
在透明导电金属层上形成的第二导电层，其中，所述第二导电层包括氧化铟锡以外的透明导电氧化物。
40.权利要求39的有机发光器件结构，其中所述透明导电金属层的厚度小于100埃。
41.权利要求39的有机发光器件结构，其中所述透明导电金属层所含金属的功函数小于4eV。
42.权利要求39的有机发光器件结构，其中所述透明导电金属层包括镁。
43.权利要求40的有机发光器件结构，其中所述透明导电金属层包括镁。
44权利要求41的有机发光器件结构，其中所述透明导电金属层包括镁。
45.权利要求42的有机发光器件结构，其中所述透明导电金属层还包括银。
46.权利要求43的有机发光器件结构，其中所述透明导电金属层还包括银。
47.权利要求44的有机发光器件结构，其中所述透明导电金属层还包括银。
48.权利要求39-47中任一项的有机发光器件结构，其中所述衬底是透明的。
49.权利要求39-47中任一项的有机发光器件结构，其中所述衬底是刚性的。
50.权利要求48的有机发光器件结构，其中所述衬底是刚性的。
51.权利要求39-47中任一项的有机发光器件结构，其中所述第一导电层是透明的。
52.权利要求48的有机发光器件结构，其中所述第一导电层是透明的。
53.权利要求49的有机发光器件结构，其中所述第一导电层是透明的。
54.权利要求50的有机发光器件结构，其中所述第一导电层是透明的。
55.权利要求39-47中任一项的有机发光器件结构，其中所述第一导电层包括反射金属层。
56.权利要求48的有机发光器件结构，其中所述第一导电层包括反射金属层。
57.权利要求49的有机发光器件结构，其中所述第一导电层包括反射金属层。
58.权利要求50的有机发光器件结构，其中所述第一导电层包括反射金属层。
59.权利要求51的有机发光器件结构，其中所述第一导电层包括反射金属层。
60.权利要求52的有机发光器件结构，其中所述第一导电层包括反射金属层。
61.权利要求53的有机发光器件结构，其中所述第一导电层包括反射金属层。
62.权利要求54的有机发光器件结构，其中所述第一导电层包括反射金属层。
CN97193731A 1996-03-06 1997-02-15 发光器件及其制造方法和有机发光器件结构 Expired - Lifetime CN1123034C (zh)

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CN1215500A (zh) 1999-04-28
US6596134B2 (en) 2003-07-22
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