CN1432198A - 基于led的发射白色的照明单元 - Google Patents

基于led的发射白色的照明单元 Download PDF

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CN1432198A
CN1432198A CN01810321A CN01810321A CN1432198A CN 1432198 A CN1432198 A CN 1432198A CN 01810321 A CN01810321 A CN 01810321A CN 01810321 A CN01810321 A CN 01810321A CN 1432198 A CN1432198 A CN 1432198A
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emission
fluorescent material
lighting unit
led
white
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A·艾伦斯
F·耶曼
M·奥斯特塔
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Osram GmbH
Ams Osram International GmbH
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Osram Opto Semiconductors GmbH
Patent Treuhand Gesellschaft fuer Elektrische Gluehlampen mbH
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Abstract

一种发射白色的发光转换LED，它采用一种除了Ca和Mg之外还含有铕掺杂的氯硅酸盐荧光材料，以及采用一种稀土的，尤其Y和/或Tb的石榴石荧光材料。因此可以达到高的显色性，以及在不同温度情况下的光技术特性的高稳定性。

Description

基于LED的发射白色的照明单元
                     技术领域
本发明涉及一种基于LED的发射白色的照明单元，其中，所述的LED初级发射UV射线或蓝色光。此外将至少一种发射黄色和一种发射绿色的荧光材料用于部分地转换初级射线。采用一种尤其含有Y和/或Tb的，Ce活化的石榴石作为黄色的荧光材料。采用一种Eu活化的氯硅酸钙镁(Ca8Mg(SiO4)4Cl2)作为绿色的荧光材料。
                     现有技术
从电化学学会杂志(J.Electrochem.Soc.)，1992，622页中已经公开了一种氯硅酸盐荧光材料，及其应用于UV和蓝色光激发，该氯硅酸盐荧光材料是用Eu掺杂的(Eu2+掺杂的磷Ca6Mg(SiO4)4Cl2的发光特性和能量变换)。这种荧光材料以绿色发光。未说明这种荧光材料的具体应用领域。
当今通过组合约在460nm上发射蓝色的Ga(In)N-LED和发射黄色的YAG∶Ce3+荧光材料，来生成输出白色光的发光转换LED(US 5 998925和EP 862 794)。由于它们的基于缺少颜色组分(首先缺少红色分量)的不良的显色性，却只能有限制地将这些白色光LED使用于通用照明目的。一个替换的方案是混合三种共同产生白色的颜色RGB(红、绿、蓝)，请参阅譬如WO 98/39805。
                     本发明的阐述
本发明的任务是提供一个按权利要求1前序部分的基于LED的照明单元，该照明单元发射白色，并尤其具有高的显色性。
通过权利要求1的特征部分来解决这些任务。在从属权利要求中可找到特别有利的扩展方案。
白色LED的迄今的解决方案尤其要么基于RGB配方，也就是混合三种颜色，即红、绿和蓝色，其中，可以通过一种荧光材料，或通过LED的初级发射来实现后者的组分。第二个简化的解决方案象开始时讨论过的那样是基于混合蓝和黄色(BG配方)的。
按本发明第一次应用一种完全新的，基于BGG混合的，也就是组合蓝、黄和绿颜色的方案。在此主要的是，黄色荧光材料此时是如此宽带的，使得它们在红色谱段中也具有足够的发射分量，尤其在≥620nm的谱段中的可见光中具有它们总发射的至少20％的分量。
一种优选具有选自Y、Tb、Gd、Lu、和/或La的SE的稀土(SE)的，Ce活化的石榴石尤其表明为合适的发射黄色的荧光材料。Y和Tb的组合是优选的。此时，在足够的红色分量的意义上通过Tb的长波的推移起着特别积极的作用。
一种按本发明用铕(Eu)掺杂的氯硅酸钙镁基本结构特别优选适合作为发射绿色的荧光材料(它的峰值发射波长优选位于500至525nm段中)。有时也可以以小的分量添加微量的其它掺杂物质，尤其是锰(Mn)用于微调。一个其它的替换方案是SrAl2O4∶Eu2+或Sr4Al14O25∶Eu2+类型的绿色的荧光材料。
绿色荧光材料的色品位置在颜色图中与黄色荧光材料的色品位置和蓝色LED(或蓝色荧光材料)的色品位置共同撑起一个宽广的三角形，因而创造了与专门要求相匹配的附加的可能性。与此相反地，不同石榴石的色品位置的变化宽度是显著较小的。可达到的色温因此也可以分散在一个典型地为4000至10000k的广阔的范围上。
就开发以白色发射的照明单元而言，本发明是特别有利的。此时涉及一个要么基于LED阵列的，要么基于各个LED的照明单元，或者直接涉及一种发光转换LED，在该发光转换LED中所述荧光材料直接或间接与芯片接触，也就是直接涂敷到芯片上，或埋入在包围它的树脂中。
通过将具有300和470nm之间发射波长(峰值)的，发射UV或蓝色光(在此总称为＂短波长的＂)的LED与本发明的荧光材料混合物相组合，可以实现白色光的生成，该荧光材料混合物完全或部分地吸收LED的射线，并且其本身在如下的谱段中发射，该荧光材料混合物与LED的光的添加混合会产生具有良好显色性的白色光。有时必须添加一个发射蓝色的附加的荧光材料组分(譬如BAM)。在约330至350nm的发射波长(峰值)时的UV-LED的情况下，和在约450至470nm的发射波长(峰值)时的蓝色LED的情况下，特别有效的激发将获得成功。
因此譬如通过混入20至50重量％的氯硅酸盐荧光材料，达到了基于石榴石荧光材料的公知白色LED的改善的显色性。发射黄色的荧光材料是一种按分子式SE3(Al，Ga)5O12∶Ce的稀土(SE)Y、Gd、Lu、La和/或Tb的石榴石，尤其是具有SE＝Y和/或Tb，尤其是符合分子式YAG∶Ce或TbAG∶Ce。
从上述科学文献中公开了荧光材料Ca8Mg(SiO4)4Cl2∶Eu2+，而在那里未说明任何具体的应用。这种荧光材料按本发明显示出一种对于在白色LED上应用的良好适用性，在由初级的UV光源(300至390nm)激发的三颜色混合物的基础上这种荧光材料特别有利。但是它也适合于在具有蓝色初级光源(430至470nm)的白色LED上的专门用途。铕的分量x有利地在x＝0.005和1.6之间，并尤其在x＝0.01和x＝1.0之间。此时假设Ca8-xEuxMg(SiO4)4Cl2为总分子式。
以小的量(直至约Eu的克分子分量的20％)添加作为除Eu之外的其它掺杂物的Mn提供了这种可能性，即有针对性地将所述的发射从绿色谱段稍微更多地向长波长的方向推移，也就是进入黄色的谱段。这有以下的优点，所述的发射可以更好与人眼适配，并因此也改善了视觉效率。Mn的分量y此时最高应位于y＝0.1。不添加锰的，在x＝0.05和0.8之间的铕的分量是特别优选的。
当使用在光源中时，尤其在LED中的情况下，铕的浓度影响发射光的色品位置。经过两种浓度Eu∶Mn之比可以附加地精细调节这种荧光材料的色品位置，在LED中这简化或优化了与可能的其它(黄色或蓝色)荧光材料的匹配。
譬如也可以在一种设备中应用本发明的荧光材料，在该设备中(初级发射UV或蓝色的)LED阵列照明了透明板上的荧光材料，或在该设备中各个LED照明了安放在透镜上的荧光材料。
为了实现高显色性的白色LED，特别有利地应用本发明的荧光材料。为此要么单独，要么以混合物涂敷所述的荧光材料，并有时与尽可能透明的粘合剂组合起来(EP 862 794)。所述的荧光材料完全或部分地吸收发射UV/蓝色光的LED的光线，并在另外的谱段中(主要为黄和绿色)重新如此宽带地(即以明显的红色分量)发射光线，使得形成一种具有所希望的色品位置的总发射。迄今几乎没有象这里所说明的荧光材料那样以其组合来良好地满足这些要求的荧光材料。它们展示了高的量子效率(70％上下)，并同时展示了一种基于人眼的敏感性被感受为亮的光谱发射。可以在广阔的范围中调节所述的色品位置。
一种LED(发光二极管)适合于作为光源，这种LED要么通过直接混合具有蓝色谱段(430至470nm)中的初级射线的、发射绿或黄色的荧光材料，要么通过借助多种荧光材料将初级发射UV的射线转换成白色的办法(借助三种荧光材料的完全的BGG混合)来生成白色光。在这里，一般蓝、黄和绿的概念应理解为在蓝色段：430至470nm，绿色段：490至525nm和黄色段：545至590nm中的发射最大值。
发射UV或蓝色的芯片的射线用作为初级的光源。用一种发射最大值位于330至370nm中的UV-LED达到特别好的结果。在特别考虑石榴石和氯硅酸盐的激发光谱的条件下在355至365nm中出现一个最佳值。譬如BAM在这里用作为蓝色的荧光材料。在蓝色的芯片上用430至470nm的峰值波长可以达到特别好的结果。在特别考虑石榴石和氯硅酸盐的激发光谱的条件下在445至460nm中出现一个最佳值。
一个具有特别好的显色性的变型方案是共同采用两种荧光材料，即一种高度含Tb的荧光材料，优选纯的TbAG∶Ce，与氯硅酸盐：Eu一起。一个具有特别好的温度稳定性的变型方案是共同采用两种荧光材料，即一种高度含Y的荧光材料，优选纯的YAG∶Ce，与氯硅酸盐：Eu一起。
一种Ga(In)N-LED，但是具有在300至360nm段中发射的任何其它的短波长发射的LED也尤其适合于作为一种将UV或蓝色射线(以下总称为短波的射线)作为初级射线来发射的LED。尤其推荐UV段320至360nm和蓝色段430至470nm中的发射段作为主要的发射段，因为这样效率是最高的。
                        附图
以下借助多个实施例详述本发明。所展示的：
图1为一种用铕掺杂的氯硅酸盐的激发和发射光谱；
图2为一种用铕掺杂的其它氯硅酸盐的反射和发射光谱；
图3为一个用作白色光光源(LED)的半导体元件；
图4为来自图3的，具有本发明荧光材料TbAG和CS∶Eu的LED的发射光谱；
图5为一种具有本发明荧光材料TbAG和CS∶Eu的其它LED的发射光谱；
图6为具有本发明荧光材料YAG和CS∶Eu的LED的温度特性；
图7为具有本发明荧光材料YAG和CS∶Eu的LED的发射光谱；
图8为具有本发明荧光材料的照明单元。
                     附图的说明
以下示范性地更准确说明Eu和Mn掺杂的氯硅酸盐Ca8Mg(SiO4)4Cl2∶(Eu2+，Mn2+)的合成。然后借助几个实例测量清楚表明这种荧光材料的适用性。
通过高温的固体反应来制备荧光材料粉末。为此譬如以7∶1∶4∶1.5的克分子比例共同混合高纯的初始材料CaCO3、MgO、SiO2和CaCl2。添加小量的Eu2O3或MnCO3用于掺杂目的，并在此代替相应克分子量的CaCO3。这相当于成分式Ca8-x-yEuxMnyMg(SiO4)4Cl2，外加0.5CaCl2。
在良好地混合了各个组分之后，在还原的气氛(H2/N2)中在1000-1200℃下将所述的粉末加热1-4小时，并因此反应成上面所说明的化合物。为了除去多余的CaCl2和其它的水溶性的异相，可以再次用完全去离子的水洗涤粉末。人们获得在400nm上下的短波波长段中激发时具有高量子效率(典型地约为70％)的荧光材料粉末。
附图1展示了一种铕掺杂粉末的典型的激发和发射光谱。Eu2O3的添加物为0.03mol，即x＝0.06。可以很好识别经越300至470nm的，优选为360至400nm的很宽广波长段的有效可激发性。由Eu2+吸收光谱带决定了可激发性在较大波长时的下降。但是在460nm时还测量到象在400nm或甚至更为短波(一直下降至约340nm)时那样的可比较的量子效率。
所述的发射光谱展示了在约507nm时具有最大值的Eu2+发射光谱带。这种发射以绿色作用到眼睛上。如果需要，可以借助用Mn的少量联合掺杂将荧光材料的发射性能更好地与眼睛的敏感性相匹配。
附图2展示了一个Eu掺杂的氯硅酸盐Ca8Mg(SiO4)4Cl2∶Eu2+(简称CS∶Eu)的其它实施例。Eu2O3的添加物为0.2mol，即x＝0.4。峰值波长位于509nm，平均波长位于522nm上。色彩坐标为x＝0.185和y＝0.615。附图2a中以任意的单位说明了在400nm时照射下的发射。在附图2b中也进一步说明了反射(以百分比)。
对于在与GaInN芯片一起的白色LED中的用途，采用譬如类似于象在US 5 998 925中所说明的那样的构造。附图3中清晰地展示了白色光的这种光源的构造。所述的光源是一个具有450nm峰值发射波长的，具有第一和第二电接头2，3的，InGaN类型的半导体元件(芯片1)，在缺口9的范围中将该半导体元件埋入到透光的基壳8中。接头中的一个3经压焊丝14与芯片1相连接。所述的缺口有一个用作为芯片1的蓝色初级射线的反射器的壁17。缺口9用一种浇铸料5充填，该浇铸料5含有环氧浇铸树脂(80至90重量％)和荧光颜料(少于15重量％)作为主要组成部分。此外其它的微小分量归于甲基醚和气溶胶(Aerosil)。
此时，将第二实施例的氯硅酸盐荧光材料(CS∶Eu)与TbAG∶Ce一起用于荧光颜料。(CS∶Eu)对TbAG的混合比为4∶6(重量分量)。这个实施例的特点在于Ra＝85的特别高的显色性。附图4中展示了这个实施例的发射光谱。
常规解决方案(BG)与本发明解决方案(BGG)的直接比较显示出以下的结果：已将发射蓝色的InGaN芯片(峰值在450nm上)与常规的YAG∶Ce共同选择为BG解决方案。已将相同的LED与TbAG∶Ce和CS∶Eu共同选择为本发明的BGG解决方案。此时，分别在具有x＝0.322和y＝0.366的色品位置上达到6000K的色温。当所述的简单的BG解决方案仅仅达到Ra＝72的显色性时，用BGG解决方案成功获得Ra＝80的显色性。甚至大大改善了红色再现，即从R9＝-22改善到R9＝10。附图5中展示了BGG解决方案的发射光谱。
除了InGaN芯片(在450nm时的蓝色发射)之外，白色LED的一个其它的优选实施例采用上面所提及的氯硅酸盐荧光材料(CS∶Eu)与YAG∶Ce的组合。象在附图6中所示的那样，这个实施例的特点在于两种荧光材料的极其相同类型的消温性能。两种荧光材料的所述的消温性能实际上在允许的使用区域(直至约100℃)上是相同的，并仅稍微依赖于温度。譬如象为了比较目的而随同分析研究的混合石榴石(Y0.33Gd0.63Ce0.04)Al5O12那样的其它石榴石，它展示出明显较差的温度稳定性(在附图6中这种混合石榴石称为(Y，Gd)AG∶Ce)。因此在这个实施例中保证了在极其不同温度条件下色品位置和其它光技术数据的特别的稳定性，该实施例以很高的程度含有Y(或甚至Tb)作为SE(SE晶格位置的至少60mol-％)。附图7中展示了这个实施例的发射光谱。它相当于8000K的色温和具有坐标x＝0.294和y＝0.309的色品位置。显色性是Ra＝77。两种荧光材料的混合比是4.6∶1。
附图8中展示了来自作为照明单元的面型照明灯20的剖视图。它由一个共同的支架21组成，一个直角平行六面体形的外壳22粘接到该支架21上。它的上侧面配备了共同的封盖23。所述的直角平行六面体形的壳体具有布置了各个半导体元件24的缺口。它们是具有360nm峰值发射的，发射UV的发光二极管。借助在所有对于UV射线可接近的面上所安置的转换层25进行白色光的转换。壳体侧壁的位于内部的表面、封盖和底部均属于此。所述的转换层25由三种荧光材料组成，这三种荧光材料在利用本发明荧光材料的条件下在黄色、绿色和蓝色谱段中发射。

Claims (10)

1.具有至少一个作为光源的LED的发射白色的照明单元，其中，所述的LED在300至470nm段中发射初级的射线，其中，通过经受着LED初级射线的荧光材料将这种射线部分或完全地转换成长波射线，其特征在于，至少借助一种发射绿色和源自Eu活化的氯硅酸钙镁族的荧光材料、并借助至少一种发射黄色和源自Ce活化的稀土石榴石族的荧光材料来进行所述的转换。
2.按权利要求1的发射白色的照明单元，其特征在于，所述发射绿色的荧光材料遵循具有在x＝0.005和x＝1.6之间的x的，和具有在y＝0和y＝0.1之间的y的总分子式Ca8-x-yEuxMnyMg(SiO4)4Cl2。
3.按权利要求1的发射白色的照明单元，其特征在于，所述发射黄色的荧光材料是一种稀土(SE)Y、Gd、Lu、La和/或Tb的，按分子式SE3(Al，Ga)5O12∶Ce的，尤其是具有SE＝Y和/或Tb的，尤其是符合分子式YAG∶Ce或TbAG∶Ce的石榴石。
4.按权利要求1的发射白色的照明单元，其特征在于，所述初级发射的射线位于波长段330至370nm中，其中，所述初级发射的射线经受到三种在蓝色(430至470nm)、绿色(490至525nm)和黄色(545至590nm)中具有发射最大值的荧光材料。
5.按权利要求1的发射白色的照明单元，其特征在于，所述初级发射的射线位于蓝色波长段430至470nm中，其中，所述初级发射的蓝色射线经受到两种在黄色(545nm至590nm)和在绿色(490至525nm)中具有发射最大值的，符合以上权利要求之一的荧光材料。
6.按权利要求1的发射白色的发光转换LED，其特征在于，采用一种短波长发射的，尤其是基于Ga(In)N的发光二极管作为初级的射线源。
7.按权利要求1的发射白色的照明单元，其特征在于，所述铕的分量位于x＝0.1和x＝1.0之间，而不外加采用Mn。
8.按权利要求1的发射白色的照明单元，其特征在于，所述的照明单元是一种所述荧光材料直接或间接与芯片接触的发光转换LED。
9.按权利要求1的发射白色的照明单元，其特征在于，所述的照明单元是一种LED阵列。
10.按权利要求9的发射白色的照明单元，其特征在于，所述荧光材料中的至少一种安放在一个布置在所述LED阵列之前的光学装置上。
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KR20030007742A (ko) 2003-01-23
US20050104503A1 (en) 2005-05-19
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US7002291B2 (en) 2006-02-21
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