CN100499186C - 氧化锌基纳米棒和半导体薄膜的p-n异质结结构、其制备和包括其的纳米器件 - Google Patents

氧化锌基纳米棒和半导体薄膜的p-n异质结结构、其制备和包括其的纳米器件 Download PDF

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CN100499186C
CN100499186C CNB2004800177881A CN200480017788A CN100499186C CN 100499186 C CN100499186 C CN 100499186C CN B2004800177881 A CNB2004800177881 A CN B2004800177881A CN 200480017788 A CN200480017788 A CN 200480017788A CN 100499186 C CN100499186 C CN 100499186C
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李圭哲
朴原一
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LG Display Co Ltd
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Abstract

一种由p型半导体薄膜和外延生长于其上的n型ZnO基纳米棒组成的异质结结构，由于促进了电子通过纳米尺寸结的隧穿和使用具有高激子能量的ZnO作为发光材料，因此该异质结结构表现出高发光效率特性，并因此其利于应用于诸如LED、场效应晶体管、光探测器、传感器等的纳米器件。

Description

氧化锌基纳米棒和半导体薄膜的P-N异质结结构、其制备和包括其的纳米器件
技术领域
本发明涉及包含p型半导体薄膜和外延生长于其上的n型ZnO基纳米棒的新型异质结结构，其提供了一种具有改善的发光特性的发光器件。
背景技术
1993年Nichia Chemical有限公司开发的氮化镓(GaN)基蓝色发光二极管(LED)使用GaN薄膜p-n结来提供蓝色和绿色LED器件，并于1997年使用氮化物半导体开发了在室温下具有约10,000小时寿命的短波长(404nm)蓝色LED。
近来，作为另一种有效的室温发光材料(λ＝380nm)，n型氧化物半导体氧化锌(ZnO)得到了关注，这是由于其引人注意的特征：(1)直接跃迁能带结构，(2)室温下用于光泵激的低功率阈值和(3)大的激子结合能(60meV)。
然而，由于难于制备p型ZnO，因此阻碍了氧化锌p-n异质结结构的发展。
发明内容
因此，本发明的一个主要目的是提供一种通过使用纳米棒形式的n-ZnO和薄膜形式的除p-znO之外的p型半导体材料形成的新型异质结结构，其利于用于诸如LED、场效应晶体管、光探测器、传感器等纳米器件。
本发明的另一个目的是提供一种该结构的制备方法。
本发明的再一个目的是提供一种包含该结构的纳米器件或其阵列。
根据本发明的一个方面，提供了一种包含p型半导体薄膜和外延生长于其上的n型ZnO基纳米棒的异质结结构。
根据本发明的另一方面，提供了一种所述异质结结构的制备方法，其包含：在400-700℃范围内的温度、0.1-10torr范围内的压力下，将含Zn金属有机化合物和含O2化合物的蒸汽作为反应物，分别与p型半导体薄膜相接触，以在半导体膜的表面上形成ZnO纳米棒。
根据本发明的再一个方面，提供了一种包含所述异质结结构的纳米器件或其阵列。
附图简述
当结合附图时，本发明的下述描述将使本发明的上述和其他目的和特点变得清楚，附图分别示出：
图1：根据本发明的例子1的p-n异质结结构制备工艺的示意图；
图2：根据本发明的包含p-n异质结结构的发光二极管器件的示意图；
图3(a)和3(b)：分别在本发明的例子1和2中得到的ZnO基p-n异质结结构的扫描电子显微镜扫描图；以及
图4：本发明的例子2中得到的LED的发光光谱，该LED包含通过在p型GaN薄膜上外延生长n型ZnO纳米棒形成的异质结结构。
发明详述
本发明的异质结结构特征在于包含p型半导体薄膜和外延生长于其上的n型ZnO基纳米棒。
此外，可以通过利用热或电子束蒸镀技术在异质结结构的p型半导体薄膜和n型纳米棒的相对表面上形成电极来制备包含所述异质结结构的纳米器件。
在本发明的异质结结构中，p型半导体薄膜可以为单晶形式、或采用传统金属有机化学气相沉积(MOCVD)方法形成在衬底上的薄膜，该MOCVD方法包含加热衬底，并使适当的前体蒸汽与衬底表面相接触。
本发明的结构的p型半导体薄膜可具有50nm-200μm范围的厚度。
适于作为用于薄膜的p型半导体的材料具有1.5-4.5eV的带隙，其代表性例子包括诸如GaN、AlN、GaP、GaAs等的III-VB族半导体；诸如ZnSe、CdSe、CdS、ZnS等的II-VIB族半导体；和诸如SrCu2O2、SiC、Si等的半导体。
另外，生长在p型半导体薄膜上的ZnO基纳米棒可以为ZnO纳米棒、或掺杂或涂敷异质材料的ZnO纳米棒。示例性的异质材料掺杂剂包括Mg、Mn、Cd、Se等；掺杂的异质材料包括Zn1-xMgxO(0<x<1)、Zn1-xMnxO(0<x<1)、Zn1-xCdx0(0<x<1)、Zn1-xSexO(0<x<1)等。
本发明的异质结结构可以通过利用金属有机化学气相沉积(MOCVD)方法在p型半导体薄膜上外延生长ZnO基纳米棒来制备，该方法包含：在400-700℃、0.1-10torr范围内的压力下，将含Zn金属有机化合物和含O2化合物的蒸汽作为反应物，分别与p型半导体薄膜相接触。
如果需要的话，可以通过在引入反应物蒸汽时或在形成ZnO纳米棒之后，引入含有诸如Mg、Mn、Cd、Se等的异质材料的化合物蒸汽来用异质材料掺杂或涂敷形成在p型半导体薄膜上的ZnO纳米棒，以形成掺杂或涂敷异质材料的ZnO纳米棒。
可根据生长期间的反应条件，诸如引入到反应腔中的气态反应物的量、沉积温度和压力等来改变形成在p型半导体薄膜上的ZnO基纳米棒的直径、长度和密度。
本发明结构的薄膜上的纳米棒可具有5-100nm范围的直径和5nm-100μm范围的长度。
可以用作本发明中的氧化锌的前体的示例性含Zn金属有机化合物包括二甲基锌[Zn(CH3)2]、二乙基锌[Zn(C2H5)2]、乙酸锌[Zn(OOCCH3)2·H2O]、乙酸酐锌[Zn(OOCCH3)2]、乙酰丙酮锌[Zn(C5H7O2)2]等，含氧化合物包括O2、O3、NO2H2O(蒸汽)、CO2、C4H8O等。
此外，可以用作本发明中纳米棒掺杂或涂敷前体的示例性含Mg金属有机化合物包括二(环戊二烯基)镁[(C5H5)2Mg]、二(甲基环戊二烯基)镁[(CH3C5H4)2Mg]、二(乙基环戊二烯基)镁[(C2H5C5H4)2Mg]、二(五甲基环戊二烯基)镁[{(CH3)5C5}2Mg]、乙酸镁[Mg(OOCCH3)2·H2O]、乙酸酐镁[Mg(OOCCH3)2]、乙酰丙酮镁[Mg(C5H7O2)2·H2O]等，含Mn金属有机化合物包括二(环戊二烯基)锰[(C5H5)2Mn]等，含Cd金属有机化合物包括二乙基镉[(C2H5)2Cd]等，含Se金属有机化合物包括二乙基硒[(C2H5)2Se]等。
由p型半导体薄膜和垂直生长于其上的n型ZnO基纳米棒组成的本发明的异质结结构可用于如图2示出的LED器件。
根据本发明的异质结结构使用具有高激子结合能的ZnO，其可以有利地用于具有由室温下激子复合带来的改善发光特性的LED。
此外，本发明的异质结结构可以是p-n纳米结，其有助于电子隧穿以增大发光区域，并包含具有高纵横比的纳米棒，由此其可用于在室温或更高温度下具有高发光效率的发光器件。
由于在本发明的异质结结构中，ZnO基纳米棒外延地生长在薄膜上，因此易于组装包含这种结构的发光器件阵列以制造出各种纳米系统。
下面的例子旨在更具体地示例本发明，但并不限制本发明的范围。
例子1：ZnO纳米棒在p型GaN薄膜上的生长
通过以下图1示出的工艺制备ZnO基p-n异质结结构。
利用传统MOCVD技术在Al2O3衬底上沉积掺Mg的GaN薄膜，并将该薄膜退火以得到具有2μm厚度的p型GaN薄膜。使用的金属有机前体为三甲基镓(TMGa)和二(环戊二烯基)镁[(C5H5)2Mg]；且氮前体为NH3。
然后，通过利用氩气(Ar)载体气体以分别在1-10sccm范围和20-100sccm范围的流速注入气态Zn(C2H5)2和O2，并使蒸气反应约1个小时，在如此得到的p型GaN薄膜上垂直生长n型ZnO纳米棒，从而得到包含生长在p-GaN薄膜上的n-ZnO纳米棒的p-n异质结结构。ZnO纳米棒生长期间的反应器压力和温度分别保持在0.1-10torr和400-700℃的范围内。
由此得到的p-n异质结结构的扫描电子显微镜(SEM)照片示于图3(a)，其显示出具有40nm直径和1μm长度的ZnO纳米棒均匀且垂直地生长在GaN薄膜的表面上。此外，X-射线衍射(XRD)分析显示出纳米棒在(0001)取向上外延生长在具有相同取向的GaN薄膜衬底上。
例子2：发光二极管的制造
以下使用例子1中制备的异质结结构制造发光二极管。
首先，通过在其上沉积绝缘材料(例如光刻胶、聚酰亚胺等)填充生长在GaN薄膜上的ZnO纳米棒周围的自由空间，然后通过采用等离子体蚀刻来暴露出纳米棒的尖端部分。接着，通过热或电子束蒸镀技术，在被蚀刻的n型纳米棒的尖端部分处形成Ti(10nm)/Au(50nm)顶部欧姆电极，和在p型GaN薄膜上形成Pt(10nm)/Au(50nm)底部电极。反应器压力约10-5mmHg、并使衬底温度保持在室温下进行的电极沉积期间，施加的加速电压和发射电流分别在4-20kV和40-400mA的范围内。
通过扫描电子显微镜(SEM)研究形成有顶部电极的ZnO纳米棒的截面形态，结果示于图3(b)中。
另外，由此获得的LED的发光光谱示于图4中。光发射强得足以在视觉上可察觉，并且其强度在长期的反复操作(几十个周期)中不会降低。此外，如图4所示，器件在570nm和470nm附近具有发射峰值。
上述结果表明本发明的p型半导体薄膜具有外延生长的n型ZnO基纳米棒的异质结结构具有良好的发光特性。
虽然已经描述和示例了本主题发明的实施例，但是显而易见地，可以在不脱离仅由附加权利要求书的范围限制的本发明的精神的情况下可以做出各种改变和变形。

Claims (11)

1、一种纳米器件，包含p型半导体薄膜和外延生长于其上的n型ZnO基纳米棒的p-n异质结结构，其中用绝缘材料填充生长在该p型半导体薄膜上的该ZnO纳米棒的尖端部分以外的部分周围的自由空间。
2、如权利要求1所述的纳米器件，其中该p型半导体薄膜由带隙能量在1.5-4.5eV范围内的材料制成。
3、如权利要求2所述的纳米器件，其中该p型半导体薄膜由选自GaN、AlN、GaP、GaAs、ZnSe、CdSe、CdS、ZnS、SrCu2O2、SiC和Si构成的组中的材料制成。
4、如权利要求1所述的纳米器件，其中该p型半导体薄膜具有在50nm-200μm范围内的厚度。
5、如权利要求1所述的纳米器件，其中该ZnO基纳米棒具有5-100nm范围内的直径和5nm-100μm范围内的长度。
6、如权利要求1所述的纳米器件，其中该ZnO基纳米棒为ZnO纳米棒或掺杂或涂敷有异质材料的ZnO纳米棒。
7、如权利要求6所述的纳米器件，其中异质材料掺杂剂包括Mg、Mn、Cd和Se。
8、如权利要求6所述的纳米器件，其中该掺杂的异质材料选自由Zn1-xMgxO、Zn1-xMnxO、Zn1-xCdxO和Zn1-xSexO构成的组，其中0<x<1。
9、一种用于制备如权利要求1所述的纳米器件的工艺，包含以下步骤：在400-700℃范围内的温度及0.1-10torr范围内的压力下，将含Zn金属有机化合物和含O2化合物的蒸汽分别与p型半导体薄膜相接触，以在该p型半导体膜的表面上形成n型ZnO纳米棒；用绝缘材料填充生长在该p型半导体薄膜上的该n型ZnO纳米棒周围的自由空间；通过采用等离子体蚀刻暴露出该n型ZnO纳米棒的尖端部分；并且在该p型半导体薄膜的表面和该n型ZnO纳米棒的尖端部分上形成电极。
10、如权利要求9所述的工艺，其中该绝缘材料是光刻胶或聚酰亚胺。
11、一种包含如权利要求1所述的纳米器件的纳米系统或集成电路。
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