CN102255018A - 带有直立式纳米线结构的led及其制作方法 - Google Patents
带有直立式纳米线结构的led及其制作方法 Download PDFInfo
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- CN102255018A CN102255018A CN2011102356962A CN201110235696A CN102255018A CN 102255018 A CN102255018 A CN 102255018A CN 2011102356962 A CN2011102356962 A CN 2011102356962A CN 201110235696 A CN201110235696 A CN 201110235696A CN 102255018 A CN102255018 A CN 102255018A
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Abstract
本发明涉及带有直立式纳米线结构的LED及其制作方法。本发明涉及发光二极管LED。具体而言,本发明涉及包括作为有源部件的纳米线的LED。根据本发明的纳米结构化LED包括基片和从该基片突出的直立式纳米线。提供有源区(120)以产生光的pn结存在于该结构内。纳米线(110)或由纳米线形成的结构形成波导(116),以将有源区中产生的光的至少一部分定向到由纳米线(110)给定的方向。
Description
本申请是申请号为200780051734.0、申请日为2007年12月22日、发明名称为“带有直立式纳米线结构的LED及其制作方法”的申请的分案申请。
技术领域
本发明涉及发光二极管LED。具体而言,本发明涉及包括纳米线的LED。
背景技术
当今发光二极管(LED)的主要类型是建立在平面技术上的。在基片上把PN结构造成多层从而给器件提供了基本水平的定向。发光复合发生在这些层的子集中。因为半导体层的折射率显著高于空气的折射率,所以生成光的很大部分会在这些层中反射并且不会对器件的有效发光有贡献。实际上这些层将作为LED的水平平面内的波导。已提出了若干措施来减轻LED光受陷于器件中的效应以及从半导体层中高效地提取光。这样的措施包括修改表面以便提供具有与水平面成不同角度的若干部分。EP1369935中提出了一种类似的方案,其中在LED器件中提供纳米大小的颗粒以对光进行散射或可选地吸收光以及生成不同波长的光。另外,平面技术在小型化和适当材料的选择方面存在约束,这将在下面进行描述。
纳米级技术的发展以及尤其是制作纳米线的能力开辟了以在平面技术中不可能的方式设计结构和组合材料的可能性。这一发展的一个基础在于纳米线的一维(1D)属性使得能够克服在用平面技术制造的器件中对不同材料之间的晶格匹配的要求。已经表明并加以利用,例如InP的纳米线能够无缺陷地生长在InAs或Si上。在Samuelson等人的US 20040075464中公开了基于纳米线结构的多种器件,例如纳米线LED。这些LED具有给出量子限制效应的内部异质结构。
US20030168964教导一种多条纳米线的组件,所述多条纳米线作为成组地安装在纳米线的下端处的导电透明基片和顶端处的透明覆盖基片之间的LED,每个单独的纳米线具有P型、N型和发光层的结构。这些纳米线据称被布置成发射光透过导电透明基片。
先前已报导了其它的纳米线LED。Hiruma等人制造了垂直的GaAs纳米线pn LED。这些纳米线被嵌入在SOG中并且用Au/Ge/Ni顶接触进行覆盖,这是在Appl.Phys.Lett.60(6)1992中的Haraguchi等人的“GaAs p-n junction formed in quantum crystals”中描述的。这些器件表现室温电致发光。如在Nanoletters中的Quian等人的“Core/Multishell Nanowire Heterostructure as Multicolor,High-Efficiency Light-Emitting Diodes”中所描述的,还制造了基于GaN的纳米线LED。
发明内容
本领域已表明可以利用纳米线来构造LED。为了提供适合于工业生产方法的高效器件,还需要进一步的改进。
本发明的目标是要提供一种纳米结构化LED以及其制作方法从而克服现有技术器件和方法的缺陷。这是由权利要求1所限定的器件和权利要求29所限定的方法来实现的。
根据本发明的纳米结构化LED包括基片和从该基片突出的直立式纳米线。提供有源区以产生光的pn结在使用期间存在于该结构内。纳米线、部分纳米线或与纳米线结合的结构形成波导,以将在有源区中产生的光的至少一部分定向到由纳米线给定的方向。
纳米结构化LED还可以包括外延地连接到纳米线的体积元件(volume element)。体积元件提供高掺杂度以一般在纳米线内或靠近纳米线形成有源区而无需对纳米线本身进行掺杂。
能够以不同的方式来改进波导的导波特性。波导具有第一有效折射率nw,而围绕至少一部分波导的材料具有第二有效折射率nc,并且通过保证该第一有效折射率大于该第二有效折射率nw>nc,给波导提供良好的导波特性。可以通过将光学活性(optically active)包层引到波导上来进一步改进导波特性。
由于本发明,可以利用所产生的光的很大一部分并且由此能够提供高效的LED。这至少部分是通过将纳米线用作波导、将所产生的光导出表面而实现的。根据本发明的纳米结构化LED非常适合于批量生产,并且所描述的方法可升级到工业使用。
纳米线作为波导的使用为将光定向明确限定的方向提供了可能性。通过使用来自光纤光学领域的概念,光束能够根据预计使用而被聚焦或分散。
纳米线技术在选择在常规体层技术中不可能的材料和材料组合方面提供了可能性。这在根据本发明的纳米结构化LED中被使用,来提供产生在常规技术不能获得的波长区内(例如紫色和UV)的光的LED。
根据本发明的设计允许在纳米线内包括异质结构以及不同掺杂的区,以便于优化电学和/光学特性。
本发明的实施例被限定于从属权利要求中。通过以下详细描述本发明并结合附图和权利要求加以考虑,本发明的其它目标、优点和新颖特征将显而易见。
附图说明
现在将参照附图来描述本发明的优选实施例,其中:
图1a-b示意性图解说明了根据本发明的纳米结构化LED的实施例;
图2示意性图解说明了根据本发明的纳米结构化LED的纳米线的波导特性;
图3a-b示意性图解说明了与根据本发明的纳米结构化LED结合使用反射层;
图4示意性图解说明了根据本发明的纳米结构化LED的实施例;
图5示意性图解说明了根据本发明的纳米结构化LED的实施例;
图6示意性图解说明了根据本发明的纳米结构化LED的实施例;
图7示意性图解说明了根据本发明的纳米结构化LED的实施例;
图8示意性图解说明了根据本发明的纳米结构化LED的实施例;
图9示意性图解说明了根据本发明的纳米结构化LED的实施例;
图10示意性图解说明了根据本发明的多个纳米结构化LED的组件;
图11示意性图解说明了结合反射平面的多个纳米结构化LED的组件;
图12示意性图解说明了根据本发明包括在平面发光结构上的纳米线的纳米结构化LED的实施例;
图13图解说明了根据本发明的方法中的基本制作步骤。
图14示意性图解说明了LED纳米结构;
图15a是根据图14的纳米结构LED的SEM图像,图15b是有源LED纳米结构的图像;
图16是在第一MOVPE步骤之后本发明的纳米线结构的SEM图像;
图17a-c是根据图14和图16的纳米线和LED纳米结构的光致发光图;
图18示出a)生长在GaP和Si上的GaAs LED的电致发光的功率相关性,b)80mA下基于GaP和基于Si的LED纳米结构的EL光谱;
图19a-b示出了用3.0sccm的NH3流速所生长的样品的SEM图像;
图20a-b示出了用1.0sccm的NH3流速所生长的样品的SEM图像;
图21a-b示出了用0.5sccm的NH3流速所生长的样品的SEM图像;以及
图22示出了用0.2sccm的NH3流速所生长的样品的SEM图像。
具体实施方式
根据本发明的纳米结构化发光二极管包括直立式纳米线。在US2003010244中描述了用于在半导体基片上生长纳米线的适当方法。在US 20040075464中可找到给外延生长的纳米线提供异质结构的方法。
对本申请来说,直立式纳米线应当被解释为从基片以某一角度突出的纳米线,该直立式纳米线例如是从基片外延生长的。与基片的角度一般将是基片和纳米线的材料、基片的表面以及生长条件的结果。通过控制这些参数,可以制作仅指向一个方向(例如垂直)或者指向有限的一组方向的纳米线。例如,闪锌矿和金刚石半导体的纳米线和基片由来自周期表的第III、V和IV列的元素组成,这些纳米线能够在[111]方向上生长并且然后在任何{111}基片表面的法向方向生长。被表示为表面法向和纳米线的轴向之间的角度的其它方向包括70.53°{111}、54.73°{100}、以及均对于{110}的35.27°和90°。因而这些纳米线限定一个方向或有限的一组方向。
根据本发明,纳米结构化LED的纳米线、纳米线的一部分或由纳米线形成的结构被用作波导以将由纳米结构化LED所产生的光的至少一部分定向由直立式纳米线所给定的方向。理想的导波纳米线LED结构包括高折射率芯层与具有比芯层折射率低的折射率的一个或多个围绕包层。该结构是圆对称的或近似圆对称的。圆对称结构中的光发生导波对于光纤应用而言是众所周知的并且与稀土掺杂光纤放大器和激光器的领域能够形成很多相似之处(parallel)。然而,一个区别在于光纤放大器是光泵浦的而所描述的纳米线LED结构可以被视为电泵浦的。一个熟知的品质因数是所谓的数值孔径,NA: 其中n1和n2分别是芯层和包层的折射率。NA确定波导所捕获的光的角度。对于在波导的芯层内生成的光,捕获角可以按来确定。NA和被捕获光的角度是优化新LED结构时的重要参数。
III-V半导体芯层材料的折射率的典型值在从2.5到3.5的范围内。当与诸如具有从1.4到2.0范围的折射率的SiO2或SiN之类的玻璃类型的包层材料组合时,捕获角可以高达65度。65度的捕获角使得高达75%的生成光能够(在两个方向上均)被该结构捕获并引导。
在优化光提取时的一个考虑因数是使得NA沿纳米线结构变化以优化从该结构的光提取。一般而言,理想的是当光生成在最远离出口位置发生时让NA最高。这会使所捕获且引导朝向出口的光最大化。相比而言,越靠近结构的出口端,可以使NA越小,原因在于所生成的光会以随机的方向辐射并且大多数辐射光会打到该结构的顶部部分的顶部和侧面并射出。在结构的顶部部分中具有较低的NA还会使光捕获并向下引导回通过该结构最小化,向下引导回通过该结构是不理想的除非在该结构的底部上插入反射器。可以通过用另一具有略低折射率的不同组分的III-V包层来包围III-V纳米线芯层,获得低的NA。
根据本发明的纳米结构化LED 100被示例性图解说明于图1中并且包括基片105和从基片以限定角θ外延生长的纳米线110。纳米线的一部分被体积元件115围绕。该体积元件115优选地外延连接到纳米线110。纳米线110的一部分被布置成作为将产生的光的至少一部分定向由纳米线的伸展方向所给出的大致方向的导波部分,并且将被称为波导116。对二极管功能所必要的pn结由纳米线110和体积元件115的组合来形成。体积元件提供高的掺杂度,因此pn结可以在不直接掺杂纳米线110的情况下或者至少不用改变纳米线110的直接掺杂的情况下形成。这是有利的,原因在于对1D结构的掺杂可能在技术上是有挑战性的并且大规模生产实施成本很高。体积元件115的功能以及纳米线110和体积元件115之间的相互作用将在下面进行进一步的讨论。接触125被提供在体积元件115上(例如在顶部)或者以绕接(wrapping)配置被提供在圆周外表面上(所描绘的)。基片105和部分直立式结构可以被覆盖层107所覆盖,例如像所示出的薄膜或者像填充包围纳米结构化LED的空间的材料。
纳米线110典型地具有大约为50nm到500nm的直径,而体积元件的直径大约为500nm到1000nm,即对于围绕纳米线的这部分体积元件而言厚度约为200nm。纳米线的波导部分116的长度典型地且优选地约为1到10μm。体积元件的长度典型地且优选地约为1到5μm。体积元件的尺寸应当使得关于例如掺杂接收性的特性是一般与体材料相关联并且根据体材料而被预料到的那些。例如厚度大于150nm的InGa:Si的体积元件已表明显现可接受的掺杂接收性。这些尺寸无论是实际数量(number)还是各部分彼此相对的数量都能够被改变以便优化特定的条件并且适应不同的材料组合。
pn结产生布置在纳米线中或者在纳米线附近的有源区120,在其中产生的光。应当注意,图1a中的有源区120的位置是非限制性示例。图2图解说明了波导部分116的波导特性。纳米结构化LED的不同构件的材料经选择以使得纳米线相对于包围材料将具有良好的导波特性,即纳米线110中的材料的折射率应当大于包围材料的折射率。如果纳米线110具有第一折射率nw,则包围波导部分116中的纳米线的材料(典型地为覆盖层107)具有第二折射率nc,而体积元件具有第三折射率nVE,nw>nc且nw>nVE。纳米结构化LED的典型值为nw≈3,nc≈1.5以及nVE≈3。
纳米线110可以被提供一个或多个包层。可以引入第一包层112以改善纳米线的表面特性,例如如果利用GaAs纳米线则已表明通过添加GaInP的包层112改善了所述特性。可以专门引入另外的包层例如光学包层113来改善纳米线110的导波特性,其方式与光纤光学领域中已完善建立的方式类似。光学包层113典型地具有在纳米线和包围材料的折射率之间的折射率。可选地,包层113具有渐变折射率,已表明这在特定情况下改善光传输。如果利用光学包层113,则纳米线的折射率nw应当就纳米线和包层两者定义有效折射率。
如上面引用文献中所描述的并且在下面例证的,可生长精确直径的纳米线的能力在本发明的一个实施例中被用来就纳米结构化LED100所产生的光的波长而言优化纳米线110或至少波导116的导波特性。如众所周知的,作为LED光产生的基础的复合过程产生在窄波长区内的光,这取决于材料特性。在实施例中,纳米线110的直径经选择以便具有与所产生的光的波长的良好对应。优选地,纳米线110的尺寸是使得沿纳米线提供针对所产生的光的特定波长所优化的均匀光学腔。芯层纳米线必须足够宽以捕获光。按经验估计直径必须大于λ/2nw,其中λ是所产生的光的波长而nw是纳米线110的折射率。
对于被布置成产生可见光区内的光的纳米结构化LED,纳米线的波导的直径应当优选地大于80nm以便纳米线成为有效的波导。在红外和近红外中,大于110nm的直径就足矣。纳米线直径的大约优选上限由生长约束给定并且大约为500nm。纳米线110的长度典型地且优选地约为1-10μm,以为有源区120提供足够的体积并且同时不会有不必要长度而造成内部吸收。
图1b图解说明了本发明的一实施例,其中体积元件115包括壳状结构的多层117、118。所述多层可以包括掺杂层117和阱层118,该掺杂层117提供p区或n区,该阱层118将包括工作时的有源区120。可选地,该阱能够由多个子层制作。因此,在这个实施例中有源区120在径向上将主要是在纳米线110之外。根据这个实施例,波导116可以由壳状结构的层117和118以及可选的其它一个或多个包层119形成,所述包层119具有增强如上所讨论的导波的特性。纳米线110可以典型地为波导116的一部分。可选地,导波被尽可能地限制到壳状结构。
在本发明的以下不同实施例中,主要示出了具有参照图1a所描述的设计。如本领域技术人员应当明白的,对于具有参照图1b所描述的壳状结构的设计,这些不同实施例应当只有很小的相关调节。
在一个实施例中有反射层108,在图3a-3b中示出为被提供在基片105上(图3a),或者可选地在覆盖层107上(图3b),如果利用覆盖层107的话。反射层的目的是对从纳米结构化LED以向下方向发射的光进行反射。优选地以多层结构的形式或者像金属膜来提供反射层108,该多层结构例如包括AlGaS/GaAs或GaN/AlGaN的反射层。
根据图4所示的本发明一个实施例,反射层108被布置成在部分波导116或者纳米线/波导/包层组合之下继续,因此形成邻近基片的茎(stem)113,茎113比上面的纳米线/包层具有更小的直径。下面将描述这种制作方法。如果茎113的直径足够小于光的波长,则大部分的定向光模会延伸到波导之外,以使得包围波导的狭窄部分的反射层108能够高效地反射。反射层108可以垂直于纳米结构化LED或者可选地被设计成使得打到反射层108上的光中的大量光会被以向上方向反射。通过以具有除90°之外的另一角度的配置来制造该层和波导,能够把光定向到与波导不同的方向上。这样的一种特定情况是当以与基片成不同于90°的角度生长纳米线的时侯。如果波导116或者纳米线+包层具有第一有效折射率nw并且反射层具有第二有效折射率ns且nw>nc,则纳米线和反射层之间的角度可以被选择为获得全内反射。
用于在波导116的下端获得反射的可选方案是将反射层109布置在纳米线下面的基片中,如图5所示。反射层可以例如是如上的多层结构,这在本领域中制作高反射表面是已知的。另一可选方案是在波导116内引入反射装置111,如图6所示。这种反射装置可以是在纳米线的生长过程期间提供的多层结构,所述多层结构包括例如SiNx/SiOx(介质)或GaAs/AlGaAs(半导体)的重复层。如果纳米结构化LED主要从纳米线的顶部发射光,则该反射装置优选地位于有源区之下,例如靠近基片,如所描绘的。可选地如果使用倒装配置并且光主要来自波导116的下端,则反射装置111应当优选地放置在有源区之上。
在图7所示的进一步实施例中,所产生的光的主要部分通过纳米线110的波导116或波导116以向下方向定向通过基片105。光能够被定向通过整个基片厚度,或者可选地基片被提供有在纳米线110基底下面的开孔130以便减小基片的厚度从而减小光在基片中的散射或吸收。基片优选地由透明材料制成。可选地,纳米结构化LED能够从基片被去除。在这种情况下,纳米线能够在其下端由绕接接触相接触。体积元件115的外表面的一部分或者优选全部可以由反射层135覆盖,这就提高所产生的光经波导116的辐射。例如由金属形成的反射层可以另外用作接触。基片和纳米线110的一部分可选地由SiO2的保护层覆盖。
在图8所示的实施例中,体积元件815被布置为分散性单元,以给出在大角度上基本均匀分布的光辐射。这种器件非常适合用于其中要求均匀照射的照明目的。有源区120可以被布置在纳米线中但可选地在体积元件内,并且位于纳米线110的上端(如所描绘的),或者径向上在纳米线之外并且可能在其之上。纳米线110在其下端应当优选地被提供有一些上面描述的反射装置,例如在纳米线内的反射装置111,以便将光向上重新定向。体积元件的几何形状能够被设计成进一步分散光。在纳米线110波导和该体积之间的结处以及另外在由体积元件115的上边界形成的边缘处提供分散。体积元件的高度和宽度经选择以使得该边缘进一步分布分散的光的角度。
纳米线LED的导波特性还提供聚集的定向束,其能够被整形并且定向性地被引导以提供期望的辐射图样。这能够通过将出口界面整形为透镜状形式和使用先前描述的可变NA方法的组合来实现。一般而言,如果期望较宽的辐射图样,则应当将靠近出口的NA渐变地或在距出口表面的某段距离处突变地更改为更小值。如果期望的是具有窄辐射图样,则这可以通过具有聚焦凹透镜状的出口表面或/和使靠近出口的纳米线LED的顶部部分处的NA维持尽可能得高来实现。芯层纳米线的直径还在整形辐射图样方面起重要作用。一般而言,直径越小,辐射图样越宽,而大直径芯层纳米线将要求更受限制的、定向的辐射图样。这种-也许跟直觉相反的-效应在光学工程中是众所周知的,因为远场辐射图样实际上是近场的傅立叶(Fourier)变换。如众所周知的,短或窄事件的傅立叶变换产生傅立叶域中长或宽事件。一个极端的示例是δ(delta)函数,δ函数的傅立叶变换是无限宽且密度恒定。与光辐射的相似之处在于点光源(近场中的δ函数)在所有方向上(在远场中“无限”宽辐射)以恒定密度进行辐射。图9示例性图解说明的本发明一个实施例是针对提供聚集的、定向的光束而优化的。相对大直径(优选大于150nm)的纳米线110延伸到体积元件115的上表面。在上端给纳米线110提供凹透镜状的出口表面112。
先前描绘的圆柱形体积元件115可用谈到的生长纳米线的方法来获得,该圆柱形体积元件115应当视为示例性形状。其它似乎合理的几何形状包括但不限于带有穹形顶的圆柱形球状物、球形/椭圆形以及金字塔形。
在典型的实施方式中,在一个器件中提供很多个纳米结构化LED。图10图解说明了这种器件的一部分。多个纳米结构化LED 100已外延生长在掺Zn的GaP基片105上。LED的纳米线110为本征GaAs并且被提供带有未掺杂InGaP的同心层。体积元件115包括掺Si的InGaP。纳米线的下部分和基片被SiO2层150覆盖。底面接触155被提供在基片上以连接多个LED,并且每个单独的LED均在体积元件115上被提供有环绕接触125。环绕接触125被连接用于逐组地寻址LED。
在一个实施例中,如上所讨论的,利用纳米线以有限的一组优选方向生长的这一固有特性。多个纳米结构化LED 1110被提供在基片1105,如图11所示。所有LED具有相同方向或者具有有限的一组方向中的一个方向。优选地,LED被布置成产生明显定向的光束。邻近这组LED以与基片成一角度提供反射装置1250,该角度对应于LED的方向以便从LED发射的光被反射装置1160以期望的方向反射。光的路径示意性地用虚箭头来表示。如果LED具有多个方向,例如对应于四个[111]方向,则可以提供相应的多个反射装置,以优选地将所有光定向到相同方向,例如垂直于基片。
作为波导的纳米线能够被用来改善常规平面LED的性能。在图12所描绘的实施例中,多个纳米线1210被布置在平面LED的表面上。在平面LED(例如GaAsP)的有源层1260中产生光。纳米线1210外延地连接到平面LED层的顶部上以便获得不同部分的良好匹配。纳米线1210可以被涂布用于保护纳米线和/或改善特性的包层1212,例如Si3N4。纳米线1210之间的表面优选地用例如Au的反射层1208来涂布。在有源区1220中产生的光的至少一部分将进入作为波导的纳米线1210,以将光导出基片平面。通过如上面所描述的相同机构,纳米线能够被布置成将光聚焦在一个或多个明确限定的方向上。
为了形成光产生所必要的pn结,至少部分纳米结构需要被掺杂。如上面所指出的,部分地提供体积元件以解决与纳米元件的掺杂相关联的一般难题以及促进良好的电接触特性。重要的是降低接入电阻以便提高器件效率。从这个角度看,纳米线就其本身而言不是最优的,因为细长性质和纳米线横截面的低面积将增加器件电阻。用于制作低电阻接触(这是一个因由纳米线几何形状给定的固有低接触表面而复杂化的任务)的主要手段是对接触的半导体侧进行高掺杂和低带隙调节,但如上所提及的,纳米元件的掺杂因若干因素而富有挑战性。然而,纳米线器件的某些其它部分不需要高掺杂,或者它们的掺杂水平不大重要并且能够与其它设计参数相权衡。还有一些器件中,关键部分的掺杂将降低器件性能。这种不利生产的掺杂效应的示例是光学区中的非发射杂质级或场效应沟道中降低迁移率的杂质散射。
根据本发明的体积元件115在三个尺度上中延展、具有大体积和大表面,由此可以避免对纳米元件的挑战性掺杂工艺,使该处理简化且更加可靠,由于掺杂以及增加的接触表面两者均可以降低接入电阻,可以充分利用将纳米线用作有源组件这一优点。
体积元件/纳米线架构增强了LED的电学和光学性能。体积元件115充当载流子库,使能从具有明确定义的(well defined)掺杂的区域到纳米线内的高载流子注入,在所述具有明确定义的掺杂的区域处能够制作低电阻接触,优选地采用环绕配置以便提高接触面积并且最小化纳米线和接触之间的距离。低内部电阻和增加的载流子量已经保证了在低正向电压下多数载流子到纳米线内的高注入。载流子到纳米线110内的高注入将高浓度的电子空穴对引入到纳米线内从而增加发光复合。与延伸到对光加以定向的波导内的有源区结合,高浓度的电子空穴对能够实现受激发射,进一步提高器件的输出。
通过在纳米线110和体积元件115中使用不同的材料组分,纳米线材料组分能够经选择以传到体积元件115内以便降低因与纳米线连接的光学扰动。在发射光的方向上延伸纳米线的长度将提高再吸收。为了降低再吸收,在发射的光的方向上调节纳米线的组分以便与发射的光的能量相比增大带隙。
一种制作纳米结构化LED的方法是首先根据上面提及的过程来生长纳米线。然后对部分纳米线进行掩模并且选择性地再生长体积元件。该方法示于图13中。体积元件轴向并径向地生长,因此当纳米线被部分掩模时,纳米线变成包围在体积元件中。适当的掩模材料例如是氮化硅、氧化硅等。
考虑到纳米线生长因诸如VLS生长的纳米线之类的物质而局部增强的系统,可通过更改生长条件而在径向生长和轴向生长之间更改的能力使得能够重复该工艺(纳米线生长、掩模形成以及后续的选择性生长)以形成更高阶的纳米线/3D序列。对于纳米线生长和选择性生长不是通过单独的生长条件进行区分的系统,可能更好的是首先沿长度生长纳米线并且通过不同的选择性生长步骤来生长不同类型的3D区或体积元件。
图13图解说明了一种根据本发明的制作方法以便制作发光pn二极管/阵列,其中(一个或多个)有源纳米线区由GaAs和InGaP形成,该方法包括以下步骤:
1、通过光刻在p+GaP基片1305上限定一个或多个局部催化剂(catalyst)。
2、从局部催化剂1331生长GaAs纳米线1310。生长参数针对催化线生长进行调节。
3、在纳米线周围径向生长薄InGaP同心层1312(包层)。
4、沉积SiO2作为掩模材料1332,
5、回蚀刻掩模1332以露出纳米线的上部分
6、选择性生长n+InGaP体积元件1315。调节生长参数以给出径向生长。
7、(未示出)在体积元件上形成接触1325并形成到基片上。
能够以已知的方式改变生长过程以例如在纳米线中包括异质结构、提供反射层等等。在一些实施中所利用的茎113通过以下步骤来提供:首先生长薄纳米线(步骤2),沉积反射层或选择性生长掩模以覆盖下部分,以及径向生长包层或纳米线以增加纳米线厚度。
根据纳米结构化LED的预计使用、适当生产过程的可用性、材料成本等等,能够针对结构的不同部分而使用各种各样的材料。另外,基于纳米线的技术允许无缺陷地组合在其它情况下不可能组合的材料。III-V半导体由于其容易实现高速低功率的电子器件的特性而尤其备受关注。基片的适当材料包括但不限于Si、GaAs、GaP:Zn、GaAs、InAs、InP、GaN、Al2O3、SiC、Ge、GaSb、ZnO、InSb、SOI(绝缘体上硅)、CdS、ZnSe、CdTe。纳米线110和体积元件115的适当材料包括但不限于GaAs(p)、InAs、Ge、ZnO、InN、GaInN、GaN、AlGaInN、BN、InP、InAsP、GaInP、InGaP:Si、InGaP:Zn、GaInAS、AlInP、GaAlInP、GaAlInAsP、GaInSb、InSb、Si。例如GaP的可能施主掺杂剂是Si、Sn、Te、Se、S等等,而对相同材料的受主掺杂剂是Zn、Fe、Mg、Be、Cd等等。应当注意,纳米线技术使得可以使用诸如GaN、InN和AlN之类的氮化物,这就便于制作发射处于常规技术不容易获得的波长区内的光的LED。商业上特别关心的其它组合包括但不限于GaAs、GaInP、GaAlInP、GaP系统。典型的掺杂水平从1018变化到1020。本领域技术人员尽管熟悉这些及其他材料但要意识到其它材料和材料组合也是可能的。
低电阻率接触材料的适当性取决于待沉积的材料,但能够使用金属、金属合金以及非金属化合物如Al、Al-Si、TiSi2、TiN、W、MoSi2、PtSi、CoSi2、WSi2、In、AuGa、AuSb、AuGe、PdGe、Ti/Pt/Au、Ti/Al/Ti/Au、Pd/Au、ITO(InSnO)等以及例如金属与ITO的组合。
根据本发明的纳米结构化LED的实现示例将被表示为在GaP和Si基片上外延生长的GaAs纳米线。在这两种基片上已确立了LED功能性。就温度相关的光致发光、电致发光和辐射图样方面进行评价这些结构。
根据实现的LED器件包括生长并集成在Si上的III-V发光纳米线二极管的阵列。每个器件被围绕直接生长在GaP或Si上的GaAs纳米线芯层构造。每个二极管的一部分作为这些单独的纳米大小的p-i-n发光结构中的有源区。
图14所示的LED器件1401包括p-i-n二极管结构1400。基片1405是器件的构成整体所必需的部分,因为其起普通p层的功能。每个纳米结构化LED 1400结构包括纳米线1410、围绕至少部分纳米线的包层1430、盖帽或球状物1415以及顶接触。p掺杂、n掺杂和本征半导体材料的顺序将取决于基片材料。在GaP上该结构是:p-GaP(基片)1405、i-GaP 1411/i-GaAs(纳米线)1410、i-InGaP(包层)1430、n-InGaP(球状物)1415。在Si上该结构是:p-Si(基片)1405、i-GaP/i-GaAs(纳米线)1410、i-InGaP(包层)1430/n-InGaP(球状物)1415。在这两个器件中,纳米线基底中的i-GaP 1411(纳米线)层大约均为60nm厚并且起双重用途:用于提高生长质量的成核段、和电子阻挡层。
下面概括该制作过程。使用THMa金属有机源和TMIn以及作为反应前导气体的AsH3、PH3和Si2H6。采用两个生长步骤。首先,通过使用随机沉积的直径大小60nm的Au悬浮微粒(粒子密度以1/μm2计)的粒子辅助生长,在p型GaP(111)B(p=~1018cm-3)和Si(111)(p≈1015cm-3)基片上生长2μm长的GaAs/GaP纳米线。用名义上晶格与GaAs匹配的40nm厚的径向InGaP包层来包围这些纳米线。在这个步骤之后,取出样品进行光致发光表征或者随后制作纳米LED。80nm厚的SiO2沉积到被排齐用于LED制作的样品上。将SiO2回蚀刻以仅覆盖基片表面并且高达纳米线侧壁的大约1μm。然后将样品重新装载到MOVPE反应器内并且在GaAs/InGaP芯层结构的上部分上选择性地生长径向的Si掺杂InGaP层。LED完全被150-300nm厚、200×200μm2的方形Ni/Ge/Au接触覆盖,每个接触覆盖大约40000个独立纳米结构化LED。P接触用导电Ag胶制作在基片的背面上。其它的接触手段例如使用透明接触在本领域内是已知的并且容易用于本方法和器件。图15a示出了该结构的扫描电子显微镜(SEM)图像。
Si和GaP器件之间的一个重要区别是在纳米线基底中异质结构顺序,在GaP上基片是p-GaP(基片)/i-GaP(纳米线)/i-GaAs(纳米线),而在Si上基片是p-Si(基片)/i-GaP(纳米线)/i-GaAs(纳米线),并且空穴注入条件和内部电阻两者都应当预期在这两种结构之间是明显不同的。
图16描绘了在第一MOVPE步骤之后的纳米线结构。所描绘的GaAs纳米线带有薄InGaP包层、在纳米线基底处的GaP成核段、以及仍附着到顶部的基于Au的种子粒子。这种结构还被转移到中性基片进行PL表征。如图16所示,在GaP和Si基片两者上成品率均基本为100%。在Si上制作纳米结构化LED被精制到如下程度:纳米线一致地对准与基片垂直的(111)方向并且基本没有纳米线生长在也从基片延伸出来的三个倾斜(111)方向上。这与在Si(111)上的III-V纳米线生长的现有技术方法形成对比。如图16所见,在Si基片上以预定阵列结构整齐对准地生长III-V纳米线是成功大规模制作光学器件以及大多数其它应用的先决条件。
LED功能可以由光致发光(PL)测量来指示。这里介绍的测量是在室温下和在10K的温度下实施的。该结果示于图17a-c的曲线图和图15b中。以473nm发射的激光器被用作激发源。PL由光学显微镜收集,经过分光计发散并且由液氮冷却的CCD相机检测。
为了在无基片影响的情况下研究来自纳米线的PL,纳米线被折断并且被从它们所生长的基片中转移,然后沉积到图案化的Au表面上。以此方式,纳米线还可以被单独地研究。如图17a所示的PL光谱是在10k下从原生的(as-grown)纳米线中获取的,该PL光谱对于从Si基片(Si)生长的纳米线和从GaP基片(GaP)生长的纳米线而言是类似的。虚线是来自仍立于基片上的(大量)纳米线的光谱。来自单独的纳米线的光谱与从GaP基片生长的纳米线相比表现出较大的不同,后者更加结构化。从Si生长的纳米线的平均PL强度大约是从GaP生长的相应纳米线的1/20。这与就Si-LED所见到的电致发光是就GaP-LED所见到的电致发光的1/30-1/10相当吻合。在室温下,光谱较宽且无特征并且这两个样品的纳米线之间的光谱差别很小。
GaP上和Si上的LED在施加正向偏压时均展示了电致发光(EL),如图Ta-b所示。光的光谱峰与GaAs带隙能量很吻合。
如图18a和b所见,示出了基于Si的(Si)和基于GaP的(GaP)LED的光功率/电流相关性。GaP上的LED在Si(40mA)的一半电流负载(20mA)时开始发光并且在60mA时功率输出大约是GaP基片上的30倍高。然而,在100mA下功率比已降低到基于Si的LED的10倍。示出了80mA下两种器件的EL光谱峰。与GaP基片器件相比,Si LED峰呈现略微红移和带有大约1.35eV的可能额外峰的尾部。峰值的偏移可以用在GaP和Si上的不同In和Ga扩散从而导致不同的InGaP组分来解释。通过使器件到达更高的电流,对于GaP器件能够在大约140mA下看到峰值功率。这对于Si器件是看不到的并且可能指示在这些电流水平下非辐射复合或竞争泄露机制仍然支配EL。
建立在GaN纳米线上的LED器件由于它们可产生其它材料组合不可获得的波长的光的能力而受到高度的商业关注。作为进一步的实施示例,要描述的是如何通过选择性区域生长而在GaN外延膜、蓝宝石、SiC或Si以及甚至自支持(self-supporting)的GaN上生长GaN纳米线。在开始基片上通过PECVD沉积一层SiNx(厚度30nm)。在随后的步骤中,通过外延束光刻EBL以及反应离子蚀刻RIE来制造点图案的GaN开口(直径大约100nm)的阵列。开口之间的间距在1.0~3.2μm变化。然后,把经过处理的样品插入到水平MOCVD腔室内以生长GaN纳米线。生长过程包括起初阶段,其中在5分钟(min)内将温度斜升(ramp up)到1000~1500℃的生长区且在75sccm的高NH3流速下退火大约60秒。在随后的纳米线生长阶段中,NH3流速被减小到3.0~0.2sccm以通过将TMG(三甲基镓)引入到腔室内开始生长。这项工作使用0.12和1.2μmol/min之间的低TMG流速。NH3流速是控制自开口的生长形态的关键因素。图19示出了用3.0sccm的NH3流速所生长的样品的SEM图像。根据俯视图像[图19(a)],可以看到自开口的选择性生长与所报导的相同。这里需要指出的一点是生长后的横向大小大于1.0μm,这比大约100nm的开口大小大很多。因而,GaN生长出开口之后的横向生长是相当大的。图19(b)示出了通过将样品倾斜35°所拍摄的SEM图像,这清楚地表明所获取的是金字塔而不是线。这些金字塔由六个等价面定界。面的悬挂键密度是16.0/nm2,这高于面的悬挂键密度(12.1/nm2)和(0001)面的悬挂键密度(11.4/nm2)[3]。从这一点来看,面和(0001)面预期在GaN生长出开口之后出现。但是,图19示出了相反的情况。因此,可能的解释是面具有N极化,这使其在NH3流速较高时是稳定的。基于这点,3sccm的NH3流速事实上对于生长由面所成小面(faceted)的GaN线而言仍然很高。图20示出了在1.0sccm的NH3流速下生长的样品的SEM表征。俯视图像[图20(a)]与图19(a)类似。但是,35°倾斜的图像[图20(b)]是不同的,即面的垂直小面(facet)开始出现在金字塔帽的下面。
图21示出了将NH3流速进一步减少到0.5sccm时的生长结果。俯视图像和35°倾斜的图像均指示横向方向上的大小收缩,尽管它们仍然大于大约100nm的开口大小。而且倾斜的图像[图21(b)]还示出了垂直小面。当NH3流速被降低到0.2sccm时,真正的GaN纳米线开始合成,如图22所示。为了制造GaN纳米线,应当调节NH3流速以便实现或可选地描述低的过饱和;从而实现迁移增强型生长。如果需要其它形状,例如金字塔,则NH3流速可以为1sccm或更高。另外的制造步骤即提供包层和球状物可以用上面描述的方式来执行。
虽然本发明已结合目前认为最实用的优选实施例进行了描述,但是要理解本发明不限于所公开的实施例,相反旨在覆盖所附权利要求内的各种修改和等价布置。
Claims (14)
1.一种包括基片(105)和多个纳米结构化LED(100)的LED,其中每个LED包括外延地连接到纳米线(110)的体积元件(115),纳米结构化LED包括由纳米线(110)和体积元件(115)的组合形成的pn结和产生光的有源区(120),其中纳米结构化LED的至少一部分形成波导截面,其将有源区中产生的光定向到由纳米线给定的方向,其中每个单独LED被提供有在体积元件上的接触(125),该接触串联连接用于逐组地寻址LED。
2.根据权利要求1所述的LED,其中串联连接的接触(125)包括InSno、金属、金属合金、或其组合的任何层。
3.根据权利要求1或2所述的LED,其中所述接触(125)是透明的。
4.根据权利要求1或2所述的LED,其中所述接触(125)是反射性的。
5.根据权利要求1-4中的任一项所述的LED,其中接触(155)被提供在基片上,连接多个LED。
6.根据权利要求5所述的LED,其中接触(155)是底面接触。
7.根据权利要求6所述的LED,其中所述底面接触(155)是反射性的。
8.根据权利要求6所述的LED,其中所述底面接触(155)是透明的。
9.根据权利要求1-6中的任一项所述的LED,其中反射层(109)在纳米结构化LED的下面。
10.根据权利要求9所述的LED,其中反射层(109)是多层结构。
11.根据权利要求1-10中的任一项所述的LED,其中光被定向通过基片。
12.根据权利要求11所述的LED,其中减小基片的至少一部分的厚度以减小光的散射或吸收。
13.根据权利要求11所述的LED,其中基片的至少一部分是由透明材料制成的。
14.根据权利要求1-4中的任一项所述的LED,其中纳米结构化LED被从基片中去除。
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KR20090096704A (ko) | 2006-12-22 | 2009-09-14 | 큐나노 에이비 | 직립 나노와이어 구조를 갖는 led 및 이를 제조하는 방법 |
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US8049203B2 (en) | 2006-12-22 | 2011-11-01 | Qunano Ab | Nanoelectronic structure and method of producing such |
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2007
- 2007-12-22 KR KR1020097012816A patent/KR20090096704A/ko active IP Right Grant
- 2007-12-22 CN CN2007800517340A patent/CN101669219B/zh not_active Expired - Fee Related
- 2007-12-22 JP JP2009542711A patent/JP5453105B2/ja not_active Expired - Fee Related
- 2007-12-22 EP EP07861099.5A patent/EP2126986B1/en not_active Not-in-force
- 2007-12-22 WO PCT/SE2007/001170 patent/WO2008079076A1/en active Application Filing
- 2007-12-22 CN CN2011102356962A patent/CN102255018B/zh not_active Expired - Fee Related
- 2007-12-27 JP JP2009542712A patent/JP5145353B2/ja not_active Expired - Fee Related
- 2007-12-27 WO PCT/SE2007/001174 patent/WO2008079079A1/en active Application Filing
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- 2007-12-27 EP EP07861102.7A patent/EP2095425B1/en not_active Not-in-force
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2010
- 2010-09-13 HK HK10108614.7A patent/HK1142170A1/xx not_active IP Right Cessation
- 2010-09-21 HK HK10109014.1A patent/HK1142718A1/xx not_active IP Right Cessation
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2015
- 2015-03-20 US US14/664,158 patent/US10263149B2/en active Active
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CN104904016A (zh) * | 2012-10-26 | 2015-09-09 | 原子能及能源替代委员会 | 配备有过渡金属缓冲层的包含纳米线的电子器件、至少一个纳米线的生长方法以及器件制造方法 |
US9991342B2 (en) | 2012-10-26 | 2018-06-05 | Commissariat A L'energie Atomique Et Aux Energies Alternatives | Electronic device containing nanowire(s), equipped with a transition metal buffer layer, process for growing at least one nanowire, and process for manufacturing a device |
CN104904016B (zh) * | 2012-10-26 | 2019-10-11 | 原子能及能源替代委员会 | 具有过渡金属缓冲层的包含纳米线电子器件、至少一个纳米线的生长方法以及器件制造方法 |
US10636653B2 (en) | 2012-10-26 | 2020-04-28 | Commissariat A L'energie Atomique Et Aux Energies Alternatives | Process for growing at least one nanowire using a transition metal nitride layer obtained in two steps |
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CN109449267A (zh) * | 2018-10-30 | 2019-03-08 | 广东工业大学 | 一种紫外发光二极管及其制作方法 |
CN109616553A (zh) * | 2018-11-22 | 2019-04-12 | 中南大学 | 一种新型纤锌矿GaAs核壳纳米线光电探测器的制备方法 |
CN109616553B (zh) * | 2018-11-22 | 2020-06-30 | 中南大学 | 一种新型纤锌矿GaAs核壳纳米线光电探测器的制备方法 |
Also Published As
Publication number | Publication date |
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WO2008079079A1 (en) | 2008-07-03 |
JP2010514207A (ja) | 2010-04-30 |
US20100283064A1 (en) | 2010-11-11 |
US20150333225A1 (en) | 2015-11-19 |
EP2126986B1 (en) | 2019-09-18 |
JP5453105B2 (ja) | 2014-03-26 |
JP2010514206A (ja) | 2010-04-30 |
JP5145353B2 (ja) | 2013-02-13 |
HK1142718A1 (en) | 2010-12-10 |
CN101669219A (zh) | 2010-03-10 |
KR20090096704A (ko) | 2009-09-14 |
EP2095425A4 (en) | 2012-10-10 |
EP2126986A4 (en) | 2012-10-10 |
CN101681918A (zh) | 2010-03-24 |
HK1142170A1 (en) | 2010-11-26 |
EP2126986A1 (en) | 2009-12-02 |
CN102255018B (zh) | 2013-06-19 |
WO2008079076A1 (en) | 2008-07-03 |
EP2095425A1 (en) | 2009-09-02 |
EP2095425B1 (en) | 2019-04-17 |
CN101669219B (zh) | 2011-10-05 |
CN101681918B (zh) | 2012-08-29 |
US10263149B2 (en) | 2019-04-16 |
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