CN101213681A - 含有半导体纳米晶体的发光器件 - Google Patents
含有半导体纳米晶体的发光器件 Download PDFInfo
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- CN101213681A CN101213681A CNA2006800125477A CN200680012547A CN101213681A CN 101213681 A CN101213681 A CN 101213681A CN A2006800125477 A CNA2006800125477 A CN A2006800125477A CN 200680012547 A CN200680012547 A CN 200680012547A CN 101213681 A CN101213681 A CN 101213681A
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- electrode
- semiconductor
- metal chalcogenide
- inorganic
- inorganic material
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- 239000004054 semiconductor nanocrystal Substances 0.000 title claims abstract description 67
- 239000004065 semiconductor Substances 0.000 claims abstract description 50
- 229910010272 inorganic material Inorganic materials 0.000 claims abstract description 44
- 239000011147 inorganic material Substances 0.000 claims abstract description 43
- 239000002159 nanocrystal Substances 0.000 claims description 120
- 239000000463 material Substances 0.000 claims description 93
- 229910052751 metal Inorganic materials 0.000 claims description 54
- 239000002184 metal Substances 0.000 claims description 54
- 238000000034 method Methods 0.000 claims description 54
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- 238000000151 deposition Methods 0.000 claims description 28
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- 238000002156 mixing Methods 0.000 claims description 13
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Images
Classifications
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- H01L33/02—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies
- H01L33/14—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies with a carrier transport control structure, e.g. highly-doped semiconductor layer or current-blocking structure
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- B65D81/26—Adaptations for preventing deterioration or decay of contents; Applications to the container or packaging material of food preservatives, fungicides, pesticides or animal repellants with provision for draining away, or absorbing, or removing by ventilation, fluids, e.g. exuded by contents; Applications of corrosion inhibitors or desiccators
- B65D81/261—Adaptations for preventing deterioration or decay of contents; Applications to the container or packaging material of food preservatives, fungicides, pesticides or animal repellants with provision for draining away, or absorbing, or removing by ventilation, fluids, e.g. exuded by contents; Applications of corrosion inhibitors or desiccators for draining or collecting liquids without absorbing them
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- H01L33/06—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies with a quantum effect structure or superlattice, e.g. tunnel junction within the light emitting region, e.g. quantum confinement structure or tunnel barrier
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- H01L33/16—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies with a particular crystal structure or orientation, e.g. polycrystalline, amorphous or porous
- H01L33/18—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies with a particular crystal structure or orientation, e.g. polycrystalline, amorphous or porous within the light emitting region
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- H01L33/36—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the electrodes
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- H10K50/115—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers comprising active inorganic nanostructures, e.g. luminescent quantum dots
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Abstract
发光器件包括多个半导体纳米晶体和包含无机材料的电荷传输层。电荷传输层可以是空穴或电子传输层。无机材料可以是无机半导体。
Description
优先权要求
本申请要求于2005年2月16日提交的申请号为60/653,094的临时美国申请的优先权,其通过引用在此引入。
技术领域
本发明涉及含有半导体纳米晶体的发光器件。
联邦资助的研究或开发
依据来自空军宇航研究(Air Force Aerospace Research)的第FA9550-04-1-0462号拨款(Grant Number FA9550-04-1-0462)和来自国家科学基金(National ScienceFoundation)的第DMR-0213282号拨款(Grant Number DMR-0213282),美国政府对本发明可具有一定的权益。
背景技术
发光器件可以用于例如显示器(如平板显示器)、荧光屏(例如计算机荧光屏)和其他需要照明的物体。因此,发光器件的亮度是该器件的重要特征。同时,低工作电压和高效率可以改进制造发光器件的耐久性。在许多应用中,期望长的器件寿命。
发光器件可响应该器件活性成分的激发而释放光子。可以通过对该器件的活性成分(例如电致发光成分)施加电压而激发发射。电致发光成分可以是聚合物,例如共轭有机聚合物或含有有机分子的电致发光部分或层的聚合物。一般,可以通过器件的层之间的受激发的电荷的辐射性复合而产生发射。发出的光具有包括最大发射波长和发射强度的发射分布(emission profile),其中发射强度以亮度测量(坎德拉/平方米(cd/m2)或功率通量(W/m2))。可以通过材料的电子结构(例如能隙)改变器件的发射分布和其他物理特性。例如,发光器件的亮度、颜色范围、效率、工作电压和工作半寿期可以基于器件的结构而改变。
发明内容
通常,发光器件可以包括多个半导体纳米晶体。该半导体纳米晶体可以是无机半导体颗粒,例如直径为1-15nm的无机半导体颗粒,该颗粒任选地以有机配体层修饰(decorate)。纳米半导体显示出强的量子限制效应,其可以用来设计自底向上的化学方法,以产生具有电子和光学性质的复杂异质结构,该电子和光学性质可以随纳米晶体的尺寸和组成而调节。
半导体纳米晶体可以在发光器件中用做发光材料(lumophore)。因为半导体纳米晶体可具有窄的发射线宽、可为光致发光有效的和发射波长可调的,所以它们可为期望的发光材料。可以将半导体纳米晶体分散在液体中并因此与薄膜沉积技术如旋涂、滴涂和浸涂相适合。然而,在固态发光器件中,由这些沉积技术产生的块状半导体纳米晶体固体的电传输性能较差。与块状固体不同,半导体纳米晶体的单层可以应用于光发射器件中。单层提供半导体纳米晶体有利的发光性能,同时使对电性能的影响最小。
使用有机材料用于空穴传输或电子传输层(或两者)的器件可以具有高的电光转换效率,但由于有机材料固有的不稳定性,器件的寿命短。如光致发光研究证实的,无机纳米晶体本身可固有地比它们的有机发光材料对应物稳定。使用半导体纳米晶体用于发光和无机半导体用于电传输的发光器件(LED)可达到优越的光电子性能和长期稳定性。可以通过低温方法例如溅射、真空气相沉积、喷墨印刷或离子镀来沉积无机半导体。
可以使用微接触印刷(microcontact printing)将半导体纳米晶体沉积到基材上。有利地,微接触印刷容许在表面上特征的微米级或纳米级(例如小于1mm、小于500微米、小于200微米、小于100微米、小于25微米或小于1微米)的图案化。特别地,可以通过微接触印刷沉积半导体纳米晶体的单层。这种方法可以在基材上图案化的半导体纳米晶体膜的基本干燥的(即基本无溶剂)的应用。由此可以使用更多类型的基材,因为基材的选用不受溶解性和表面化学条件的限制。
一方面,发光器件包括:与第一电极接触的第一电荷传输层,该第一电荷传输层包括第一无机材料,该第一电极被布置以在第一电荷传输层中引入电荷;第二电极;和布置在第一电极和第二电极之间的多个半导体纳米晶体。该发光器件可以包括与第二电极接触的第二电荷传输层,其中布置第二电极以引入电荷。
第一无机材料可以是无定形的或多晶的。第一无机材料可以包括无机半导体。第二电荷传输层可以包括第二无机材料。第二无机材料可以是无定形的或多晶的。第二无机材料可为无机半导体。无机半导体可以包括金属硫族化物。金属硫族化物可为混合的金属硫族化物。金属硫族化物可以包括氧化锌、氧化钛、氧化铌、硫化锌、氧化铟锡、或其混合物。第一电荷传输层可以是空穴传输层,或者第一电荷传输层可以是电子传输层。多个半导体纳米晶体可以形成单层。该多个半导体纳米晶体可以是半导体纳米晶体的基本上单分散群体(monodisperse population)。多个半导体纳米晶体可以排列成图案。该器件可以是透明的。
另一方面,形成器件的方法包括:沉积包括第一无机材料的第一电荷传输层到电极上;在电极上沉积多个半导体纳米晶体,其中该多个纳米晶体与第一电荷传输层电接触。
沉积多个半导体纳米晶体包括将多个半导体纳米晶体沉积作为单层。沉积多个半导体纳米晶体包括形成图案。沉积第一无机材料可包括溅射。
该方法可以包括:沉积包括第二无机材料的第二电荷传输层到电极上,其中该多个纳米晶体与第二电荷传输层电接触。沉积第二无机材料可包括溅射。
另一方面,发光的方法包括提供包括第一电极、第二电极、与第一电极接触的包括第一无机材料的第一电荷传输层、和配置在第一电极和第二电极间的多个半导体纳米晶体的器件,以及跨越(across)第一电极和第二电极施加发光电势。
该器件可以进一步包括含有第二无机材料的第二电荷传输层。
另一方面,一种含有多个发光器件的显示器,其中至少一个发光器件包括:与第一电极接触的第一电荷传输层,该第一电荷传输层包括第一无机材料,该第一电极被布置以在第一电荷传输层中引入电荷;第二电极;和布置在第一电极和第二电极之间的多个半导体纳米晶体。
本发明其他的特征、目的和优点将从以下描述和附图以及权利要求中明晰。
附图说明
图1为描述发光器件的示意图。
图2为描述形成发光器件的方法的图。
图3A-3E为描述发光器件的示意图。
图4A为发光器件的示意性能量图。图4B是描述发光器件的电致发光性能的图。
图5为描述发光器件的电致发光性能的图。
图6A-6B为描述发光器件的电致发光性能的图。
具体实施方式
发光器件可以包括将该器件的两个电极分离的两层。一层的材料可以基于材料传输空穴的能力而选择,或空穴传输层(HTL)。另一层的材料可以基于材料传输电子的能力而选择,或电子传输层(ETL)。电子传输层一般包括电致发光层。当施加电压时,一个电极将空穴(正电荷载流子)注入到空穴传输层中,同时另一个电极将电子注入到电子传输层中。注入的空穴和电子各自向相反电荷的电极迁移。当电子和空穴定位于同一分子上时,形成激子,其可以复合而发光。该器件可在HTL和ETL之间包括发射层。发射层可包括对于其发射性能例如发射波长或线宽而选择的材料。
发光器件可以具有例如图1所示的结构,其中有第一电极2、与电极2接触的第一层3,与层3接触的第二层4,和与第二层4接触的第二电极5。第一层3可以为空穴传输层,而第二层4可以为电子传输层。至少一层可以为非聚合的。所述层可含有无机材料。该结构的电极之一与基材1接触。每个电极可以与电源接触,以跨越该结构提供电压。当对异质结构施加适当极性的电压时,可以通过异质结构的发射层产生电致发光。第一层3可以包括多个半导体纳米晶体,例如,纳米晶体的基本上单分散群体。或者,单独的发射层(图1未示出)可以包括在空穴传输层和电子传输层之间。单独的发射层可以包括多个纳米晶体,包括纳米晶体的层可以为纳米晶体的单层。
含有半导体纳米晶体的发光器件可以通过旋转浇铸(spin-casting)包含HTL有机半导体分子和半导体纳米晶体的溶液得到,其中HTL通过相分离在半导体纳米晶体单层下形成(参见,例如2003年3月28日提交的美国专利申请US10/400,907,和美国专利申请公开US2004/0023010,将每篇的全文引入作为参考)。这种相分离技术可再现地将半导体纳米晶体的单层置于有机半导体HTL和ETL之间,因此可以有效的地利用半导体纳米晶体的有利的的发光性能,同时也减小了使其对电子性能的影响最小化。采用这种技术制得的器件受到如下的限制来自:溶剂纯度;和;必须使用如半导体纳米晶体一样能可溶解到于同一溶剂中的有机半导体分子。这用该相分离技术不适用于将半导体纳米晶体的单层沉积到HTL和HIL两层两者的上边顶部(因为溶剂破坏下边在下面的有机薄膜)。该技术该相分离方法也不适用于容许控制在同一基材上控制发射不同颜色的半导体纳米晶体的位置;该技术还不容许控制适用于在同一基材上形成可发射不同颜色的纳米晶体的图案化。
而且,在传输层(即空穴传输、空穴注入或电子传输层)中使用的有机材料可不如发射层中的半导体纳米晶体稳定。结果,有机材料的使用寿命限制器件的寿命。在传输层中具有较长寿命的材料的器件可用于形成较长耐久的发光器件。
基材可以是不透明或透明的。透明基材可以用在透明LED的制造中,参见,例如:Bulovic,V.等,Nature 1996,380,29;和Gu,G.等,Appl..Phys.Lett.1996,68,2606-2608,将每篇都引入本文做为参考。透明LED可于应用例如在头盔护目镜或车辆挡风玻璃上的平视显示器(head-up display)。基材可以是刚性的或柔性的。基材可以是塑料、金属或玻璃。第一电极可以是例如高功函空穴注入导体,例如氧化铟锡(ITO)层。其他的第一电极材料可以包括氧化镓铟锡、氧化锌铟锡、氮化钛或聚苯胺。第二电极可以是例如低功函(例如小于4.0eV)的电子注入金属,例如Al、Ba、Yb、Ca、锂-铝合金(Li:Al)、或镁银合金(Mg:Ag)。第二电极如Mg:Ag可以用于保护阴极层免于空气氧化的不透明保护金属层如Ag层覆盖,或用相对薄的基本透明的ITO层覆盖。第一电极的厚度可以为约500埃~4000埃。第一层的厚度可以为约50埃~约5微米,例如100埃~100纳米、100纳米~1微米或1微米~5微米。第二层的厚度可以为约50埃~约5微米,例如100埃~100纳米、100纳米~1微米或1微米~5微米。第二电极的厚度可以为约50埃至大于约1000埃。
电荷传输层(HTL)或电子传输层(ETL)可以包括无机材料,例如无机半导体材料。无机半导体可为能带隙大于发射材料的发射能量的任意材料。无机半导体材料可以包括金属硫族化物、金属磷族元素化物或元素半导体,例如金属氧化物、金属硫化物、金属硒化物、金属碲化物、金属氮化物、金属磷化物、金属砷化物、或金属砷化物。例如,无机材料可以包括氧化锌、氧化钛、氧化铌、氧化铟锡、氧化同、氧化镍、氧化钒、氧化铬、氧化铟、氧化锡、氧化镓、氧化锰、氧化铁、氧化钴、氧化铝、氧化铊、氧化硅、氧化锗、氧化铅、氧化锆、氧化钼、氧化铪、氧化钽、氧化钨、氧化镉、氧化铱、氧化铑、氧化钌、氧化锇、硫化锌、硒化锌、碲化锌、硫化镉、硒化镉、碲化镉、硫化汞、硒化汞、碲化汞、碳化硅、钻石(碳)、硅、锗、氮化铝、磷化铝、砷化铝、锑化铝、氮化镓、磷化镓、砷化镓、锑化镓、氮化铟、磷化铟、砷化铟、锑化铟、氮化铊、磷化铊、砷化铊、锑化铊、硫化铅、硒化铅、碲化铅、硫化铁、硒化铟、硫化铟、碲化铟、硫化镓、硒化镓、碲化镓、硒化锡、碲化锡、硫化锡、硫化镁、硒化镁、碲化镁、或其混合物。金属氧化物可以是混合的金属氧化物,例如ITO。在器件中,纯金属的氧化物的层(即具有单独的基本纯的金属的金属氧化物)随着时间可生长结晶区域,降低器件的性能。与使用纯金属氧化物相比,混合的金属氧化物较不容易形成这样的结晶区域,提供较长的器件寿命。金属氧化物可以是掺杂的金属氧化物,其中掺杂是例如氧缺陷、卤素掺杂物或混合的金属。无机半导体可以包括掺杂物。通常,掺杂物可以是p型或n型掺杂物。HTL可以包括p型掺杂剂,而ETL可以包括n型掺杂剂。
在LED中已提出单晶无机半导体用于电荷传输到半导体纳米晶体。单晶半导体通过需要将被涂覆的基材加热到高温的技术沉积。然而,顶层半导体必须直接沉积在纳米晶体层上,该纳米晶体层不耐高温处理,也不适合于容易的外延生长。外延技术(例如化学蒸发沉积)的制造也可为昂贵的,且通常不能用于覆盖较大面积(即大于12英寸直径的晶片)。
有利地,无机半导体可在低温例如通过溅射沉积到基材上。溅射通过对低压气体(例如氩)施加高电压以产生高能状态的电子和气体离子的等离子体而进行。增能的等离子体离子撞击所需涂覆材料的靶,导致原子从该靶具有足够的能量地排出,以移动到基材并与其结合。
在生长过程中,基材或制造的器件被冷却或加热以控制温度。温度影响沉积材料的结晶度,也影响它与它沉积的表面之间如何相互作用。沉积材料可以是多晶或无定形的。沉积的材料具有尺寸在10埃~1微米范围内的结晶域(domain)。掺杂浓度可以通过改变气体或气体混合物进行控制,该气体或气体混合物用于等离子体溅射。掺杂的性质和程度可以影响沉积膜的导电性,也影响其光学猝灭邻近激子的能力。通过在另一材料顶部上生长一种材料,可产生p-n或p-i-n二极管。为传递电荷到半导体纳米晶体单层,可以优化器件。
该层可以通过旋涂、浸涂、气相沉积、溅射或其他薄膜沉积方法沉积在电极之一的表面上。第二电极可以夹在、溅射或蒸发到固体层的暴露表面上。可以对电极之一或二者图案化。通过导电路径,可以将器件的电极连接到电压源。在施加电压时,从器件中发出光。
微接触印刷提供将材料涂覆到基材上预定区域的方法。该预定区域是在基材上其中选择性涂覆材料的区域。可以对材料和基材进行选择,使得材料基本上完全保持在预定区域内。通过选择形成图案的预定区域,将材料涂覆到基材上,使得材料形成图案。图案可以是规则图案(例如阵列或一系列线)或不规则图案。一旦在基材上形成材料的图案,基材可具有含有材料的区域(预定区域)和基本上不含材料的区域。在有些情况下,材料在基材上形成单层。预定区域可以是非连续区域。换句话说,当材料涂覆到基材的预定区域时,含有材料的位置被基本上不含材料的其他位置分开。
通常,微接触印刷从形成图案化模具开始。模具的表面具有凸起和凹陷的图案。例如通过用液体聚合物前体涂覆模具表面,形成具有与凸起和凹陷互补的图案的印记,该液体聚合物前体当与模具的图案化表面接触时固化。然后将印记上墨,即,将印记与要沉积到基材的材料接触。材料可逆地粘附到印记上。然后将上墨的印记与基材接触。印记凸起的部分可与基材接触,而凹陷的部分可与基材分离。在上墨的印记接触基材时,墨材料(或其至少一部分)从印记转印到基材上。采用这种方式,凸起和凹陷的图案从印记转移到基材上,作为基材上含有材料的区域和不含有材料的区域。微接触印刷和相关的技术描述在例如美国专利No.5,512,131、6,180,239和6,518,168中,将每篇的全文引入做为参考。在有些情况下,印记可以是具有墨图案的无特征印记,当墨施加到印记上时形成图案。参见2005年10月21号提交的美国专利申请No.11/253,612,将其全文引入做为参考。
图2描述了概述微接触印刷过程的基本步骤的流程图。首先,采用标准的半导体加工工艺制造硅母版(master),该加工工艺在硅表面上形成图案,例如凸起和凹陷的图案(或者,对于无图案沉积,可使用空白硅母版)。然后混合聚二甲基硅氧烷(PDMS,例如Sylgard 184)前体,脱气,倒入母版中,再脱气,在室温下固化(或高于室温以便于加速固化)(步骤1)。然后将表面具有硅母版图案的PDMS印记从模具中取出,裁切成需要的形状和大小。然后将该印记涂覆表面化学层,该表面化学层选择为容易地根据需要粘附和释放墨。例如,该表面化学层可以是化学气相沉积的聚对二甲苯-C层。表面化学层可为例如0.1~2μm厚,取决于待复制的图案(步骤2)。然后,将该印记上墨,例如通过旋转浇注、注射泵分配、或喷墨印刷半导体纳米晶体的溶液(步骤3)。溶液可以例如在氯仿中1-10mg/ml的浓度。可以根据所需结果改变浓度。然后上墨的印记可与基材接触,并施加温和的压力,例如30秒,以将墨(即半导体纳米晶体单层)完全转移到新基材上(步骤4)。图2A和2B描绘了ITO涂覆的玻璃基材的制备。将包括有机半导体的电荷传输和/或电荷注入层(分别为HTL和HIL)热蒸发到ITO基材上。将图案化的半导体纳米单层转移到该HTL层,然后加入器件的其余部分(例如,电子传输层(ETL)、电子注入层(EIL)和金属接点)(步骤5)。参见,例如,2005年10月21日提交的美国专利申请No.11/253,595和11/253,612以及2005年1月11日提交的11/032,163,将每篇的全文引入做为参考。
当电子和空穴定位于纳米晶体上,可在发射波长处产生发射。发射频率与量子局限的(confined)半导体材料的能带隙相应。该能带隙是纳米晶体尺寸的函数。小直径的纳米晶体可以具有介于物质的分子形式和整体形式之间中间的性质。例如,基于半导体材料的小直径的纳米晶体在所有三维空间中可表现出电子和空穴二者的量子局限(quantum confinement),这导致材料的有效能带隙随晶体尺寸的减小而增加。因此,随着微晶尺寸的减小,纳米晶体的光学吸收和发射移动到蓝色或更高的能量。
来自纳米晶体的发射可为窄的高斯发射带,其可以通过改变纳米晶体的尺寸、纳米晶体的组成或二者在光谱的紫外、可见光或红外区域的全部波长范围上调节。例如,CdSe可以在可见光区域内调整,以及InAs可以在红外区域内调整。纳米晶体群体的窄尺寸分布可以导致在窄光谱范围内的光的发射。该群体可以为单分散的,并且可展现出纳米晶体的直径的小于15%rms偏差,优选为小于10%,更优选为小于5%。可以观察到对于在可见光范围内发射的纳米晶体在不大于约75纳米、优选60纳米、更优选40纳米和最优选30纳米的半高宽(FWHM)的窄范围内的光谱发射。IR发射纳米晶体的FWHM可不大于150纳米,或不大于100纳米。用发射能量来表示时,该发射的FWHM可不大于0.05eV,或不大于0.03eV。发射宽度随着纳米晶体直径的分散性的降低而减小。半导体纳米晶体可以具有高量子发射效率,例如大于10%、20%、30%、40%、50%、60%、70%或80%。
形成纳米晶体的半导体可以包括II-VI族化合物、II-V族化合物、HI-VI族化合物、III-V族化合物、IV-VI族化合物、I-HI-VI族化合物、H-IV-VI族化合物、或II-IV-V族化合物,例如,ZnS、ZnS、ZnSe、ZnTe、CdO、CdS、CdSe、CdTe、MgO、MgS、MgSe、MgTe、HgO、HgS、HgSe、HgTe、AlN、AlP、AlAs、AlSb、GaN、GaP、GaAs、GaSb、InN、InP、InAs、InSb、TlN、TlP、TlAs、TlSb、TlSb、PbS、PbSe、PbTe、或其混合物。
单分散半导体纳米晶体的制备方法包括注入热的配位溶剂中的有机金属反应物例如二甲基镉的热解。这容许离散成核,并导致宏观量的纳米晶体的受控增长。纳米晶体的制备和处理描述于例如,美国专利6,322,901和6,579,291以及美国专利申请No.60/550,314中,其各自全文在此引入做为参考。纳米晶体的制造方法是胶体生长法。通过将M给体和X给体快速注入热的配位溶剂中而产生胶体生长。注入产生核,该核可以受控方式生长以形成纳米晶体。可以温和地加热反应混合物以生长纳米晶体,并使之退火。样品中纳米晶体的平均尺寸和尺寸分布取决于生长温度。保持稳定生长所必需的生长温度随平均晶体尺寸的增加而升高。该纳米晶体是纳米晶体群体的成员。由于离散成核和受控生长,获得的纳米晶体群体具有窄的直径单分散分布。直径单分散分布也可以指尺寸。成核后的在配位溶剂中纳米晶体的受控生长和退火的过程也可导致均匀的表面衍生(surface derivatization)和规则的核结构。随着尺寸分布锐化,可以升高温度以保持稳定生长。通过加入更多M给体或X给体,可以缩短生长周期。
M给体可以为无机化合物、有机金属化合物或元素金属。M为镉、锌、镁、汞、铝、镓、铟或铊。X给体为能够与M给体反应形成通式MX的材料的化合物。典型地,X给体为硫族化物给体或磷族元素化物给体,例如膦硫族化物、二(甲硅烷基)硫族化物、双氧、铵盐、或三(甲硅烷基)磷族元素化物。合适的X给体包括双氧、二(三甲基甲硅烷基)硒化物((TMS)2Se)、三烷基膦硒化物例如(三-正辛基膦)硒化物(TOPSe)或(三-正丁基膦)硒化物(TBPSe)、三烷基膦碲化物例如(三-正辛基膦)碲化物(TOPTe)或六丙基磷三酰胺碲化物(HPPTTe)、二(三甲基甲硅烷基)碲化物((TMS)2Te)、二(三甲基甲硅烷基)硫化物((TMS)2S)、三烷基膦硫化物例如(三-正辛基膦)硫化物(TOPS)、铵盐例如卤化铵(例如,NH4Cl)、三(三甲基甲硅烷基)磷化物((TMS)3P)、三(三甲基甲硅烷基)砷化物((TMS)3As)、或三(三甲基甲硅烷基)锑化物((TMS)3Sb)。在某些实施方式中,M给体和X给体可以为相同分子中的部分。
配位溶剂可以有助于控制纳米晶体的生长。配位溶剂是具有给体孤对的化合物,其例如具有可以配位到生长纳米晶体表面的孤电子对。溶剂配位可以使生长纳米晶体稳定化。典型的配位溶剂包括烷基膦、烷基膦氧化物、烷基膦酸或烷基次膦酸,但是其他配位溶剂例如吡啶、呋喃和胺也可以适用于制备纳米晶体。合适的配位溶剂的实例包括吡啶、三-正辛基膦(TOP)、三-正辛基膦氧化物(TOPO)和三-羟丙基膦(tHPP)。可以使用工业级TOPO。
通过监控颗粒的吸收线宽可以估计在反应的生长阶段过程中的尺寸分布。响应于颗粒吸收光谱中变化的反应温度的改变容许在生长过程中保持尖锐的粒度分布。在晶体生长过程中,可以将反应物加入到成核溶液中以生长更大的晶体。通过在特定的纳米晶体平均直径处停止生长以及选择半导体材料的适当组成,对于CdSe和CdTe,可以在300纳米~5微米,或400纳米~800纳米的波长范围连续调整纳米晶体的发射光谱。纳米晶体的直径小于150埃。纳米晶体的群体的平均直径为15埃~125埃。
该纳米晶体可以为具有窄尺寸分布的纳米晶体群体成员。纳米晶体可以为球形、棒形、盘形或其他形状。纳米晶体可以包括半导体材料的核。纳米晶体可以包括具有式MX的核,其中M为镉、锌、镁、汞、铝、镓、铟、铊或其混合物,并且X为氧、硫、硒、碲、氮、磷、砷、锑或其混合物。
核可以在其表面上具有外涂层。外涂层可以为具有组成不同于核的组成的半导体材料。纳米晶体表面上的半导体材料的外涂层可以包括II-VI族化合物、II-V族化合物、III-VI族化合物、III-V族化合物、IV-VI族化合物、I-III-VI族化合物、II-IV-VI族化合物、或II-IV-V族化合物,例如,ZnO、ZnS、ZnSe、ZnTe、CdO、CdS、CdSe、CdTe、MgO、MgS、MgSe、MgTe、HgO、HgS、HgSe、HgTe、AlN、AlP、AlAs、AlSb、GaN、GaP、GaAs、GaSb、InN、InP、InAs、InSb、TlN、TlP、TlAs、TlSb、PbS、PbSe、PbTe、或其混合物。例如,ZnS、ZnSe或CdS外涂层可以在CdSe或CdTe纳米晶体上生长。外涂层工艺描述于例如,美国专利6,322,901中。通过在外涂覆过程中调整反应混合物的温度和监控核的吸收光谱,可以获得具有高量子发射效率和窄尺寸分布的外涂层材料。外涂层可为1~10单层的厚度。
可以用对于纳米晶体的不良溶剂例如甲醇/丁醇通过尺寸选择沉淀进一步精制粒度分布,如描述于美国专利6,322,901中。例如,纳米晶体可以分散在己烷的10%丁醇溶液中。可以将甲醇逐滴加入到搅拌的溶液中,直至乳白光持续。通过离心分离上层清液和絮凝物,在样品中产生富含最大微晶的沉淀物。可重复进行该步骤直至不再发现光学吸收光谱的进一步锐化。尺寸选择沉淀可以在各种溶剂/非溶剂对中进行,包括吡啶/己烷和氯仿/甲醇。尺寸选择的纳米晶体群体可以具有从平均直径不大于15%rms偏差,优选10%rms偏差或更小,更优选5%rms偏差或更小。
纳米晶体的外表面可以包括来自生长工艺中使用的配位溶剂的化合物。该表面可以通过重复暴露于过量的竞争配体基团中来改性。例如,封端的(capped)纳米晶体的分散体可以用配位有机化合物例如吡啶处理,以制备容易分散于吡啶、甲醇和芳香化合物,但不再分散于脂族溶剂中的微晶。这种表面交换工艺可以用任何能够与纳米晶体的表面配位或结合的化合物进行,包括例如膦、硫醇、胺和磷酸盐(phosphates)。纳米晶体可以暴露于短链聚合物,该聚合物显示出对表面的亲和性,并且在对悬浮或分散介质具有亲和性的部分中止。该亲和性改善悬浮液的稳定性,并且阻碍纳米晶体的絮凝。纳米晶体配位化合物描述于美国专利No.6,251,303中,其全文引入做为参考。
更具体地,配位配体可以具有下式:
(YXL)
k-n n
其中k为2、3或5,并且n为1、2、3、4或5,以使k-n不小于0;X为O、S、S=O、SO2、Se、Se=O、N、N=O、P、P=O、As或As=O;Y和L各自独立地为芳基、杂芳基或直链或支链C2-12烃链,该烃链任选含有至少一个双键、至少一个三键或至少一个双键和一个三键。该烃链可任选被一个或多个C1-4烷基、C2-4链烯基、C2-4炔基、C1-4烷氧基、羟基、卤素、氨基、硝基、氰基、C3-5环烷基、3-5元杂环烷基、芳基、杂芳基、C1-4烷基羰氧基、C1-4烷氧基羰基、C1-4烷基羰基或甲酰基。该烃链还可任选被-O-、-S-、-N(Ra)-、-N(Ra)-C(O)-O-、-O-C(O)-N(Ra)-、-N(Ra)-C(O)-N(Rb)-、-O-C(O)-O-、-P(Ra)-或-P(O)(Ra)-间隔。Ra和Rb各自独立地是氢、烷基、链烯基、炔基、烷氧基、羟烷基、羟基或卤代烷基。
芳基可以是芳基取代或未取代的环状芳香基。实例包括苯基、苄基、萘基、甲苯基、蒽基、硝基苯基或卤代苯基。杂芳基为环上具有一个或多个杂原子的芳基,例如呋喃基、吡啶基、吡咯基、菲基。
合适的配位配体可以从市场上购得,或通过常规有机合成技术制备,例如描述于J.March,Advanced Organic Chemistry中,在此引入其全文做为参考。
透射电子显微镜(TEM)可以提供有关纳米晶体群体的尺寸、形状和分布的信息。粉末X射线衍射(XRD)图形可以提供有关纳米晶体的晶体结构的类型和量的最完整的信息。也可估计尺寸,因为粒径通过X射线相干长度反比于(inverselyrelated to)峰宽度。例如,纳米晶体的直径可以通过透射电子显微镜直接测量或使用例如Scherrer方程从X射线衍射数据估计。也可以从UV/Vis吸收光谱估计。
可以在单一基材的多个区域形成单独的器件以形成显示器。该显示器可以包括在不同波长发射的器件。通过图案化具有不同颜色发射材料的阵列的基材,可形成含有不同颜色象素的显示器。在有些应用中,基材可以包括底板(backplane)。该底板包括活性或非活性电子器件,以控制或转换施加到像素上的电力。具有该底板可以应用于领域如显示器、传感器、或成像器。特别地,底板可以设置成有源矩阵、无源矩阵、固定格式、直接驱动或混合型。显示器可以设置用于静止图像、动态图像或照明。照明显示器可以提供白光、单色光或彩色可调光。参见例如2005年10月21号提交的美国专利申请No.11/253,612,将其全文引入做为参考。
该器件在受控的(无氧和无水)环境下制造,防止制造过程中抑制发光效率。可以使用其他多层结构,以改善器件性能(参见,例如2003年3月28日提交的美国专利申请No.10/400,907和10/400,908,将每篇的全文引入做为参考)。阻挡层如电子阻挡层(HBL)、空穴阻挡层(HBL)或空穴和电子阻挡层(eBL)可以引入该结构中。阻挡层可以包括3-(4-联苯基)-4-苯基-5-叔丁基苯基-1,2,4-三唑(TAZ)、3,4,5-三苯基-1,2,4-三唑、3,5-双(4-叔丁基苯基)-4-苯基-1,2,4-三唑、浴铜灵(BCP)、4,4′,4″-三{N-(3-甲苯基)-N-苯基氨基}三苯基胺(m-MTDATA)、聚亚乙基二氧噻吩(PEDOT)、1,3-二(5-(4-二苯基氨基)苯基-1,3,4-噁二唑-2-基)苯、2-(4-联苯基)-5-(4-叔丁基苯基)-1,3,4-噁二唑、1,3-二[5-(4-1,1-二甲基乙基)苯基-1,3,4-噁二唑-2-基]苯、1,4-二(5-(4-二苯基氨基)苯基-1,3,4-噁二唑-2-基)苯。
可以通过增加有机发光器件的效率、缩小或增宽它们的发射光谱、或偏振它们的发射,改善有机发光器件的性能。例如,参见Bulovic等的Semiconductors andSemimetals 64,255(2000);Adachi等的Appl.Phys.Lett.78,1622(2001);Yamasaki等的Appl.Phys.Lett.76,1243(2000);Dirr等的Jpn.J.Appl.Phys.37,1457(1998)和D’Andrade等的MRS Fall Meeting,BB6.2(2001),在此将每篇的全文引入做为参考。纳米晶体可以包括在有效的混合有机/无机发光器件中。
纳米晶体的窄FWHM可以产生饱和色发射。即使在可见光谱的红色和蓝色部分中,这也可产生有效的纳米晶体发光器件,因为在纳米晶体发射器件中,没有光子进行红外和UV发射。在单一材料系统的整个可见光光谱中,该广泛可调的饱和色发射是任何种类的有机生色团不匹配的(参见,例如,Dabbousi等的J.Phys.Chem.101,9463(1997),将其全文引入做为参考)。纳米晶体的单分散群体将发射跨越窄波长范围的光。包括超过一种尺寸的纳米晶体的器件发射在超过一种窄波长范围内的光。可以通过选择器件中纳米晶体的尺寸和材料的适当组合来控制观察者观察的发射光的颜色。纳米晶体的能带边缘能级的间并度促进所有可能激子的捕获和辐射复合,无论是通过直接电荷注入还是通过能量转移产生的。因此,最大理论纳米晶体发光器件的效率是可与磷光有机发光器件的整体效率比较的。纳米晶体的激发态寿命(τ)(τ~10ns)远大于典型的磷光体(τ>0.5μs),使得纳米晶体发光器件即使在高电流密度下也能有效工作。
可以制备发射可见光或红外光的器件。可以选择半导体纳米晶体的尺寸和材料,以使纳米晶体发射选定波长的可见或红外光。该波长可以为300~2500纳米或更高,例如300~400纳米、400~700纳米、700~1100纳米、1100~2500纳米或大于2500纳米。
可以在同一基材的多个区域形成单独的器件以形成显示器。该显示器可以包括可发射不同波长光的器件。通过图案化具有不同颜色发射的半导体纳米晶体的阵列的基材,可形成含有不同颜色象素的显示器。
将p型半导体例如NiO沉积到透明电极例如氧化铟锡(ITO)上,以形成器件。透明电极可以设置在透明基材上。然后,使用适用于大面积相容的单独单层沉积技术例如微接触印刷或朗缪尔-布洛杰特(LB)技术沉积半导体纳米晶体。随后,在该层顶部上,通过例如溅射法涂覆n型半导体(例如ZnO或TiO2)。在这之上可热蒸发金属电极以完成器件。更复杂的器件结构也是可能的。例如,邻近纳米晶体层可包括轻微掺杂层,以使非辐射损失最小化,该损失是由于通过传输层中的无束缚的电荷载流子的激子猝灭引起的。
可以通过分别生长两个传输层和使用弹性体例如聚二甲基硅氧烷(PDMS)物理地涂覆电触点,进而装配器件。这避免在纳米晶体层上直接沉积材料的需要。
在涂覆所有的传输层后,可以热处理器件。热处理可以进一步增强电荷向纳米晶体的注入,还消除纳米晶体上的有机封端(capping)基团。封端基团的不稳定性可有助于器件的不稳定性。
所使用的无机传输层,特别是金属氧化物材料可以做为阻挡层,以阻止O2和H2O进入到器件的活性层(半导体纳米晶体层)。无机层的保护性质可以为包装提供设计选择。例如,由于无机层可以阻碍水和/或氧,可制造器件,而不需要额外组件以阻止这些污染物达到发射材料。使用金属氧化物和聚合物的交替层制造密封剂涂层例如BAPIX(由Vitex制造)。在这种阻挡层中,金属氧化物阻止O2和H2O,聚合物层使金属氧化物层中的针孔缺陷随机化。因此,在使用金属氧化物作为传输层的情况下,器件本身起到对半导体纳米晶体的保护层的作用。
图3A-3E显示了可能的器件结构。它们是标准的p-n二极管设计(图3A),p-i-n二极管设计(图3B),透明器件(图3C),倒转器件(图3D,通过薄膜晶体管(TFT)工艺优化接触),柔性(flexible)器件(图3E)。在柔性器件的情况中,可以为每个单独层的金属氧化物层引入滑动层,即金属氧化物/金属/金属氧化物型三层结构。这已显示增加金属氧化物薄膜的柔性、增加导电性,同时保持透明性。这是因为金属层(典型为银)非常薄(大约每层12nm),因此,不吸收很多光。这样,采用这种技术,适合的和可能甚至柔性显示器是可实现的。
由于掺杂的无机半导体的高导电性,与采用有机传输材料制得的器件相比,该器件本身可具有较低电压。因为具有无机发光团和传输层,该器件也具有增加的电致发光寿命。尽管在本领域中的寿命受到驱动故障或线接触故障的限制,外延制备的无机LED的实验室寿命超过100,000小时。最后,因为器件通过通过将载流子直接注入到纳米晶体中而专门地工作,单线态和三线态都有效的转换成发光激子。因此器件可通过以上四个因素而更有效。
实施例
制备LED,其中通过化学和电学更稳定的高能带隙(>3ev)的无机空穴传输层代替有机TPD膜。基于能带偏移考虑(相对于CdSe纳米晶体)、易于沉积、和其与CdSe纳米晶体的化学相容性,选择NiO。另外,早期研究已表明,透明的p型NiO膜可通过NiO或Ni靶的接近室温的反应性溅射得到,且可以在电光器件中用做空穴传输/注入层。参见,例如H.Sato等的Thin Solid Film 236,1-2(1993);K.Suga等的Sens.Actrators B 14,598(1993);和W.Y.Lee等的Appl.Phys.Lett.72,1584(1998),将每篇文章的全文引入做为参考。所研究的LED器件的能带结构说明在图4A中,其中NiO空穴传输层和Alq3电子传输层把纳米晶体发光层夹在中间。
为制造高效率的NiO QD-LED,通过NiO中自由电荷载流子的高密度的纳米晶体单层发光的猝灭是需要克服的基本光物理问题。观测到与沉积到高导电性(ρ≈5×10-4Ω.cm)NiO和ITO薄膜的上部的纳米晶体的猝灭发光相反,沉积到电阻性(ρ≈1Ω.cm)NiO或ITO薄膜的上部的单独纳米晶体的光致发光效率保持很高,由此解决了上述问题。该观测与早期的理论和实验工作是一致的,早期的理论和实验工作证明通过电介质的有机和无机发光团的光致发光猝灭可以通过控制发色团介电距离(chromophore-dielectric distance)和通过调节电介质的介电常数进行调节,这些随着器件中NiO层中的空穴浓度而改变。参见,例如K.H.Drexhage等的Ber.Bunsenges.Phys.Chem.70,1179(1966);H.Kuhn和D.Mobius,Angew.Chem.10,620(1971);R.R.Chance等的J.Chem.Phys.60,2744(1974);I.Larkin等的Phys.Rev.B 69,121403(R)(2004)和H.Morawitz,Phys.Rev.187,1792(1969),将每篇文章的全文引入做为参考。
LED的制备如下。在沉积NiO薄膜之前,将预涂了ITO的玻璃基材(具有薄膜电阻为30Ω/□(欧姆每平方))通过在清洁剂溶液、去离子水和丙酮中顺序漂洗而清洁,然后在异丙醇中煮沸5分钟。清洁完毕后,将基材在氮气中干燥并暴露于紫外-臭氧以清除任何吸附的有机材料。然后将基材放入氮手套箱中,其通过高真空传输线与溅射和蒸发室连接。在溅射室中,通过在Ar/O2气体混合物中NiO靶的反应性RF磁控管溅射沉积30nm厚的NiO薄膜。溅射前的基础压力为10-7托,RF功率固定为200W,等离子体压力为6毫托,O2和Ar的气流速率比为2.5%,这导致NiO的沉积速率为0.03nm/s。在以上沉积参数下,NiO膜为p型,其电阻率为ρ=5Ω.cm(薄膜电阻为2Ω/□(欧姆每平方)),在波长λ=625nm(纳米晶体发射峰的中心)处的光透射率为80%。它们在空气和在纳米晶体的化学处理过程时使用的有机溶剂中是稳定的。将玻璃/ITO/NiO基材传输回手套箱中,其中通过旋转浇注出氯仿将它们用CdSe/ZnS核/壳纳米晶体的单层涂覆。旋转浇注的纳米晶体膜的厚度通过改变氯仿中纳米晶体的浓度和/或旋涂过程中旋转的速度进行调节。然后基材无需暴露于空气而转移到蒸发室中,在10-6托和沉积速度为~0.2nm/s的条件下蒸发40nm厚Alq3电子传输层。然后通过荫罩板蒸发100nm厚Ag/Mg(重量比为1/10)和30nm厚Ag电子注入电极,形成1mm直径的圆形电极(电极面积为0.78mm2)。在有些器件中,在沉积Alq3层之前,将10nm厚的3-(4-联苯基)-4-苯基-5-叔丁基苯基-1,2,4-三唑(TAZ)空穴阻挡层的膜蒸发到纳米晶体层上(参见S.Coe-Sullivan等的Proc.Of SPIEvol.5739,p.108(2005),将其全文引入做为参考)。将刚制得的器件从集成沉积系统中取出,不经过组装,直接在空气中进行测试。
相对于接地Ag阴极测量NiO纳米晶体LED的典型正向偏压电流-电压(I-V)特性,将结果绘图于图4B中。对于大多数纳米晶体LED,J∝Vn,在(6±1)V以下1<n<1.5,和在较高电压下6<n<7。这里,n是电荷导电机理的特征,且与温度、有机或无机材料中阱状态(trap state)的密度和能量分布有关。这些I-V曲线与在CdSe/ZnS密堆集膜和OLED中阱协助空间电荷有限传导的早先报道一致。参见,例如R.A.M.Hikmet等的J.Appl.Phys.93,3509(2003);P.E.Burrows和S.R.Forrest,Appl.Phys.Lett.64,2285(1994);和P.E.Burrows等的J.Appl.Phys.79,7991(1996),将每篇文章的全文引入做为参考。达到的最大稳态电流密度一般为~4A/cm2。在此电流密度下,在发光纳米晶体层的每个纳米晶体中每秒可注入8×107个载流子。因为在纳米晶体器件中单线态激子复合时间≤10ns,在该高电流水平下,每个纳米晶体的激子密度可达到40%。参见例如C.R.Kagan等的Phys.Rev.B 54,3633(1996);和C.R.Kagan等的Phys.Rev.Lett,76,1517(1996);将每篇的全文引入做为参考。
图5描绘了电流密度为200mA/cm2下,具有电阻性NiO层(ρ=5Ω.cm)的NiO纳米晶体LED的EL光谱。30nmFWHM纳米晶体发射峰的中心在λ=625nm,该峰为EL谱的主峰。在λ=530nm处的较宽的肩是由于弱的Alq3发射。纳米晶体和Alq3的HOMO能级之间的1eV能带偏移(参见图4A中的能带图)使得空穴能够注入到Alq3层中。反向偏压时没有观察到EL。图5的插图显示了对于相同的电阻性NiO器件ηEL作为电流密度函数的变化,该器件驱动直到J>200mA/cm3的转换点(breaking point)。典型的I-V特性在整个该组纳米晶体LED中与ηEL≤0.18%和亮度最高到40Cd/m2一致。
图6描绘了低电阻NiO(10-2Ω.cm)对纳米晶体LED光谱的不利影响。对于这些器件ηEL<10-3%。与图5相反(图5中器件包括较高电阻性的NiO),在图6中,电流密度低于300mA/cm2时,检测到EL的将近50%来自Alq3层(图6A中的星号标记)。该效果归因于由高掺杂的NiO薄膜引起的电子和空穴注入器件中的不平衡,该NiO薄膜增强了空穴密度。增加的空穴注入使激子复合区域转移到Alq3层,并且在发光纳米晶体附近的过量NiO空穴降低了纳米晶体单层的电致发光效率。另外,CdSe纳米晶体中过量的空穴可导致超快(~100ps)非辐射Auger驰豫(relaxation)。参见V.I.Klimov等Science 287,1011(2000),将其全文引入做为参考。在1500mA/cm2(图6A中的实线)时,85%的EL来自纳米晶体。纳米晶体光谱贡献随电流的增加归因于器件中电荷载流子浓度密度的再平衡和较高电场下纳米晶体充电(nanocrystal charging)的降低,较高电场是造成较高的电流密度的原因。在图6B中,空圆和空的菱形分别表示了Alq3和纳米晶体EL峰下集成区域的变化。
总之,使用p型NiO膜作为空穴传输层制造纳米晶体LED。NiO电阻性的仔细优化防止纳米晶体发光的降低和容许纳米晶体LED的外部量子效率高达0.18%。与使用TPD空穴传输层的所报道的最好的纳米晶体LED相比,尽管本发明的纳米晶体LED的效率要低,但本发明的纳米晶体LED中使用更稳定的金属氧化物膜。由于NiO溅射界面的粗糙,大部分注入电流被分流通过器件。使用较光滑的NiO膜,可以预期纳米晶体LED效率的显著增加。不像在溶剂敏感的有机薄膜顶部旋转浇注,使用共价结合的化学稳定的无机空穴或电子注入层使得能够进行任何纳米晶体的溶液的旋转浇注沉积。因此,引入金属氧化物发展和简化了纳米晶体LED的制作过程。
其他实施方式在随附的权利要求书中。
Claims (69)
1.发光器件,包括:
包括第一无机材料的第一电荷传输层,其与第一电极接触,该第一电极被布置以在该第一电荷传输层中引入电荷;
第二电极;和
布置在该第一电极和第二电极之间的多个半导体纳米晶体。
2.如权利要求1所述的发光器件,进一步包括与该第二电极接触的第二电荷传输层,其中第二电极被布置以在该第二电荷传输层中引入电荷。
3.如权利要求1所述的发光器件,其中该第一无机材料是无定形的或多晶的。
4.如权利要求1所述的发光器件,其中该第一无机材料是无机半导体。
5.如权利要求4所述的发光器件,其中该无机半导体包括金属硫族化物。
6.如权利要求5所述的发光器件,其中该金属硫族化物是混合的金属硫族化物。
7.如权利要求5所述的发光器件,其中该金属硫族化物包括氧化锌、氧化钛、氧化铌、硫化锌、氧化铟锡、或其混合物。
8.如权利要求1所述的发光器件,其中该第二电荷传输层包括第二无机材料。
9.如权利要求8所述的发光器件,其中该第二无机材料是无定形的或多晶的。
10.如权利要求8所述的发光器件,其中该第二无机材料是无机半导体。
11.如权利要求10所述的发光器件,其中该无机半导体包括金属硫族化物。
12.如权利要求11所述的发光器件,其中该金属硫族化物是混合的金属硫族化物。
13.如权利要求11所述的发光器件,其中该金属硫族化物包括氧化锌、氧化钛、氧化铌、硫化锌、氧化铟锡、或其混合物。
14.如权利要求1所述的发光器件,其中该第一电荷传输层是空穴传输层。
15.如权利要求1所述的发光器件,其中该第一电荷传输层是电子传输层。
16.如权利要求1所述的发光器件,其中该多个半导体纳米晶体形成单层。
17.如权利要求1所述的发光器件,其中该多个半导体纳米晶体是半导体纳米晶体的基本上单分散群体。
18.如权利要求1所述的发光器件,其中该多个半导体纳米晶体以图案排列。
19.如权利要求1所述的发光器件,其中该器件是透明的。
20.制备发光器件的方法,包括:
将含有第一无机材料的第一电荷传输层沉积到电极上;和
在该电极上沉积多个半导体纳米晶体;
其中,该多个纳米晶体与该第一电荷传输层电接触。
21.如权利要求20所述的方法,其中沉积多个半导体纳米晶体包括将多个半导体纳米晶体沉积作为单层。
22.如权利要求20所述的方法,其中沉积多个半导体纳米晶体包括形成图案。
23.如权利要求20所述的方法,其中沉积第一无机材料包括溅射。
24.如权利要求23所述的方法,其中该第一无机材料是无机半导体。
25.如权利要求24所述的方法,其中该无机半导体材料包括金属硫族化物。
26.如权利要求25所述的方法,其中该金属硫族化物是混合的金属硫族化物。
27.如权利要求26所述的方法,其中该金属硫族化物包括氧化锌、氧化钛、氧化铌、硫化锌、氧化铟锡、或其混合物。
28.如权利要求20所述的方法,进一步包括:将含有第二无机材料的第二电荷传输层沉积到电极上;
其中,该多个纳米晶体与该第二电荷传输层电接触。
29.如权利要求28所述的方法,其中沉积第二无机材料包括溅射。
30.如权利要求29所述的方法,其中该第二无机材料是无机半导体。
31.如权利要求30所述的方法,其中该无机半导体材料包括金属硫族化物。
32.如权利要求31所述的方法,其中该金属硫族化物是混合的金属硫族化物。
33.如权利要求31所述的方法,其中该金属硫族化物包括氧化锌、氧化钛、氧化铌、硫化锌、氧化铟锡、或其混合物。
34.如权利要求20所述的方法,其中该器件是透明的。
35.发光方法,包括:
提供器件,该器件包括:第一电极、第二电极、与第一电极接触的包括第一无机材料的第一电荷传输层、和布置在该第一电极和第二电极之间的多个半导体纳米晶体;和
跨越该第一电极和第二电极施加发光电势。
36.如权利要求35所述的方法,其中该第一无机材料是无定形的或多晶的。
37.如权利要求36所述的方法,其中该第一无机材料是无机半导体。
38.如权利要求37所述的方法,其中该无机半导体包括金属硫族化物。
39.如权利要求38所述的方法,其中该金属硫族化物是混合的金属硫族化物。
40.如权利要求38所述的方法,其中该金属硫族化物包括氧化锌、氧化钛、氧化铌、硫化锌、氧化铟锡、或其混合物。
41.如权利要求35所述的方法,其中该器件进一步包括含有第二无机材料的第二电荷传输层。
42.如权利要求41所述的方法,其中该第二无机材料是无定形的或多晶的。
43.如权利要求42所述的方法,其中该第二无机材料是无机半导体。
44.如权利要求43所述的方法,其中该无机半导体包括金属硫族化物。
45.如权利要求44所述的方法,其中该金属硫族化物是混合的金属硫族化物。
46.如权利要求44所述的方法,其中该金属硫族化物包括氧化锌、氧化钛、氧化铌、硫化锌、氧化铟锡、或其混合物。
47.如权利要求35所述的方法,其中该多个半导体纳米晶体形成单层。
48.如权利要求35所述的方法,其中该多个半导体纳米晶体是半导体纳米晶体的基本上单分散群体。
49.如权利要求35所述的方法,其中该多个半导体纳米晶体以图案排列。
50.如权利要求35所述的方法,其中该器件是透明的。
51.含有多个发光器件的显示器,其中至少一个发光器件包括:
包括第一无机材料的第一电荷传输层,其与第一电极接触,该第一电极被布置以在该第一电荷传输层中引入电荷;
第二电极;和
布置在该第一电极和第二电极之间的多个半导体纳米晶体。
52.如权利要求51所述的显示器,进一步包括与该第二电极接触的第二电荷传输层,其中该第二电极被布置以在第二电荷传输层中引入电荷。
53.如权利要求51所述的显示器,其中该第一无机材料是无定形的或多晶的。
54.如权利要求51所述的显示器,其中该第一无机材料是无机半导体。
55.如权利要求54所述的显示器,其中该无机半导体包括金属硫族化物。
56.如权利要求55所述的显示器,其中该金属硫族化物是混合的金属硫族化物。
57.如权利要求55所述的显示器,其中该金属硫族化物包括氧化锌、氧化钛、氧化铌、硫化锌、氧化铟锡、或其混合物。
58.如权利要求51所述的显示器,其中该第二电荷传输层包括第二无机材料。
59.如权利要求58所述的显示器,其中该第二无机材料是无定形的或多晶的。
60.如权利要求58所述的显示器,其中该第二无机材料是无机半导体。
61.如权利要求60所述的显示器,其中该无机半导体包括金属硫族化物。
62.如权利要求61所述的显示器,其中该金属硫族化物是混合的金属硫族化物。
63.如权利要求61所述的显示器,其中该金属硫族化物包括氧化锌、氧化钛、氧化铌、硫化锌、氧化铟锡、或其混合物。
64.如权利要求51所述的显示器,其中该第一电荷传输层是空穴传输层。
65.如权利要求51所述的显示器,其中该第一电荷传输层是电子传输层。
66.如权利要求51所述的显示器,其中该多个半导体纳米晶体形成单层。
67.如权利要求51所述的显示器,其中该多个半导体纳米晶体是半导体纳米晶体的基本上单分散群体。
68.如权利要求51所述的显示器,其中该多个半导体纳米晶体以图案排列。
69.如权利要求51所述的显示器,其中该器件是透明的。
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2006
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CN103311442A (zh) * | 2012-03-06 | 2013-09-18 | 海洋王照明科技股份有限公司 | 电致发光器件及其制备方法 |
CN102610725A (zh) * | 2012-03-29 | 2012-07-25 | 华北电力大学 | 一种半导体量子点发光二极管及其制备方法 |
CN102610725B (zh) * | 2012-03-29 | 2015-01-07 | 华北电力大学 | 一种半导体量子点发光二极管及其制备方法 |
CN102820391A (zh) * | 2012-08-27 | 2012-12-12 | 中国科学院半导体研究所 | 硅基上的近红外量子点电致发光的器件及制备方法 |
CN102820391B (zh) * | 2012-08-27 | 2014-12-03 | 中国科学院半导体研究所 | 硅基上的近红外量子点电致发光的器件及制备方法 |
CN104120388A (zh) * | 2013-04-26 | 2014-10-29 | 三星显示有限公司 | 纳米晶形成方法和制造有机发光显示装置的方法 |
CN104120388B (zh) * | 2013-04-26 | 2018-06-12 | 三星显示有限公司 | 纳米晶形成方法和制造有机发光显示装置的方法 |
CN105206757A (zh) * | 2015-11-05 | 2015-12-30 | 京东方科技集团股份有限公司 | 有机发光二极管及其制作方法、显示基板和显示装置 |
CN106450013A (zh) * | 2016-10-11 | 2017-02-22 | Tcl集团股份有限公司 | Qled器件 |
CN110970534A (zh) * | 2018-09-29 | 2020-04-07 | Tcl集团股份有限公司 | 一种氧化镍薄膜及其制备方法、量子点发光二极管 |
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KR101257780B1 (ko) | 2013-04-24 |
EP2546192A3 (en) | 2014-08-27 |
US20070103068A1 (en) | 2007-05-10 |
US10014438B2 (en) | 2018-07-03 |
JP5528672B2 (ja) | 2014-06-25 |
CN107507895A (zh) | 2017-12-22 |
US20120292595A1 (en) | 2012-11-22 |
US8232722B2 (en) | 2012-07-31 |
KR20070107708A (ko) | 2007-11-07 |
EP1864341A1 (en) | 2007-12-12 |
JP5806895B2 (ja) | 2015-11-10 |
MY168191A (en) | 2018-10-15 |
WO2006088877A1 (en) | 2006-08-24 |
PL2546192T3 (pl) | 2020-05-18 |
JP2012023388A (ja) | 2012-02-02 |
TWI440206B (zh) | 2014-06-01 |
US20170125635A1 (en) | 2017-05-04 |
TW200727514A (en) | 2007-07-16 |
EP2546192A2 (en) | 2013-01-16 |
US20120238047A1 (en) | 2012-09-20 |
US9550614B2 (en) | 2017-01-24 |
EP2546192B1 (en) | 2019-12-18 |
EP1864341B1 (en) | 2019-11-13 |
KR20130007649A (ko) | 2013-01-18 |
CN107507895B (zh) | 2020-12-01 |
JP2008530802A (ja) | 2008-08-07 |
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