TW200917536A - Composite substrate for forming light emitting element and method for manufacturing the composite substrate - Google Patents

Composite substrate for forming light emitting element and method for manufacturing the composite substrate Download PDF

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TW200917536A
TW200917536A TW097133884A TW97133884A TW200917536A TW 200917536 A TW200917536 A TW 200917536A TW 097133884 A TW097133884 A TW 097133884A TW 97133884 A TW97133884 A TW 97133884A TW 200917536 A TW200917536 A TW 200917536A
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light
layer
substrate
phase
oxide
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Fumito Furuuchi
Hideki Hirayama
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Ube Industries
Riken
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Abstract

A uniform nitride buffer layer is formed over the entire surface of a substrate including both an Al2O3 phase and an oxide phase which has a garnet type structure and emits fluorescence, for forming a nitride semiconductor layer. A composite substrate for forming the light emitting element is composed of a light conversion material substrate and a nitride layer formed on the light conversion material substrate. The light conversion material substrate has a structure wherein at least two or more oxide layers are continuously and three-dimensionally entwined with each other. Each oxide layer includes the Al2O3 phase and at least one oxide phase which emits fluorescence. The nitride layer has a nitride layer including at least Al on an interface to the light conversion substrate, preferably, at least one layer of AlxGa1-xN (0<x=1).

Description

200917536 九、發明說明: 【發明所屬之技術領域3 本申請案係根據西元2007年9月4日向日本國專利廳申 請之發明申請案第2007-229263號基礎案主張優先權,並於 5 此援用其申請案之内容。 本發明係有關於可利用於顯示器、照明、背光光源等 之發光元件形成用複合基板及其製造方法,特別是有關於 一種使用發出螢光之光變換材料之發光二極體元件用之形 成用複合基板及其製造方法。 10 【先前技術】 近年來,使用氮化物系化合物半導體(InxAlyGa^-y N、〇Sx$l、〇$y$l、〇Sx + y$ 1)之藍色發光元件為發 光源之白色發光二極體之開發研究蓬勃發展中。白色發光 二極體之重量輕,且不使用水銀,壽命長,因此預測今後 15的需求將會急速擴大。以使藍色發光元件之藍色光轉換成200917536 IX. Description of the invention: [Technical field 3 of the invention] This application claims priority based on the basic application of the invention application No. 2007-229263 filed on September 4, 2007, to the Japanese Patent Office, and is hereby incorporated by reference. The content of its application. The present invention relates to a composite substrate for forming a light-emitting element that can be used for a display, an illumination, a backlight source, and the like, and a method of manufacturing the same, and more particularly to a method for forming a light-emitting diode element using a light-emitting material that emits fluorescence. Composite substrate and method of manufacturing the same. [Prior Art] In recent years, a blue light-emitting element using a nitride-based compound semiconductor (InxAlyGa^-y N, 〇Sx$l, 〇$y$l, 〇Sx + y$ 1) is a white light-emitting source. The development of diodes is booming. The white light-emitting diode is light in weight and does not use mercury, and has a long life. Therefore, it is predicted that the demand for the next 15 will rapidly expand. To convert the blue light of the blue light-emitting element into

白色光之方法而言,其中最平常進行的方法,如日本國發 明申請案公開公報第2000-208815號所揭示,在發出藍色光 之發光元件的前面設有含有吸收部分藍色光而發出黃色光 之螢光體之塗層及將光源的藍色光和來自塗層之黃色光混 20色之成形層,使處於補色關係之藍色及黃色混色,得到虛 擬的白色。迄今,以塗層而言’採用以鈽活化之 d AI5 〇ι2 : Ce)粉末及環氧樹脂之混合物。但是本方法中, 塗佈塗層時’被指摘容易產生所含之螢光體粉末之分布不 均、每個發光二極體個體之螢光體粉末量之偏差等,以及 5 200917536 因其引起之發光二極體之顏色不均等問題。 為避免上述問題,本發明人乃在PCT/JP2005/019739 (W02006/043719)中提出一種方法,在由陶瓷複合氧化物構 成之光變換材料基板上形成由Ii^AlyGa^yN (OSxgl、 5 1、丨)構成之氮化物半導體層,使發光層 所發光之藍色光直接射入基板,由基板本身發出均質的黃 色螢光,使得可在不用含有螢光體粉末之塗層之狀態下, 只用發光晶片’即可得到無顏色不均且均質的白色。 惟,在使用GaN作為專利文獻2之實施例所示之緩衝層 10之方法中,有易於Al2〇3相上優先地形成氮化物半導體層之 問題衍生。為此,優先地形成於Al2〇3相之氮化物半導體係 於Ah 〇3相之外的領域互為孤立’因此難以實施良好的元件 形成。為了迴避如此問題,而欲以氮化物半導體層覆蓋基 板表面全面時,必須先厚膜化。惟,一進行厚膜化,除了 15使臈厚增加,另外因為基板與氮化物半導體層之晶格常數 與熱膨脹係數間的不同,最終發生變形,對於元件特性帶 來不良影響之傾向漸增。因此為了得到良好特性之元件, 由形成氮化物半導體層之初期開始,即在基板全面上形成 均勻的層之事就顯得重要。為了實現如此要點,乃需要由 20 α!2〇3相及具有石榴石型構造且發出螢光之氧化物相兩相 互相形成同樣的氮化物半導體層之步驟,經由同—步驟來 製作發光元件時,即可期待所得到之元件之特性的提昇。 本發明人發現:在於光變換材料基板上形成氮化物半 導體層之時,以與氮化物半導體層成長溫度同樣之溫度, 200917536 或,在該成長溫度以上之高溫下,形成至少含有八丨之氮化 物層,作為緩衝層使用時,亦可由基板中之發出螢光之氧 化物相,與Al2〇3相同樣,進行氮化物半導體層之晶體成長 者;終完成本發明。 5 【發明内容】 即’本發明係有關於一種發光元件形成用複合基板, 其特徵在於:在光變換材料基板上形成有至少含A1之氮化 物緩衝層,該緩衝層覆蓋光變換材料基板全面者。 進而,在本發明中較佳之型態係一種發光元件形成用 10複合基板,其特徵在於:螢光體相係至少含有γ元素、A1 元素、Ce元素之石榴石型構造。 進而,在本發明中較佳之型態係有關於一種發光元件 形成用複合基板,其特徵在於:前述緩衝層係形成於以 Al2〇3相之C面及螢光體相之(112)面同時作為主面之光變 15 換材料基板上者。 又’有關於一種發光元件形成用複合基板之製造方 法,其特徵在於光變換材料基板上形成至少含A1之氮化物 缓衝層,且藉該緩衝層覆蓋光變換材料基板全面者。 進而,一較佳之型態係有關於一種發明元件形成用複 20合基板之製造方法,其特徵在於:前述氮化物半導體層之 形成係以有機金屬氣相反應法進行者。 進而’一較佳之型態係有關於一種發明元件形成用複 合基板之製造方法,其特徵在於:前述含A1之氮化物緩衝 層係以900°C以上且小於140CTC之溫度形成者。 7 200917536 在如此製作之發光元件形成用複合基板中’可由具有 ai2〇3相及具有石權石型構造且發出蟹光之氧化物相之兩 相^相同樣形成氮化物半導體層,經由同―步驟,即可數 作高特性之白色發光元件。 5 對於形成如此發光層之氣化物半導體層,以In the method of white light, the most common method is disclosed in Japanese Laid-Open Patent Publication No. 2000-208815, which is provided with a blue light containing an absorbing portion and a yellow light in front of a light-emitting element that emits blue light. The coating of the phosphor and the blue layer of the light source and the yellow light from the coating are mixed into a 20-color forming layer, and the blue and yellow colors in the complementary color relationship are mixed to obtain a virtual white color. Heretofore, in the case of coating, a mixture of powder and epoxy resin activated by hydrazine d AI5 〇ι 2 : Ce was used. However, in the method, when the coating is applied, the uneven distribution of the phosphor powder contained in the coating is easily caused, and the amount of the phosphor powder of each of the individual light-emitting diodes is varied, and 5 200917536 The color of the LED is not uniform. In order to avoid the above problem, the present inventors have proposed a method in the PCT/JP2005/019739 (W02006/043719) to form Ii^AlyGa^yN (OSxgl, 5 1) on a substrate of a light conversion material composed of a ceramic composite oxide. And 丨) the nitride semiconductor layer is formed such that the blue light emitted by the luminescent layer directly enters the substrate, and the substrate itself emits a homogeneous yellow fluorescing, so that the coating layer containing the phosphor powder can be used only With the luminescent wafer', a colorless and uniform white color can be obtained. However, in the method of using GaN as the buffer layer 10 shown in the embodiment of Patent Document 2, there is a problem that it is easy to preferentially form a nitride semiconductor layer on the Al2〇3 phase. For this reason, the nitride semiconductors preferentially formed in the Al2〇3 phase are isolated from each other in the field other than the Ah 〇 3 phase. Therefore, it is difficult to perform good element formation. In order to avoid such a problem, when it is desired to cover the surface of the substrate with a nitride semiconductor layer, it is necessary to thicken the film first. However, as a result of the thick film formation, in addition to the increase in the thickness of the ruthenium, the difference between the lattice constant of the substrate and the nitride semiconductor layer and the thermal expansion coefficient eventually causes deformation, and the tendency to adversely affect the device characteristics is increasing. Therefore, in order to obtain an element having good characteristics, it is important to form a uniform layer from the beginning of the formation of the nitride semiconductor layer, that is, to form a uniform layer over the entire substrate. In order to achieve such a point, it is necessary to form a light-emitting element by the same step by a step of forming a nitride semiconductor layer of 20 α! 2 〇 3 phase and a garnet-type oxide structure having two phases. At that time, the characteristics of the obtained components can be expected to be improved. The present inventors have found that when a nitride semiconductor layer is formed on a substrate of a light conversion material, at least the temperature of the growth temperature of the nitride semiconductor layer, 200917536 or at a high temperature above the growth temperature, a nitrogen containing at least eight bismuth is formed. When the compound layer is used as a buffer layer, the crystal growth of the nitride semiconductor layer may be carried out in the same manner as the Al 2 〇 3 phase from the oxide phase in the substrate. The present invention has been completed. [Invention] The present invention relates to a composite substrate for forming a light-emitting element, characterized in that a nitride buffer layer containing at least A1 is formed on a substrate of a light conversion material, and the buffer layer covers the entire surface of the light conversion material substrate. By. Further, a preferred embodiment of the present invention is a composite substrate for forming a light-emitting element, characterized in that the phosphor phase contains at least a garnet structure of a γ element, an A1 element, and a Ce element. Further, a preferred embodiment of the present invention relates to a composite substrate for forming a light-emitting element, characterized in that the buffer layer is formed on the C-plane of the Al2〇3 phase and the (112) plane of the phosphor phase. As the main surface of the light change 15 on the material substrate. Further, a method for producing a composite substrate for forming a light-emitting element, characterized in that a nitride buffer layer containing at least A1 is formed on a substrate of the light conversion material, and the entire surface of the light conversion material substrate is covered by the buffer layer. Further, a preferred embodiment relates to a method for producing a composite substrate for forming an inventive device, characterized in that the formation of the nitride semiconductor layer is carried out by an organometallic gas phase reaction method. Further, a preferred embodiment relates to a method for producing a composite substrate for forming an inventive device, characterized in that the nitride buffer layer containing A1 is formed at a temperature of 900 ° C or more and less than 140 CTC. 7 200917536 In the composite substrate for forming a light-emitting element thus produced, a nitride semiconductor layer can be formed by a two-phase phase having an ai2〇3 phase and a stone-bearing structure and emitting an ice oxide phase. In the step, the white light-emitting element with high characteristics can be counted. 5 for the vaporized semiconductor layer forming such a light-emitting layer,

InxAlyGa丨_x_yN (〇$xgi 氮化物半導體層為佳。 [圖式簡單說明] 1、〇gx + yS ”所構成之 第1A及1B圖係模式地顯示本發明之發光元件形成用 10複合基板之一實施型態之剖視圖。 第圖係‘,、、頁示光變換材料之組織構造例之電子顯微 照片。 第3圖係實_ 1所得狀GaN狀輪制面照片。 第4圖係比較例1所得到之GaN層之顯微鏡剖面照片。 15 【貧方式】 本發明之發光元件形成用複合基板之-種型態,例如 在如第1A圖所示般之光變換材料基板】之表面上不管複雜 纏繞-起之Al2〇3相13及發出螢光之氧化物相狀晶體間 之不同,全面性地形成緩衝層2。該緩衝層2含有一至少含 2〇 A1之氮化物層2a。又,為了提昇如第⑺圖所示之複合基板 表面之均質性,亦可在含A1之氮化物層上形成GaN層2b。 本發明之構成發光元件形成用複合基板之光變換材料 基板係由下述凝固體所構成,該凝固體係使由單一金屬氧 化物及複合金屬氧化物中所選擇之至少2個以上之氧化物 200917536 相連續且相互纏繞成三維空間形成者,該凝固體中之氧化 物相中至少有一個是Ah a晶相,又,前述凝固體中之氧化 物相中至少一個是含有可發出螢光之金屬元素氧化物。單 金屬氧化物係指1種金屬的氧化物,複合金屬氧化物是指 5 2種以上的金屬之氧化物。各種氧化物都形成為單晶狀態, 成為相互纏繞成三維空間之構造。如此單一金屬氧化物係 可舉下述氧化物,諸如氧化鋁(Abo3)、氧化鍅(Zr〇2)、氧 化鎂(MgO)、氧化矽(Si〇2)、氧化鈦(Ti〇2)、氧化鋇(Β&amp;〇)、 氧化鈹(Be0)、氧化鈣(CaO)、氧化鉻(Cr2〇3)等之外,另舉 1〇 有稀土類元素氧化物(La203、Y2〇3、Ce〇2、Pr6〇n、 Nd2 〇3、Sm2 〇3、Gd2 〇3、邮 〇3、Tb4 〇、以2 〇3 h〇2 〇3 Er2〇3、Tm203、Yb2〇3、Lu203)為例。又,複合金屬氧化 物可舉有LaA103、CeA103、PrA103、NdA103、SmA103、 EuA1〇3、GdAl〇3、DyA103、ErA103、Yb4 Al2 〇9、γ3 Al5 〇丨2、 b Er3Al5〇12、Tb3Al5〇i2、11Al2〇3 山办、iiai办·InxAlyGa丨_x_yN (the x$xgi nitride semiconductor layer is preferable. [FIG. 1A and 1B] FIG. 1A and 1B are schematic diagrams showing the 10 composite substrate for forming a light-emitting element of the present invention. A cross-sectional view of one embodiment. The figure is an electron micrograph of a structure of a light-converting material. The third figure is a photograph of a GaN-like wheel surface obtained by _1. Photograph of a microscopic cross section of the GaN layer obtained in Comparative Example 1. [Purity mode] The surface of the composite substrate for forming a light-emitting element of the present invention, for example, on the surface of a light conversion material substrate as shown in Fig. 1A The buffer layer 2 is formed in a comprehensive manner regardless of the difference between the complex winding-like Al 2 〇 3 phase 13 and the fluorescing oxide phase crystal. The buffer layer 2 contains a nitride layer 2a containing at least 2 Å A1. Further, in order to improve the homogeneity of the surface of the composite substrate as shown in the above (7), the GaN layer 2b may be formed on the nitride layer containing A1. The optical conversion material substrate constituting the composite substrate for forming a light-emitting element of the present invention Composed of the following solidified body, the solidified body Forming at least one of the oxide phases of at least one of the oxides of the single metal oxide and the composite metal oxide continuously and intertwined into a three-dimensional space, wherein at least one of the oxide phases in the solidified body is Ah a crystal In addition, at least one of the oxide phases in the solidified body contains a metal element oxide which emits fluorescence, and the single metal oxide refers to an oxide of one metal, and the composite metal oxide refers to more than 52 kinds. The oxide of the metal. The various oxides are formed into a single crystal state and become a structure in which they are entangled into a three-dimensional space. Such a single metal oxide may be an oxide such as alumina (Abo3) or yttrium oxide (Zr〇). 2), magnesium oxide (MgO), cerium oxide (Si〇2), titanium oxide (Ti〇2), cerium oxide (Β &amp; 〇), cerium oxide (Be0), calcium oxide (CaO), chromium oxide (Cr2 〇 3), etc., another rare earth element oxide (La203, Y2〇3, Ce〇2, Pr6〇n, Nd2 〇3, Sm2 〇3, Gd2 〇3, 〇3, Tb4 〇, Take 2 〇3 h〇2 〇3 Er2〇3, Tm203, Yb2〇3, Lu203) as an example. The compound may be LaA103, CeA103, PrA103, NdA103, SmA103, EuA1〇3, GdAl〇3, DyA103, ErA103, Yb4 Al2 〇9, γ3 Al5 〇丨2, b Er3Al5〇12, Tb3Al5〇i2, 11Al2〇3 Office, iiai office

Nd2〇3、3Dy2〇3.5Al2〇3、2Dy203 .Al203、UAl203 · Pr2〇3、EuA1&quot;〇18、2Gd203 ·Α1203、11Α12〇3 .Sm203、Nd2〇3, 3Dy2〇3.5Al2〇3, 2Dy203.Al203, UAl203 · Pr2〇3, EuA1&quot;〇18, 2Gd203 ·Α1203,11Α12〇3 .Sm203,

Yb3Al5〇12、CeAlu〇18、Er4Al2〇9 等為例。 光變換材料基板由2種以上之氧化物相構成,因此藉其 2〇組合,可選擇各種晶格間隙。為此,可配合發光二極體的 各種半導體之晶格間隙,晶體構造上之匹配性良好,可進 行缺陷少之良好半導體層的成膜,由半導體層内所形成之 發光層,可得到效率佳之發光。進而,光變換材料基板也 疋瑩光體’因此藉由半導體層中之發光層之光,亦可發出 200917536 均勻的螢光。 5 10 15 發光二極體用半導體層為氮化物半導體層時,在構成 光變換材料基板之前述凝固體之中,可舉含有單—金屬氧 化物之Ah〇3晶體之組合為佳之凝固體為例。如上述,這是 因為Al2〇3晶體係與構成發出可見光之氮化物半導體層: 代表性化合物之InGaN,在晶體構造上匹配性佳,可形成氮 ㈣半導體之良好發光層所致者。又,可舉从〇3晶體與= ;以鈽活化之複合金屬氧化物之石榴石型晶體單晶之組合 更佳之凝固體為例。石榴石型晶體係以Α3χ5〇&quot;之構造式 表不,且在構造式中,Α含有選自由γ、Tb、Sm、Gd、」、 &amp;之群中之1種以上之㈣,同樣在構造式中,X含有選自 =Al、Ga中之!種以上之元素時特佳。這是因為由這特佳组 &amp;所構成之光變換材料由紫色光-邊使藍色光穿透,一邊 =收其中—部分,而發出黃色螢光的緣故。其中又和以飾 活化之Y3Al5〇12之組合可發光強螢光,因此為佳。 第1A及1B圖所示之—實施型態之Al2(VY3Al5〇12:Ce 換材料基板係由ΑΙΑ單晶和YAW : ^單晶構 ^氧化物相連續且相互纏繞成三輕間地形成,整體 ^是由曰2^晶的相所構成。各相為單晶之型態是極為重Yb3Al5〇12, CeAlu〇18, Er4Al2〇9, etc. are taken as examples. Since the light conversion material substrate is composed of two or more oxide phases, various lattice gaps can be selected by the combination of the two. For this reason, it is possible to match the lattice gap of various semiconductors of the light-emitting diode, and the crystal structure has good matching property, and it is possible to form a good semiconductor layer with few defects, and the light-emitting layer formed in the semiconductor layer can obtain efficiency. Good light. Further, the light conversion material substrate is also a phosphorescent material. Therefore, it is possible to emit uniform fluorescent light of 200917536 by the light of the light-emitting layer in the semiconductor layer. 5 10 15 When the semiconductor layer for a light-emitting diode is a nitride semiconductor layer, among the solidified bodies constituting the substrate of the light conversion material, a combination of Ah- 3 crystals containing a single-metal oxide is preferable. example. As described above, this is because the Al2〇3 crystal system and the nitride semiconductor which constitutes the nitride semiconductor layer emitting visible light: a representative compound have good crystal structure matching, and can form a good light-emitting layer of a nitrogen (tetra) semiconductor. Further, a solidified body of a combination of a ruthenium 3 crystal and a ruthenium-type crystal single crystal of a composite metal oxide activated by ruthenium is exemplified. The garnet-type crystal system is represented by the structural formula of Α3χ5〇&quot;, and in the structural formula, Α contains one or more (four) selected from the group consisting of γ, Tb, Sm, Gd, ", &amp; In the formula, X contains one selected from =Al, Ga! It is especially good when the above elements are used. This is because the light-converting material composed of the special group &amp; is caused by the purple light-side to allow the blue light to pass through, and the one side to receive the - part, and the yellow fluorescent light is emitted. Among them, the combination of Y3Al5〇12 activated by the decoration can emit strong fluorescence, so it is preferable. The Al2 (VY3Al5〇12:Ce material exchange substrate) shown in Figs. 1A and 1B is formed by a single crystal and a YAW: ^ single crystal structure oxide phase continuous and intertwined into three light spaces. The whole ^ is composed of a phase of 曰 2 ^ crystal. The phase of each phase is extremely heavy.

光變播疋單日日彳就不4成品質良好的氮化物半導體層。 =換材料基板可藉下述方法形成,例如將上述AW 要^〇r:ce之凝㈣切斷成狀厚度,將表面研磨到必 得到者。光變換材料基板之切出方位尤 1203之卿υ面作為主面時為佳。躺隸有與氮化 20 200917536 物系化合物半導體之Inx Aly Gai_x_yN類似之晶體構造, Al2〇3(〇〇〇l)面與InxAlyGai-x-yN間之晶格間隔之差小,匹配 性佳。為此,利用Al2〇3之(0001)面,可得到品質良好之氮 化物半導體層,形成良好的發光層。 5 構成用於本發明之光變換材料之凝固體係藉熔解原料 金屬氧化物之後凝固製作者。例如,藉將已放入維持在預 定溫度之堝鍋中之熔融物’一邊控制冷卻溫度一邊冷卻凝 結之簡單方法,可得到凝固體,但最佳的是藉單向凝固法 製造者。這是因為經由單向凝固之進行,使所含之晶相以 10單晶狀態連續成長,使得各相形成單一晶體方位的緣故。 本發明所使用之光變換材料除了含有至少有1相發出 螢光之金屬元素氧化物之外,亦可為與本申請案申請人先 前揭露於曰本發明申請案公開公報第H07-149597號、第 H07-187893 號、第 H08-81257 號、第 H08-253389 號、第 15 H08-253390號及第H09-67194號及與其等對應之美國申請 案(美國專利第5,569,547號、第5,484,752號、第5,902,963號) 等公報中之陶瓷複合材料同樣之化合物,可以其等申請案 (專利)所揭示之製造方法製造者。於此援用其等申請案或專 利之揭露内容。 2〇 形成於發光元件形成用複合基板上之氮化物半導體層 係由多數氮化物系化合物半導體之層所構成。多數氮化物 系化合物半導體之層各藉以通式Inx Aly Ga,_x_yN(0芸x各i、 OSyS卜OSx + y各1)所示之氮化物系化合物構成者為佳。 又’氮化物半導體層至少具有發出可見光之發光層。為了 200917536 形成良好的發光層’在各層’堆疊已調整成最適於各機能 之組成之多數氮化物系化合物半導體之層者為佳。多數之 氮化物系化合物半導體之層及其等層之形成方法,如】 Appl. Phys. Vol.34(1995), L797等文獻所揭露的,為公知之 5 技術。具體方法可有下述方法,在基板上,藉M〇CVD等方 法依序堆疊GaN之緩衝層(厚度30nm)、形成η電極之n型一In the case of a light-changing broadcast, it is not a good quality nitride semiconductor layer. = The material substrate can be formed by, for example, cutting the above-mentioned AW to be condensed into a thickness, and grinding the surface to the extent necessary. It is preferable that the cut surface of the light conversion material substrate is particularly the main surface of the 1203. The crystal structure similar to Inx Aly Gai_x_yN of the compound semiconductor of nitridation 20 200917536 is lying, and the difference in lattice spacing between the Al 2 〇 3 (〇〇〇l) plane and the InxAlyGai-x-yN is small, and the matching is good. For this reason, a nitride semiconductor layer of good quality can be obtained by using the (0001) plane of Al2〇3 to form a favorable light-emitting layer. 5 A solidification system constituting the optical conversion material used in the present invention is produced by solidifying a metal oxide. For example, a solidified body can be obtained by a simple method of cooling and coagulating a molten material which has been placed in a crucible maintained at a predetermined temperature while controlling the cooling temperature, but it is preferable to manufacture by a one-way solidification method. This is because the crystal phase contained is continuously grown in a single crystal state by unidirectional solidification so that each phase forms a single crystal orientation. The optical conversion material used in the present invention, in addition to the metal element oxide which emits at least one phase of the fluorescing, may be disclosed in the applicant's publication No. H07-149597, as disclosed in the present application. U.S. Patent Nos. H07-187893, H08-81257, H08-253389, 15H08-253390, and H09-67194, and the corresponding US application (U.S. Patent Nos. 5,569,547, 5,484,752, No. 5,902,963) The same compound as the ceramic composite material in the publication can be manufactured by the manufacturing method disclosed in the application (patent). The disclosure of such applications or patents is hereby incorporated. 2) The nitride semiconductor layer formed on the composite substrate for forming a light-emitting element is composed of a layer of a plurality of nitride-based compound semiconductors. It is preferable that each of the layers of the nitride-based compound semiconductor is composed of a nitride-based compound represented by the general formula Inx Aly Ga, _x_yN (0 芸 x each, OSyS, OSx + y each). Further, the nitride semiconductor layer has at least a light-emitting layer that emits visible light. In order to form a good luminescent layer for 200917536, it is preferable to stack a layer of a plurality of nitride-based compound semiconductors which are adjusted to be optimal for each functional layer in each layer. A layer of a nitride-based compound semiconductor layer and a method for forming the same layer, as disclosed in Appl. Phys. Vol. 34 (1995), L797, and the like, are well-known 5 techniques. The specific method may be as follows. On the substrate, a buffer layer of GaN (thickness: 30 nm) is sequentially stacked by a method such as M〇CVD, and an n-type of an n-electrode is formed.

GaN : Si接觸層(厚度5/zm)、η型—AlcuGa^N : Si層、η型 —Ino.QsGao.MN : Si層、形成單量子井構造型發光層之〗nGaN 層、p型一AlojGao.gN : Mg障壁層、形成p電極之p型—GaN : 10 Mg層而得到。發光層之構造另為多重量子井構造、均質 (homo)構造、雜質(hetero)構造或雙雜構造,亦可。惟,在 本發明中,上述基板是使用本發明之發光元件形成用複合 基板,形成在發光元件形成用複合基板上之氮化物半導體 層,由於發光元件形成用複合基板在表面具有含A1之氮化 I5 物層’因此可省略GaN之緩衝層(厚度30nm)。 形成在本發明之發光元件形成用複合基板之氮化物半 導體層中之發光層係以發出可見光者為佳。可見光穿透構 成本發明之發光元件形成用複合基板之光變換材料基板 時’使業經波長轉換之螢光和變換前之可見光混合,因應 20 已混合之光線的波長,可得到新的虛擬之光線。進而,可 見光係以發出藍色或紫色為佳。發光色為藍色或紫色時, 來自發光層之藍光或紫光射入基板之YAG : Ce單晶時,由 Y3 AI5 : Ce晶體發出黃色榮光,在AI2 〇3晶體時,則藍 色或紫色之光線就這樣透射過去。其等光線藉光變換材料 12 200917536 單晶基板内之連續且相互纏繞成三維空間的組織混合後放 射,因此可得到沒有顏色不均且均質之白色。為此,氮化 物半導體層中之發光層係由InxGai χΝ(〇$χ$ ”構成者為 佳。改變形成前述發光層之所含之匕的莫耳比,可 5 使發光波長變化。 δ史置本發明之緩衝層時’較佳的是在其上形成前述氮 化物半導體層。使用本發明之形成有氮化物緩衝層之發光 兀件形成用複合基板,便可在無須新設置緩衝層之狀態下 直接形成前述氮化物半導體層。又,一般來說,氮化物半 10導體層之形成係以氣相成長反應進行,因此希望基板的表 面是均勻的。為此,與氮化物半導體層之形成同樣,針對 剛述緩衝層之形成,亦是藉可得到高品質之緩衝層之氣相 反應法進行者為佳。尤其從品質及成長速度之觀點來看, 以藉有機金屬化學氣相成長法(下述中稱為M0CVD)形成 15者為佳。MOCVD係-種將原料之有機金屬氣體擠流在藉 Hz或N2加熱之基板上,在基板表面上引起晶體成長之方 法。有關剛述緩衝層之原料氣體,八丨源可使用TMA(三甲鋁) 或TEA(二乙鋁)等,Ga#可使用tmG(三甲鎵)或TEG(三乙 錄)等’ N源可使用氨或聯麟,可使用—般圖(:¥〇中之氮 20化物半導體層之形成時所使用之材料。 本發明之氮化物緩衝層係全面地覆蓋於基板表面者為 特徵所在。藉此,在氮化物半導體層之形成時,可在光變 換材料基板之八丨2〇3相與螢光體相之間沒有境界之狀態 下’穩定地形成疊層構造。又,由A1203相優先地進行成長, 13 200917536 亦可得到均勻的面,但是如果沒有本發明之氮化物緩衝層 存在,只使用光變換材料基板(含有ALA相及螢光體相之 複合氧化物)形成氮化物半導體層之均勻面時,乃必須厚膜 化,即使得到均勻面,因其形變,導致產生裂痕或使基板 5扭曲,對元件帶來不良的影響。但是使用本發明之形成有 緩衝層之複合基板時,無須厚膜化,可做到充分之薄膜化, 幾乎不會對元件特性有影響。 本發明之緩衝層含有至少含八比氮化物層者為特徵所 在。具體上以含有AlxGai-xN(0&lt;XSl)表示之氮化物層為 10佳。更佳的是含有A1N。又以成為與氮化物半導體同程度以 上之形成度般之900 至1400°C之溫度條件形成者為 佳。更佳的是以115〇t至140(TC之溫度條件形成為佳。9〇〇 °C至1200°C時,使成長在Alz a相與螢光體相之氮化物層均 勻是有困難,不過在螢光體相時亦可形成氮化物層。進而, 15藉以更高溫形成氮化物層時,更容易得到均勻的面。又, 該緩衝層,其晶體性對形成在該緩衝層上之氮化物半導體 層之元件特性有很大影響,以晶體性更佳者為合適。含A1 之氮化物層,以提昇AlxGai-xN(0&lt;xS1)之晶體性之方法而 s,無關於溫度條件,有益於氮化物半導體層之元件特性 20的提昇。例WM0CVD,更高溫時,在所得到之AlxGai_xN(0 &lt;x$l)組成上Ga必然減少。由形成為緩衝層之氮化物層之 品質來看,以Ga組成低者較佳。 又’在前述含A1之氮化物層之上,以橫向晶體成長速 度變快之條件形成GaN時更適合。含A1之氮化物層之形成 200917536 係與光變換材料基板之A丨2 〇3相與螢光體相同樣進行晶核 形成,但是Al —Ν與Ga —Ν相比,鍵結能較高,表面的遷移 率杈小,因此只有含A1之氮化物層時,Α1ζ〇3相與螢光體相 中之氮化物層之稍微差異便在晶體性與表面型態上產生差 5異而顯現。使GaN成長,容易在成長於Aha相與螢光體相 之氮化物晶體上造成移動(migrati〇n),可消除各晶相的差異 者。以使橫向晶體成長速度加快之條件形成GaN時,藉&amp;、GaN: Si contact layer (thickness 5/zm), n-type-AlcuGa^N: Si layer, n-type-Ino.QsGao.MN: Si layer, nGaN layer forming a single quantum well structured light-emitting layer, p-type one AlojGao.gN : Mg barrier layer, p-type p-type GaN: 10 Mg layer. The structure of the light-emitting layer may be a multiple quantum well structure, a homo structure, a hetero structure or a double structure. In the present invention, the substrate is a nitride semiconductor layer formed on the composite substrate for forming a light-emitting element using the composite substrate for forming a light-emitting element of the present invention, and the composite substrate for forming a light-emitting element has a nitrogen containing A1 on the surface. The I5 layer "can therefore omit the buffer layer of GaN (thickness 30 nm). The light-emitting layer formed in the nitride semiconductor layer of the composite substrate for forming a light-emitting element of the present invention is preferably one which emits visible light. When the visible light penetrates the light conversion material substrate constituting the composite substrate for forming a light-emitting element of the present invention, 'the wavelength-converted fluorescent light and the visible light before the conversion are mixed, and a new virtual light can be obtained in response to the wavelength of the 20 mixed light rays. . Further, it is preferred that the light system emits blue or purple. When the illuminating color is blue or purple, when the blue or violet light from the luminescent layer is incident on the YAG: Ce single crystal of the substrate, the yellow glory is emitted by the Y3 AI5 : Ce crystal, and the blue or purple AI2 〇 3 crystal is used. The light is transmitted through it. The light-transmissive light-transforming material 12 200917536 The continuous and intertwined structures in the three-dimensional space in the single crystal substrate are mixed and then emitted, so that white color having no color unevenness and homogeneity can be obtained. For this reason, it is preferable that the light-emitting layer in the nitride semiconductor layer is composed of InxGai® (〇$χ$). The molar ratio of the germanium contained in the light-emitting layer is changed to change the light-emitting wavelength. When the buffer layer of the present invention is disposed, it is preferable to form the nitride semiconductor layer thereon. By using the composite substrate for forming a light-emitting element having the nitride buffer layer of the present invention, it is possible to eliminate the need for a new buffer layer. The nitride semiconductor layer is formed directly in the state. Further, in general, the formation of the nitride half-conductor layer is performed by a vapor phase growth reaction, and therefore it is desirable that the surface of the substrate is uniform. For this, with the nitride semiconductor layer The formation of the buffer layer is also preferably carried out by a gas phase reaction method in which a high-quality buffer layer can be obtained, especially from the viewpoint of quality and growth rate, by chemical vapor growth of an organic metal. The method (hereinafter referred to as M0CVD) is preferably formed by 15. The MOCVD system extrudes the organic metal gas of the raw material on a substrate heated by Hz or N2 to cause crystal growth on the surface of the substrate. For the raw material gas of the buffer layer, the Bagua source can use TMA (trimethylaluminum) or TEA (diethylaluminum), etc., Ga# can use tmG (trimethylgallium) or TEG (three-e-record), etc. When ammonia or lining is used, a material used in the formation of a nitrogen semiconductor film layer in the general image can be used. The nitride buffer layer of the present invention is characterized by covering the surface of the substrate in its entirety. Therefore, when the nitride semiconductor layer is formed, the laminated structure can be stably formed in a state where the boundary between the octagonal phase and the phosphor phase of the optical conversion substrate is not present. Further, the A1203 is preferred. Growth is carried out, 13 200917536 can also obtain a uniform surface, but if there is no nitride buffer layer of the present invention, only a light conversion material substrate (composite oxide containing ALA phase and phosphor phase) is used to form a nitride semiconductor layer. In the case of a uniform surface, it is necessary to form a thick film, and even if a uniform surface is obtained, cracks may occur or the substrate 5 may be twisted due to deformation thereof, which may adversely affect the element. However, when the composite substrate having the buffer layer of the present invention is used, ,no Thick filming can achieve sufficient filming and hardly affect the element characteristics. The buffer layer of the present invention is characterized by containing at least an eight-by-nitride layer. Specifically, it contains AlxGai-xN (0&lt;XSl). The nitride layer is preferably at least 10. More preferably, it contains A1N, and it is preferably formed at a temperature of 900 to 1400 ° C which is more than the degree of formation of the nitride semiconductor. 115 〇 t to 140 (the temperature condition of TC is preferably formed. When 9 〇〇 ° C to 1200 ° C, it is difficult to make the nitride layer grown in the Alz a phase and the phosphor phase uniform, but in the phosphor A nitride layer can also be formed in the phase. Further, when a nitride layer is formed at a higher temperature, it is easier to obtain a uniform surface. Further, the crystallinity of the buffer layer greatly affects the element characteristics of the nitride semiconductor layer formed on the buffer layer, and is more suitable for crystallinity. The nitride layer containing A1, in order to enhance the crystallinity of AlxGai-xN (0&lt;xS1), irrespective of temperature conditions, is advantageous for the enhancement of the element characteristics 20 of the nitride semiconductor layer. For example, WM0CVD, at a higher temperature, Ga is necessarily reduced in the composition of the obtained AlxGai_xN (0 &lt; x$l). From the viewpoint of the quality of the nitride layer formed as a buffer layer, it is preferable to have a low Ga composition. Further, it is more preferable to form GaN on the nitride layer containing A1 above, in the case where GaN is formed under conditions in which the lateral crystal growth rate becomes faster. The formation of the nitride layer containing A1 200917536 is the same as the phosphor phase of the A丨2 〇3 phase of the substrate of the light conversion material, but the bonding energy of Al-Ν is higher than that of Ga-Ν. The mobility of the surface is small, so that only the nitride layer containing A1, the slight difference between the Α1ζ〇3 phase and the nitride layer in the phosphor phase is different in crystallinity and surface morphology. When GaN is grown, it is easy to cause movement on the nitride crystal which grows in the Aha phase and the phosphor phase, and the difference in each crystal phase can be eliminated. When GaN is formed under conditions that increase the growth rate of the lateral crystal, borrow &amp;

Ge、Se、Te等雜質之摻雜,俟n型化後,可使上述效果及n 型一GaN接觸層之形成並行,因此合適。要提高(3&amp;1^之朝 10橫向成長之晶體成長速度,可使用所謂改變晶體成長溫 度、v/m比等之成長條件之公知方法,而不是選擇其方法 者。又,有關於前述含A1之氮化物層,使用藉控制原料氣 體之供給法,優先地進行移動之方法,亦可得到同樣的效 果。 15 使用依本發明之發光元件形成用複合基板,可在無緩 衝層之狀態下形成氮化物半導體層。在氮化物半導體層之 形成上一般是使用氣相成長法。因為形成氮化物半導體 層,而在加熱時’易使氮缺損。—邊流人職原料氣體一邊 加熱時,可減少氮缺損,可形成穩定的氮化物半導體層。 20 又,依本發明,亦可使用光變換材料基板,且於其基 板上形成與本發明之發光元件形成用複合基板同一構造之 缓衝層’且連續該層而形成氡化物半導體層。在形成氮化 物半導體層時,沒有因再加熱所造成之氮缺損,可得到具 有同樣特性之發光元件。 15 200917536 實施例 以下舉具體型態例,更詳細地說明本發明。 (實施例1) 秤量出以八103/2換算下6^—八1203粉末(純度99.99%) 5 0.82莫耳、以Y03/2換算下Y203粉末(純度99·9%)0·175莫 耳、Ce02粉末(純度99.9%)0.005莫耳。使其等粉末在乙醇 中,藉球磨機濕式混合16小時後,使用蒸發器,使乙醇脫 媒,得到原料粉末。該原料粉末在真空爐中預備溶解,作 為單向凝固之原料。 10 其次,就這樣將原料裝入鉬堝鍋,安裝在單向凝固裝 置,在1.33xHT3Pa(l〇-5Torr)之壓力下熔解原料。其次,在 同一環境氣體下使堝鍋以20mm/小時下降,得到由Al2〇3 (藍寶石)相及(Y、Ce)3Al5012相之2個氧化物相構成之凝固 體。 15 與凝固體之凝固方向垂直之剖面組織示於第2圖。白色 的部分是Y3A15012 : Ce晶體,黑色的部分為Al2〇3晶體。 知道具有兩種晶體相互纏在一起之組織。 所得到之凝固體係藉X線繞射,進行極點圖之測定,檢 查晶體轴的方向’進行以A〗2 〇3晶相之C面為主面之基板之 20 切出。已進行切出之光變換材料係進行研磨、洗淨,以此 作為光變換材料基板。所得到之光變換材料基板再度進行X 線繞射測定,確認到基板表面與Al2〇3之C面間之誤差為&lt; ±2°以内者。 供發光元件形成用複合基板之用之緩衝層之形成是使 16 200917536 用一般的MOCVD爐進行的。原料氣體係使用TMA作為A1 源,使用TMG作為Ga源,使用TES作為Si源(四氫呋喃)。原 料氣體係藉H2而導入反應爐内,在業已加熱之光變換材料 基板上進行晶體成長。 5 已安裝(settlng)在爐内之光變換材料基板係於H2環境 氣體下進行昇溫、加熱,將基板清淨化。將設定改變到目 標之溫度,流入原料氣體,形成含八】之氮化物層。接著在 促進橫向之成長之條件下進行4#m2GaN : si的成長,製 造目標之發光元件形成用複合基板。 10 $ A1之氮化物層係以1300 C形成300nm之A1N後,使用 該物。藉由電子顯微鏡觀察的結果,如第3圖之GaN層剖面 之照片所示,不能觀測到位於Ah 〇3相與螢光體相之間的境 界,形成有均勻的GaN表面。基板之較黑部分為Ai2〇3相, 較白部分為YAG相。GaN薄膜係成長為Ai2〇3相及YAG相兩 15相。其結果是表面為平滑者。在第3圖中,符號la為基板之 Al2〇3相、符號lb為Y3A15012: Ce相,符號2a為A1N緩衝層, 符號2b為GaN : Si層。A1N緩衝層2a係於基板上沿橫向連續 延伸。 (比較例1) 20 對於光變換材料基板’使用與實施例1同樣製作之基 板,按照前述揭示之論文Jpn. J. Appl. Phys. Vol.34(1995), L797 ’在550°C形成30nm之GaN ’代替含A1之氮化物層,接 著,以與實施例1同一條件形成η型一GaN : Si層。使GaN形 成30nm之厚度作為緩衝層之理由是為了和上面所形成之n 17 200917536 型一GaN . Si層間之晶格匹配良好者(如下述,增加緩衝GaN 層之厚度,結果亦同)。 第4圖顯示GaN層之剖面照片。八12 03相上很明顯地可 確認到GaN之形成。在螢光體相中,藉由a1203相之橫向成 5 長’使其表面有部分被GaN覆蓋,不過不能確認來自螢光 體相之GaN的成長’知道表面的平滑性劣化。在第4圖中, 在Ah 〇3相1 a上成長之GaN層2係於使缓衝GaN層(30nm)2c 及η型一GaN : Si層(4&quot;m)2d—起之GaN層2之整體上,亦未 橫向連續者(因此,使緩衝GaN層2c之厚度比實施例1之 10 300nm更厚,例如形成4&quot;m,結果亦同)。 (實施例2、比較例2) 為檢查兀件特性,對於與實施例丨、比較例丨同樣形成 之GaN: Si層,接著形成n型—A1〇iGa〇9N:以層、n型—The doping of impurities such as Ge, Se, and Te, after the 俟n type, can achieve the above effects and the formation of the n-type GaN contact layer in parallel, which is suitable. In order to increase the crystal growth rate of the horizontal growth of 3 &amp; 1^, a well-known method of changing the growth conditions of the crystal growth temperature, the v/m ratio, or the like can be used instead of selecting the method. The nitride layer of A1 can be preferentially moved by the method of supplying the raw material gas, and the same effect can be obtained. 15 The composite substrate for forming a light-emitting element according to the present invention can be used without a buffer layer. A nitride semiconductor layer is formed. In the formation of the nitride semiconductor layer, a vapor phase growth method is generally used. Since the nitride semiconductor layer is formed, it is easy to cause nitrogen deficiency during heating. Further, a nitrogen nitride defect can be reduced, and a stable nitride semiconductor layer can be formed. Further, according to the present invention, a light conversion material substrate can be used, and a buffer having the same structure as the composite substrate for forming a light-emitting element of the present invention can be formed on the substrate. The layer 'continues the layer to form a germanide semiconductor layer. When the nitride semiconductor layer is formed, there is no nitrogen defect caused by reheating, and it is obtained. Light-emitting elements having the same characteristics. 15 200917536 EXAMPLES Hereinafter, the present invention will be described in more detail with reference to specific examples. (Example 1) 6^-eight 1203 powder (purity 99.99%) was weighed and measured in eight 103/2. 5 0.82 mol, Y203 powder (purity 99.9%) 0.175 mol, Ce02 powder (purity 99.9%) 0.005 mol in Y03/2 conversion, so that the powder is in ethanol, wet mixing by ball mill After 16 hours, the ethanol was de-intermediated using an evaporator to obtain a raw material powder which was preliminarily dissolved in a vacuum furnace as a raw material for unidirectional solidification. 10 Next, the raw material was charged into a molybdenum crucible and mounted in a single The raw material was melted at a pressure of 1.33 x HT3Pa (10 Torr - 5 Torr) to the solidification apparatus. Secondly, the crucible was lowered at 20 mm/hr under the same ambient gas to obtain an Al2〇3 (sapphire) phase and (Y, Ce). A solidified body composed of two oxide phases of 3Al5012 phase. 15 The cross-sectional structure perpendicular to the solidification direction of the solidified body is shown in Fig. 2. The white part is Y3A15012: Ce crystal, and the black part is Al2〇3 crystal. a group of two crystals intertwined The obtained solidification system is diffracted by X-rays, and the pole pattern is measured, and the direction of the crystal axis is checked. The substrate of the C surface of the A 2 3 〇 3 crystal phase is cut out. The light conversion material was polished and washed to obtain a substrate for a light conversion material. The obtained optical conversion material substrate was subjected to X-ray diffraction measurement again, and it was confirmed that the error between the surface of the substrate and the C surface of Al2〇3 was &lt; Within ±2° The buffer layer for the composite substrate for forming a light-emitting element is formed by using 16 200917536 in a general MOCVD furnace. The feed gas system uses TMA as the A1 source, TMG as the Ga source, and TES as the Si source (tetrahydrofuran). The raw material gas system is introduced into the reaction furnace by H2, and crystal growth is performed on the heated light conversion material substrate. 5 Installed (settlng) The substrate of the light conversion material in the furnace is heated and heated under H2 ambient gas to purify the substrate. The setting is changed to the target temperature, and the raw material gas is flowed to form a nitride layer containing eight. Then, the growth of 4#m2GaN:si is carried out under the conditions of promoting lateral growth, and a target composite substrate for forming a light-emitting element is produced. The nitride layer of 10 $ A1 is formed by forming 300 nm of A1N at 1300 C. As a result of observation by an electron microscope, as shown in the photograph of the cross section of the GaN layer in Fig. 3, the boundary between the Ah 〇 3 phase and the phosphor phase was not observed, and a uniform GaN surface was formed. The darker portion of the substrate is the Ai2〇3 phase, and the whiter portion is the YAG phase. The GaN thin film system is grown into two phases of Ai2〇3 phase and YAG phase. The result is that the surface is smooth. In Fig. 3, the symbol la is the Al2〇3 phase of the substrate, the symbol lb is the Y3A15012: Ce phase, the symbol 2a is the A1N buffer layer, and the symbol 2b is the GaN: Si layer. The A1N buffer layer 2a is continuously extended in the lateral direction on the substrate. (Comparative Example 1) 20 A substrate prepared in the same manner as in Example 1 was used for the optical conversion substrate, and 30 nm was formed at 550 ° C according to the above-mentioned paper Jpn. J. Appl. Phys. Vol. 34 (1995), L797 '. The GaN ' replaced the nitride layer containing A1, and then an n-type GaN : Si layer was formed under the same conditions as in Example 1. The reason why GaN is formed to have a thickness of 30 nm as a buffer layer is to have a good lattice match with the n 17 200917536 type GaN. Si layer formed above (as described below, the thickness of the buffer GaN layer is increased, and the result is also the same). Figure 4 shows a cross-sectional photograph of the GaN layer. It is apparent that the formation of GaN is confirmed on the phase of the eight 12 03 phase. In the phosphor phase, a part of the surface of the a1203 phase is covered with GaN by a lateral length of 5, but the growth of GaN from the phosphor phase cannot be confirmed, and the smoothness of the surface is known to be deteriorated. In Fig. 4, the GaN layer 2 grown on the Ah 〇 3 phase 1 a is bonded to the GaN layer 2 which is a buffer GaN layer (30 nm) 2c and an n-type GaN : Si layer (4 &quot; m) 2d. As a whole, there is also no lateral continuity (thus, the thickness of the buffer GaN layer 2c is made thicker than 10300 nm of the first embodiment, for example, 4 &quot; m, and the result is the same). (Example 2, Comparative Example 2) In order to examine the characteristics of the element, the GaN: Si layer formed in the same manner as in Example 比较 and Comparative Example ,, followed by formation of n-type - A1 〇 i Ga 〇 9 N: layer, n type -

In〇.05GaQ.95N :Si層、形成單—量子井構造型發光層之化⑽ 層、p型-A1〇.lGa〇.9N:Mg障壁層、形成有p電極之p型—In〇.05GaQ.95N : Si layer, forming a single-quantum well structured light-emitting layer (10) layer, p-type-A1〇.lGa〇.9N: Mg barrier layer, p-type formed with p-electrode

GaN . Mg層’在n型接觸層及p型接觸層進行電極形成,製 作發光二極體元件。 在實施例2巾,與製作前述發光元件形成職合基板同 樣,每一半導體層都可均勾地形成,可確認來自全面之發 在比較例2中, 得到充分的發光。 由其型態做電極之形成是困難的,不能 比較所製作之發光二極 以下匯整以實施例丨為基準而 體元件之外部量子效率之結果。 18 25 200917536 試料 外部量子效率比(以實施例1為基準) 實施例2 1 比較例2 0.01 (實施例3) 對於含A1之氮化物層,以1150°C形成300nm之AlojGao.g N或Al0.25Ga0.75N,除了使用這個之外,其餘與實施例1同樣 5 進行。藉電子線顯微鏡觀察之結果,與實施例1同樣,不能 觀測到ai2o3相與螢光體相之境界,在複合基板上已形成均 勻之GaN表面。其樣態係與第3圖同樣。 由以上之結果明白,使用本發明之具有緩衝層之發光 元件形成用複合基板,更有效地靈活運用光變換材料基 10 板,可做到良好的白色發光元件之形成者。 【圖式簡單說明3 第1A及1B圖係模式地顯示本發明之發光元件形成用 複合基板之一實施型態之剖視圖。 第2圖係顯示光變換材料之組織構造例之電子顯微鏡 15 照片。 第3圖係實施例1所得到之G aN層之顯微鏡剖面照片。 第4圖係比較例1所得到之GaN層之顯微鏡剖面照片。 【主要元件符號說明】 1...光變換材料基板 la. · _Al2〇3 相 lb. ..氧化物相 2…緩衝層 2a...氮化物層 2b.,.GaN 層 2c._.謝UGaN 層 2d...n型一GaN : Si層 19The GaN. Mg layer' is formed by electrodes on the n-type contact layer and the p-type contact layer to form a light-emitting diode element. In the same manner as in the case of fabricating the above-mentioned light-emitting element forming substrate, each of the semiconductor layers was formed in a uniform manner, and it was confirmed that the film was completely emitted in Comparative Example 2, and sufficient light emission was obtained. It is difficult to form the electrode by its type, and it is not possible to compare the results of the external quantum efficiency of the body element based on the embodiment of the light-emitting diode. 18 25 200917536 Sample external quantum efficiency ratio (based on Example 1) Example 2 1 Comparative Example 2 0.01 (Example 3) For a nitride layer containing A1, AlojGao.g N or Al0 at 300 nm was formed at 1150 °C. .25Ga0.75N was carried out in the same manner as in Example 1 except that this was used. As a result of observation by an electron beam microscope, in the same manner as in Example 1, the boundary between the ai2o3 phase and the phosphor phase could not be observed, and a uniform GaN surface was formed on the composite substrate. The appearance is the same as in Figure 3. From the above results, it is understood that the use of the composite substrate for forming a light-emitting element having a buffer layer of the present invention can more effectively utilize the optical conversion material substrate 10, and can form a good white light-emitting element. BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1A and FIG. 1B are cross-sectional views showing an embodiment of a composite substrate for forming a light-emitting element of the present invention. Fig. 2 is an electron microscope 15 photograph showing an example of the structure of a light conversion material. Fig. 3 is a photomicrograph of a photomicrograph of the GaN layer obtained in Example 1. Fig. 4 is a photomicrograph of a GaN layer obtained in Comparative Example 1. [Main component symbol description] 1...Light conversion material substrate la. · _Al2〇3 phase lb. .. oxide phase 2...buffer layer 2a...nitride layer 2b.,.GaN layer 2c._. UGaN layer 2d...n type GaN: Si layer 19

Claims (1)

200917536 十、申請專利範圍: h —種發光件形成用複合基板,包含有: 光變換材料基板;及 形成在該光變換材料基板上之氮化物層, 5 則述光變換材料基板具有至少2層以上之氧化物層連 續且相互輯成三維空間之㈣’且前述氧化物層含有 Al2〇3相及至少發出1種螢光之氧化物相, 前述氮化物層於與前述光變換材料基板之界面至少 具有1層至少含A1之氮化物層。 1〇 2.如中請專利範圍第1項之發統件形成用複合基板,其中 前述氮化物層内至少含A1之氮化物層係以組成式 A1xGai_xN(0&lt;x$i)表示, 且其他氮化物層係以組成式ΙηχΑ^ ㈣χ ^ 1、OSySl、OSx + ygi)表示。 15 3.如申請專利範圍第丨項之發光元件形成用複合基板,其中 前述光變換材料基板中之發㈣光之氧化物相之一相, 其組成成分具有至少含γ元素、似素及、&amp;元素 之石榴石型構造。 ” ” 20 4. 如申請專利範圍第3項之發光元件,其中前述光變換材料 基板係以彻3相之⑽與具有硕石型構造且發 之氧化物相之(112)面同時作為主面。 5. -種發光讀,係於中請專利範圍第…項巾任— 發光元件形成賴合基板之前述氮化物層上,具 化物糸化合物半導體構成之發光層。 20 200917536 6. 如申請專利範圍第5項之發光元件,其中前述發光層係由 InxAlyGa^.yNeSxS :l、0SyS ;l、0Sx + yS 1)所構成者。 7. —種發光元件形成用複合基板之製造方法,係於光變換 材料基板上形成氮化物層, 5 該光變換材料基板具有至少2層以上之氧化物層連續 且相互纏繞成三維空間之組織,且該氧化物層含有ai2o3 相及至少發出1種螢光之氧化物相, 並且,該氮化物層於與該光變換材料基板間之界面至 少具有1層至少含A1之層。 10 8.如申請專利範圍第7項之發光元件形成用複合基板之製 造方法,其中前述氮化物層之形成中,利用有機金屬化 合物氣相成長法進行至少1層之形成。 9.如申請專利範圍第7項之發光元件形成用複合基板之製 造方法,其中前述氮化物層之形成中,利用有機金屬化 15 合物氣相成長法,以900°C以上、小於1400°C以下之溫度 形成含A1之氮化物層。 21200917536 X. Patent application scope: h—a composite substrate for forming a light-emitting member, comprising: a substrate for optical conversion material; and a nitride layer formed on the substrate of the light conversion material, 5 wherein the substrate of the light conversion material has at least 2 layers The above oxide layer is continuously and mutually formed into a three-dimensional space (four)' and the oxide layer contains an Al2〇3 phase and at least one fluorescent oxide phase, and the nitride layer is on the interface with the optical conversion material substrate. There is at least one nitride layer containing at least one layer of A1. 1. The composite substrate for forming a hair piece according to the first aspect of the invention, wherein the nitride layer containing at least A1 in the nitride layer is represented by a composition formula A1xGai_xN (0&lt;x$i), and the other The nitride layer is represented by the composition formula ΙηχΑ^ (4) χ ^ 1, OSySl, OSx + ygi). The composite substrate for forming a light-emitting element according to the invention of claim 2, wherein one of the oxide phases of the light (four) light in the light conversion material substrate has a composition containing at least a γ element, a phenotype, and The garnet structure of the &amp; element. 4. The light-emitting element of claim 3, wherein the light-converting material substrate has a three-phase (10) and a (112) surface having a gem-type structure and an oxide phase as a main surface. . 5. A kind of illuminating reading, which is a luminescent layer composed of a bismuth compound semiconductor formed on the nitride layer of the substrate. The light-emitting element of claim 5, wherein the light-emitting layer is composed of InxAlyGa^.yNeSxS:1, 0SyS; 1, 0Sx + yS 1). 7. A method of producing a composite substrate for forming a light-emitting element, wherein a nitride layer is formed on a substrate of a light conversion material, and the substrate of the light conversion material has at least two or more oxide layers continuously and intertwined into a three-dimensional space. And the oxide layer contains an ai2o3 phase and an oxide phase emitting at least one type of phosphor, and the nitride layer has at least one layer containing at least one layer of A1 at an interface with the substrate of the light conversion material. In the method of producing a composite substrate for forming a light-emitting element according to the seventh aspect of the invention, in the formation of the nitride layer, at least one layer is formed by an organometallic compound vapor phase growth method. 9. The method for producing a composite substrate for forming a light-emitting element according to claim 7, wherein the formation of the nitride layer is performed by a vapor phase growth method of an organometallic compound, and is 900 ° C or more and less than 1400 °. The temperature below C forms a nitride layer containing A1. twenty one
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