TW201232824A - Transparent thin film, light emitting device comprising the same, and methods for preparing the same - Google Patents

Transparent thin film, light emitting device comprising the same, and methods for preparing the same Download PDF

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TW201232824A
TW201232824A TW100146371A TW100146371A TW201232824A TW 201232824 A TW201232824 A TW 201232824A TW 100146371 A TW100146371 A TW 100146371A TW 100146371 A TW100146371 A TW 100146371A TW 201232824 A TW201232824 A TW 201232824A
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layer
electrode
nitride semiconductor
emitting device
contact layer
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TW100146371A
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Chinese (zh)
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Suk-Hun Lee
Hae-Gwon Lee
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Quantum Device Inc
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/02—Semiconductor devices with at least one potential-jump barrier or surface barrier 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
    • H01L33/025—Physical imperfections, e.g. particular concentration or distribution of impurities
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/02—Semiconductor devices with at least one potential-jump barrier or surface barrier 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
    • H01L33/12—Semiconductor devices with at least one potential-jump barrier or surface barrier 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 stress relaxation structure, e.g. buffer layer
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/36—Semiconductor devices with at least one potential-jump barrier or surface barrier 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
    • H01L33/40—Materials therefor
    • H01L33/42—Transparent materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/44—Semiconductor devices with at least one potential-jump barrier or surface barrier 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 coatings, e.g. passivation layer or anti-reflective coating
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2933/00—Details relating to devices covered by the group H01L33/00 but not provided for in its subgroups
    • H01L2933/0008—Processes
    • H01L2933/0016—Processes relating to electrodes

Abstract

The invention relates to a transparent film, a light emitting device including the same, and a method for manufacturing the same. A nitride semiconductor light emitting device with composition formula AlxInyGa(1-x-y)N (0 ≤ x ≤ 1, 0 ≤ y ≤ 1, 0 ≤ x+y ≤ 1) of this invention includes a substrate, a buffer layer, a first electrode contact layer, a first cover layer, an active layer, a second cover layer, a second electrode contact layer, and a transparent electrode of ZnO film. The transparent electrode of ZnO film is formed on the second electrode contact layer and, at the same time, doped with at least one n-type impurity selected from the group consisting of group III elements of B, Al, Ga, In and F, Cl, H, and at least one p-type impurity selected from the group consisting of group V elements of N, P, As, Sb and Li, Na, C. A first electrode pad formed on one side of the upper part of the first electrode contact layer, and a second electrode pad formed on one side of the upper part of the transparent electrode.

Description

201232824 40534pif 六、發明說明： 【發明所屬之技術領域】 本發明係關於一種透明薄膜、包含該薄臈之發光装置 及其製備方法，特別是關於一種同時摻雜有如Ga之〜型 雜質與如As之p-型雜質之ZnO(Zinc oxide，氧化鋅）薄膜、 包含該薄膜之發光裝置及其製備方法。 、 【先前技術】 發光裝置之材料、特別是氮化物半導體因優異之物 理、化學特性，作為如半導體發光二極體(LED， Emitting Diode)或雷射二極體(LD，Laser Di〇de)之發光裝 置之核心材料而倍受青睞。通常，氮化物半導體=具^ AlxInyGa(1-x-y)N(0^x$l、Ogyy、+ 之組成 式之GaN系物質構成。圖1是概略性地表示利用有普通之 AlInGaN线化物半導體之發光裝置之積層構造的剖面 圖。於利用有AlInGaN系氮化物半導體之發光裝置之擊備 過程中，積層成長基板(101)、緩衝層（1〇3)、作^第丨電極 接觸層而發揮個之η·型氮化物半導體層⑽）、〜型氮化 物包覆層（107)、活性層（109)、p_型氮化物包覆層（lli)、p_ 型氮化物半導體層（113)、咖型第2電極接觸層（ii5)。此 後，於忠片（chip)製備過程中，透明電極層、特別是 mxmdium Tin Oxide，氧化銦锡)透明電極 於 n/p-型第2電極接觸層（115)上’最終如圖i所示般形成用 以線結合(wire bonding)之p-型電極塾(121)盘&型電極塾 4201232824 40534pif VI. Description of the Invention: [Technical Field] The present invention relates to a transparent film, a light-emitting device comprising the same, and a method of fabricating the same, and more particularly to a method of simultaneously doping a dopant such as Ga with an impurity such as As A ZnO (Zinc oxide) thin film of p-type impurities, a light-emitting device comprising the same, and a method for preparing the same. [Prior Art] The material of the light-emitting device, particularly the nitride semiconductor, is excellent in physical and chemical properties, such as a semiconductor light emitting diode (LED) or a laser diode (LD, Laser Di〇de). The core material of the illuminating device is favored. In general, a nitride semiconductor = a GaN-based material having a composition formula of AlxInyGa(1-xy)N (0^x$l, Ogyy, and +). Fig. 1 is a view schematically showing the use of a conventional AlInGaN linearized semiconductor. A cross-sectional view of a laminated structure of a light-emitting device. In the process of using a light-emitting device having an AlInGaN-based nitride semiconductor, a growth substrate (101), a buffer layer (1〇3), and a second electrode contact layer are laminated. Η-type nitride semiconductor layer (10)), a nitride-coated layer (107), an active layer (109), a p-type nitride cladding layer (lli), and a p-type nitride semiconductor layer (113) , coffee type second electrode contact layer (ii5). Thereafter, during the preparation of the chip, a transparent electrode layer, particularly an mxmdium Tin Oxide, indium tin oxide transparent electrode is formed on the n/p-type second electrode contact layer (115), which is finally shown in FIG. A p-type electrode 121(121) disk & type electrode 塾 4 for wire bonding is generally formed.

Sy 201232824 (119)。 基板’)主要使用具有六邊形結晶構造之石基 板。為了使因藍寶石基板(1G1)與η·型氮化物半導體 之晶格常數及熱膨脹係數之差而產生之結晶缺陷最〕、化， 緩衝層（103)可成長於基板⑽)上。緩衝層⑽)可於遍 °C〜60G°C之低溫下，由呈非晶質結晶性之具有％⑽以 下厚度之GaN系或A1N系氮化物形成。另外，於緩衝層（1〇3) 上，可進一步形成非摻雜GaN層。而且，為了於 度設為刚代〜則代左右之範_形成料有助^ 導率（electrical conductivity)之載子之電子，成長以1〜 5xl018/cm3左右之摻雜濃度摻雜有矽之〜型氮化物半導體 層（105)。上述n-型氮化物半導體層（1〇5)用作與n型電極 墊(119)電性接觸之第1電極接觸層。於在n_型氮化物半導 體層（105)上形成n-型氮化物包覆層（1〇7)後，將成長溫度降 至 700。(：〜800。(：而形成 InGaN/GaN、InGaN/InGaN 之單一 或多重量子井構造之活性層（109)。此後，於活性層（1〇9) 上’形成P-型氮化物包覆層（111)、p_型氮化物半導體層 (113)、及n/p-型第2電極接觸層（115)。 於n/p-型第2電極接觸層（115)之形成過程中，作為雜 質而摻雜有Cp2Mg或DMZn。於使用DMZn作為雜質之 情形時’Zn原子於n/p-型第2電極接觸層（115)内，作為受 體而以深能級(deep energy level)，，定位，藉此用以形成 作為載子之電洞之活化能(activation energy)非常高，故於 施加偏壓時，作為載子之電洞濃度限定於〜l〇17/cm3左 201232824 40534pit 右。因此’作為用以使n/p-型第2電極接觸層（i15)成長之 雜質，活化能相對較低之Cp2Mg用作摻雜源。於將Cp2Mg 作為摻雜源而使第2電極接觸層（115)成長之情形時，在 GaN層内形成與用作氮(N)源之NH3源氣體、及自摻雜源 分離之氫(H)鍵結之Mg-H錯合體(complex)，具有〜106 ohm.cm以上之高電阻絕緣體特性。於上述活性層（1〇9) 中，為了電洞與電子藉由再結合過程(recombination process) 而射出光，無法以摻雜有作為高電阻之Mg之狀態使用， 必需用以破壞Mg-H錯合體之鍵結之活化步驟(activati〇n process)。上述活化步驟係於6〇〇t〜8〇〇。(：範圍之溫度條 件及N2或沁/〇2環境下’藉由熱處理步驟(annealing pr〇cess) 而執行，但第2電極接觸層（115)内所存在之Mgi活化效 率較低，因此即便進行活化步驟，第2電極接觸層（115)與 作為第1電極接觸層之η-型氮化物半導體層（1〇5)相比，亦 具有非常高之電阻雜。於活化步驟後，上述第2電極接 觸，（115)内之Mg原子濃度（at〇mic撃如财㈣為 10 /cm〜l〇21/cm3左右，但作為有助於電導率之載子之電 洞之濃度僅為lG17/em3左右，且制移動雜也⑽磁y) 亦非常低至KW/Vsec。另外，於上述第2電極接觸層_ ^未完全構成活化而殘留之Mg、Mg_H錯合體、結晶缺陷 荨在捕獲(trap)自上述活性層⑽)向表面方向射出之光、或 施加高電流之情形時，藉由相對而言非常高之上述第2電 mm 極^觸層（115)之電阻特性而產生熱，因此縮短發光裝置之 哥中而對可靠性產生惡劣影響。特別是，於1 201232824 4U>34pit 20 ηιΑ^Γ輪出發光裝置之情形時’施加遠遠大於現 ί /η接Ϊ高電流，因此導致如下之結果： 於ρ-/η-接面產± _以上之接面溫 咖 temperature) ’從而對發光裝置之 ^ 之影響，且對使用於要及了成致〒性 听…猫私為 “輸出之應用產品而言具有極 二原因在於因未於第2電極接觸層(出)内活 化成載子而殘留之過剩Mg原 電阻成分之增加與藉此產生g Η :體 未解決課題。另外，先前之D/n广㈣娜且殘存為 „ ；；^： ：Γ；Ν ί ^ .电蚀祛觸層之上述η-型氮化物半 ^體層（105)之情㈣，與作為播雜源之卿或祕之产 1 =加對應:之敎摻雜濃度呈線性比例而增加，且於結曰^ 性付到臨界厚度㈣㈣邮⑽相容易地“ =:r:6xl〇18/cm3範圍内’但於第2電極接觸層 (115)之情形時，即便增加作為摻雜 最多地摻雜有〜102VCm3以上之M s π P g之机量而 於電導率之載子，電、、同作為純粹有助 电守千 電洞，農度亦限制於lxl〇i7/cm3〜 P_/n-接碎光f置之•二Γ祕之摻雜分佈之 Ρ η接面I九裝置之構造。如上所述，第2電極接觸 之較低之載子濃度及較高之電阻特性使内部量子 (mt觀1 quantum effieieney)降低，限制細 αι = 化物半導體發光裝置之實現。 糸氣 於AlInGaN系氮化物半導體發光装置 接觸層（H5)之較高之_5]電阻特性，藉由電子=電洞^ 201232824 40534pifSy 201232824 (119). The substrate ') mainly uses a stone substrate having a hexagonal crystal structure. The buffer layer (103) can be grown on the substrate (10) in order to maximize the crystal defects caused by the difference between the lattice constant and the thermal expansion coefficient of the sapphire substrate (1G1) and the ?-type nitride semiconductor. The buffer layer (10) may be formed of a GaN-based or A1N-based nitride having an amorphous crystallinity and having a thickness of less than % (10) at a low temperature of from °C to 60 °C. Further, on the buffer layer (1〇3), an undoped GaN layer can be further formed. In addition, in order to set the degree to the nearest generation to the next generation, the electrons of the carrier having the electrical conductivity are grown at a doping concentration of about 1 to 5 x 1018 /cm 3 . A type-nitride semiconductor layer (105). The n-type nitride semiconductor layer (1〇5) serves as a first electrode contact layer in electrical contact with the n-type electrode pad (119). After the n-type nitride cladding layer (1?7) was formed on the n-type nitride semiconductor layer (105), the growth temperature was lowered to 700. (: ~800. (: The active layer (109) of a single or multiple quantum well structure of InGaN/GaN, InGaN/InGaN is formed. Thereafter, a P-type nitride coating is formed on the active layer (1〇9) a layer (111), a p-type nitride semiconductor layer (113), and an n/p-type second electrode contact layer (115). During formation of the n/p-type second electrode contact layer (115), Cp2Mg or DMZn is doped as an impurity. When DMZn is used as an impurity, 'Zn atoms are in the n/p-type second electrode contact layer (115), and a deep energy level is used as a receptor. Positioning, whereby the activation energy for forming a hole as a carrier is very high, so when a bias voltage is applied, the hole concentration as a carrier is limited to ~l〇17/cm3 left 201232824 40534pit right Therefore, as an impurity for growing the n/p-type second electrode contact layer (i15), Cp2Mg having a relatively low activation energy is used as a dopant source. The second electrode is contacted by using Cp2Mg as a dopant source. When the layer (115) is grown, a Mg-H bond formed in the GaN layer with a hydrogen (H) source gas which is used as a nitrogen (N) source and a self-doping source is formed. Complex, having a high-resistance insulator characteristic of ~106 ohm.cm or more. In the above active layer (1〇9), light is emitted by holes and electrons by a recombination process. It is used in the state of Mg as a high resistance, and it is necessary to activate the activation process of the bond of the Mg-H complex. The above activation step is performed at 6〇〇t~8〇〇. The temperature condition and the N2 or 沁/〇2 environment are performed by the annealing step, but the Mgi activation efficiency existing in the second electrode contact layer (115) is low, so even if the activation step is performed The second electrode contact layer (115) also has a very high resistance impurity as compared with the n-type nitride semiconductor layer (1〇5) which is the first electrode contact layer. After the activation step, the second electrode contacts The atomic concentration of Mg in (115) is at least 10/cm~l〇21/cm3, but the concentration of the hole as a carrier that contributes to conductivity is only about lG17/em3. And the system movement is also (10) magnetic y) is also very low to KW / Vsec. In addition, in the above 2nd The contact layer _ ^ is not completely composed of activated Mg, Mg_H complex, crystal defect 荨 when trapping light from the active layer (10) to the surface direction, or applying a high current, by relative In the case where the resistance of the second electric mm electrode layer (115) is extremely high, heat is generated, so that the light-emitting device is shortened and the reliability is adversely affected. In particular, in the case of 1 201232824 4U>34pit 20 ηιΑ^Γ when the light-emitting device is turned on, 'the application is much higher than the current high voltage, which results in the following results: ρ-/η- junction production ± _ Above the junction temperature temperature)) and thus the impact of the illuminating device ^, and the use of the singularity of the singularity of the singularity of the cat The increase in the excess Mg primary resistance component remaining in the second electrode contact layer (outlet) by activation of the carrier and the generation of g Η are not solved. In addition, the previous D/n is broad (4) and remains as „ ; ;^: :Γ;Ν ί ^ . The above-mentioned η-type nitride half-body layer (105) of the electrolytically etched contact layer (4), and the product of the Qing or the secret source as the source of the miscellaneous source 1 = plus: The doping concentration increases linearly, and the crucible is added to the critical thickness (4). (4) The postal (10) phase is easily "=:r:6xl〇18/cm3" but in the case of the second electrode contact layer (115). At the time, even if the doping is most doped with a mass of Ms π P g of more than ~102 VCm3, the carrier of conductivity, electricity, The same as the purely helpful electric gate hole, the degree of agriculture is also limited to lxl〇i7/cm3~ P_/n- 接 碎 碎 • • Γ Γ Γ 掺杂 掺杂 掺杂 掺杂 掺杂 I I 九 九As described above, the lower carrier concentration and higher resistance characteristics of the second electrode contact lower the internal quantum (mt), limiting the implementation of the fine-α semiconductor semiconductor light-emitting device. Helium is used in AlInGaN. The higher the _5] resistance characteristic of the contact layer (H5) of the nitride semiconductor light-emitting device, by electron = hole ^ 201232824 40534pif

再結合過程而自相當於與第2電極接觸層（115)電性接觸之 P-型電極墊（121)之下端部分的活性層（1〇9)之InGaN/GaN 多重量子井層射出光。然而，p-型電極墊(121)於封裝步驟 中藉由線結合與Au線(wire)連接，因此可導致如下之結 果.整體金屬厚度較厚地沉積成1 μιη以上，從而自活性 層（109)射出之光無法通過較厚之金屬。特別是，因第2電 極接觸層（115)之較高之電阻特性’於橫向(lateral directi〇n) 上無均勻之電流散佈(current spreading)，而產生局部性地 集中於Ρ·型電極墊（121)部分之電流集中（叫订邮 concentrating)，藉此存在因極其大之散熱而高效/高可靠性 之發光裝置之製作較難之問題點。因此，需要光透過率優 異，且具有與第2電極接觸層（115)之較低之接觸電阻之透 明電極，以便可改善發光裝置之電流集中，達成均勻之電 流散佈至活性層（109)之實際發光面積為止。伴隨此種技術 必需性，提出有如下之方案：對上述A1InGaN系氮化物半 導體之磊晶片（Epi-Wafer)成長技術之極限，開發芯片（chip) v驟技術並應用’藉此解決先前之AUnGaN系氮化物半導 體之上述問題點。首先，試圖於上述第2電極接觸層（115) 上應用較薄之Ni/Au合金而降低接觸電阻。即，為了提高 第2電極接觸層（115)之電流散佈而增加發光效率，使用具 有20 nm以下之較薄之厚度之Ni/Au合金作為電極物質: 用作電極物質之Ni/Au合金作為抗透過性金屬，於與第2 電極接觸層（115)之接觸時’在界面形成非常薄之Ni〇膜而 接觸電阻下降，但光透過率相對較低至5〇%〜6〇%左右，In the bonding process, light is emitted from the InGaN/GaN multiple quantum well layer of the active layer (1〇9) corresponding to the lower end portion of the P-type electrode pad (121) electrically contacting the second electrode contact layer (115). However, the p-type electrode pad (121) is connected to the Au wire by wire bonding in the packaging step, and thus can result in the following result. The overall metal thickness is thickly deposited to 1 μm or more, thereby self-active layer (109). The light that is emitted cannot pass through the thicker metal. In particular, since the higher resistance characteristic of the second electrode contact layer (115) has no uniform current spreading in the lateral direction, localized concentration on the electrode pad is locally concentrated. (121) Part of the current concentration (called concentrating), whereby there is a problem that it is difficult to manufacture a light-emitting device with high efficiency and high reliability due to extremely large heat dissipation. Therefore, a transparent electrode having excellent light transmittance and having a low contact resistance with the second electrode contact layer (115) is required, so that current concentration of the light-emitting device can be improved, and a uniform current can be distributed to the active layer (109). The actual luminous area is up. Along with the necessity of such technology, a proposal has been made to develop a chip and apply the technology to the limit of the Epi-Wafer growth technology of the above-mentioned A1InGaN nitride semiconductor, thereby solving the previous AUnGaN. The above problems of nitride semiconductors. First, an attempt is made to reduce the contact resistance by applying a thin Ni/Au alloy to the second electrode contact layer (115). That is, in order to increase the light emission efficiency by increasing the current dispersion of the second electrode contact layer (115), a Ni/Au alloy having a thin thickness of 20 nm or less is used as the electrode material: Ni/Au alloy used as an electrode material is used as an anti-electrode The contact metal forms a very thin Ni tantalum film at the interface when the contact with the second electrode contact layer (115), and the contact resistance decreases, but the light transmittance is relatively low to about 5〇% to about 6〇%.

S 201232824 4U5J4plt 故咼效發光裝置之實現較難。為了改善此種問題點，光透 過率較尚且接觸電阻較低之IT〇(In2〇3: Sn)取代Ni/Au抗透 過性金屬作為透明電極，廣泛應用於在2〇〇2年後正式量產 之移動終％、葦δ己型電腦、pC(personai c〇mpUter，個人電 腦）、顯不器、LCD(LiqUid Crystal Display，液晶顯示 器)TV(Television)背光單元、照明製品等。藉由將IT〇用 作透明電極’實現了發光裝置之光輸出約提高3〇%之劃時 代之技術進步。 TO透明電極層（Η?)可利用與濺鍍法（SpUtterjng deposition)及電子束蒸鍍法(e_beam evap〇rati〇n)相關之設 備而沉積，且光透過率為85%以上，接觸電阻為1〇·5 ohm.cm級別，具備具有〜型電導率之非晶質或多晶質之 結晶性，且於沉積後，為了恢復結晶性而必需後續之熱處 理步驟。藉由多晶之結晶構造，自第2電極接觸層（115)之 下=部相對於活性層（109)之垂直方向(vertical directi〇n)之 電流流動較為容易，但相對於橫向〇ateraldirecti〇n)之電流 流動較垂直方向之電流流動非常小，因此處於要求有對該 情形之改善之情況。另外，持續執行用以用作發光裝置之 透明電極之ITO物質本身之性能改善的研究開發，但其結 果處於未完成之狀態。最近，相較對IT0物質本身之研究 開發藉由對ιτο透明電極之圖案化(pattering)或紋理化 (texturing)步驟技術之開發而謀求發光裝置之性能改善，但 現狀為動作電壓增加，從而實際上無法應用於量產製品。 另外，構成ITO物質之銦(In)之埋藏量極其有限，故存在 201232824 40534pif 得非常高之輸’特別是最近對稀有元素之 貝源武裔化之傾向變得白熱化而其程度日益嚴峻。 改盖】=為:編必系氮化物悔發光裝置之性能 成本’迫切需求可代替現有之1το物質 為了滿足智慧型手機(_ =型，心顯示器、LCD用背光單元或照明製品之 f ’迫切需求具有5G%以上之光效率且高效之發光裝 置’旦現狀為因對蟲晶片成長技術及芯片步驟之技術性極 限而無法滿足該需求十於A1InGaN ^化物半導體發 光裝置之蟲晶片成長技射’投人極其大之費賴人力進 行用以將内部量子效率改善5%以上之研究開發’，、但處於 未完成=狀態。另外，為了克服蟲晶片成長技術之技術性 極限，藉由芯片步驟技術之開發進行用以發光裝置之性能 改善之努力’但未發現令人矚目的成果。為了克服此種技 術難關，最近積極進行對Zn0透明電極之研究開發，該 ZnO透明電極係作為代替用作A1InGaN系氮化物半導體發 光裝置之透明電極之ITO物質之物質。 可用作發光裝置之透明電極之Zn0薄膜具有85%以 上之優異之光透過率，具有與AlInGaN系氮化物半導體發 光裝置相同之六邊形結晶構造，熱穩定性(thermal stability) 優異而可有效地應用於大面積/高輸出發光裝置，且具有較 局之折射率(refractive index)與能帶隙(energy bandgap)調 節較為容易之優點。另外，於ZnO薄膜之情形時，具有可 易於在結晶成長方向上形成柱狀微構造（columnar 201232824 4U534pit' microstmcture)之優點。而且，於Zn〇薄膜之情形時，使 用遠遠豐富於現有之ITO透明電極之銦(In)之辞(Zn)，因此 具有可實現低彳貝之順利且穩定之原料物質之供給。於可代 替先前之ITO透明電極之Zn〇物質之情形時，形成於作為 第2電極接觸層之ρ-GaN層上，具有與p_GaN層相同之六 邊形之結晶構造，且使用於沉積之設備與技術可相同地適 用，因此具有可容易地獲得優質之結晶性之優點。Zn〇物 質中，光透過率可藉由較高之折射率與較低之吸收係數等 而較高地變為90%以上，且亦可藉由形成構造之變化，使 自InGaN/InGaN或InGaN/GaN活性層向表面方向射出之 光之飛離角（escape angle)發生變化而提高發光裝置之透過 效率。 於發光裝置之情形時，就發光之方面而言，必須與較 高之光透過率一併滿足電阻設計(resistance design)技術， 方可實質地應用於量產，該電阻設計技術係為了於活性層 上增加電子與電洞之再結合效率，將與p_/n_電極之接觸電 阻最小化，從而即便施加較低之電壓，内部量子效率亦可 極大化。為了形成ZnO透明電極，向如下方向進行研究開 發：對利用濺鍍法、電子束蒸鍍法之含有添加物之非晶質 及多晶構造進行成長之方向；及對利用分子束遙晶法 (MBE ’ molecular beam epitaxy)、有機金屬化學氣相沉積法 (MOCVD，metal organic chemical vapor deposition)或脈衝 雷射沉積法(PLD ’ pulse laser deposition)之摻雜有雜質之單 晶構造進行成長之方向。利用上述成長方法，可藉由Zn〇 201232824 40534pif 物質本身或構造之變更而容易地獲得較高之透過率特性， 但迄今為止未獲得具有根據較低之接觸電阻產生之較高之 電導率的結果。ZnO透明電極之開發方向可較大地分為如 下開發：對用以改善光透過率之奈米柱(職〇r〇d)與奈米線 (nanowire)形態之開發；及用以改善光透過率與電導率之以 5000 A以下之厚度之薄膜形態添加或摻雜有助於電導率 之雜質之n-/p-摻雜構造之開發。特別是，於後者之開發方 向上，報告有對用以改善電導率之雜質及摻雜有雜質之 AZO(ZnO:Al)、GZO(ZnO:Ga)、IZO(ZnO:In)薄膜之研究結 果。若具體地觀察研究開發結果’則首先於電子開發方向 上’在 Sung Jin An 'Near ultraviolet light emitting diode composed of n-GaN/ZnO coaxial nanoroad heterostructures on a p-GaN layer', Applied Physics Letters 91,123109(2007). Xiao-Mei Zhang 等'Fabrication of a High-Brightness Blue-Light-Emitting Diode Using a ZnO-Nanowire Array Grown on p-GaN Thin Film', Advanced Materials.Vol.21，pp.2767-2770(2009)’論文等中報告有 ZnO 奈米柱、奈米線。然而，評價如下：ZnO形態之變更係可 容易地實現，但決定電導率之電阻值相對而言非常高，故 發光裝置之動作電壓具有非常高之極限。於後者之開發方 向上，在 K. Nakahara 'Two different features of ZnO:S 201232824 4U5J4plt Therefore, the realization of the light-emitting device is difficult. In order to improve such a problem, IT〇(In2〇3: Sn), which has a relatively low light transmittance and low contact resistance, replaces Ni/Au anti-transmissive metal as a transparent electrode, and is widely used in a formal amount after 2〇〇2 years. The mobile end%, 苇δ-type computer, pC (personai c〇mpUter, personal computer), display device, LCD (LiqUid Crystal Display), TV (Television) backlight unit, lighting products, and the like. By using IT〇 as a transparent electrode, the technological advancement of the light output of the light-emitting device is increased by about 3%. The TO transparent electrode layer (Η?) can be deposited by a device related to sputtering (SpUtterjng deposition) and electron beam evaporation (e_beam evap〇rati〇n), and the light transmittance is 85% or more, and the contact resistance is The order of 1 〇·5 ohm.cm has crystallinity of amorphous or polycrystalline having a conductivity of ~, and after deposition, a subsequent heat treatment step is necessary in order to restore crystallinity. By the crystal structure of polycrystal, it is easier to flow from the vertical direction of the second electrode contact layer (115) to the vertical direction of the active layer (109), but relative to the lateral direction 〇ateraldirecti〇 The current flow of n) is very small compared to the flow in the vertical direction, and therefore is required to improve the situation. Further, the research and development of the performance improvement of the ITO material itself used as the transparent electrode of the light-emitting device was continuously performed, but the result was in an unfinished state. Recently, compared with the research on the IT0 substance itself, the performance of the illuminating device has been improved by the development of the patterning or texturing step technology of the ιτο transparent electrode, but the current situation is that the operating voltage is increased, so that the actual Can not be applied to mass production products. In addition, the amount of indium (In) constituting the ITO substance is extremely limited, so there is a very high output of 201232824 40534pif, and in particular, the tendency of the rare source of rare elements has become hotter and the degree has become increasingly severe. Change the cover] =: The performance cost of the nitride-repented illuminating device must be replaced by the urgent need to replace the existing 1το substance in order to satisfy the smart phone (_ = type, heart display, LCD backlight unit or lighting product f 'urgently A light-emitting device that requires more than 5G% of light efficiency and is highly efficient. The current situation is due to the technical limitations of the wafer growth technology and the chip step, and the demand for the insect growth of the A1InGaN semiconductor light-emitting device is not satisfied. It is extremely costly to invest in research and development to improve internal quantum efficiency by more than 5%, but in an unfinished state. In addition, in order to overcome the technical limits of the technology of wafer growth, chip-step technology The development of the performance of the illuminating device has been carried out, but no remarkable results have been found. In order to overcome this technical difficulty, the research and development of the Zn0 transparent electrode has recently been actively carried out, and the ZnO transparent electrode is used as a substitute for A1InGaN. A substance of an ITO material of a transparent electrode of a nitride semiconductor light-emitting device. It can be used as a transparent electrode of a light-emitting device. The Zn0 film has an excellent light transmittance of 85% or more, and has the same hexagonal crystal structure as the AlInGaN nitride semiconductor light-emitting device, and has excellent thermal stability and can be effectively applied to large-area/high-output light emission. The device has the advantages of easier refractive index and energy bandgap adjustment. In addition, in the case of a ZnO thin film, it is easy to form a columnar microstructure in the crystal growth direction ( Columnar 201232824 4U534pit' microstmcture). Moreover, in the case of Zn〇 film, the indium (In) word (Zn) which is far richer than the existing ITO transparent electrode is used, so that it can achieve low mussels smoothly. The supply of a stable raw material is formed on the ρ-GaN layer as the second electrode contact layer and has the same hexagonal crystal structure as the p-GaN layer in the case of replacing the Zn 〇 material of the previous ITO transparent electrode. And the apparatus and technology used for deposition can be applied in the same manner, and therefore has the advantage that the crystallinity of high quality can be easily obtained. In the Zn〇 substance, the light transmittance can be It is higher than 90% by a higher refractive index, a lower absorption coefficient, etc., and light which is emitted from the InGaN/InGaN or InGaN/GaN active layer toward the surface direction by a change in the formation structure. The escape angle changes to improve the transmission efficiency of the illuminating device. In the case of the illuminating device, in terms of illuminating, it is necessary to satisfy the resistance design technique together with the higher light transmittance. Substantially applied to mass production, the resistor design technique is to increase the recombination efficiency of electrons and holes on the active layer, and minimize the contact resistance with the p_/n_ electrode, so that even if a lower voltage is applied, the internal quantum Efficiency can also be maximized. In order to form a ZnO transparent electrode, research and development have been carried out in the following directions: the growth direction of the amorphous and polycrystalline structures containing the additive by the sputtering method and the electron beam evaporation method; and the use of the molecular beam telecrystal method ( The single crystal structure doped with impurities of MBE 'molecular beam epitaxy), metal organic chemical vapor deposition (MOCVD) or pulsed laser deposition (PLD 'pulse laser deposition) is grown in the direction of growth. With the above growth method, higher transmittance characteristics can be easily obtained by the change of the material or structure of Zn〇201232824 40534pif, but the result of having higher conductivity due to lower contact resistance has not been obtained so far. . The development direction of ZnO transparent electrodes can be broadly divided into the following developments: development of nano-pillars and nanowires for improving light transmittance; and to improve light transmittance. The development of an n-/p-doped structure that contributes to impurities of conductivity is added or doped with a film having a thickness of 5000 A or less. In particular, in the development direction of the latter, research results on AZO (ZnO:Al), GZO(ZnO:Ga), and IZO(ZnO:In) thin films for impurities and impurities doped with impurities have been reported. . If the research and development results are specifically observed, then first in the direction of electronic development, 'Sung Jin An 'Near ultraviolet light emitting diode composed of n-GaN/ZnO coaxial nanoroad heterostructures on a p-GaN layer', Applied Physics Letters 91, 123109 (2007). Xiao-Mei Zhang et al. 'Fabrication of a High-Brightness Blue-Light-Emitting Diode Using a ZnO-Nanowire Array Grown on p-GaN Thin Film', Advanced Materials. Vol. 21, pp. 2767-2770 ( 2009) 'The paper has reported ZnO nano columns and nanowires. However, the evaluation is as follows: the change in the morphology of ZnO can be easily realized, but the resistance value for determining the conductivity is relatively high, so that the operating voltage of the light-emitting device has a very high limit. In the latter development, at K. Nakahara 'Two different features of ZnO:

transparent ZnO:Ga electrode for InGaN-LED and homoepitaxial ZnO films for UV-LEDs.' Zinc Oxide Materials and Devices, Proc. Of SPIE 12Transparent ZnO: Ga electrode for InGaN-LED and homoepitaxial ZnO films for UV-LEDs.' Zinc Oxide Materials and Devices, Proc. Of SPIE 12

201232824 4U3J4piI201232824 4U3J4piI

Vol.6122，pp61220N(2006)論文中’報告有如下之發光裝 置，即，於利用分子束磊晶法(ΜΒΕ)成長Ζη〇薄膜之過程 中’使用摻雜鎵(Ga)作為摻雜源而具有η_型電導率之 GZO(ZnO:Ga)/p-GaN層透明電極，從而具有8〇%以上之光 透過率者’但未能提出對各種製品所要求之較低之動作電 壓之條件。另外，於 Gary S. Tompa ’Large Area Multi_\Vafef MOCVD of Transparent and Conducting ZnO Fils', Mater. Res· Soc. Symp. V〇1.957(2007)論文中，報告有如下之發光 裝置，即，於利用有機金屬化學氣相沉積法(M〇CVD)成長 ZnO薄膜之過程中，使用摻雜鋁(A1)作為摻雜源而具有〜 型電導率之ΑΖΟ(ΖηΟ:Α1)透明電極，從而為80%以上之光 透過率，且較ΙΤΟ透明電極改善1〇%以上者，但評價為動 作電壓相對較高。 ' 通常’使用Β、Α卜Ca、In等III族元素與F、Cl、Η 等作為具有η_型電導率之Ζη〇薄膜之摻雜源，從而可容易 地形成η-型ZnO薄膜。使用p、As、Ν、C、Li、F、Na 等作為具有P-型電導率之ZnO薄膜之摻雜源，但於形成 Zn〇薄膜時’藉由氧空位(vacancy)、本質缺陷(natiVe defect) 及自動補償(selfcompensation)效果，產生無助於電導率之 非發光缺陷中心(nonradiative defect center)而具有η-型 ZnO特性，因此非常難以形成卜型Ζη〇薄膜。為了解決此 種問題點，最近提出有對Ga-N、F-Ni、Ga-C、Ga-H等η-里型雜質摻雜源之同時摻雜(co-doped)技術，而積極進 打對具有較高之電洞載子之p-型ZnO薄膜之研究，但迄今 13 201232824 40534pif 為止無表示令人滿意之結果之報告。具體而言，於 US6,291，〇85之情形時，利用脈衝雷射沉積法(pld)使 As-doped p-ZnO薄膜形成於n_GaAs基板上，從而獲得電 洞之摻雜濃度、移動率及比電阻分別為l〇i5/cm3、1〜5〇 cm2/Vsec及1 ohm.cm之電特性，但係關於利用p_型zn〇 單晶薄膜而並非透明電極之n/p_接面ZnO發光裝置者。於 US6,458,673之情形時’利用脈衝雷射沉積法(此⑼吏H_Ga co-doped n-GaN薄膜形成於玻璃(glass)基板上，從而提出 較而之光透過率及較高之電子濃度，但未能提出發光裝置 之透明電極之開發。於US6,527,858中，提出利用分子束 磊晶法(MBE)而藉由N-Ga(CIn)co-doped具有低電阻之p_ 型ZnO單晶薄膜，但係關於並非透明電極之應用之p/n_ 接面ZnQ發S裝置者，❿未揭^^作為電極而提高光 透過率與電導率之發光裝置之内容。於US6,896,731之情 形時，利用分子束蟲晶法_E)使進行F-Ga cooped及作 為追加對Mg、Be元素進行2次摻雜而具有低電阻之p_型 Zn〇單晶薄膜成長’從而欲應用於p/n接面Zn〇發光裝 置’但作為㈣電極未揭轉實際光妓率及電導率之内Vol. 6122, pp61220N (2006), 'Reporting the following illuminating device, that is, using a doped gallium (Ga) as a doping source in the process of growing a Ζη〇 film by molecular beam epitaxy (ΜΒΕ) A GZO (ZnO:Ga)/p-GaN layer transparent electrode having η_type conductivity, thereby having a light transmittance of 8 〇 or more, but failing to propose a lower operating voltage condition required for various products . In addition, in the paper of Gary S. Tompa 'Large Area Multi_\Vafef MOCVD of Transparent and Conducting ZnO Fils', Mater. Res. Soc. Symp. V〇 1.957 (2007), the following illuminating device is reported, that is, utilized In the process of growing a ZnO thin film by organometallic chemical vapor deposition (M〇CVD), a doped aluminum (A1) is used as a doping source and has a ~-type conductivity (ΑΖΟηΟ:Α1) transparent electrode, thereby being 80%. The above light transmittance is improved by 1% or more compared with the transparent electrode, but it is evaluated that the operating voltage is relatively high. A group of elements such as lanthanum, lanthanum, Ca, and the like, and F, Cl, lanthanum or the like are used as a dopant source of the Ζη〇 film having η-type conductivity, so that the η-type ZnO thin film can be easily formed. Use p, As, yttrium, C, Li, F, Na, etc. as the doping source of ZnO thin film with P-type conductivity, but when forming Zn 〇 thin film 'by vacancy, essential defect (natiVe The defect and the selfcompensation effect have a non-radiative defect center which does not contribute to the conductivity and have η-type ZnO characteristics, so that it is very difficult to form a Ζ-type 〇 〇 film. In order to solve such a problem, a co-doped technique of η-type impurity doping sources such as Ga-N, F-Ni, Ga-C, and Ga-H has recently been proposed, and actively For the study of p-type ZnO thin films with higher hole carriers, no report of satisfactory results has been reported so far until 13 201232824 40534pif. Specifically, in the case of US Pat. No. 6,291, 〇85, an As-doped p-ZnO thin film is formed on an n-GaAs substrate by pulsed laser deposition (pld) to obtain a doping concentration and a mobility of the hole and The specific resistances are electrical characteristics of l〇i5/cm3, 1~5〇cm2/Vsec, and 1 ohm.cm, respectively, but are related to n/p_ junction ZnO which is not a transparent electrode using a p_type zn〇 single crystal film. Light-emitting device. In the case of US 6,458,673 'by pulsed laser deposition (this (9) 吏H_Ga co-doped n-GaN film is formed on a glass substrate to provide a light transmittance and a higher electron concentration, However, the development of a transparent electrode for a light-emitting device has not been proposed. In US Pat. No. 6,527,858, a p-type ZnO single crystal film having low resistance by N-Ga(CIn)co-doped is proposed by molecular beam epitaxy (MBE). However, for the application of the p/n_ junction ZnQ S device which is not a transparent electrode application, the illuminating device which improves the light transmittance and the conductivity as an electrode is not disclosed. In the case of US 6,896,731, By using the molecular beam crystallization method _E), the F-Ga cooped and the p_ type Zn〇 single crystal film having a low resistance doped twice with the Mg and Be elements are grown to be applied to p/n. Junction Zn〇 light-emitting device 'but as (four) electrode is not exposed within the actual optical transmittance and conductivity

發衫署^ _Ll共„推雜P-Zn〇單晶，而關於P/n_接面ZnO ί實際光透膜層Ϊ，但作為透明電極未揭示 Θ貝丨不7L逐過年及電導率之内容。 【發明内容】 201232824 為了克服上述問題點，本發明之目的在於提供一種同 日轉雜如Ga之n_型雜質與如As之卜型雜質而同時具有較 面之光透過率與織的電導率之翻賴、特暇Zn〇薄 膜、包含該薄膜之發光裝置及其製備方法。 本發明之另—目的在於提供—種製備高效之發光裳 置之方法，該發光裝置係利用分子束遙晶法_E)同時換 之:型雜質與如As>型雜質而使透明薄膜、特 別疋Zn⑽膜成長，藉此不僅可應用於大量量產，而且星 有較高之光透過率、較低之動作電壓及高可靠性。八 j明之又-目的在於提供—種製備高效之發光裝 fvt ’、Ϊ發光裝置係湘有機金屬化學氣相沉積法 )、原子層沉積法(ALD)、原子層磊晶法(ALE， a:=:r epitaxy)中之至少一者’同時摻雜如Ga之… ^AS Ο型㈣而使透明薄膜、特別是Zn0薄 Π，錯此不僅可應用於量產，而且具有較高之光透過 率、較低之動作電壓及高可靠性。 為了達成上述目的，根據本發明之一形離， 括·其:1^=卜09 + %1)之組成式者，其特徵在於包 声，衝層’其形成於上述基板上；第1電極接觸 ^二:上述緩衝層上；第1包覆層，其形成於上述 第2 ;活性層，其形成於上述第1包覆層上； C 形成於上述活性層上；第2電極接觸層， 、少：上述第2包覆層上：㈤薄膜之透明電極，其形 15 201232824 40534pif 成於上述第2電極接觸層上，且同時換 Ga、In之III族元素與F、α、H構二有選自由B、A1、 η-型雜質、與選自由.卜&,之^群中之至少-個 C構成之群t之至少一個㈣雜質 於上述第1電極接觸層之上部一側 ，極墊，其形成 成於上述透明電極之上部-側；且同時換雜電極墊，其形 質與上述P-型雜質中，上述n•型雜質為使== 型雜 主要，因，上述p_型雜質為使光特性變之^子之 …較理想之實施例之特徵在於，上述1型1原因： 上述p-型雜質為As。另外，特徵在於上明電跡a 子束蟲晶法_E)形成。另外，特，月f亟错由分 由有機金μ學氣相㈣法^^^；4^電^ (ALD)及原子層蟲晶法(ALE)中之任一者形子層/儿積法 根據本發明之另-形態，可提供—種氮化物半導體 先裝置製備方法，其係製備具有Α1χΙηρυ(〇^ 卜OSyShOSx + ygl)之組成式之氮化物半導體發光裝 置之方法，其特徵在於包括如下步驟：提供基板之步驟； 於上述基板上，形成緩衝層之步驟；於上述緩衝層上，形 成第1電極接觸層之步驟；於上述第丨電極接觸^上，^ 成第1包覆層之步驟；於上述第i包覆層上，形&活性‘ 之步驟；於上述活性層上，形成第2包覆層之步驟；於丄 述第2包覆層上，形成第2電極接觸層之步驟；於上述第 2電極接觸層上，形成ZnO薄膜之透明電極之步驟，此處 選自由B、A卜Ga、In之III族元素與F、cn、H構成之群 201232824 4U^J4pit 中之至少一個n_型雜質 元素與Li、Na、C構成之群^之=,Sb之V族 雜於上述Zn〇薄膜上;及於上述透明電時摻 二=墊2驟，時摻雜之上述鳴質—:上: •雜質中’上述n-型雜質為使電特性變良 j述 因，上述P-型雜質為使光特性變良好之主要原因。主要原 較理想之實施例之特徵在於，上述n 上述P-型雜質為AS。另外’特徵在於上述透明二G:: 子束遙晶法_)形成。另外，特徵在於上述透明 由有機金屬化學氣相沉積法(M()CVD) 、: _)及原子層線，之任一者形成。另層外;^ 本發明之另-形態之氮化物半導體發光裝置製備方法^ = =述第1電極接觸層之上部-側，形 [發明之效果] 根據本發明，可期待如下之效果。 根據本發明，可提供_種同時摻雜如⑶之〜型雜質 與如As之ρ·型雜質而_具有較高之絲過率與較高的 電導率之透明義、特別是⑽薄膜、包含該薄膜之發 裝置及其製備方法。 另外，根據本發明，可提供一種製備高效之發光裝置 之方法，該發光裝置係利用分子束磊晶法(MBE)同時摻雜 如Ga之η-型雜質與如八8之？_型雜質而成長透明薄膜、特 別是ΖηΟ薄膜，藉此不僅可應用於大量量產，而且具有較 17 201232824 40534pif 尚之光透過率、較低之動作電壓及高可靠性。 另外，根據本發明，可提供一種製備高效之發光裝置 之方法，該發光裝置係利用有機金屬化學氣相沉積法 (M〇CVD)、原子層沉積法(ALD)及原子層磊晶法(ALE)中 之任-者，同時摻雜如Ga之n_型雜質與如Asip_型雜質 '^長透明相、制是ZnC)薄膜，藉此*僅可應用於大 f里產1¾且具有較焉之光透過率、較低之動作電壓及 可靠性。 ° 另外，根據本發明，將以埋藏量較IT0物質之鋼 相對豐富而可改善製備成本之鋅(Ζη)為基礎而同時摻雜如 ^之，⑨雜質與如^之卩·型雜質之a。薄膜用作透明電 ^ =可提供—種可將轉效益極尬之透明薄膜、包 含_膜之發光襄置及其製備方法。 另外’根據本發明，可提供—鮮限定於發光 =用於可代替先前之1το物質之觸控板、有機EL(electro 、太陽電池(論，#各種應用 貝域之翻電極及其製備方法。 【實施方式】 施二說:照=圖明之較理想之實 便標示於符號時’對相同之構成要素而言，即 外，於對本^式上亦儘可能地使具有相同之符號。另 、、X進行_時’在麟為對相關之公知構成 18 S. 201232824 40534pit 或功能之具體說明可混淆本發明之主旨時’省略其詳細之 說明。 本發明係關於一種同時摻雜(co-doped)如Ga之η-型雜 質與如As之ρ·型雜質之透明薄膜、包含該薄膜之發光裝 置及其製備方法。為了便於說明，本發明之同時摻雜有如 Ga之η-型雜質與如As之？_型雜質之透明薄膜設為zn〇 薄膜，但並不限定於此。另外，為了便於說明，本發明之 發光裝置設為氮化物半導體發光裝置、特別是具有 AlxInyGa(1-x-y)N(〇Sx$l、OSygl、OSx + ygi)之組成 式之氮化物半導體發光裝置，但並不限定於此。另外，為 了便於說明’本發明之透明薄膜設為利用分子束磊晶法 (MBE)而形成者’但並不限定於此，較理想的是，利用有 機金屬化學氣相沉積法(M0CVD)、原子層沉積法(ALD)及 原子層磊晶法(ALE)中之至少一者形成透明薄膜之方面亦 包含於本發明之技術範圍内。以下，為了便於對本發明之 说明，同時摻雜有如Ga之η-型雜質與如As之p-型雜質之 透明薄膜為ZnO薄膜，發光裝置為具有AixInyGa(i x_y)N(〇The hairdressing agency ^ _Ll „ 推 P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P P SUMMARY OF THE INVENTION 201232824 In order to overcome the above problems, an object of the present invention is to provide an n-type impurity of the same day as Ga and an impurity such as As, while having a relatively high light transmittance and a woven conductance. Rate responsive, special Zn 〇 film, illuminating device comprising the film and preparation method thereof. Another object of the present invention is to provide a method for preparing a highly efficient luminescent device, which utilizes molecular beam remote crystal At the same time, the method _E) is replaced with a type of impurity and an impurity such as As> to grow a transparent film, particularly a 疋 Zn(10) film, thereby not only being applied to mass production, but also having a high light transmittance and a low operating voltage. And high reliability. Eight J Mingzhi - the purpose is to provide a kind of high-efficiency luminescent installation fvt ', Ϊ 装置 系 系 有机 有机 organic metal chemical vapor deposition method), atomic layer deposition (ALD), atomic layer epitaxy (ALE, a:=:r epitaxy) to One is 'doping at the same time as Ga... ^AS Ο type (4) makes transparent film, especially Zn0 thin, which is not only applicable to mass production, but also has high light transmittance, low operating voltage and high reliability. In order to achieve the above object, according to one aspect of the present invention, the composition of the formula: 1^=Bu 09 + %1) is characterized by a sound of a package, which is formed on the substrate; a first electrode layer formed on the first cladding layer; C formed on the active layer; Layer, and less: on the second cladding layer: (5) transparent electrode of the film, the shape 15 201232824 40534pif is formed on the second electrode contact layer, and at the same time, the elements of the group III of Ga and In are replaced with F, α, H The second structure has at least one (four) impurity selected from the group consisting of B, A1, and η-type impurities and at least one C selected from the group consisting of a group of <>, and the impurity is on the upper portion of the first electrode contact layer. a side pad, which is formed on the upper side of the transparent electrode; and at the same time, the electrode pad is replaced, and its shape is In the above P-type impurity, the n-type impurity is mainly caused by == type impurity, and the p-type impurity is a component which changes optical characteristics. A preferred embodiment is characterized in that the type 1 is Cause: The above-mentioned p-type impurity is As. In addition, it is characterized by the formation of the a-beam ion crystal method _E). In addition, the special value of the moon is determined by the organic gold μ gas phase (four) method ^^ a method for preparing a nitride semiconductor device according to another aspect of the present invention, which is a method for preparing a nitride semiconductor device, A method for preparing a nitride semiconductor light-emitting device having a composition formula of Α1χΙηρυ (〇^ OS OS OS OS Sh OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS OS a step of forming a first electrode contact layer on the buffer layer; a step of forming a first cladding layer on the second electrode contact; and a step of forming a & activity on the ith cladding layer; a step of forming a second cladding layer on the active layer; and forming a second layer on the second cladding layer a step of forming a contact layer; a step of forming a transparent electrode of a ZnO thin film on the second electrode contact layer, wherein the group consisting of a group III element of B, A, Ga, In, and F, cn, H is 201232824 4U ^J4pit at least one of the n-type impurity elements and the group consisting of Li, Na, and C =, the V group of Sb is mixed with the Zn 〇 film; and when the transparent electricity is mixed with the second = pad 2, The above-mentioned sound quality of doping:: Upper: • In the impurity, the above-mentioned n-type impurity is a factor for improving the electrical characteristics, and the P-type impurity is a factor for improving the optical characteristics. A principally preferred embodiment is characterized in that the above-mentioned P-type impurity is AS. Further, the feature is formed by the above-described transparent two G:: beamlet crystal method. Further, it is characterized in that the above transparency is formed by any one of an organometallic chemical vapor deposition method (M() CVD), : _) and an atomic layer line. In addition, the method of preparing a nitride semiconductor light-emitting device of another aspect of the present invention is as follows: [Effect of the invention] According to the present invention, the following effects can be expected. According to the present invention, it is possible to provide a transparent type, such as a (3) film, including a (3)-type impurity and a ρ-type impurity such as As, having a higher silk pass rate and a higher electrical conductivity. The film hair device and the preparation method thereof. Further, according to the present invention, there can be provided a method of producing a highly efficient light-emitting device which is simultaneously doped with a η-type impurity such as Ga by a molecular beam epitaxy method (MBE) and such as 八八? The _-type impurity grows a transparent film, in particular, a ΖηΟ film, which is not only applicable to mass production, but also has a light transmittance, a lower operating voltage and a high reliability than the 17 201232824 40534pif. In addition, according to the present invention, there can be provided a method for preparing a highly efficient light-emitting device which utilizes organometallic chemical vapor deposition (M〇CVD), atomic layer deposition (ALD) and atomic layer epitaxy (ALE). In the middle of the process, the n-type impurity such as Ga is doped simultaneously with a thin transparent phase such as Asip_type impurity, which is a ZnC film, whereby * can only be applied to large-scale production and has a ratio of 13⁄4 Light transmittance, low operating voltage and reliability. In addition, according to the present invention, the zinc (Ζη) which is relatively rich in burial amount compared with the material of the IT0 substance can be simultaneously doped with zinc (Ζη), and 9 impurities and a kind of impurity such as . The film is used as a transparent electric ^ = a transparent film capable of transferring the benefits, a luminescent film containing the film, and a preparation method thereof. In addition, according to the present invention, it can be provided that it is rarely limited to luminescence = a touch panel which can replace the previous 1 τ substance, an organic EL (electro ray, a solar cell, and a preparation method thereof). [Embodiment] Shi 2 said: If the ideal reality is shown in the figure, the same symbol is used for the same component, that is, the same symbol is used as much as possible. When X is performed _ when 'Lin is a well-known composition 18 S. 201232824 40534pit or a detailed description of the function may confuse the subject matter of the present invention. The detailed description is omitted. The present invention relates to a simultaneous doping (co-doped). a transparent film such as Ga η-type impurity and ρ· type impurity such as As, a light-emitting device comprising the film, and a preparation method thereof. For convenience of explanation, the present invention is doped with an η-type impurity such as Ga and The transparent film of As-type impurity is a zn〇 film, but is not limited thereto. For convenience of explanation, the light-emitting device of the present invention is a nitride semiconductor light-emitting device, particularly having AlxInyGa(1-xy). N (〇Sx The nitride semiconductor light-emitting device of the composition formula of $1, OSygl, OSx + ygi) is not limited thereto. For the sake of convenience, the transparent film of the present invention is formed by molecular beam epitaxy (MBE). 'But' is not limited thereto, and it is preferable to form a transparent film by at least one of organometallic chemical vapor deposition (M0CVD), atomic layer deposition (ALD), and atomic layer epitaxy (ALE). The aspect is also included in the technical scope of the present invention. Hereinafter, in order to facilitate the description of the present invention, a transparent film doped with an η-type impurity such as Ga and a p-type impurity such as As is a ZnO thin film, and the light-emitting device has AixInyGa(i x_y)N(〇

SxSl、〇^ygl、〇gx + y^丨)之組成式之氮化物半導體 發光裝置（以下，稱為AlInGaN系氮化物半導體發光裝 置）’且設為利用分子束磊晶法(MBE)形成Zn〇薄膜。 另外，為了便於對本發明之說明，同時摻雜於透明薄 膜、特別是ZnO薄膜之η-型雜質與p_型雜質主要設為Qa 與As，但並不限定於此，較理想的是，〜型雜質為選自由 B、Al、Ga、In之m族元素與F、α、η構成之群中之至 201232824 40534pif 少一個，p_型雜質為選自由N、P、As、Sb之v族元素與 Li、Na、C構成之群中之至少一個之方面亦包含於本發明 之技術範圍内。 用以形成本發明之同時摻雜(co-doped)Ga與As之 ZnO薄膜(以下’稱為ZGA0(Zn0:Ga_As)薄膜或ZGA〇單 晶溥膜)之分子束蟲晶設備（以下，稱為MBE設備)較大地 區分為裝料室、處理室及成長室。特別是，Zn〇薄臈、較 理想的是ZnO單晶薄膜之成長室為了維持丨〇-9 t〇rr之超高 真空及最大限度地去除污染成分之潔淨之成長環境，各個 空間由閘閥(gate valve)分離。圖2是概略性地表示用作本 發明之較理想之實施例之AlInGaN系氮化物半導體發光裝 置的透明電極之ZGAO薄膜之形成過程之順序圖。參照圖 2，用以形成用作本發明之A1InGaN系氮化物半導體發光 裝置之透明電極之ZGAO薄膜的MBE設備係1〇·9 torr以 下之超高真空設置，具有於非常潔淨之環境下，使膜按照 原子級別而非常精緻地成長之優點。製備本發明之ZGA〇 薄膜及採用該薄膜之AlInGaN系氮化物半導體發光裝置之 γΒΕ設備於高真空之成長環境下，使用高純度、較理想的 士 99.999%以上之入卜In、Ga、Zn、As、Sb金屬旋劑㈣㈣， 疋位有收納各金屬源之炼爐與加熱器(heater)，且由對流量 進行控制之獨立之個個單元（cell)構成。利用RF(radi〇 frequency，射頻）電漿使高純度、較理想的是99 9999%以 上之氧(〇2)解離而用作氣體源。為了提高本發明之ZGa〇 薄膜、較理想的是ZGAO單晶薄膜之結晶性，較理想的是 t 201232824 4uyj4pit 加熱基板。如上料，作為同時_MZn◦薄臈之 質較理想的是Ga，但可為選自由B、A卜Ga、In之Ιπ族 成之群中之至少一個，作為ρ-型雜質 車乂里心的疋As，但可為選自由N、p、As、Sb 與^，、0構成之群中之至少—個。 私兀素 包，作為形成有本發明之ZGAO薄膜、較理想的是 =GAO單晶_之對象物之基板的發光構造物設為^有較 『之電阻雜、與於表面上不活化成作域子之電洞而殘 邊之Mg、Mg-H錯合體、過剩(excess)Mg等不穩定之六邊 形構造之Mg-doped p-GaN薄膜，但並不限定於此。於本 發明之ZGAG _、較理想的是ZGA〇單晶_之成長方 法中’首先具有AlInGaN錢㈣半導歸光裝置構造之 包含基板之發光構造物於升溫至適當之熱處理溫度後，降 溫至用以形成本發明之ZGA〇薄膜、較理想的是zga〇單 晶薄膜之溫度(步驟2G1)。母縣板之鱗理溫度較理相的 是約為5(KTC〜7G(TC之範圍。為了最佳之流量控制，^包 含基板之發㈣造物之熱處理過程同時，將定位有Α^、 =Mg、Zn、As源之各單元之溫度維持為最佳 度條件(步驟施）。於各單μ，最佳 驗0_、_想的是ZGAG單晶_之成長條件而不康 同，且可根據放置於各早疋内之材料之量與構造而不同。 例如，與Zn材料相應之單元之溫度較佳為約·。〇〜㈣ °C之範圍，與Ga材料相應之單元溫度較佳為約獅。卜 麵C之犯圍’與As材料相應之單元溫度較佳為約载 21 201232824 40534pif 〜400°C之範圍’且可於此種範圍内設定各單元之最佳之流 量條件。於本發明所屬之技術領域内具有常識者應當瞭 解，上述各單元之較佳之溫度範圍僅為一實施例，可根據 设備規格進行各種變更。 於藉由步驟201及203而已準備最佳之成長環境之狀 態下’對包含基板之發光構造物確定最佳成長溫度，並於 最佳成長溫度得以確定後，旋轉基板(步驟2〇5)。此後，相 對於包含旋轉之基板之發光構造物，與步驟過程相應地開 放已準備各個材料之單元之擋閘（步驟207)。於步驟2〇7 中，能夠以與步驟過程相應之方式，進一步供給藉由利用 RF電漿對氧(〇2)進行解離而獲得之氧源。以 應之方式開放各單元之擔問而收納於單元内之二= 發到，包含基板之發光構造物，且以與步驟過程相應之方 式進一步供給氧，從而本發明之ZGAO _、較理^ 晶薄购勻地絲，藉此形朗時摻雜有作為n- 之型摻雜源之AS，並且具有因較高 (而步::9)。於上述步驟過程中，大部分之ζί;;: 而形成氧化鋅(ζηο)之單晶薄膜。 乳紙 於氧之情形時，通常以分子狀態存在， 發明之步驟，受到解離而 -马了進仃本 产之=可 ZGA0單晶薄臈之形成，則關閉各單元之擋閘A nitride semiconductor light-emitting device (hereinafter referred to as an AlInGaN-based nitride semiconductor light-emitting device) of a composition formula of SxS1, 〇^ygl, 〇gx + y^丨) is formed by molecular beam epitaxy (MBE) to form Zn 〇 film. Further, in order to facilitate the description of the present invention, the n-type impurity and the p-type impurity doped in the transparent film, particularly the ZnO thin film, are mainly set to Qa and As, but are not limited thereto, and it is preferable that ~ The type impurity is one selected from the group consisting of B, Al, Ga, In and the group of F, α, η to 201232824 40534pif, and the p_ type impurity is selected from the group V of N, P, As, Sb. Aspects of at least one of the elements and the group consisting of Li, Na, and C are also included in the technical scope of the present invention. A molecular beam crystal device for forming a ZnO thin film of a co-doped Ga and As (hereinafter referred to as a ZGA0 (Zn0:Ga_As) thin film or a ZGA〇 single crystal germanium film) (hereinafter, referred to as For MBE equipment, the larger area is divided into charging room, processing room and growth room. In particular, Zn 〇 thin 臈, ideally, the growth chamber of the ZnO single crystal thin film in order to maintain the ultra-high vacuum of 丨〇-9 t〇rr and to clean the clean environment of the pollution components to the maximum extent, each space is controlled by a gate valve ( Gate valve) separation. Fig. 2 is a sequence diagram schematically showing a process of forming a ZGAO thin film which is used as a transparent electrode of an AlInGaN-based nitride semiconductor light-emitting device which is a preferred embodiment of the present invention. Referring to Fig. 2, an MBE apparatus for forming a ZGAO thin film which is used as a transparent electrode of an A1InGaN-based nitride semiconductor light-emitting device of the present invention has an ultra-high vacuum setting of 1 〇·9 torr or less, and is provided in a very clean environment. The film grows very delicately at the atomic level. The ZGA(R) film of the present invention and the γΒΕ device of the AlInGaN-based nitride semiconductor light-emitting device using the film are used in a high-vacuum growth environment, and a high-purity, more desirable 99.999% or more of In, Ga, Zn, As, Sb metal spinning agent (4) (4), the furnace has a furnace and a heater for accommodating each metal source, and is composed of independent cells that control the flow rate. High-purity, ideally, 99 9999% or more oxygen (〇2) is used as a gas source by using RF (radiation frequency) plasma. In order to improve the crystallinity of the ZGa 薄膜 film of the present invention, preferably a ZGAO single crystal film, it is preferable to heat the substrate by t 201232824 4uyj4pit. As described above, it is preferable that Ga is preferable as the mass of the simultaneous _MZn ◦ thin 臈, but may be at least one selected from the group consisting of B, A, Ga, and In Ι π, as a ρ-type impurity rut疋As, but may be at least one selected from the group consisting of N, p, As, Sb and ^, and 0. The luminescent material of the substrate of the ZGAO film of the present invention, which is preferably a target of the GAO single crystal, is set to have a resistance impurity and is not activated on the surface. The Mg-doped p-GaN thin film having an unstable hexagonal structure such as Mg, Mg-H, or excess Mg in the region of the hole is not limited thereto. In the ZGAG _, preferably ZGA 〇 single crystal _ growth method of the present invention, the luminescent structure including the substrate having the AlInGaN carbon (four) semi-conductor device structure is first cooled to a suitable heat treatment temperature, and then cooled to The ZGA(R) film used in the present invention is preferably a temperature of the zga(R) single crystal film (step 2G1). The temperature of the maternal plate is about 5 (KTC ~ 7G (the range of TC. For the best flow control, ^ the substrate containing the hair (four) the heat treatment process of the creation, at the same time, will be positioned Α ^, = The temperature of each unit of the source of Mg, Zn, and As is maintained at the optimum condition (step application). For each single μ, the best test 0_, _ thinks the growth condition of ZGAG single crystal _ is not the same, and can Depending on the amount and structure of the materials placed in each of the early crucibles, for example, the temperature of the unit corresponding to the Zn material is preferably about 〇 ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( About the lion. The surface temperature corresponding to the As material is preferably about 21 201232824 40534pif ~ 400 °C range and the optimal flow conditions for each unit can be set within this range. It should be understood by those skilled in the art to which the present invention pertains that the preferred temperature range of each of the above units is only one embodiment, and various modifications can be made according to the device specifications. The optimal growth environment is prepared by steps 201 and 203. In the state of the 'light-emitting structure containing the substrate After the optimum growth temperature is determined and the optimum growth temperature is determined, the substrate is rotated (step 2〇5). Thereafter, the unit in which the respective materials have been prepared is opened corresponding to the step of the step with respect to the light-emitting structure including the rotating substrate. Blocking (step 207). In step 2〇7, the oxygen source obtained by dissociating oxygen (〇2) by RF plasma can be further supplied in a manner corresponding to the step process. The second unit stored in the unit is included in the unit, and includes the light-emitting structure of the substrate, and further supplies oxygen in a manner corresponding to the step, so that the ZGAO _ of the present invention is relatively thin. The wire, by which the shape is doped with AS as a doping source of n- type, and has a higher (step::9). During the above steps, most of the ζ; A single crystal film of zinc (ζηο). When the paper is in the case of oxygen, it usually exists in a molecular state, and the steps of the invention are dissociated - the horse is introduced into the product, and the ZGA0 single crystal is formed. Block of each unit

S 22 201232824 4υ534ρι1 例之表示_有本發明之較理想之一實施 明之較;?圖:r略性地表示利用綱 氣化物主：ί 例之包含ZGA0薄臈的A1InGaN系 4 θ 之發絲置之積層構造之剖面圖。圖3及圖 日1胺、4歹4生地對本發明之ZGA〇薄膜（包括ZGAO單 發域置、_是湘有AUnGaN系氮化 ^導體之發光裝置之㈣進行綱者，本發明之技術範 ^可限定於此而解釋。圖3及圖4所示之利用有秦⑽ 系亂化物半導體之發光裝置包括“發光二《(Emitting Light D1〇de，LED)” 及“雷射器二極體(User Di〇de， LD)。於圖3及圖4所示之利用有本發明之AiInGaN系 氮化物半導體之發光裝置中，對與圖1所示之先前之利用 有普通之AlInGaN系氮化物半導體之發光裝置相同之部 分，省略具體之說明。於圖3及圖4所示之利用有本發明 之AlInGaN系氮化物半導體之發光裝置中，基板(3〇1)、緩 衝層(303)、作為第1電極接觸層而發揮功能之心型氮化物 半導體層(305)、n-型氮化物包覆層(307)、活性層（309)、p_ 型氮化物包覆層(311)及p-型氮化物半導體層（313)依次積 層。於p-型氮化物半導體層(313)上，n/p-型第2電極接觸 層（315、316)可形成為具有平坦之表面之平坦型（行站 type)(圖3之315)、或具有粗糙之表面之粗糙型（r〇ugh type)。於第2電極接觸層(315、316)上，可與下部之第2 電極接觸層（315、316)之表面狀態相應地，進一步形成較 23 201232824 4U534pif 薄之 p-InGaN 層或 n+-InGaN 層、InGaN/InGaN 超晶格層、 n-InGaN/GaN超晶格層等。即，於第2電極接觸層（315)為 平坦型之情形時，可於第2電極接觸層（315)上形成平坦型 之車父薄之厚度之p-InGaN層或n+-InGaN層、InGaN/InGaN 超晶格層、n-InGaN/GaN超晶格層等，於第2電極接觸層 (316)為粗糙型之情形時，可於第2電極接觸層（316)上形成 粗縫型之較薄之厚度之p-InGaN層或n+-InGaN層、S 22 201232824 4 υ ρ ρ 例 _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ υ υ υ υ υ υ υ υ υ υ υ υ υ ; υ υ υ ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; A sectional view of the laminated structure. FIG. 3 and FIG. 1 show that the ZGA(R) film of the present invention (including the ZGAO single-emitting region, and the light-emitting device of the AU-GaN-based nitriding conductor) can be used as an outline of the present invention. ^ can be limited to this explanation. The light-emitting device using the Qin (10) system of the semiconductor semiconductor shown in FIG. 3 and FIG. 4 includes "Emitting Light D1" (LED) and "Laser Diode" (User Di〇de, LD). In the light-emitting device using the AiInGaN-based nitride semiconductor of the present invention shown in FIG. 3 and FIG. 4, the conventional AlInGaN-based nitride used in the prior art shown in FIG. In the light-emitting device using the AlInGaN-based nitride semiconductor of the present invention shown in FIGS. 3 and 4, the substrate (3〇1) and the buffer layer (303) are the same as those of the semiconductor light-emitting device. A core-type nitride semiconductor layer (305), an n-type nitride cladding layer (307), an active layer (309), a p-type nitride cladding layer (311), and a functioning as a first electrode contact layer The -type nitride semiconductor layer (313) is sequentially laminated. On the p-type nitride semiconductor layer (313), the n/p-type second electric The contact layer (315, 316) may be formed into a flat type (row type) having a flat surface (315 of Fig. 3) or a rough type having a rough surface. Contact at the second electrode On the layer (315, 316), a thin p-InGaN layer or an n+-InGaN layer, InGaN/InGaN super is formed in accordance with the surface state of the second electrode contact layer (315, 316) of the lower portion; 201232824 4U534pif A lattice layer, an n-InGaN/GaN superlattice layer, etc., that is, when the second electrode contact layer (315) is of a flat type, a flat type of the parent can be formed on the second electrode contact layer (315). a thin p-InGaN layer or an n+-InGaN layer, an InGaN/InGaN superlattice layer, an n-InGaN/GaN superlattice layer, or the like, when the second electrode contact layer (316) is rough, Forming a thin-thickness p-InGaN layer or an n+-InGaN layer of a thick slit type on the second electrode contact layer (316),

InGaN/InGaN超晶格層、n-lnGaN/GaN超晶格層等。本發 明之平坦型可藉由對Mg流量進行控制而執行。較理想的 是，本發明之基板(301)、緩衝層（3〇3)、作為第1電極接觸 層而發揮功能之型氮化物半導體層(305)、η-型氮化物包 覆層(307)、活性層(309)、ρ-型氮化物包覆層(3丨υ、ρ_型氮 化物半導體層(313)、第2電極接觸層(315、316)、形成於 第2+電極接觸層(315、316)上之較薄之厚度之p_InGaN層 或 n+-IiiGaN 層、InGaN/InGaN 超晶格層、n_InGaN/GaN 超 晶格層等利用有機金屬化學氣相沉積法(m〇cvd)而成 長，但並不限定於此。於圖3及圖4所示之本發明之發d 裝ί中:7, 1 摻雜物之雜質源為矽⑸)，摻雜總 別為10 /cm〜10 /cm左右，特別是，於與作為 極墊之第i電極墊(319)電性接觸而用作第！ f極接觸層之 η-型^化物半導體層(305)之情形時，歡換 5X10 W左右’且於2〜> 之厚度範圍内成長。用竹 P-型摻雜物之㈣源為鎂(Mg)，於活化步 敝 P腦啦執純，作為載子之制之摻賴度呈有卜 24InGaN/InGaN superlattice layer, n-lnGaN/GaN superlattice layer, and the like. The flat type of the present invention can be performed by controlling the Mg flow rate. Preferably, the substrate (301), the buffer layer (3〇3), the type nitride semiconductor layer (305) functioning as the first electrode contact layer, and the n-type nitride cladding layer (307) ), an active layer (309), a p-type nitride coating layer (3丨υ, a p-type nitride semiconductor layer (313), a second electrode contact layer (315, 316), and a contact at the 2+th electrode Thin metal thickness p_InGaN layer or n+-IiiGaN layer, InGaN/InGaN superlattice layer, n_InGaN/GaN superlattice layer, etc. on layer (315, 316) using organometallic chemical vapor deposition (m〇cvd) And growing, but not limited to this. In the present invention shown in Figures 3 and 4, the impurity source of the 7,1 dopant is 矽(5)), and the doping is always 10 /cm. ~10 /cm or so, in particular, used as the first in electrical contact with the i-th electrode pad (319) as a pole pad! In the case of the n-type semiconductor layer (305) of the f-electrode contact layer, it is changed by about 5×10 W and grows in the thickness range of 2 to >. The (4) source of the bamboo P-type dopant is magnesium (Mg), which is pure in the activation step 敝 P brain, and the blending degree of the carrier as a carrier is confusing.

201232824 4U^J4piI =:/:1左範圍。特別是’第2電極接觸層(315、 316)=為P·型電極塾之第2電極墊(321)電性接觸 nm〜500 nm之厚声銘阁如上ρ Αυ 載子之電洞濃度^化。蚊昭圖=由活化步驟使作為 ^ ^ ^ ϋ興參照圖1進行說明之先前之剎 包含;錢化物半導體的發光裝®同樣地， 二導中：Λ?明之·aN系氮化 _ 中的苐2電極接觸層(315、316)具 /下，、面·於單晶薄膜内部與表面上包含過剩 inch之減之表面。因此，為了獲得 勻之散佈與注入產生之較高之光輸 出之同放發找置，準確地掌歸光構造201232824 4U^J4piI =:/:1 left range. In particular, the 'second electrode contact layer (315, 316) = the second electrode pad (321) which is the P-type electrode 电 electrically contacts the thick sound of nm~500 nm. The hole concentration of the above ρ Αυ carrier ^ Chemical. Mosquito diagram = by the activation step, the previous brake is described as a reference to Fig. 1; the illuminating device of the cryptic semiconductor is similarly, in the second conductor: Λ?明之·aN nitriding _ The 电极2 electrode contact layer (315, 316) has/below, and the surface contains a surface of excess reduction of the inner inch and the surface of the single crystal film. Therefore, in order to obtain a uniform distribution of the light output generated by the uniform dispersion and injection, accurate palm return light structure

造古表面粗链、電特性)，藉此要求與此後形成之七 ^#^^^©^f.i^#(interface control technology) 〇 #± 參照圖3及圖4 ’如參照圖2進行說明般於上述 接觸層(315、316)上’可與第2電極接觸層(3l5、316)之 面狀態相應地形成本發明之透板、軸是z g A 透明電極(317、318)。#，較理想的是，於第2電極接觸 層⑽)為平坦型之情_，在第2電極接_( 成平坦型之ZGA0薄膜透明電極(317，圖3之情形），於第 2電極接觸層(316)為祕型之情形時，在第2電極接 (316)上’形成粗糙型之ZGA〇薄膜透明電極(318，圖*之 情形），但並不限定於此。最終，如圖3及圖4所示般形 25 201232824 40534pif 用以線結合(Wire bonding)之第i電極塾(319)與第2電極塾 (321)。如圖i所示，第2電極墊(321)亦能夠以直接連接於 第2電極接觸層(315、316)之方式形成。於本發明中，代 替用=先前之發光裝置之透明電極之ΙΤ〇物f而以形成具 有較高之光輸出與較低之動作電壓、及長期之壽命的且^ 面效/高可靠性之發綠置之透明電極之方式所要㈣The ancient surface has a thick chain and electrical characteristics. Therefore, it is required to form an interface control technology. 〇#± Refer to FIG. 3 and FIG. 4' as described with reference to FIG. The above-mentioned contact layer (315, 316) can be formed in accordance with the surface state of the second electrode contact layer (3l5, 316), and the axis of the invention is a zg A transparent electrode (317, 318). #, Preferably, the second electrode contact layer (10) is flat-type, and the second electrode is connected to the second electrode (the flat ZGA0 thin film transparent electrode (317, in the case of FIG. 3), at the second electrode When the contact layer (316) is a secret type, a rough ZGA thin film transparent electrode (318, in the case of FIG. *) is formed on the second electrode connection (316), but is not limited thereto. Finally, Figure 3 and Figure 4 show the shape of 25 201232824 40534pif for the wire bonding (i) electrode 319 (319) and the second electrode 塾 (321). As shown in Figure i, the second electrode pad (321) It can also be formed directly connected to the second electrode contact layer (315, 316). In the present invention, instead of using the object f of the transparent electrode of the previous light-emitting device, it is formed to have a higher light output and lower. The action voltage, and the long-term life and ^ surface effect / high reliability of the green transparent transparent electrode method (4)

Zn〇薄膜具有如下之優點··^藉由結晶構造與作為第 象物之發光構造物之第2電極接觸層(315、316)相同之 f薄膜’使光透過率極大化1可藉由峰型雜f之同時 捧雜，控制載子之電特性而將接觸電阻最小化，從 導率變大。本發明之Zn0薄膜之特徵在於如下方面：藉由 與作為成長之對象物之發光構造物、特別衫2電極接觸 =(315、316)之界面控制及如&之>型雜f之摻 電洞(hole)。 愚 作為本發明之透明電極之ζ_單晶薄膜即、 =於c-axis成長方向上成長為包含具有六邊形結晶構造之 =之發光構造物，特別是可成長為於第2電極接觸層 、316)上具有糊之六邊職晶構造之單晶薄膜且 可藉由最佳之摻雜控财現電阻，因 之 質與多晶質之加_減，具轉越之光透料ί = 率。包括AlInGaN錢化物半導體之發光裝置之第 接觸層(315、316)混合有作為基f物f (hQst)之如地、氮 空位(vacancy)及活化步驟後之1〇2/cm3以上之過剩The Zn 〇 film has the following advantages: The f-film which is the same as the second electrode contact layer (315, 316) which is the luminescent structure of the first object, maximizes the light transmittance by 1 At the same time, the type of impurity f is mixed, and the electrical characteristics of the carrier are controlled to minimize the contact resistance, and the conductivity is increased. The Zn0 film of the present invention is characterized in that it is controlled by an interface with a light-emitting structure which is a target of growth, a contact of a special shirt 2 (=315, 316), and a blend of a type such as & Hole.单晶 作为 作为 作为 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶 单晶316) A single crystal film with a hexagonal crystal structure and can be controlled by the best doping, because of the addition and subtraction of the quality and polycrystal, with the light transmissive = rate. The first contact layer (315, 316) of the light-emitting device including the AlInGaN carbon semiconductor is mixed with, for example, the ground material f (hQst), the nitrogen vacancy, and the excess of 1 〇 2 /cm 3 or more after the activation step.

Mg-H錯合體等，而處於具有較高之電阻與粗社表面之Mg-H is a complex, etc., and has a high electrical resistance and a coarse surface.

26 S 201232824 的狀態。根據本發明之較理想之實施例，於在 2電極接觸層(315、316)上成長zGA〇單晶薄膜 If)時，在成長初期作為Zn〇單晶薄膜之基質物質 之於同真空狀態下，自上述第2電極接觸層即、別) ^& nCh表面置換至Ga之位置(ZnGa)，從而於ZGAO單 w _(3Π、318)與上述第2電極接觸層(315、316)之界面 上形成局部性之(l〇calized)Zn摻雜GaN層。另外，於活化 步驟後’局部性地殘留於上述第2電極接觸層(315 、316) 表面上之Mg-H錯合體藉由作為Zn<3單晶薄膜之基質之氧 (〇)而進。行OH鍵結，藉此氫(H)脫離，結果Mg置換至在 ZGAO單晶賴(317、31_λ述第2電極接觸層(315、⑽ 之界面上藉由懸空鍵(dangiing b〇n(j)而殘留之作為基質之 Ga的>^£(MgGa)，形成作為載子之電洞之摻雜濃度局部 性地非常高之1)_〇1〇1^(1層，並且接觸電阻可於zga〇單晶 薄膜(317、318)與上述第2電極接觸層（315、316)之界面上 大幅降低。此後，ZGA0單晶薄膜(317、318)一面進行成 長，一面於c-axis方向上成長，但產生因具有氧空位、於 結晶成長中形成之本質缺陷(native defect)之非對稱之化學 計量的組成比產生之較高之電阻。為了提高因此種非發光 中心(nonradiative center)產生之較低之電導率，需要應用最 佳之摻雜技術。於本發明之實施例中，為了 Zn〇薄膜用作 高效發光裝置之透明電極而同時摻雜作為n_型雜質之Ga 與作為P-型雜質之As，藉此可使非發光缺陷中心與自體補 償(self compensation)之影響最小化，並且改善電導率。即， 27 201232824 40534pif 換至料基質之211位置，同時換雜 分最小為基質之◦之位置，並且使電阻成 里之ZGA〇i曰：長均勻之電流散佈與電流注入效率優 ，、之ZGAO早日日溥膜(3! 7、3 ^ 8) 〇 曰5疋表示與η-型(Ga)與p-型(as)雜質對廡之電产 lltllT ^m n^(Ga)# -仆二U理想之—實施例而成長於利用有A1InGaN系 亂化物4*導體之發綠置之第2電極接觸層上之z 膜。 寸 土明者人為了觀察與摻雜於Zn0薄臈之雜質對鹿之 利用有AlInGaN錢化物半導體之發光裝置的電特性:利 用MBE設備，使具有與發光構造物相同之六邊形結晶構 造之約250G A厚度之Zn〇單晶薄膜成長於利用有平坦型 的AlInGaN綠化物半導體之發絲置之第2電極接觸層 上。通常，半導體物質之電阻依存於所_之n型與p_ 型雜質之濃度，因此為了確認與…型㈣與p_型(A雜質 之摻雜、及該等之同時摻雜對應之電特性，發明者於在將 ZnO薄膜厚度u定為25GG a後使未摻雜之Zn〇薄膜 (imdoped ZnO)、摻雜 Ga 之 Zn〇 薄膜(Ga Zn〇)、摻 雜As之ZnO薄臈(As doped Zn〇)、及同時捧雜Ga As之 ZnO薄膜(Ga-As CO-d〇ped ZnO)成長而以具有相同之距離 之方式形成銦電極後，確認電流-電壓特性。另外，發明者 將包含2英吋之藍寳石基板之AUnGaN系氮化物半^體發 光裝置之發光構造物分割成1/4塊而確認電特性，藉此確26 S 201232824 Status. According to a preferred embodiment of the present invention, when a zGA germanium single crystal film If) is grown on the 2-electrode contact layer (315, 316), it is used as a host material of the Zn〇 single crystal film in the initial vacuum state under the same vacuum state. From the second electrode contact layer, that is, the ^& nCh surface is replaced by the position of Ga (ZnGa), so that the ZGAO single w _ (3 Π, 318) and the second electrode contact layer (315, 316) A localized (Zn) Zn-doped GaN layer is formed on the interface. Further, the Mg-H complex which is locally left on the surface of the second electrode contact layer (315, 316) after the activation step is advanced by oxygen as a matrix of the Zn<3 single crystal thin film. The OH bond is formed, whereby hydrogen (H) is detached, and as a result, Mg is substituted to the ZGAO single crystal ray (317, 31_λ, the second electrode contact layer (315, (10) interface by dangling b〇n (j And the residue of the Ga as the substrate, Mg (MgGa), forms a doping concentration of the hole as a carrier, which is locally very high. 1) _〇1〇1^ (1 layer, and the contact resistance can be The interface between the zga〇 single crystal thin film (317, 318) and the second electrode contact layer (315, 316) is greatly reduced. Thereafter, the ZGA0 single crystal thin film (317, 318) is grown while being in the c-axis direction. Growing up, but producing a higher resistance due to the composition ratio of the asymmetric stoichiometry with oxygen vacancies and the native defect formed in the crystal growth. In order to improve the nonradiative center The lower conductivity requires the application of an optimum doping technique. In the embodiment of the present invention, the Zn〇 film is used as a transparent electrode of a high-efficiency light-emitting device while doping Ga as an n-type impurity and as a P As-type impurity As, thereby making non-luminous defect center and self-compensation (self compe The effect of nsation is minimized and the conductivity is improved. That is, 27 201232824 40534pif is changed to the position of the material 211, and the change of the impurity is at least the position of the matrix, and the resistance is made into ZGA〇i曰: long uniform The current dispersion and current injection efficiency are excellent, and the ZGAO early diurnal film (3! 7, 3 ^ 8) 〇曰 5 疋 indicates the electrical property of the η-type (Ga) and p-type (as) impurities. lltllT ^mn^(Ga)# - servant U U ideal - the example is grown on the z-film on the second electrode contact layer using the A1InGaN-based disordered 4* conductor greening. An electrical property of a light-emitting device using an AlInGaN carbon semiconductor with an impurity doped with Zn0 thin: a Zn 约 having a thickness of about 250 G A having a hexagonal crystal structure identical to that of the light-emitting structure by an MBE apparatus The single crystal thin film is grown on the second electrode contact layer of the hair of the flat AlInGaN green semiconductor. Generally, the resistance of the semiconductor material depends on the concentration of the n-type and p-type impurities, so Type (4) and p_ type (doping of A impurity, and at the same time The inventors have made an undoped Zn〇 film (imdoped ZnO), a Ga-doped Zn〇 film (Ga Zn〇), and doped As after the ZnO film thickness u is set to 25 GG a. The ZnO thin ruthenium (As doped Zn 〇) and the Ga As As ZnO thin film (Ga-As CO-d ped ZnO) were grown to form the indium electrode at the same distance, and the current-voltage characteristics were confirmed. In addition, the inventors have divided the light-emitting structure of the AUnGaN-based nitride semiconductor light-emitting device including the sapphire substrate of 2 inches into 1/4 blocks, and confirmed the electrical characteristics.

28 201232824 保對各個摻雜影響及效果之準確度。參照圖5，可知於未 摻雜之ZnO薄膜之情形時，在〇2 v之施加電壓下表示 5305 ohm之非常高之電阻值。評價為此種結果係因於未換 雜之ZnO單晶薄膜之成長中途產生之如本質結晶缺陷 (native defect)、氧(〇2)空位(vacancy)之原因而產生，且可 知如載子之捕獲等般對電導率造成惡劣影響，結果表示具 有較尚之電阻值。然而，於摻雜Ga之ZnO薄膜之情形時， 於相同之施加電壓下，電阻值為6 7 〇hm，表示與作為未 摻雜之ZnO薄膜之電阻值之5305 ohm相比變小至可無視 之程度。判斷為此種結果係因Ga置換至氧(〇2)空位之位 置’從而形成多個Ga-O與Zn-Ga鍵。另外，於摻雜As 之ZnO薄膜之情形時，可知於相同之施加電壓下，電阻值 再次增加至397 ohm。此種結果推測為As不僅置換至Zn 之位置，而且置換至氧(〇2)空位之位置，並且藉由Zn_As 與As-Ο鍵，結果電阻值與摻雜Ga之Zn〇薄膜之電阻值 相比再次增加。於同時摻雜Ga_As之Zn〇薄膜之情形時， 可知於相同之施加電壓下，電阻值為17 6〇hm，且可知該 電阻值略高於摻雜Ga之ZnO薄膜之電阻值，但與摻雜^ 之ZnO薄膜之電阻值相比非常低。此種結果推測為因同時 摻雜Ga與As，於具有本質結晶缺陷與氧(〇2)空位之基質 ZnO薄膜之成長中，與因由Ga形成之多個^_〇鍵盥 Ga-Ζη鍵引起之電阻減少、及由As形成之多個a.鍵與 As-Ο鍵同時一併進行Ga_As鍵結，從而與未換雜之 薄臈或摻雜As之ZnO薄膜相比，具有非常低之電阻值。 29 201232824 40534pif 以如圖5所示之電特性為基礎’可形成可用作AlInGaN系 氮化物半導體發光裝置之透明電極之具有與低電阻對應之 較尚之電導率之ZGAO薄膜。如圖5所示’發明者可確認 藉由4點探針(4 point probe)測定之未摻雜之ZnO薄膜 (xmdoped ZnO)、摻雜 Ga 之 ZnO 薄膜(Ga doped ZnO)、摻 雜As之ZnO薄膜(As doped ZnO)、及同時摻雜Ga_As之 ZnO 薄膜（Ga-As co-doped ZnO)之薄層電阻（sheet resistance ’ RS)分別為 6·5 K〇hm/sq、7 2 〇hm/sq、^ ohm/sq、及45 ohm/sq，且評價為與根據摻雜影響之電阻值 變化之電流-電壓特性曲線一致之具有可靠性之結果。 圖6是將與n_型(Ga)與化型(As)雜質對應之電流-電壓 特性對比於與先前之IT〇透日㈣極之發光裝置對應的電流 -電壓特性之圖表，該―㈣與ρ•型㈣雜質係摻雜於根 ί ί2想之另—實施例而成長於利用有Α1Ιη_ 、導體之發光裝置之第2電極接觸層上。發明者 鍵法(e_beam eVap〇rati〇n meth〇d)使先前之 〇_,月:極沉積為2200 A之厚度，從而於 執仃1分鐘之熱處理。 反卜 Ζη〇 化物半導體發光裝置之積層構造物與 同。件與圖5之情形相 加ΨΒτ 先則之IT0透明電極於0.2 V之施 之具二3i;=r阻值，且該值較具有17.6_ 如夂昭円〜之以〇薄膜高2倍以上。 “、、圖5及圖6觀察般，可知於本發明之同時推雜28 201232824 Guarantee the accuracy of each doping effect and effect. Referring to Fig. 5, it is understood that in the case of an undoped ZnO thin film, a very high resistance value of 5305 ohm is indicated at an applied voltage of 〇2 v. It is evaluated that such a result is caused by a natural defect or an oxygen (〇2) vacancy which occurs in the middle of the growth of the unsubstituted ZnO single crystal thin film, and it is known as a carrier. The capture and the like have a bad influence on the conductivity, and the result indicates that the resistance value is relatively high. However, in the case of a Ga-doped ZnO thin film, the resistance value is 6 7 〇hm at the same applied voltage, which means that it is small compared to the 5305 ohm which is the resistance value of the undoped ZnO thin film. The extent of it. It was judged that such a result was caused by the substitution of Ga to the position of the oxygen (〇2) vacancy, thereby forming a plurality of Ga-O and Zn-Ga bonds. Further, in the case of the As-doped ZnO thin film, it was found that the resistance value was again increased to 397 ohm at the same applied voltage. This result presumes that As is not only displaced to the position of Zn, but also displaced to the position of the oxygen (〇2) vacancy, and by the Zn_As and As-Ο bond, the resistance value is compared with the resistance value of the Ga-doped Zn〇 film. The ratio increases again. In the case of a Zn〇 film doped with Ga_As at the same time, it can be seen that the resistance value is 17 6 〇hm under the same applied voltage, and it is known that the resistance value is slightly higher than that of the Ga-doped ZnO thin film, but mixed with The resistance value of the ZnO thin film is very low. This result is presumed to be caused by simultaneous doping of Ga and As in the growth of a bulk ZnO thin film having an intrinsic crystal defect and an oxygen (〇2) vacancy, and a plurality of ^_〇 bond 盥Ga-Ζη bonds formed by Ga. The resistance is reduced, and the a. bond formed by As and the As-Ο bond are simultaneously bonded to the Ga_As bond, thereby having a very low resistance compared to the undoped thin tantalum or As-doped ZnO thin film. value. 29 201232824 40534pif Based on the electrical characteristics shown in Fig. 5, a ZGAO thin film having a relatively low electrical resistance corresponding to a low electric resistance which can be used as a transparent electrode of an AlInGaN-based nitride semiconductor light-emitting device can be formed. As shown in FIG. 5, the inventors can confirm an undoped ZnO thin film (xmdoped ZnO), a Ga doped ZnO thin film (Ga doped ZnO), and doped As as measured by a 4-point probe. The sheet resistance 'RS of ZnO thin film (As doped ZnO) and ZnO thin film (Ga-As co-doped ZnO) doped with Ga_As are respectively 6.5 K〇hm/sq, 7 2 〇hm /sq, ^ ohm/sq, and 45 ohm/sq, and was evaluated as a result of reliability consistent with the current-voltage characteristic curve according to the change in the resistance value of the doping effect. 6 is a graph comparing current-voltage characteristics corresponding to n-type (Ga) and chemical (As) impurities to current-voltage characteristics corresponding to a previous illuminating device of the IT 〇 day (fourth) pole, The ρ•-type (four) impurity is doped in the second electrode contact layer of the light-emitting device having the Α1Ιη_ and the conductor. The inventor's bond method (e_beam eVap〇rati〇n meth〇d) causes the previous 〇_, month: pole to be deposited to a thickness of 2200 Å, thereby performing a heat treatment for 1 minute. The laminated structure of the antimony semiconductor semiconductor light-emitting device is the same. Adding ΨΒτ to the case of Figure 5, the first IT0 transparent electrode is applied at 0.2 V with a value of 2i; = r, and the value is more than 2 times higher than the film with 17.6_夂夂夂~ . ", as shown in Fig. 5 and Fig. 6, it can be seen that the present invention is simultaneously mixed.

30 201232824 4U>34pit30 201232824 4U>34pit

Ga-As之Zn〇(即，ZGA〇薄膜）中，在同時掺雜之如&之 卜型雜質與如As^P_型雜質中，如Ga之n_型雜質為使電 特性變良好之主要相。如上所述，根據本發明，利用分 子束磊晶法(MBE)等方法，形成利用濺鍍法（spmtering method)與電子束蒸鑛法(e-beam evaporation method)形成 之ITO透明電極、或與低於Zn〇透明電極之電阻對應之電 導率優異之ZGAO薄膜、較理想的是ZGA〇單晶薄膜作為 AlInGaN系氮化物半導體發光裝置之透明電極，藉此可對In the Zn〇 of Ga-As (i.e., ZGA〇 film), in the doping of impurities such as & and the impurity such as As^P_ type, such as the n-type impurity of Ga, the electrical characteristics are improved. The main phase. As described above, according to the present invention, an ITO transparent electrode formed by a sputter method and an e-beam evaporation method is formed by a method such as molecular beam epitaxy (MBE), or A ZGAO thin film having a lower electrical conductivity than the Zn〇 transparent electrode, and preferably a ZGA 〇 single crystal thin film as a transparent electrode of the AlInGaN nitride semiconductor light-emitting device, can be used

AlInGaN系氮化物半導體發光裝置保證可靠性，並且 大量量產。 ’ 一圖7是表示與η-型(Ga)與p-型(As)雜質對應之電特性 及光特性之®，該η·型(Ga)與ρ·型(As)雜質係摻雜於根據 本發明之較理想之一實施例而成長於利用有A1InGaN系氮 化物半導體之發光裝置之第2電極接觸層上。參照圖7 , 使未摻雜之ZnO薄膜(und〇ped ZnO)、摻雜Ga之ZnO薄獏 (Ga doped ZnO)、摻雜 As 之 Zn〇 薄膜(As d〇ped Zn〇)、及 同時摻雜Ga-As之Zn〇薄膜(Ga-As co-doped ZnO)成長於 包含2英吋藍寶石基板之利用有AUnGaN系氮化物半導體 之發光裝置之第2電極接觸層上，從而測定電特性與光特 性而表示。圖7所示之結果係於與圖4相同之條件下而測 定，即於各試料上以相同之大小與距離形成銦電極而測 定。如圖7所示，於摻雜GaiZn〇薄膜之情形時，可確 認隨著摻雜Ga而整體之電阻值減少，但相對地光輸出減 少。於摻雜As之ZnO薄膜之情形時，可確認隨著摻雜〜 31 201232824 40534pif 而光輸出成為最大’但電阻值較摻雜Ga^Zn()薄膜 阻值增加。此觀科料隨著雜As， 形 ，〇le)注入中心㈣咖。請η㈣而光輸出增加， k合用於AlInGaN系氮化物半導體發光裝置 電阻值。於本發明之同時雜Ga_As之Zn〇薄膜== 時’ ^確認出隨著同時摻雜Ga_As❿光輸出較推雜&月‘ ZnO薄膜略減少’但具有低於先前之ιτ〇透明電極之電阻 值。因此’本發明之同時摻雜Ga_As之Ζη〇薄膜評價為可 ，為AlInGaN錢化物半導體發絲置之透日㈣極而實現 量產。 如上所述，於本發明之同時摻雜Ga-As之ZnO(即， ZGAO薄膜）中’在同時摻雜之如⑶之n型雜質與如& 之P-型雜質中，如Ga之η-型雜質為使電特性變良好之主 要原因，如參照圖7觀察般，可知於同時摻雜之如Ga之 η-型雜負與如As之p-型雜質中，如as之p_型雜質為使光 特性變良好之主要原因。根據本發明，可提供一種製備高 效發光裝置之方法，該發光裝置係利用分子束磊晶= (MBE)、有機金屬化學氣相沉積法(M〇CVD)、原子層二積 法(ALD)及原子層磊晶法(ALE)等方法，使Zn〇薄長 為單晶，藉此不僅可應用於大量量產，而且具有較高之光 輸出、低電阻與較高電流傳導率之電特性，該Zn〇薄膜係 將具有六邊形單晶構造之AlInGaN系氮化物半導體發光穿' 置之發光構造物本身作為基板，具有幾乎不存在晶格不二 致之六邊形結晶構造，且同時摻雜有使電特性變良好之如The AlInGaN nitride semiconductor light-emitting device ensures reliability and is mass-produced. ' Figure 7 shows the electrical and optical properties corresponding to η-type (Ga) and p-type (As) impurities. The η-type (Ga) and ρ-type (As) impurities are doped in According to a preferred embodiment of the present invention, the second electrode contact layer of the light-emitting device using the A1InGaN-based nitride semiconductor is grown. Referring to FIG. 7, an undoped ZnO thin film, gamma-doped ZnO thin doped (Ga doped ZnO), As-doped Zn tantalum thin film (As d〇ped Zn〇), and simultaneously doped Ga-As co-doped ZnO (Ga-As co-doped ZnO) is grown on a second electrode contact layer of a light-emitting device using an AUnGaN-based nitride semiconductor including a 2-inch sapphire substrate, thereby measuring electrical characteristics and light. Expressed by characteristics. The results shown in Fig. 7 were measured under the same conditions as in Fig. 4, i.e., indium electrodes were formed on the respective samples at the same size and distance. As shown in Fig. 7, in the case of doping a GaiZn〇 film, it was confirmed that the overall resistance value decreased with the doping of Ga, but the relative light output decreased. In the case of the As-doped ZnO thin film, it was confirmed that the light output became maximum with the doping of ~31 201232824 40534pif, but the resistance value of the doped Ga^Zn() film increased. This view material is injected into the center (four) coffee along with the Mis, Shape, and 〇le). Please η (4) and the light output is increased, and k is used for the resistance value of the AlInGaN nitride semiconductor light-emitting device. At the same time as the present invention, the Zn〇 film of the hetero-Ga_As == '^ confirms that the light output of the GaN film is slightly reduced with the simultaneous doping of Ga_As, but has a lower resistance than that of the previous transparent electrode. value. Therefore, the Ζη〇 film which is doped with Ga_As at the same time as the present invention is evaluated as a thin-film (four) electrode of the AlInGaN bulk semiconductor semiconductor. As described above, in the ZnO doped with Ga-As (i.e., ZGAO thin film) of the present invention, 'n-type impurity such as (3) and P-type impurity such as & The -type impurity is a main cause of improving the electrical characteristics. As observed with reference to FIG. 7, it can be seen that the η-type hetero-negative such as Ga and the p-type impurity such as As are simultaneously doped, such as the p_ type of as. Impurities are the main cause of improving optical characteristics. According to the present invention, there can be provided a method for preparing a high-efficiency light-emitting device using molecular beam epitaxy = (MBE), organometallic chemical vapor deposition (M〇CVD), atomic layer two-product method (ALD), and Atomic layer epitaxy (ALE) method makes Zn 〇 thin into a single crystal, thereby not only being applicable to mass production, but also having high optical output, low resistance and high current conductivity, the Zn The ruthenium film system has a hexagonal crystal structure in which a light-emitting structure of an AlInGaN-based nitride semiconductor having a hexagonal single crystal structure is used as a substrate, and has a hexagonal crystal structure having almost no crystal lattice, and is doped at the same time. Making electrical properties better

S » 32 201232824S » 32 201232824

想之實施例之將 ZGAO單晶薄膜形成為透明電極之In the embodiment, the ZGAO single crystal film is formed into a transparent electrode.

Ga之η-型，質、與使光特性變良好之如之 圖8疋表不對叙於帝廊，----Ga η-type, quality, and light characteristics become better as shown in Figure 8 疋 不 叙 叙 帝 帝 帝 , , , , , , , , , ,

AlInGaN系氮化物半導體發光裝置之咖芯片步驟之執 後而測定。參照圖8，表示有對發光裝置之電特性之綠圖 (mapping資訊，該發光裝置之電特性係於在使本發明之 ZGAO單晶薄膜成長於具有相同之A1InGaN系氮化物半導 體發光裝置之積層構造物的2英叶蟲晶片之第2電極接觸 層上後執行實際之LED芯片步驟後而測定。為了確認作為 本發明之實施例之透明電極之ZGA〇單晶薄膜的電特性''， 發明者將ZGAO單晶薄膜之厚度設為約2500 A左右，並 將2英忖發光裝置切割成1/2，剩餘之一塊係於將先前之 ITO透明電極設為500〜1200 a範圍内進行沉積及熱處 理，從而對電特性進行比較評價。另外，發明者將LED芯 片尺寸(chip size)及施加電流分別設為ιι〇〇χ600以瓜2、95 mA，此後於執行磨削、研磨、拋光等後續步驟後，對LED 芯片進行封裝而藉由積分球測定光輸出。如圖8所示，於 作為低電流之1 # A施加電流下，VF1 (forward voltage， 順向電壓)於ZGAO與ITO透明電極中相同地為2.10 V， 於95 μΑ施加電流下’ VF2於ZGAO與ΙΤΟ透明電極中仍 相同為 3·08 V，且於 450 nm 之 WD(dominant wavelength， 33 201232824 40534pif 主波長)下，ZGAO與IT0透明電極之光輸出分別為ι〇5 mW與115 mW而表示均勻之分散。光輸出根據測定設備 之選擇而存在差異，圖8所示之光輸出表示相對值。根據 ZGAO與ITO透明電極之光輸出分散，可確認出具有約ι〇 mW左右之差異，但於在對發光裝置之led芯片進行磨 削、研磨、拋光後分離成個個LED糾裸⑽⑹而安裝至 相同之封裝體後，湘積分棚定整體之光輸丨，结果於 先前之ΙΤΟ透明電極之情形時$ 1〇3 mW，於zGA〇透明 電極之情料為108.7 mW，從而確認^本發明之ZGA〇 透明電極錢前之ΓΓΟ透明電極相比，具有相對較高之 值。於本發明中，先前之加透明電極較zga〇透明電極 厚度約薄2.5倍以上’因此可藉由ZGAQ _之厚度及作 為η-，雜質之Ga與作為p•型雜質之&換雜控制，使光輸 出提兩10〜20%以上。 上述說明僅係示例性地對本發明之技術思想進行說 明’於本發明所屬之技術領軸具有常識者可於不脫離本 發明之本質特性之範圍内進行各種修正及變形。因此’本 發明所揭示之實施例並_以限定本發明之技術思想而是 用^說明，且並减㈣種實施例㈣林發明之技術思 想範圍。本發明之保護範圍應根據以下之中請專利範圍而 解釋’且__與祕於_之範_之所有技術思想 均包含於本發明之權利範圍内。 【圖式簡單說明】 34 S. 201232824 HUDj^pir ，圖i是概略性地表示利用有普通之他⑽系氣化物 半導體之發光裝置之積層構造的剖面圖。 圖2是概略性地表示用作本發明之較理想之實施例之 AlInGaN系氮化物半導體發光裝置的透明電極之zga〇薄 膜之形成過程之順序圖。 圖3是概略性地表示利用有本發明之較理想之一實施 例之包含ZGAO薄膜的AlInGaN系、氮化物半導體之發光裝 置之積層構造之剖面圖。 X 、 圖4是概略性地表示利用有本發明之較理想之另一實 施例之包含ZGAO薄膜的A1InGaN系氮化物^ 裝置之積層構造之剖面圖。 圖5是表示與n_型(Ga)# p•型(As)雜質對應之電流_ =特性之圖表，該η-型(Ga)與_(As)雜質係換雜於根 ，本發明之較理想之-實_而成長於有她祕系 鼠化物半導體之發絲置之第2電極接觸層上之Zn〇薄 膜。 圖6是將與n_型(Ga)與P-型(As)雜質對應之電流.電壓 特性對比於與先前之⑽透明電歡發光裝置對應之電流 撼電^寺性之圖表，該哨叫與p_型㈣雜質係摻雜於根 ^發明之較理想之另—實施例而成長於利財她⑽ 系氮化物半導體之發光裝置之第2電極接觸層上。 圖7是表示與n_s(Ga)與p_s(As)雜質 生之圖，該，與p_型剛 X之較理想之-實施例而成長於利用有A1InGaN系氣 35 201232824 4U534pit 化物半導體之發光裝置之第2電極接觸層上。The steps of the coffee chip step of the AlInGaN nitride semiconductor light-emitting device were measured. Referring to Fig. 8, there is shown a green map of the electrical characteristics of the light-emitting device. The electrical characteristics of the light-emitting device are based on the growth of the ZGAO single crystal thin film of the present invention in a laminate having the same A1InGaN nitride semiconductor light-emitting device. After the actual electrode chip step was performed on the second electrode contact layer of the two-leaf worm wafer of the structure, the electric characteristics of the ZGA 〇 single crystal film which is a transparent electrode of the embodiment of the present invention were confirmed. The thickness of the ZGAO single crystal film is set to about 2500 A, and the 2 inch light-emitting device is cut into 1/2, and the remaining one is deposited in the range of 500 to 1200 a of the previous ITO transparent electrode. The heat treatment was used to compare and evaluate the electrical characteristics. In addition, the inventors set the LED chip size and the applied current to ι 2, 95 mA, respectively, and then perform grinding, polishing, polishing, etc. After the step, the LED chip is packaged and the light output is measured by the integrating sphere. As shown in Fig. 8, VF1 (forward voltage) is applied to ZGAO and ITO at a current of 1 # A as a low current. The same electrode in the bright electrode is 2.10 V, and the current is applied at 95 μΑ. 'VF2 is still the same as 3·08 V in ZGAO and ΙΤΟ transparent electrode, and WD (dominant wavelength, 33 201232824 40534pif dominant wavelength) at 450 nm. The light output of ZGAO and IT0 transparent electrodes is ι〇5 mW and 115 mW, respectively, indicating uniform dispersion. The light output varies according to the selection of the measuring equipment, and the light output shown in Fig. 8 indicates the relative value. According to ZGAO and ITO transparent The light output of the electrode is dispersed, and it can be confirmed that the difference is about ι〇mW. However, after the LED chip of the light-emitting device is ground, polished, and polished, it is separated into individual LEDs (10) and mounted to the same package. After that, Xiang Xiang set the overall light transmission, and the result was $1〇3 mW in the case of the previous transparent electrode, and 108.7 mW in the zGA〇 transparent electrode, thus confirming the ZGA〇 transparent electrode of the present invention. Compared with the transparent electrode before the money, it has a relatively high value. In the present invention, the previous transparent electrode is about 2.5 times thinner than the thickness of the zga 〇 transparent electrode, so it can be made by the thickness of ZGAQ _ For the η-, the impurity Ga and the p-type impurity & the impurity control, the light output is increased by two 10~20% or more. The above description merely exemplifies the technical idea of the present invention. The technical lead of the present invention can be variously modified and modified without departing from the essential characteristics of the present invention. Therefore, the embodiments disclosed in the present invention are defined by the technical idea of the present invention, and And reduce (four) kinds of examples (four) the scope of the technical ideas of the forest invention. The technical scope of the present invention should be construed in accordance with the following claims, and all technical ideas of the invention are included in the scope of the present invention. BRIEF DESCRIPTION OF THE DRAWINGS 34 S. 201232824 HUDj^pir , FIG. 1 is a cross-sectional view schematically showing a laminated structure of a light-emitting device using a conventional (10)-based vaporized semiconductor. Fig. 2 is a sequence diagram schematically showing a process of forming a zga thin film of a transparent electrode used as an AlInGaN nitride semiconductor light-emitting device of a preferred embodiment of the present invention. Fig. 3 is a cross-sectional view schematically showing a laminated structure of an AlInGaN-based or nitride semiconductor light-emitting device including a ZGAO thin film according to an embodiment of the present invention. X and Fig. 4 are cross-sectional views schematically showing a laminated structure of an A1InGaN-based nitride device including a ZGAO thin film according to another preferred embodiment of the present invention. 5 is a graph showing a current_= characteristic corresponding to an n-type (Ga)#p• type (As) impurity, the η-type (Ga) and _(As) impurities are mixed with a root, and the present invention Preferably, the Zn film is grown on the second electrode contact layer of the hairline of her secret mouse compound semiconductor. 6 is a graph comparing current and voltage characteristics corresponding to n_type (Ga) and P-type (As) impurities with currents corresponding to the previous (10) transparent electroluminescent device, the whistle The p-type (four) impurity is doped in the second embodiment of the invention, and is grown on the second electrode contact layer of the light-emitting device of the nitride semiconductor. Fig. 7 is a view showing the generation of impurities with n_s(Ga) and p_s(As), which is preferably formed in a light-emitting device using an A1InGaN-based gas 35 201232824 4U534pit semiconductor with an ideal embodiment of p_-type X-- The second electrode is in contact with the layer.

圖8是表示對動作電壓(VF1、VF2)、逆向洩漏電流 (IR)、波長（WD)及光輸出（IV)分佈等電特性之繪圖 (mapping)資訊之圖’該等動作電壓(VF〗、vF2)、逆向茂漏 電流(IR)、波長(WD)及光輸出州分佈係於對本發明之較 理想之實施例之將ZGA0單晶薄膜形成為透明電極之 AlInGaN系氮化物半導體發光裝置之LED芯片步驟之執行 後所測定。 T 【主要元件符號說明】 101、301 :基板 103、303 :緩衝層 105、305 : η-型氮化物半導體層 107、307 : η-型氮化物包覆層 109、309 :活性層 111、311 : ρ-型氮化物包覆層 113、313 : ρ-型氮化物半導體層 115、315、316 :第2電極接觸層 117 : ΙΤΟ透明電極層 119、319 : η·型電極墊 121、321 : ρ-型電極墊 201〜211 :步驟 317、318 : ZGAO薄膜透明電極 36Fig. 8 is a diagram showing mapping information on electrical characteristics of operating voltage (VF1, VF2), reverse leakage current (IR), wavelength (WD), and light output (IV) distribution, and the operating voltage (VF) , vF2), reverse leakage current (IR), wavelength (WD), and light output state distribution are in an AlInGaN-based nitride semiconductor light-emitting device in which a ZGA0 single crystal thin film is formed as a transparent electrode in a preferred embodiment of the present invention. Measured after the execution of the LED chip step. T [Description of main component symbols] 101, 301: substrate 103, 303: buffer layers 105, 305: n-type nitride semiconductor layers 107, 307: n-type nitride cladding layers 109, 309: active layers 111, 311 : ρ-type nitride cladding layers 113, 313 : ρ - type nitride semiconductor layers 115, 315, 316 : second electrode contact layer 117 : ΙΤΟ transparent electrode layers 119 , 319 : η · type electrode pads 121 , 321 : Ρ-type electrode pads 201 to 211: Steps 317, 318: ZGAO thin film transparent electrode 36

SS

Claims (1)

201232824 4U5J4pit 七、申請專利範圍： 二二種氮化物半導體發光裝置，其係 徵在於包括：1、〇^ +以D之組成式者，其特 基板； ^衝層’其形成於上述基板上； 接觸層’其形成於上述緩衝層上； 活性，其形成於上述第1電極接觸層上； 其形成於上述第1包覆層上； = <層，其形成於上述活性層上； Ζη〇薄雷f形成於上述第2包覆層上； 上，且同時摻雜有選自上述第2電極接觸層 CM構成之群中之至:一 As、Sb之t 尘雜質、與選自由N、P、 P-型雜質族凡素與^^冓成之群令之至少-個 側；及電姆細成於上述第1電極接觸層之上部-第2電極墊’其形成於上述 η·型雜質為使電特性變良好之 P，雜質中，上述 使光特性變良好之主要原因。，、因’上述p-型雜質為 2.如申請專利範圍第】項所 裝置’其一雜質為-，上述P-型雜/為導:發光 37 201232824 40534pif 3·如申請專利範圍第1項所述之氮化物半導體發光 裝置，其中上述透明電極藉由分子束磊晶法(ΜΒΕ)形成。 4·如申請專利範圍第1項所述之氮化物半導體發光 裝置，其中上述透明電極藉由有機金屬化學氣相沉積法 (MOCVD)、原子層沉積法(ALD)及原子層蟲晶法中 之任一者形成。 人5. 一種氮化物半導體發光裝置製備方法，其係製備包 含 AlxInyGa(1—-y)N_⑸、Wya、osx+ysi)之组 成式之氮化物半導體發絲置之方法，其特徵在於包括如 下步驟： 提供基板之步驟； 於上述基板上形成緩衝層之步驟； 於上述緩衝層上形成第丨電極接觸層之步驟； 於上述第1電極接觸層上形成第1包覆層之步驟· 於上述^包覆層上形成活性層之步,^之々驟’ 於上述活性層上形成第2包覆層之步驟； 於上述第2包覆層上形成第2電極接觸層之步驟； 牛驟於第2電極接觸層上形成Zn〇薄膜之透明電極之 =此處選自由B、A1、Ga，之m族元素與f電= 之群中之至少-個η-型雜質、與選自由N、p、As、 Sb之v族元素與Li、Na、c構成之一 、 雜質同時摻雜於上述Zn〇薄膜；及 夕卜型 且於上述透明電極之上部一側形成第2電極塾之步驟； 38 201232824 4U^J4pif 门時推雜之上述n-形雜暂纺？ i、+， ，為使電特性良好=上因 光特性良好之主要原因。要原因上述p_型雜質為使 裳置5項所述之氮化物半導體發 3備方法，射上述η姻質為仏，上述。爾 裝置明^述之氮化物半導體發光 形成。 、中上述透明電極由分子束磊晶法(MBE) 果』二圍第5項所述之氮化物半導體發光 裝置氣備方法’其中上述透明電極藉由有機金屬化 ==_CVD)、料層㈣法(ald)及好層遙= (ALE)中之任一者形成。 9·如申請專利範圍第5項所述之氮化物半導體發 裝置製備方法’其更包括如下之步驟：於上述第1電極接 觸層之上部一側形成第1電極墊之步驟。 39201232824 4U5J4pit VII. Patent application scope: Two or two kinds of nitride semiconductor light-emitting devices, which are characterized by: 1, 〇 ^ + with the composition of D, its special substrate; ^ punching layer ' it is formed on the above substrate; a contact layer formed on the buffer layer; an active layer formed on the first electrode contact layer; formed on the first cladding layer; = < a layer formed on the active layer; Ζη〇 a thin ray f is formed on the second cladding layer; and is doped with a dust selected from the group consisting of the second electrode contact layer CM: a dust impurity of As, Sb, and selected from N, P, P-type impurity species, and at least one side of the group; and the electric electrode is finely formed on the upper portion of the first electrode contact layer - the second electrode pad' is formed in the above η type The impurity is P which is excellent in electrical characteristics, and among the impurities, the above-mentioned optical characteristics are improved. , because the above p-type impurity is 2. As described in the scope of the patent application, the impurity is -, the above P-type impurity / is the guide: illuminating 37 201232824 40534pif 3 · as claimed in the first item In the nitride semiconductor light-emitting device, the transparent electrode is formed by a molecular beam epitaxy method. 4. The nitride semiconductor light-emitting device according to claim 1, wherein the transparent electrode is formed by an organic metal chemical vapor deposition (MOCVD), an atomic layer deposition (ALD) method, and an atomic layer crystal method. Either form. Human 5. A method for preparing a nitride semiconductor light-emitting device, which is a method for preparing a nitride semiconductor hair strand comprising a composition formula of AlxInyGa(1-—y)N_(5), Wya, osx+ysi), which comprises the following steps a step of providing a substrate; a step of forming a buffer layer on the substrate; a step of forming a second electrode contact layer on the buffer layer; and a step of forming a first cladding layer on the first electrode contact layer; a step of forming an active layer on the cladding layer, a step of forming a second cladding layer on the active layer, and a step of forming a second electrode contact layer on the second cladding layer; a transparent electrode forming a Zn 〇 film on the electrode contact layer = here selected from at least one η-type impurity of a group of elements of group B, A1, Ga, and f =, and selected from N, p a group of elements of As, Sb, and one of Li, Na, and c, and an impurity doped simultaneously with the Zn〇 film; and a step of forming a second electrode 于 on the upper side of the transparent electrode; 201232824 4U^J4pif The above n-shaped miscellaneous ? i, +, , are the main reasons for good electrical characteristics = good optical properties. The reason for the above-mentioned p_ type impurity is a method for preparing a nitride semiconductor according to item 5, and the above-mentioned η-ring is 仏, as described above. The nitride semiconductor of the device is formed to emit light. The above-mentioned transparent electrode is prepared by a molecular beam epitaxy method (MBE). The method for preparing a nitride semiconductor light-emitting device according to item 5, wherein the transparent electrode is organic metallization==_CVD, and the layer (4) Any one of the law (ald) and the good layer (=ALE) is formed. The method for producing a nitride semiconductor device according to claim 5, further comprising the step of forming a first electrode pad on the upper side of the first electrode contact layer. 39
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