TW201737317A - 製造複合GaN奈米柱之方法及由此方法製得之發光結構 - Google Patents

製造複合GaN奈米柱之方法及由此方法製得之發光結構 Download PDF

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TW201737317A
TW201737317A TW105141477A TW105141477A TW201737317A TW 201737317 A TW201737317 A TW 201737317A TW 105141477 A TW105141477 A TW 105141477A TW 105141477 A TW105141477 A TW 105141477A TW 201737317 A TW201737317 A TW 201737317A
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nano
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安納 沃克法
維拉迪姆 伊凡索夫
亞歷山大 瑟金
班傑明 A 哈斯寇
哈森 S 艾爾－葛洛力
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傲思丹度科技公司
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Abstract

本發明揭示一種用於在基板上生長強對準均一橫截面半導體複合奈米柱之方法。該方法包括：(a)在該基板表面上形成琢面化錐形凹陷；(b)在該等凹陷之該等琢面上起始成核；以及；(c)促進核朝向該等凹陷之中心生長，在此中心處該等核藉由雙晶作用聚結且隨後一同長成為複合奈米柱。可在該等奈米柱之側壁上生長多量子井、核殼奈米柱異質結構。此外，可藉由該等奈米柱之過度生長形成連續半導體磊晶層以有助於製造高品質平面裝置結構或發光結構。

Description

製造複合GaN奈米柱之方法及由此方法製得之發光結構
本發明大體上係關於半導體材料及裝置。更特定言之，本發明係關於生產用於光電及其他應用之非極性半導體奈米柱之方法。
半導體奈米結構出現於大於二十年以前，不僅在量子實驗室中做研究用物件，而且作為搜尋裝置整合之方法中的步驟以進一步擴展其操作功能。在各種半導體奈米結構中，歸因於存在適合於導電而非穿隧之單一非受限方向，一維(1D)奈米柱(例如，奈米線及奈米鬚)在用於各種應用中具有格外吸引力。 相較於二維層，一維奈米柱幾何結構在無負荷表面上提供有利的橫向應變鬆弛，該無負荷表面在高晶格失配異質結構中作為應力消除路徑之功能為尤其重要的。 由GaN及相關第III族氮化物化合物製造之奈米柱在光電(太陽能電池、新穎發光及雷射二極體)至高頻電子(兆赫發射極、高電子遷移率電晶體及Gunn二極體)之廣泛應用中具有前景。有助於高速光通信之超小共振器及化學傳感器以及基於奈米線之裝置被期望使用此等結構或類似結構(參看S.J. Pearton、B.S. Kang、B.P. Gila、D.P. Norton、O. Kryliouk、F. Ren、Young-Woo Heo、Chih-Yang Chang、Gou-Chung Chi、Wei-Ming Wang及Li-Chyong Chen, GaN, ZnO and InN Nanowires and Devices, J. Nanosci. Nanotechnol. 8 (2008) 99-110)。 自碳奈米管內部之生長(參看W. Han、S. Fan、Q. Li及Y. Hu, Synthesis of Gallium Nitride Nanorods through a Carbon Nanotube-Confined Reaction, Science 277, 1287 (1997))開始，已使用各種方法合成1D GaN奈米結構。在催化劑塗佈之基板上之催化性化學蒸氣沈積(Cat-CVD)最常用。在Cat-CVD方法中，將氣態反應物溶解於奈米級液滴直至其過飽和，且藉由蒸氣-液體-固體(VLS)機制發生後續受小液滴限制之GaN生長。柱生長通常在藍寶石、SiC或Si基板上利用Au、Ni、Fe或In作為金屬催化劑材料進行。 在美國專利第7,745,315號中揭示一種在基板上形成豎直對準奈米線之方法，該方法使用金屬原子之單層以形成均一尺寸化金屬島，其充當用於第III族氮化物奈米線之金屬有機化學氣相沈積(MOCVD)之催化劑。該方法包含在結晶模板基板之表面上沈積催化劑金屬原子；加熱結晶模板以誘使催化劑金屬原子之表面擴散以形成複數個金屬奈米簇；以及使鎵前驅體與氮前驅體分子在金屬奈米簇處反應以形成與結晶模板基板磊晶對準之豎直定向、單晶GaN奈米線。描述氮前驅體與鎵前驅體之大於一的比率。雖然認為此對於連續磊晶層之生長為常見現象，但其對於奈米結構材料之生長並不同樣顯而易見。儘管此方法在使奈米線直徑減少至幾奈米中具有優勢，但此方法具有至少兩個主要缺點。第一，幾乎不可能控制最終界定奈米線之分佈及橫截面的催化劑奈米簇的自發演進。第二，VLS「由下而上」生長之常見缺點為金屬催化劑引起奈米線潛在污染，該金屬催化劑由於生長之後留於材料中之金屬殘餘物而在半導體中具有有限及非零分配係數。 在美國專利第8,410,496號中描述一種用於藉由遮罩輔助MOCVD技術產生GaN奈米線之無催化劑方法。在所描述之方法中，在基板上方形成用於選擇性奈米線生長之遮罩。此選擇性生長遮罩包括複數個圖案化孔口，其曝露部分基板。半導體材料首先使用選擇性及所謂「非脈衝生長」模式在遮罩之開口內部生長。隨後，在遮罩上方，生長以脈衝模式延續。在脈衝生長模式期間，交替引入第III族及第V族前驅體。藉由繼續脈衝生長模式，第III族氮化物奈米線沿單一方向在遮罩之頂部上方延伸，且維持開口之橫截面特徵。 前述方法之主要缺點為其對脈衝生長模式之參數的極端靈敏度。已判定在所描述之方法中規則至脈衝MOCVD生長之轉換的時機為尤其關鍵的(參看S.D. Hersee、X. Sun及X. Wang, The Controlled Growth of GaN Nanowires, Nano Lett., 6 (2006) 1808-1811)。若維持非脈衝方案，則一旦奈米線自生長遮罩出現，便開始發生橫向生長且損失奈米線幾何結構。亦認為脈衝序列內之步驟的持續時間為關鍵的，且因此必須對不同生長反應器組態進行最佳化。 在一系列學術著作中(參看H.M. Kim、D.S. Kim、D.Y. Kim、T.W. Kang、Y.H. Cho、K.S. Chung, Growth and Characterization of Single-crystal GaN Nanorods by Hydride Vapor Phase Epitaxy, Appl. Phys. Lett. 81, No. 12 (2002) 2193-2195； H.M. Kim、D.S. Kim、Y.S. Park、D.Y. Kim、T.W. Kang、K.S. Chung, Growth of GaN Nanorods by a Hydride Vapor Phase Epitaxy Method, Adv. Mater. 14, No. 13-14 (2002) 991-993； H.M. Kim、D.S. Kim、D.Y. Kim、T.W. Kang、K.S. Chung, Structural and Cathodoluminescence Properties of Gallium Nitride Nanorods by HVPE, J. Korean Phys. Soc. 42 (2003) S222-S225； H.M. Kim、Y.H. Cho、H. Lee、S.I. Kim、S.R. Ryu、D.Y. Kim、T.W. Kang、K.S. Chung, High-Brightness Light Emitting Diodes Using Dislocation-Free Indium Gallium Nitride/Gallium Nitride Multiquantum-Well Nanorod Arrays, Nano Lett. 2004, 4, 1059-1062)，已描述一種用於藉由氫化物氣相磊晶(HVPE)技術生長GaN及InGaN/GaN奈米棒及奈米棒陣列之催化劑及無遮罩方法。生長在水平反應器中在2吋藍寶石基板上在約480℃之溫度下進行。在生長方法期間，GaCl前驅體經由HCl氣體與Ga金屬之反應在750℃下在反應器之源區域中合成。其藉由氮氣運載氣體傳送至反應器之生長區域。在那裏，GaCl與氣態氨(NH3 )一起混合以形成沿基板上c軸方向定向之具有80-120 nm直徑之GaN奈米棒。形成奈米棒而非連續磊晶層為活性組分之低生長溫度及高V/III比率(超過60)的結果。令人遺憾地，所描述之方法存在奈米棒在基板之整個區域上之不可控制自發分佈及難以操縱奈米柱之直徑，認為兩者為奈米裝置應用之重要缺陷。 在美國專利第8,338,818號中描述一種用於形成非平面奈米線、奈米線陣列及奈米線網路之方法。根據該專利，揭示內容之非平面奈米線描述為以受控方式在具有非平面定向之表面上形成。在一所描述之實施例中，選擇性生長遮罩安置於至少兩個半導體側壁上，且複數個第III-N族奈米線藉由選擇性生長遮罩選擇性安置於至少兩個半導體側壁中之每一者上。所形成之第III-N族奈米線在同一半導體側壁上沿單一方向定向且各奈米線保持恆定橫截面特徵，其中在至少兩個半導體側壁之不同側壁上之相鄰第III-N族奈米線合併在一起，由此形成一或多個奈米線分支。 所描述之方法的明顯缺點為使生長晶體界面之分離部分合併在一起通常破壞性地干涉其單結晶度之損失，而替代地形成具有廣角晶粒界之多晶體。所描述之方法的又一另外缺點為忽略在奈米線與上面合成該等奈米線之基板之間存在磊晶協調之溫度依賴性。先前觀測展示(參看H.Y. Peng、N. Wang、X.T. Zhou、Y.F. Zheng、C.S. Lee、S.T. Lee, Control of growth orientation of GaN nanowires, Chemical Physics Letters 359 (2002) 241-245)無催化劑GaN奈米線具有在900℃與950℃之間的溫度下垂直於{101 1}平面生長且在更低800-900℃溫度下沿[0001]方向生長之趨勢。此外，奈米線之形狀在相同溫度序列中自豎直變化成不規則，其使得此方法之實際實施成問題。 在本發明之一個態樣中，提供一種用於均一直徑第III族氮化物奈米柱之無催化劑生長，且該等奈米柱定序陣列無先前技術方法中發現之前述不足的方法，該等不足包括(1)沿著預定結晶方向之非均一直徑奈米柱；(2)奈米柱之不可控位置；以及(3)奈米柱之溫度依賴性結晶定向，如在此之附件A中論述，標題為「On the origin of the spontaneous transition to non-polar a-plane GaN growth on c-plane sapphire」，V. Ivantsov等人，其全部內容併入本文中。 複合奈米柱在本發明之基板上的位置由成核平面之陣列的共同中心界定。由於奈米柱由在聚結期間在雙晶作用之後形成之至少三個對稱子奈米柱組成，所以在與新興凹角相關之各奈米柱之中心處存在較佳成核位點。在奈米柱之頂部上較佳成核之外觀控制最高生長速率之方向與奈米柱軸線對準。 複合奈米柱之軸線生長速度勝過其側面生長速度，不僅在擴散上而且在動力學受限生長模式中提供均一奈米柱直徑。對於奈米級結構之生長，包括來自第III族氮化物之奈米級結構的生長，奈米柱可以比先前技術方法能夠提供之參數範圍寬得多的生長參數範圍生產。此外，奈米柱生長之方向可選自具有適合雙晶作用協調之極性或非極性定向，由此允許選擇。複合奈米柱提高研發例如改良之光電及高頻電子裝置之可能性。本發明之另外目標及優勢進一步闡述於之後的描述中。
相關申請案之交叉參考 本申請案主張2015年12月14日申請之美國臨時專利申請案第62/267,117號之權益。 揭示一種用於在基板上生長強對準均一橫截面半導體複合奈米柱之方法。該方法可包含(a)在基板表面上形成一或多個琢面化錐形凹陷或凹槽；(b)在凹陷之琢面上起始成核；以及(c)促進核朝向凹陷之中心生長，從而使其藉由雙晶作用聚結且共同長成一或多個複合奈米柱。理想地，可在奈米柱之頂部或側壁上生長多量子井、核殼奈米柱異質結構。可藉由奈米柱之過度生長形成連續半導體磊晶層以有助於製造高品質平面裝置結構。本發明之奈米柱可例如用作發光結構中之元件或作為適應性插件用於減輕可在其上生長之連續磊晶層中之應力及缺陷密度。 在一較佳實施例中，本發明之複合第III族氮化物奈米柱經描述為使用氫化物氣相磊晶(HVPE)生長，但其亦可使用金屬有機化學氣相沈積(MOCVD)、分子束磊晶法(MBE)或類似方法形成。奈米柱生長可在藉由多區域電阻式鍋爐加熱之水平管石英反應器中進行。儘管水平反應器由於易於適應所需組分源而為較佳的，但應理解本發明之實施並不限於特定反應器組態，而係亦可使用對溫度、氣流及基板定位提供所需控制之其他組態。雖然反應器管較佳具有圓柱形狀，但亦可使用諸如矩形橫截面之其他反應器組態。 圖1之流程圖大致說明用於在HVPE生長設備中製造複合GaN奈米柱之較佳方法。參看圖1，將磊晶矽預備基板(例如藍寶石)插入至磊晶反應器之生長區域中(110)。基板定向較佳與藍寶石之(0001)平面一致或位於其附近。在後續步驟中，在生長區域之溫度下在氨(NH3 )氣流中進行基板之第一氮化(120)。氨氣流較佳在約0.5至約20標準公升/分鐘(slm)之範圍內，其視反應器幾何結構而定。如所測定最佳於經由HVPE化學方法之GaN的生長，生長區域之溫度可在約900℃至約1100℃之範圍內。 如擴散及活性氮離子與藍寶石之表面反應所需要，第一氮化可持續約4分鐘至約90分鐘。在圖1流程圖步驟130期間，歸因於藉由氯化氫(HCl)與氨之氣體混合物進行(0001)藍寶石表面當場蝕刻，出現用於生長子奈米柱之傾斜{101 2}成核平面(r-平面)。錐形{101 2}藍寶石成核平面受限且製造三角形蝕刻凹陷，在此處開始{112 0}a-平面GaN子奈米柱之生長。 r-平面藍寶石琢面化蝕刻凹陷之產生不僅可如本文所述當場進行，而且可使用乾式及濕式蝕刻中之任一者或兩者異地進行。在任一情況下，蝕刻凹陷之直徑界定子奈米柱之間的距離，及隨後所得複合奈米柱之直徑。 圖1之步驟140在氨氣流中提供經蝕刻基板之約10分鐘長第二氮化，其中氣流及溫度參數類似於第一氮化之參數。 在圖1之步驟150期間藉由使氯化鎵及氨穿過基板上方來實現GaN子奈米柱及複合奈米柱之生長。 藉由將具有奈米柱之基板自生長反應器移除來停止方法(160)。 本發明之奈米柱形成之進一步描述提供於圖2中。在c-平面藍寶石基板210上形成蝕刻凹陷220且將其藉由三個r-平面230琢面化。藍寶石之r-平面為a-平面GaN之成核位置。三個a-平面GaN子奈米柱240隨著{101 3}雙晶作用彼此聯結且豎直增長為由三個120度旋轉域組成之a-平面複合奈米柱250。複合奈米柱之六個側壁處於與GaN之三對+c及-c平面平行。歸因於-c-平面在高生長溫度下之較低熱穩定性，-c-平面可藉由穩定的+c平面來過度生長，由此產生僅由+c-平面限制之三角形橫截面的慣態。 現參看圖3，本發明之複合奈米柱結構之其他細節在俯視圖SEM影像中可見。自c-平面藍寶石基板上之當場所產生蝕刻凹陷進行複合a-平面奈米柱310之HVPE生長。奈米柱由三個相鄰a-平面GaN子奈米柱320、330及340組成。由於奈米柱310係自r-平面琢面化藍寶石蝕刻凹陷中演進出，所以其側壁之位置由基板表面上蝕刻凹陷之定向界定。 藉由參看圖4更充分描述作為奈米柱之複合結構的奈米柱與磊晶層之相互定向。圖4中{101 3}XRD反射之極圖獲自複合a-平面奈米柱及c-平面GaN磊晶層周圍且由圖410表示。為簡化理解所繪示之極圖，針對純c-平面及純a-平面GaN量測之兩個相對應{101 3}極圖分別展示於420及430中。可見複合奈米柱及磊晶層之極圖410可由與c-平面磊晶層相關之一者420以及三個120度旋轉a-平面極圖430組成。三個a-平面極圖中之每一者可歸屬於a-平面子奈米柱中之一者。其與磊晶層相比轉動約30度，此係因為後者之定向由與基板之磊晶關係界定，而前者之定向歸因於蝕刻凹陷定向。 參看圖5，展示根據本發明生長之GaN複合奈米柱的另一SEM影像。如上文所述，奈米柱之定向對應於a-平面GaN垂直於c-平面藍寶石基板生長。環繞奈米柱之非平面GaN磊晶層沿c軸定向且與奈米柱並行生長。 參看圖6，展示本發明之GaN複合奈米柱以及磊晶層周圍之側視圖SEM影像。奈米柱之高度相反地視其直徑而定，其繼而藉由奈米柱源於其中之蝕刻凹陷之直徑判定。 在本發明之一替代性較佳實施例中，在2吋c-平面藍寶石基板之表面上的複合奈米柱可用作藉由連續GaN磊晶層進行磊晶橫向過度生長的成核部位。奈米柱可藉由基板表面遮罩中蝕刻之規則間隔開口生長。 在此實施例中，第一，可使用例如遠程電漿增強式化學氣相沈積(PECVD)技術將約50 nm厚SiO2 遮罩沈積於基板上。 第二，可進行使用SF6 及Ar反應性離子蝕刻(RIE)之標準光微影以在此例示性實施例中在遮罩中製造約4 μm直徑及約5 μm間距之孔圖案。 第三，藍寶石表面上經曝露遮罩開口之濕式蝕刻可使用基於H3 PO4 之溶液在約300-400℃之蝕刻溫度下及以約120-140 s之蝕刻時間進行。 在蝕刻之後，在晶格結構中之開口的底部形成具有平坦r-平面琢面之三角形蝕刻凹陷。 最終，可使用如先前所描述之HVPE起始GaN生長且持續直至複合奈米柱自遮罩開口出現，在其上部邊緣上方延伸約3-5 μm。 應注意在本發明之方法中氯化鎵及氨氣流的增加導致GaN生長速率增加。在遮罩過度生長期間之V/III比率較佳設定於約30與約35之間。由於側壁不可接近性，GaN過度生長僅自奈米柱之頂部(或頂部琢面)繼續進行。因此，奈米柱與彼此合併且變成充分聚結GaN膜。聚結方法可在約10 μm之膜厚度內完成。膜懸掛於奈米柱上，且若其厚度足以避免破裂，則可剝離以便製備獨立式GaN晶體。可自約100 μm厚度開始獲得無裂痕材料。 在圖7及圖8中描繪之又一更佳實施例中，可在複合GaN奈米柱上生長諸如發光二極體(LED)之發光結構。 用於使用本發明之奈米柱製造發光結構之方法步驟的較佳集合在圖7之方法流程圖中說明。第一，如在本說明書中先前所描述生長GaN複合奈米柱(710)。在奈米柱製造之後，藉由引入矽烷(SiH4 )作為摻雜劑在奈米柱之頂部、側壁及環繞底部生長n型GaN (720)。隨後諸如藉由電漿增強式化學氣相沈積(PECVD)將SiO2 膜沈積於n型GaN之頂部上(730)。諸如藉由反應性離子蝕刻(RIE)將SiO2 膜自奈米柱之頂部移除(740)。隨後，在n型a-平面頂部奈米柱之頂部上形成InGaN/GaN量子井(QW)結構(750)，且在InGaN/GaN QW之頂部上生長a-平面連續p型GaN磊晶層(760)。隨後，諸如藉由電子束(EB)蒸發形成與頂部a-平面p型磊晶層之接觸(770)。隨後在環繞奈米柱的底部c-平面n型GaN磊晶層之表面上進行RIE蝕刻(780)，且諸如藉由EB蒸發形成與底部c-平面n型磊晶層之接觸(790)。 奈米柱如上文所述使用其上具有c-平面GaN層840之藍寶石基板810中之蝕刻凹陷820生長。在此LED實施例中，在生長步驟期間，可在氣流中引入矽烷(SiH4 )以添加矽雜質，有助於奈米柱及相鄰磊晶層或磊晶層中之n型傳導。 約20 nm厚SiO2 膜850可隨後藉由如上文所述之PECVD技術沈積於奈米柱及磊晶層上，且可進行反應性離子蝕刻或「RIE」。因為RIE之蝕刻速率視離子束朝向基板之方向而定，所以豎直蝕刻速率快於水平蝕刻速率。因此使用者可控制RIE參數以便移除a-平面複合奈米柱之頂部上的SiO2 且同時將殘餘SiO2 860留在奈米柱之側壁上，使得側壁經10 nm厚SiO2 膜鈍化。奈米柱830之頂部因此呈現無氧化物、複合a-平面表面，其適合於發光磊晶層之後續再生長。在圖8中，假定基板區域經遮蔽，因此氧化物層850將保留。 在後續步驟中，將具有奈米柱之生長模板轉移至MOCVD生長反應器，在此處InGaN/GaN量子井結構880使用例如三甲基鎵Ga(CH3 )3 、三甲基銦In(CH3 )3 及氨(NH3 )作為氣體載劑沈積於n型奈米柱之頂部上。n-襯墊870可設置於c-平面n型GaN層840上。發光結構亦可形成為InGaN/GaN多層量子井結構。反射膜亦可視情況形成於n型半導體層上。 進一步生長可藉由雙(環戊二烯基)鎂(Cp2 Mg)進行以產生頂部a-平面p型傳導磊晶層。在p型GaN生長期間，氨及三甲基鎵以及運載氣體之流動速率可逐漸升高以擴寬奈米柱之直徑且最終將其合併且形成平面a-平面p型GaN磊晶層890。 其後，Ni/氧化銦錫(ITO)可藉由例如電子束(EB)氣相沈積設備中之氣相沈積形成為p型磊晶層表面上之透明電極。可在透明電極上形成Au p型電極以形成p-襯墊821。 類似地，Ti/Au或其他合適n型電極可藉由EB氣相沈積設備中之氣相沈積在n型GaN磊晶層之RIE蝕刻表面上形成，以形成n型接觸850以便完成發光二極體(LED)結構。可類似地形成GaN及AlGaN光偵測器結構以及複合奈米柱場發射結構及供電裝置。 所形成LED結構包含附接於n型GaN磊晶層表面之n型電極(第一電極)850；複數個a-平面n型GaN複合奈米柱830，其中在奈米柱830之頂部上InGaN/GaN發光結構(奈米柱LED)依序堆疊，該等奈米柱轉而由磊晶層環繞；形成於透明電極811之表面上的p型連續GaN磊晶層及p型電極或襯墊(第二電極)821。 因此圖8之LED結構為在c-平面極性GaN 850上起始磊晶生長製程形成a-平面非極性GaN LED結構之方法的實施例。此方法克服在r-平面藍寶石上非極性GaN之磊晶生長中通常遭遇的困難，包括但不限於在r-平面藍寶石/a-平面GaN界面處之應力管理及位錯形成。因此在c-平面藍寶石上可能使用經充分理解及可信賴的生長來獲得a-平面LED結構，其具有可由該結晶平面實現之優勢，諸如更低應變、顯著更低的穿透位錯密度、更高效能及在a-平面LED結構之InGaN QW中更潛在地更高銦引入率。因此圖8之實施例使得能夠實現具有充分高In比率x之Inx Ga( 1 - x ) N QW LED結構，以實現長可見光譜波長，諸如紅色650-nm，其在顯示應用中極其受歡迎。 熟習此項技術者應認識到如在圖8之區塊890中所說明，在生長發光結構之前可在奈米柱之間發生GaN之橫向聚結，可能具有n型或未摻雜GaN而非p型GaN。生長次序之該反轉可用於生長鬆弛平面發光二極體及雷射二極體，其利用所產生材料中之低應力及疵點密度。該等結構可更輕易地黏接至用於封裝於薄膜光發射器結構中之載體晶圓或子基座。 雖然上文所述之LED實施例在奈米柱之頂部表面上採用磊晶生長，但熟習此項技術者應認識到亦可替代地遮蔽奈米柱之頂部表面且在豎直側壁上生長發光結構。該方法可為例如製造邊緣發射雷射二極體提供優勢。替代地，發光層可在側壁及頂部表面兩者上生長。在此情形下，可定製生長方法以使兩個相異結晶平面上之銦併入率不同，由此分別自奈米柱之頂部表面及側面產生不同發射波長。該色彩混合可在用於發光及顯示應用之高效白色LED的製造中提供獨特優勢。此外在本文之許多情況下，已在LED之情形下描述所產生之結構，不過結構中之多者經或可易於經熟習此項技術者修改成雷射結構且易於用作雷射二極體。因此如本文所使用，LED與雷射二極體之間存在一致性，其統稱為發光結構。 在前文揭示內容中，使用c-平面藍寶石作為例示性基板材料，不過c-平面藍寶石僅為例示性的，因為亦可使用各種其他基板材料，僅舉幾例該等其他材料，諸如c-平面藍寶石GaN、碳化矽、矽、a-平面藍寶石、鋁酸鋰或尖晶石材料。在彼方面，由於由晶格失配產生之不利影響可使用將不視為用於GaN生長之傳統基板材料的基板材料來實踐本發明，如沿橫向方向之錐形凹陷之正常尺寸較佳在10奈米至50微米之範圍內，且更佳低於1微米，避免若欲生長GaN之均一層則將遭遇的晶格失配累積。此外在前文揭示內容中，GaN用作奈米柱及子奈米柱之例示性材料。然而亦可使用其他材料，包括AlN、AlGaN、InGaN、AlInN或AlInGaN。 雖然在所選擇之實施例方面說明本發明，但在不背離隨附申請專利範圍之精神及範疇的情況下可對所說明實例進行更改及修改。此外，雖然可已相對於僅若干實施例揭示本發明之特定特徵，但該等特徵可與如對於任何給定或特定功能可為所需及有利的一或多個其他特徵組合。 考慮本文中所揭示之本發明之說明書及實踐，熟習此項技術者將清楚本發明之其他實施例。意欲本說明書及實例僅視為例示性的，其中本發明之真正範疇及精神藉由以下申請專利範圍指示。
110‧‧‧步驟
120‧‧‧步驟
130‧‧‧步驟
140‧‧‧步驟
150‧‧‧步驟
160‧‧‧步驟
210‧‧‧基板/c-平面藍寶石基板
220‧‧‧凹陷/蝕刻凹陷
230‧‧‧側壁/r-平面
240‧‧‧分支/a-平面GaN子奈米柱
250‧‧‧複合奈米柱/a-平面複合奈米柱
310‧‧‧複合a-平面GaN奈米柱
320‧‧‧a-平面GaN奈米柱
330‧‧‧a-平面GaN奈米柱
340‧‧‧a-平面GaN奈米柱
410‧‧‧{1013}GaN反射之XRD極圖/複合奈米柱及磊晶層之極圖
411‧‧‧c-平面磊晶層
412‧‧‧複合GaN奈米柱
420‧‧‧在c-平面藍寶石上針對c-平面磊晶層的{1013}反射之極圖/針對純c-平面量測之極圖
421‧‧‧{1013}反射
430‧‧‧在r-平面藍寶石上針對a-平面磊晶層的{1013}反射之極圖/針對純a-平面GaN量測之極圖
431‧‧‧a-平面磊晶層
710‧‧‧步驟
720‧‧‧步驟
730‧‧‧步驟
740‧‧‧步驟
750‧‧‧步驟
760‧‧‧步驟
770‧‧‧步驟
780‧‧‧步驟
790‧‧‧步驟
810‧‧‧藍寶石基板
811‧‧‧透明電極
820‧‧‧蝕刻凹陷
821‧‧‧p-襯墊/p型電極或襯墊(第二電極)
830‧‧‧奈米柱/a-平面n型GaN複合奈米柱
840‧‧‧c-平面GaN層/c-平面n型GaN層
850‧‧‧SiO2膜/氧化物層/n型接觸/n型電極(第一電極)/c-平面極性GaN
860‧‧‧殘餘SiO2
870‧‧‧n-襯墊
880‧‧‧InGaN/GaN量子井結構
890‧‧‧平面a-平面p型GaN磊晶層/區塊
本發明之特徵及優勢將由下文所闡述之圖式及實施方式變得更加顯而易見。本文呈現之圖示不意欲為任何特定半導體材料、結構或裝置之實際視圖，而僅為用以描述本發明之實施例的示意性表示。 圖1為展示根據本發明之實施例中之一或多者在c-平面藍寶石基板上生產複合a-平面GaN奈米柱之方法的流程圖。 圖2為結構之透視圖，其展示自三個分支240形成複合奈米柱250，該等分支自蝕刻於基板210中之凹陷220的側壁230增長且藉由雙晶作用合併在一起。 圖3為本發明之複合a-平面GaN奈米柱310之俯視圖SEM影像，該複合a-平面GaN奈米柱藉由HVPE生長且由三個相鄰a-平面GaN奈米柱320、330及340組成。 圖4為在根據本發明之c-平面藍寶石上生長之{101 3}GaN反射的XRD極圖410，包括由c-平面磊晶層411環繞之複合GaN奈米柱412。為簡化極圖410之描述，展示在c-平面藍寶石上針對c-平面磊晶層的{101 3}反射421之極圖420，以及在r-平面藍寶石上針對a-平面磊晶層431的{101 3}反射421之極圖430。 圖5為根據本發明之本方法生長之GaN複合奈米柱的SEM影像。奈米柱之定向對應於a-平面GaN。C-平面藍寶石用作基板。環繞奈米柱之波狀磊晶層為c-平面GaN。 圖6為本發明之GaN複合奈米柱的橫截面SEM影像。奈米柱之高度相反地視其直徑而定且由蝕刻凹陷之直徑界定，奈米分支在蝕刻凹陷中產生。 圖7為展示根據本發明之實施例，使用在c-平面藍寶石基板上之複合a-平面GaN奈米柱製造發光結構(諸如發光二極體結構或雷射二極體結構)之程序的流程圖。 圖8為複合奈米柱發光結構之示意圖。
810‧‧‧藍寶石基板
811‧‧‧透明電極
820‧‧‧蝕刻凹陷
821‧‧‧p-襯墊/p型電極或襯墊(第二電極)
830‧‧‧奈米柱/a-平面n型GaN複合奈米柱
840‧‧‧c-平面GaN層/c-平面n型GaN層
850‧‧‧SiO2膜/氧化物層/n型接觸/n型電極(第一電極)/c-平面極性GaN
860‧‧‧殘餘SiO2
870‧‧‧n-襯墊
880‧‧‧InGaN/GaN量子井結構
890‧‧‧平面a-平面p型GaN磊晶層/區塊

Claims (45)

  1. 一種用於生長複合奈米柱之方法，其包含以下步驟： 在基板之表面上形成凹陷； 在該凹陷中起始複數個子奈米柱成核；以及； 促進複數個子奈米柱朝向該凹陷之中心生長，在此中心處該等子奈米柱聚結以形成單個奈米柱。
  2. 如請求項1之方法，其中該凹陷為琢面化錐形凹陷。
  3. 如請求項2之方法，其中該琢面化錐形凹陷係藉由在基於H3 PO4 之溶液中的濕式化學蝕刻形成。
  4. 如請求項3之方法，其中該等子奈米柱包含GaN材料，且其中該等GaN子奈米柱及複合奈米柱具有非極性a-平面定向。
  5. 如請求項2之方法，其中該琢面化錐形凹陷在橫向尺寸中之大小為次微米。
  6. 如請求項2之方法，其中該琢面化錐形凹陷在橫向尺寸中之大小係在10奈米至50微米之範圍內。
  7. 如請求項2之方法，其進一步包含複數個錐形凹陷，且其中該等錐形凹陷係在該基板之表面上使用遮罩以在該基板表面上產生琢面化錐形凹陷之二維晶格圖案來形成。
  8. 如請求項7之方法，其中該等子奈米柱包含GaN材料，且其中該等GaN子奈米柱及複合奈米柱具有非極性a-平面定向。
  9. 如請求項7之方法，其中該等子奈米柱及複合奈米柱係藉由氫化物氣相磊晶技術生長。
  10. 如請求項1之方法，其中該基板係選自由c-平面藍寶石、GaN、碳化矽、a-平面藍寶石、鋁酸鋰或尖晶石材料組成之材料的群。
  11. 如請求項1之方法，其中該複合奈米柱包含第III族氮化物半導體材料。
  12. 如請求項1之方法，其中該基板為c-平面藍寶石基板。
  13. 如請求項12之方法，其中該錐形凹陷之琢面平行於該c-平面藍寶石基板之r-平面。
  14. 如請求項1之方法，其中該凹陷為琢面化錐形凹陷且該琢面化錐形凹陷係藉由在含有HCl之氣體混合物中蝕刻該基板來形成。
  15. 如請求項14之方法，其中該基板為c-平面藍寶石基板且其中該錐形凹陷之琢面平行於該c-平面藍寶石基板之r-平面。
  16. 如請求項1之方法，其中該等子奈米柱及複合奈米柱為GaN、AlN、InN、AlGaN、InGaN、AlInN或AlInGaN子奈米柱及複合奈米柱。
  17. 如請求項16之方法，其中該方法進一步包含生長複合奈米柱多層GaN及InGaN發光結構。
  18. 如請求項16之方法，其中該方法進一步包含在該複合奈米柱之頂部上生長複合奈米柱多層GaN及InGaN發光結構。
  19. 如請求項16之方法，其中該方法進一步包含在該複合奈米柱之側面上生長複合奈米柱多層GaN及InGaN發光結構。
  20. 如請求項16之方法，其中該方法進一步包含在該複合奈米柱上生長複合奈米柱多層GaN及AlGaN光偵測器結構。
  21. 如請求項16之方法，其中該方法進一步包含在該複合奈米柱之頂部上生長複合奈米柱多層GaN及AlGaN光偵測器結構。
  22. 如請求項16之方法，其中該方法進一步包含在該複合奈米柱之側面上生長複合奈米柱多層GaN及AlGaN光偵測器結構。
  23. 如請求項16之方法，其中該方法進一步包含在該複合奈米柱上生長複合奈米柱場發射結構。
  24. 如請求項16之方法，其中該方法進一步包含在該複合奈米柱上生長供電裝置。
  25. 如請求項1方法，其進一步包含在該奈米柱上生長複合奈米柱多層GaN及InGaN發光結構，其中基於該等發光結構在該複合奈米柱上面生長之結晶琢面，該等發光結構發射不同波長。
  26. 一種複合奈米柱，其包含： 在基板表面上之琢面化錐形凹陷； 在該錐形凹陷之該等琢面上的複數個子奈米柱；以及； 該複數個子奈米柱經聚結以形成單個奈米柱。
  27. 如請求項26之複合奈米柱，其中該基板為c-平面藍寶石、GaN、碳化矽、a-平面藍寶石、鋁酸鋰或尖晶石材料中之一者。
  28. 如請求項26之複合奈米柱，其中該複合奈米柱包含第III族氮化物半導體材料。
  29. 如請求項28之複合奈米柱，其中該基板為c-平面藍寶石基板且其中該錐形凹陷之琢面平行於該c-平面藍寶石基板之r-平面。
  30. 如請求項28之複合奈米柱，其中該等子奈米柱包含GaN材料，且其中該等GaN子奈米柱及複合奈米柱具有非極性a-平面定向。
  31. 如請求項26之複合奈米柱，其中該基板為c-平面藍寶石基板。
  32. 如請求項31之複合奈米柱，其中該錐形凹陷之琢面平行於該c-平面藍寶石基板之r-平面。
  33. 如請求項26之複合奈米柱，其中該琢面化錐形凹陷之大小為次微米。
  34. 如請求項26之複合奈米柱，其中該琢面化錐形凹陷之大小係在10奈米至50微米之範圍內。
  35. 如請求項26之複合奈米柱，其中該等子奈米柱及複合奈米柱為GaN、AlN、InN、AlGaN、InGaN、AlInN或AlInGaN子奈米柱及複合奈米柱。
  36. 如請求項35之複合奈米柱，其中該複合奈米柱進一步包含在該複合奈米柱上之複合奈米柱多層GaN及InGaN發光結構。
  37. 如請求項36之複合奈米柱，其中該複合奈米柱多層GaN及InGaN發光結構基於其所位處之結晶琢面發射不同波長。
  38. 如請求項35之複合奈米柱，其中該複合奈米柱進一步包含在該複合奈米柱之頂部上之複合奈米柱多層GaN及InGaN發光結構。
  39. 如請求項35之複合奈米柱，其中該複合奈米柱進一步包含在該複合奈米柱之側面上之複合奈米柱多層GaN及InGaN發光結構。
  40. 如請求項35之複合奈米柱，其中該複合奈米柱進一步包含在該複合奈米柱上之複合奈米柱多層GaN及AlGaN光偵測器結構。
  41. 如請求項35之複合奈米柱，其中該複合奈米柱進一步包含在該複合奈米柱之頂部上之複合奈米柱多層GaN及AlGaN光偵測器結構。
  42. 如請求項35之複合奈米柱，其中該複合奈米柱進一步包含在該複合奈米柱之側面上之多層GaN及AlGaN光偵測器結構。
  43. 如請求項35之複合奈米柱，其中該複合奈米柱進一步包含在該複合奈米柱上之場發射結構。
  44. 如請求項35之複合奈米柱，其進一步包含在該複合奈米柱上之供電裝置。
  45. 如請求項26之複合奈米柱，其中該等子奈米柱包含GaN材料，且其中該等GaN子奈米柱及複合奈米柱具有非極性a-平面定向。
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