TWI714740B - 經圖案加工的基板的製造方法及發光元件的製造方法 - Google Patents
經圖案加工的基板的製造方法及發光元件的製造方法 Download PDFInfo
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Classifications
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G73/00—Macromolecular compounds obtained by reactions forming a linkage containing nitrogen with or without oxygen or carbon in the main chain of the macromolecule, not provided for in groups C08G12/00 - C08G71/00
- C08G73/06—Polycondensates having nitrogen-containing heterocyclic rings in the main chain of the macromolecule
- C08G73/10—Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
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- G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
- G03F7/004—Photosensitive materials
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- G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
- G03F7/004—Photosensitive materials
- G03F7/022—Quinonediazides
- G03F7/023—Macromolecular quinonediazides; Macromolecular additives, e.g. binders
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- G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
- G03F7/004—Photosensitive materials
- G03F7/027—Non-macromolecular photopolymerisable compounds having carbon-to-carbon double bonds, e.g. ethylenic compounds
- G03F7/032—Non-macromolecular photopolymerisable compounds having carbon-to-carbon double bonds, e.g. ethylenic compounds with binders
- G03F7/037—Non-macromolecular photopolymerisable compounds having carbon-to-carbon double bonds, e.g. ethylenic compounds with binders the binders being polyamides or polyimides
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- G—PHYSICS
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- G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
- G03F7/004—Photosensitive materials
- G03F7/09—Photosensitive materials characterised by structural details, e.g. supports, auxiliary layers
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- G03F7/26—Processing photosensitive materials; Apparatus therefor
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- G—PHYSICS
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Abstract
本發明提供一種蝕刻用罩幕抗蝕劑組成物,其特徵在於:包含(A)以通式(1)所表示的結構單元為主成分的聚醯亞胺、以及(B)光酸產生劑的組成物,其中聚醯亞胺(A)的醯亞胺基當量為0.0025莫耳/g以上,蝕刻用罩幕抗蝕劑組成物即便於成為100℃~300℃的高溫下的高功率乾式蝕刻處理中亦不會產生抗蝕劑燃燒或碳化,且即便於低溫下進行抗蝕劑硬化,亦可獲得高的耐蝕刻性,因此可獲得面內均勻性高的藍寶石圖案。
Description
本發明是有關於一種蝕刻用罩幕抗蝕劑組成物、使用其的基板的製造方法及發光元件(二極體(diode))的製造方法。
發光二極體(LED:Light Emitting Diodes)是利用半導體的特性,將電能轉換為光能的元件的一種。LED由於能量轉換效率良好或長壽命,故而作為各種照明器件或照明(illumination)、顯示器等電子設備用途而不斷普及。因此,近年來,要求LED中使用的發光元件的進一步的高亮度化。
此種LED中使用的發光元件具有於基板上依次形成有n型GaN層等n型半導體層、InGaN層等發光層及p型GaN層等p型半導體層的結構,成為藉由自n型半導體層中注入的電子與自p型半導體層中注入的電洞於發光層中再結合而產生光的結構。
此種結構的發光元件中,已知如下技術:於基板的結晶上,利用將GaN系半導體整齊地排列於基底基板的結晶面上而進行結晶成長的磊晶成長法,來形成GaN系半導體層。結晶成長用基板多使用機械特性、熱特性、化學穩定性、透光性優異的單晶藍寶石基板(pattern sapphire substrate,PSS)。
但是,若於單晶藍寶石基板上使GaN層進行結晶成長,則由於藍寶石的晶格常數與GaN的晶格常數之間存在差,故而存在於成長時,GaN結晶的排列紊亂而產生缺陷的問題。另外,由於藍寶石基板的折射率與GaN系半導體層的折射率存在差,故而於發光層上產生的光於藍寶石-GaN系半導體的層界面上產生全反射,存在光封閉於GaN系半導體層中的問題。由於該些問題,向外部取出的光減少的方面為課題。
作為用以提高來自發光層的光取出效率的方法,已知如下方法:於藍寶石基板上形成抗蝕劑圖案,將其作為罩幕而對藍寶石基板進行乾式蝕刻,藉此於藍寶石基板表面形成凸圖案(例如參照專利文獻1~專利文獻3)。藉由凸圖案的形成,於GaN系半導體層形成時,沿著凸圖案而推進結晶的位錯,因此與使用平滑的藍寶石基板的情況相比,GaN層的缺陷減少。另外,藉由使發光層中產生的光散射、繞射,可抑制層界面上的全反射。
[現有技術文獻]
[專利文獻]
[專利文獻1]日本專利第3595277號公報
[專利文獻2]日本專利特開2011-91374號公報
[專利文獻3]日本專利特開2014-191002號公報
然而,專利文獻1中記載的抗蝕劑中,若為了製程的縮短化而以
高功率進行乾式蝕刻,則基板的溫度上升而產生抗蝕劑燃燒或碳化,因此存在無法獲得所需的藍寶石圖案的問題。
專利文獻2中記載的抗蝕劑中,提出了抑制抗蝕劑燃燒或碳化的製程,但必須追加如下步驟:於光微影步驟後一邊進行熱處理一邊進行紫外線(ultraviolet,UV)硬化,進而進行後烘烤;因此存在製程的縮短化不充分的問題。
專利文獻3中記載的抗蝕劑中,為了獲得充分的耐蝕刻性而必需300℃以上的抗蝕劑硬化,並且於250℃以下的抗蝕劑硬化中存在如下問題:蝕刻時基板面內的蝕刻速度有偏差,從而無法獲得面內均勻性高的藍寶石圖案。
本發明的目的在於提供一種蝕刻用罩幕抗蝕劑組成物,所述蝕刻用罩幕抗蝕劑組成物即便於成為100℃~300℃的高溫下的高功率乾式蝕刻處理中亦不會產生抗蝕劑燃燒或碳化,且即便於低溫下進行抗蝕劑硬化亦可獲得高的耐蝕刻性,且可獲得面內均勻性高的藍寶石圖案。
本發明為一種蝕刻用罩幕抗蝕劑組成物,其特徵在於:包含(A)以通式(1)所表示的結構單元為主成分的聚醯亞胺、以及(B)光酸產生劑的組成物,其中聚醯亞胺(A)的醯亞胺基當量為0.0025莫耳/g以上。
(通式(1)中,R1表示碳數2~50的二價的有機基;R2表示碳數2~50的三價或四價的有機基;m1為0或1的整數,c1為0或1的整數,當m1=0時,c1=1,當m1=1時,c1=0)
本發明的蝕刻用罩幕抗蝕劑組成物即便於成為100℃~300℃的高溫下的高功率乾式蝕刻處理中亦不會產生抗蝕劑燃燒或碳化,且即便於低溫下進行抗蝕劑硬化亦可獲得高的耐蝕刻性。因此,可獲得面內均勻性高的藍寶石圖案。
本發明的蝕刻用罩幕抗蝕劑組成物包含(A)以通式(1)所表示的結構單元為主成分且醯亞胺基當量為0.0025莫耳/g以上的聚醯亞胺、以及(B)光酸產生劑。
以下,關於本發明的蝕刻用罩幕抗蝕劑組成物的各成分而詳細進行說明。再者,下文為例示,本發明並不受下文的任何限定。
<(A)聚醯亞胺>
(A)聚醯亞胺為本發明的蝕刻用罩幕抗蝕劑組成物中的樹脂成分。於本發明中,(A)聚醯亞胺以通式(1)所表示的結構單元為主成分。
通式(1)中,R1表示碳數2~50的二價的有機基。R2表示碳數2~50的三價或四價的有機基。m1為0或1,c1為0或1,當m1=0時,c1=1,當m1=1時,c1=0。
所謂此處所述的主成分,是指於(A)聚醯亞胺中佔60重量%以上、較佳為80重量%以上的成分。(A)聚醯亞胺可為實質上包含通式(1)所表示的結構單元的聚醯亞胺。再者,「實質上包含通式(1)所表示的結構單元的聚醯亞胺」並不排除於不損及本發明的效果的範圍內包含其他結構單元的情況。
通式(1)所表示的結構單元的含量可藉由如下方法來估算:對所獲得的樹脂直接利用紅外分光法(FT-IR(Fourier Transform Infrared Spectroscopy,傅立葉轉換紅外光譜法))、核磁
共振(Nuclear Magnetic Resonance,NMR)、熱重量測定-質量分析(Thermo gravimetry Mass Spectrometry,TG-MS)、飛行時間型二次離子質量分析法(Time-of-Flight Secondary Ion Mass Spectrometry,TOF-SIMS)等進行分析,或使樹脂分解於各構成成分後利用氣相層析法(Gas Chromatography,GC)、高效液相層析法(High Performance Liquid Chromatography,HPLC)、質量分析(Mass Spectrometry,MS)、FT-IR、NMR等進行分析,進而於高溫下使樹脂灰化後利用元素分析等進行分析等。
(二胺殘基)
通式(1)中,R1表示二胺殘基。就對作為顯影液的鹼性水溶液的溶解性、感光性能的方面而言,二胺殘基較佳為具有羥基的二胺殘基。
作為提供具有羥基的二胺殘基的胺成分,可列舉:雙(3-胺基-4-羥基苯基)六氟丙烷、雙(3-胺基-4-羥基苯基)碸、雙(3-胺基-4-羥基苯基)丙烷、雙(3-胺基-4-羥基苯基)亞甲基、雙(3-胺基-4-羥基苯基)醚、雙(3-胺基-4-羥基)聯苯、雙(3-胺基-4-羥基苯基)茀、雙(4-胺基-3-羥基苯基)六氟丙烷、雙(4-胺基-3-羥基苯基)碸、雙(4-胺基-3-羥基苯基)丙烷、雙(4-胺基-3-羥基苯基)亞甲基、雙(4-胺基-3-羥基苯基)醚、雙(4-胺基-3-羥基)聯苯、雙(4-胺基-3-羥基苯基)茀等,但並不限定於該些。
就抗蝕劑硬化後的耐乾式蝕刻性的觀點而言,二胺殘基(R1)更佳為下述通式(8)所示的結構。
通式(8)中,R17表示單鍵、選自C(CF3)2、C(CH3)2、SO2、O、S、CH2中的至少一種所表示的有機基。進而佳為C(CF3)2、SO2,最佳為SO2。
另外,二胺殘基亦可包含不具有羥基的二胺殘基。作為提供此種二胺殘基的胺成分,可列舉:3,5-二胺基苯甲酸、3-羧基-4,4'-二胺基二苯基醚等含羧基的二胺、3-磺酸-4,4'-二胺基二苯基醚等含磺酸的二胺、二硫代羥基苯二胺、3,4'-二胺基二苯基醚、4,4'-二胺基二苯基醚、3,4'-二胺基二苯基甲烷、4,4'-二胺基二苯基甲烷、3,4'-二胺基二苯基碸、4,4'-二胺基二苯基碸、3,4'-二胺基二苯基硫醚、4,4'-二胺基二苯基硫醚、1,4-雙(4-胺基苯氧基)苯、間苯二胺、對苯二胺、1,5-萘二胺、2,6-萘二胺、雙(4-胺基苯氧基苯基)碸、雙(3-胺基苯氧基苯基)碸、雙(4-胺基苯氧基)聯苯、雙{4-(4-胺基苯氧基)苯基}醚、1,4-雙(4-胺基苯氧基)苯、2,2'-二甲基-4,4'-二胺基聯苯、2,2'-二乙基-4,4'-二胺基聯苯、3,3'-二甲基-4,4'-二胺基聯苯、3,3'-二乙基-4,4'-二胺基聯苯、2,2',3,3'-四甲基-4,4'-二胺基聯苯、3,3',4,4'-四甲基-4,4'-二胺基聯苯、2,2'-二(三氟甲基)-4,4'-
二胺基聯苯、或者將該些的芳香族環的氫原子的一部分以烷基或鹵素原子取代的化合物,或環己基二胺、亞甲基雙環己基胺等脂肪族二胺等,但並不限定於該些。
該些的二胺殘基亦可作為二胺、或於二胺殘基的結構中代替胺基而鍵結有異氰酸酯基或鍵結有三甲基矽烷基化胺而成的異氰酸酯化合物或三甲基矽烷基化二胺而使用。
另外,亦可使用基於上文所例示的二胺的二胺殘基的氫原子經甲基、乙基等碳數1~10的烷基、三氟甲基等碳數1~10的氟烷基、羥基、胺基、磺酸基、磺酸醯胺基或磺酸酯基、F、Cl、Br、I等取代1個~4個而成者。
(酸殘基)
通式(1)中,R2表示三-羧酸殘基或四-羧酸殘基(以下,稱為「酸殘基」)。
作為提供酸殘基的較佳的三羧酸的例子,可列舉:偏苯三甲酸、均苯三甲酸、二苯基醚三羧酸、聯苯三羧酸等。
作為提供酸殘基的較佳的四羧酸的例子,可列舉:均苯四甲酸、3,3',4,4'-聯苯四羧酸、2,3,3',4'-聯苯四羧酸、2,2',3,3'-聯苯四羧酸、3,3',4,4'-二苯甲酮四羧酸、2,2',3,3'-二苯甲酮四羧酸、2,2-雙(3,4-二羧基苯基)六氟丙烷、2,2-雙(2,3-二羧基苯基)六氟丙烷、1,1-雙(3,4-二羧基苯基)乙烷、1,1-雙(2,3-二羧基苯基)乙烷、雙(3,4-二羧基苯基)甲烷、雙(2,3-二羧基苯基)甲烷、雙(3,4-二羧基苯基)碸、雙(3,4-二羧基苯基)醚、1,2,5,6-萘四羧酸、2,3,6,7-萘四
羧酸、2,3,5,6-吡啶四羧酸、3,4,9,10-苝四羧酸等芳香族四羧酸,或環丁烷四羧酸、1,2,3,4-環戊烷四羧酸、環己烷四羧酸、雙環[2.2.1.]庚烷四羧酸、雙環[3.3.1.]四羧酸、雙環[3.1.1.]庚-2-烯四羧酸、雙環[2.2.2.]辛烷四羧酸、金剛烷四羧酸等脂肪族四羧酸等。
該些酸可單獨或者組合兩種以上來使用。
另外,亦可使用基於上文例示的三羧酸、四羧酸的羧酸殘基的氫原子經羥基、胺基、磺酸基、磺酸醯胺基或者磺酸酯基取代1個~4個而成者。
就抗蝕劑硬化後的耐熱性、耐乾式蝕刻性的觀點而言,酸殘基(R2)較佳為包含芳香環及/或脂肪族環,更佳為包含選自下述通式(9)~通式(11)所示的結構中的至少一種。
通式(9)~通式(11)中,R12~R16分別獨立地表示鹵素原子或碳數1~3的一價的有機基。b5~b7分別獨立地為0~2
的整數,b8~b9為0~3的整數。
作為提供酸殘基的三羧酸或四羧酸的最佳的例子,可列舉:均苯四甲酸、3,3',4,4'-聯苯四羧酸、2,3,3',4'-聯苯四羧酸、2,2',3,3'-聯苯四羧酸、萘四羧酸等。該些酸可單獨使用或組合兩種以上來使用。
進而,視需要亦可使用1,3-雙(對羧基苯基)-1,1,3,3-四甲基二矽氧烷、1-(對羧基苯基)-3-鄰苯二甲酸-1,1,3,3-四甲基二矽氧烷、1,3-雙鄰苯二甲酸-1,1,3,3-四甲基二矽氧烷等具有矽氧烷鍵的羧基化合物。藉由含有源自該些具有矽氧烷鍵的羧基化合物的酸殘基,可提高對基板的黏接性,進而可提高耐乾式蝕刻性。
就提高耐乾式蝕刻性的觀點而言,本發明中所使用的(A)聚醯亞胺的醯亞胺基當量為0.0025莫耳/g以上。較佳為0.003莫耳/g以上,更佳為0.0032莫耳/g以上。最佳為0.0034莫耳/g以上。
關於該醯亞胺基當量,是如以下般進行算出。將結構單元中的醯亞胺基數設為A(莫耳),將結構單元的分子量設為B(g)。
關於A、B,例如於為下述結構單元的情況下,分別為A=2、B=534。
另外,於為下述結構單元的情況下,為A=2、B=836。
該些是由A、B算出醯亞胺基當量A/B。
另外,於為A=2、B=534的聚醯亞胺結構單元80莫耳%與B=600的聚醯亞胺以外的結構單元20莫耳%的共聚物的情況下,醯亞胺基當量是由(2×0.8)/(534×0.8+600×0.2)算出。
(封端劑)
本發明中所使用的(A)聚醯亞胺亦可利用酸酐、單羧酸化合物、醯氯化合物及單胺化合物等封端劑將聚合物末端密封。藉由將聚合物的末端密封,可將聚合物對於鹼性水溶液的溶解速度調整為較佳範圍。
作為此種酸酐的例子,可列舉:鄰苯二甲酸酐、順丁烯二酸酐、納迪克酸酐、環己烷二羧酸酐、3-羥基鄰苯二甲酸酐、
1,10-蒽二羧酸酐、1,2-蒽二羧酸酐、2,3-蒽二羧酸酐等。
作為單羧酸化合物的例子,可列舉:2-羧基苯酚、3-羧基苯酚、4-羧基苯酚、2-羧基苯硫酚、3-羧基苯硫酚、4-羧基苯硫酚、1-羥基-8-羧基萘、1-羥基-7-羧基萘、1-羥基-6-羧基萘、1-羥基-5-羧基萘、1-羥基-4-羧基萘、1-羥基-3-羧基萘、1-羥基-2-羧基萘、1-巰基-8-羧基萘、1-巰基-7-羧基萘、1-巰基-6-羧基萘、1-巰基-5-羧基萘、1-巰基-4-羧基萘、1-巰基-3-羧基萘、1-巰基-2-羧基萘、2-羧基苯磺酸、3-羧基苯磺酸、4-羧基苯磺酸、1-羧基蒽、2-羧基蒽、3-羧基蒽等。
作為醯氯化合物的例子,可列舉:所述單羧酸化合物的羧基進行醯氯化而成的單醯氯化合物,對苯二甲酸、鄰苯二甲酸、順丁烯二酸、環己烷二羧酸、3-羥基鄰苯二甲酸、5-降冰片烯-2,3-二羧酸、1,2-二羧基萘、1,3-二羧基萘、1,4-二羧基萘、1,5-二羧基萘、1,6-二羧基萘、1,7-二羧基萘、1,8-二羧基萘、2,3-二羧基萘、2,6-二羧基萘、2,7-二羧基萘等二羧酸類的僅一個羧基進行醯氯化而成的單醯氯化合物。或者亦可使用藉由該些單醯氯化合物與N-羥基苯并三唑或N-羥基-5-降冰片烯-2,3-二羧基醯亞胺的反應而獲得的活性酯化合物。
作為單胺化合物的例子,可列舉:苯胺、萘基胺、胺基吡啶、3-乙炔基苯胺、4-乙炔基苯胺、3-胺基-4,6-二羥基嘧啶、2-胺基苯酚、3-胺基苯酚、4-胺基苯酚、5-胺基-8-羥基喹啉、4-胺基-8-羥基喹啉、1-羥基-8-胺基萘、1-羥基-7-胺基萘、1-羥基-6-胺基
萘、1-羥基-5-胺基萘、1-羥基-4-胺基萘、1-羥基-3-胺基萘、1-羥基-2-胺基萘、1-胺基-7-羥基萘、2-羥基-7-胺基萘、2-羥基-6-胺基萘、2-羥基-5-胺基萘、2-羥基-4-胺基萘、2-羥基-3-胺基萘、1-胺基-2-羥基萘、1-羧基-8-胺基萘、1-羧基-7-胺基萘、1-羧基-6-胺基萘、1-羧基-5-胺基萘、1-羧基-4-胺基萘、1-羧基-3-胺基萘、1-羧基-2-胺基萘、1-胺基-7-羧基萘、2-羧基-7-胺基萘、2-羧基-6-胺基萘、2-羧基-5-胺基萘、2-羧基-4-胺基萘、2-羧基-3-胺基萘、1-胺基-2-羧基萘、2-胺基煙鹼酸、4-胺基煙鹼酸、5-胺基煙鹼酸、6-胺基煙鹼酸、4-胺基水楊酸、5-胺基水楊酸、6-胺基水楊酸、3-胺基-鄰甲苯甲酸、三聚氰酸一醯胺(Ammelide)、2-胺基苯甲酸、3-胺基苯甲酸、4-胺基苯甲酸、2-胺基苯磺酸、3-胺基苯磺酸、4-胺基苯磺酸、5-胺基-8-巰基喹啉、4-胺基-8-巰基喹啉、1-巰基-8-胺基萘、1-巰基-7-胺基萘、1-巰基-6-胺基萘、1-巰基-5-胺基萘、1-巰基-4-胺基萘、1-巰基-3-胺基萘、1-巰基-2-胺基萘、1-胺基-7-巰基萘、2-巰基-7-胺基萘、2-巰基-6-胺基萘、2-巰基-5-胺基萘、2-巰基-4-胺基萘、2-巰基-3-胺基萘、1-胺基-2-巰基萘、3-胺基-4,6-二巰基嘧啶、2-胺基苯硫酚、3-胺基苯硫酚、4-胺基苯硫酚、1-胺基蒽、2-胺基蒽、3-胺基蒽等。
該些酸酐、單羧酸化合物、醯氯化合物及單胺化合物等封端劑可單獨或者組合兩種以上來使用,亦可併用其以外的封端劑。
就提高耐乾式蝕刻性的方面而言,作為特佳的聚醯亞胺
末端結構的例子,可列舉包含選自下述通式(2)、通式(3)、通式(4)中的至少一種者。
R18、R19、R20表示碳數9~18的縮合多環式芳香族烴基,縮合多環式芳香族烴基上的氫原子可經碳數1~4的烷基取代。
作為較佳的R18,可列舉:1-胺基蒽、2-胺基蒽、3-胺基蒽、1-胺基芘、2-胺基芘、3-胺基芘等單胺的殘基,但並不限定於該些。
作為較佳的R19,可列舉:1,10-蒽二羧酸酐、1,2-蒽二羧酸酐、2,3-蒽二羧酸酐、1,2-芘二羧酸酐、2,3-芘二羧酸酐、3,4-芘二羧酸酐等酸酐的殘基,但並不限定於該些。
作為較佳的R20,可列舉:1-羧基蒽、2-羧基蒽、3-羧基蒽等單羧酸的殘基,但並不限定於該些。
所述酸酐、單羧酸化合物、醯氯化合物、單胺化合物等封端劑的含量較佳為構成羧酸殘基及胺殘基的成分單體的添加莫耳數的0.1莫耳%~60莫耳%的範圍,更佳為5莫耳%~50莫耳%。藉由設為此種範圍,可獲得塗佈時的溶液的黏性為適度,且具有
優異的膜物性的蝕刻用罩幕抗蝕劑組成物。
本發明中所使用的(A)聚醯亞胺可使三羧酸、四羧酸、或該些的酸酐或醯氯、活性酯、活性醯胺與二胺、或與其對應的二異氰酸酯化合物、三甲基矽烷基化二胺進行聚合反應而獲得。
本發明中所使用的(A)聚醯亞胺的重量平均分子量較佳為5000~80000。更佳為10000~60000,最佳為20000~40000。
藉由設為此種範圍,可製成耐乾式蝕刻性高且蝕刻後的抗蝕劑去除性優異的組成物。
另外,本發明中所使用的(A)聚醯亞胺可為於聚合結束後,於甲醇或水等對於聚醯亞胺而言為不良溶媒中進行沈澱化後,進行洗滌、乾燥而獲得者。藉由進行沈澱化,聚合時使用的酯化劑、縮合劑及醯氯的副產物或低分子量成分等可去除,因此具有硬化圖案的耐熱性提高的優點。
<(B)光酸產生劑>
本發明的蝕刻用罩幕抗蝕劑組成物含有(B)光酸產生劑。藉此可形成曝光部被作為顯影液的鹼性水溶液去除的正型圖案。
作為光酸產生劑,可列舉醌二疊氮化合物、或鋶鹽、鏻鹽、重氮鎓鹽、錪鹽等鎓鹽化合物等。其中,本發明的蝕刻用罩幕抗蝕劑組成物較佳為包含醌二疊氮化合物,就提高耐乾式蝕刻性的觀點而言,更佳為除了醌二疊氮化合物以外亦包含鎓鹽。
作為醌二疊氮化合物,可列舉:醌二疊氮的磺酸以酯鍵鍵結於多羥基化合物而成者、醌二疊氮的磺酸以磺醯胺鍵鍵結於
多胺化合物而成者、醌二疊氮的磺酸以酯鍵及/或磺醯胺鍵鍵結於多羥基多胺化合物而成者等。特佳為作為該些的醌二疊氮鄰醌二疊氮的鄰醌二疊氮化合物。
該些多羥基化合物或多胺化合物的所有的官能基可未經醌二疊氮取代,較佳為官能基整體的50莫耳%以上經醌二疊氮取代。藉由50莫耳%以上經醌二疊氮取代而具有如下優點:樹脂膜對鹼性顯影液的溶解性變良好,可獲得與未曝光部的對比度高的精細的圖案。藉由使用此種醌二疊氮化合物,可獲得對作為一般的紫外線的水銀燈的i射線(365nm)、h射線(405nm)、g射線(436nm)感光的、具有正型感光性的蝕刻用罩幕抗蝕劑組成物。
作為多羥基化合物的具體例,可列舉以下的化合物(均為本州化學工業(股)製造)。
多胺化合物可列舉:1,4-苯二胺、1,3-苯二胺、4,4'-二胺基二苯基醚、4,4'-二胺基二苯基甲烷、4,4'-二胺基二苯基碸、4,4'-二胺基二苯基硫醚等。
另外,多羥基多胺化合物可列舉:2,2-雙(3-胺基-4-羥基苯基)六氟丙烷、3,3'-二羥基聯苯胺等。
於本發明中,醌二疊氮可較佳地使用5-萘醌二疊氮磺醯基、4-萘醌二疊氮磺醯基的任一者。4-萘醌二疊氮磺醯基酯化合物於水銀燈的i射線區域中具有吸收,適合於i射線曝光。5-萘醌二疊氮磺醯基酯化合物於直至水銀燈的g射線區域中具有吸收,適合於g射線曝光。
於本發明中,較佳為根據進行曝光的波長來選擇4-萘醌二疊氮磺醯基酯化合物、5-萘醌二疊氮磺醯基酯化合物。另外,亦可獲得於同一分子中併用4-萘醌二疊氮磺醯基及5-萘醌二疊氮磺醯基的萘醌二疊氮磺醯基酯化合物,亦可併用4-萘醌二疊氮磺醯基酯化合物與5-萘醌二疊氮磺醯基酯化合物。
另外,醌二疊氮化合物的分子量較佳為300以上,更佳為350以上。另外,較佳為1500以下,更佳為1200以下。若分子量為300以上,則具有曝光感度變高的優點,若為1500以下,則具有加熱處理後的耐熱性被膜的機械特性提高的優點。
本發明中所使用的醌二疊氮化合物可由特定的酚化合物並藉由如下方法來合成。例如,有如下方法等:使5-萘醌二疊氮磺醯氯與酚化合物於三乙基胺存在下進行反應。酚化合物的合成方法有如下方法等:於酸觸媒下,使α-(羥基苯基)苯乙烯衍生物與多元酚化合物進行反應。
作為本發明中所使用的鎓鹽化合物,較佳為選自鋶鹽、鏻鹽、重氮鎓鹽中的化合物。藉由使用該些而圖案的解析度顯著提高。進而,就耐乾式蝕刻性的觀點而言,較佳為使用鋶鹽。鋶鹽中,特別更佳為使用通式(12)~通式(14)所表示的結構者。
通式(12)~通式(14)的R21~R23可分別相同亦可不同,表示碳數1~20的有機基。
作為較佳例,可列舉:甲基、乙基、丙基、異丙基、丁基、第三丁基等烷基,環戊基、環己基等環烷基,苯基、萘基等芳基等。另外,亦可使用環戊基、環己基、苯基、萘基的氫原子的1個~4個經甲基、乙基等碳數1~4的烷基、甲氧基、乙氧基等碳數1~4的烷氧基、三氟甲基等碳數1~4的氟烷基、羥基、胺基、磺酸基、磺酸醯胺基、磺酸酯基、F、Cl、Br或I等取代而成者。
R24、R25表示單鍵、醚基、硫醚基、碸基、酮基。Z-表示選自R26SO3 -、R26COO-、SbF6 -中的陰離子部。R26表示碳數1~20的有機基。
作為較佳例,可列舉:十二烷基等碳數1~18的烷基,三氟甲基等碳數1~10的氟烷基,環戊基、環己基等環烷基,苯
基、萘基等芳基,7,7-二甲基-2-氧代雙環[2.2.1]庚烷-1-亞甲基等。
另外,亦可使用環戊基、環己基、苯基、萘基的氫原子的1個~4個經甲基、乙基等碳數1~4的烷基、甲氧基、乙氧基等碳數1~4的烷氧基、三氟甲基等碳數1~4的氟烷基、羥基、胺基、磺酸基、磺酸醯胺基、磺酸酯基、F、Cl、Br或I等取代而成者。
以下示出通式(12)所表示的鋶鹽的具體例。
以下示出通式(13)所表示的鋶鹽的具體例。
以下示出通式(14)所表示的鋶鹽的具體例。
就耐乾式蝕刻性的觀點而言,特佳者可列舉通式(15)所表示的三芳基鋶鹽。
式中,R27可分別相同亦可不同,表示氫原子或碳數1~20的有機基的任一者。
作為較佳例,可列舉:甲基、乙基等碳數1~4的烷基,甲氧基、乙氧基等碳數1~4的烷氧基,三氟甲基等碳數1~4的氟烷基,羥基,胺基,磺酸基,磺酸醯胺基,磺酸酯基,F,Cl,Br或I等。
R28表示碳數1~20的有機基。作為較佳例可列舉:十二烷基等碳數1~18的烷基,三氟甲基等碳數1~10的氟烷基,環戊基、環己基等環烷基,苯基、萘基等芳基,7,7-二甲基-2-氧代雙環[2.2.1]庚烷-1-亞甲基等。另外,亦可使用環戊基、環己基、苯基、萘基的氫原子的1個~4個經甲基、乙基等碳數1~4的烷基、甲氧基、乙氧基等碳數1~4的烷氧基、三氟甲基等碳數1~4的氟烷基、羥基、胺基、磺酸基、磺酸醯胺基、磺酸酯基、F、Cl、Br或I等取代而成者。
b10~b12分別表示0~5的整數。
以下示出通式(15)所表示的三芳基鋶鹽的具體例。
相對於蝕刻用罩幕抗蝕劑組成物中的樹脂整體100重量份,(B)光酸產生劑的含量較佳為1重量份以上,更佳為3重量份以上。另外,較佳為50重量份以下,更佳為40重量份以下。
若處於該範圍,則具有加熱處理後的耐熱性被膜的機械特性變良
好的優點。
另外,本發明的蝕刻用罩幕抗蝕劑組成物亦可含有未經酯化的具有酚性羥基的化合物。藉由含有此種具有酚性羥基的化合物,所獲得的蝕刻用罩幕抗蝕劑組成物於曝光部中對鹼性水溶液的溶解性提高。另外,於未曝光部中,萘醌二疊氮化合物與具有酚性羥基的化合物產生氫鍵,因此對鹼性水溶液的溶解性降低。因此,可實現高感度化。
相對於蝕刻用罩幕抗蝕劑組成物中的樹脂整體100重量份,具有酚性羥基的化合物的含量較佳為1重量份~40重量份,更佳為3重量份~30重量份。再者,具有酚性羥基的化合物可含有兩種以上,於含有兩種以上的情況下,較佳為該些的總量為所述範圍。
<(C)通式(5)及通式(6)所表示的化合物>
進而,就耐蝕刻性、蝕刻後的抗蝕劑去除性的觀點而言,本發明的蝕刻用罩幕抗蝕劑組成物較佳為包含下述(C)通式(5)、通式(6)所表示的化合物的至少一種。
通式(5)、通式(6)中,R3、R5及R7表示氫原子或下述通式(7)所表示的結構的基。R3中的30莫耳%~100莫耳%為下述通式(7)所表示的結構的基。就耐乾式蝕刻性的觀點而言,較佳為40莫耳%~90莫耳%,更佳為50莫耳%~80莫耳%。另外,R5及R7的合計量中的30莫耳%~100莫耳%為下述通式(7)所表示的結構的基。就耐乾式蝕刻性的觀點而言,較佳為40莫耳%~90莫耳%,更佳為50莫耳%~80莫耳%。
R4、R6及R8表示碳數1~6的有機基。X1為單鍵、O、S、NH、SO2、CO或碳數1~3的二價的有機基或者該些的兩個以上連結而成的二價的交聯結構。a1、a2、a3、b1、b2及b3表示1以上的整數,d1、d2、d3表示0以上的整數,a1+b1+d1≦6,a2+b2+d2≦5及a3+b3+d3≦5。
通式(7)中,R9表示碳數1~6的二價的有機基。作為較佳例,可列舉:甲基、乙基、丙基等碳數1~6的烷基、及該些經由醚、硫醚、醯胺、酯連結而成的基、三氟甲基等碳數1~6的氟烷基、及該些經由醚、硫醚、醯胺、酯連結而成的基、環戊基、
環己基等環烷基、苯基等。
R10及R11表示碳數1~8的有機基。作為較佳例,可列舉:甲基、乙基、丙基等碳數1~8的烷基,三氟甲基等碳數1~8的氟烷基,環戊基、環己基等環烷基,苯基、甲氧基苯基等。
a4表示1以上的整數,b4表示0以上的整數,a4+b4=3。
作為較佳的(5)、(6)的具體例,可列舉下述所示結構者,但並不限定於該些。
相對於蝕刻用罩幕抗蝕劑組成物中的樹脂整體100重量份,(C)通式(5)及通式(6)所表示的化合物的含量較佳為1重量份以上,更佳為3重量份以上。另外,較佳為20重量份以下,更佳為10重量份以下。若處於該範圍,則具有加熱處理後的耐熱性被膜的機械特性變良好的優點。
<其他樹脂>
本發明的蝕刻用罩幕抗蝕劑組成物亦可含有聚醯亞胺以外的
鹼可溶性樹脂。具體而言可列舉:將丙烯酸共聚而成的丙烯酸聚合物、酚樹脂、矽氧烷樹脂、多羥基苯乙烯、或於該些中導入羥甲基、烷氧基甲基或環氧基等交聯基而成的樹脂、該些的共聚聚合物等。
就耐乾式蝕刻性的觀點而言,較佳為包含(D)選自酚樹脂及多羥基苯乙烯中的至少一種。此處所述的酚樹脂及多羥基苯乙烯中包含在該些中導入羥甲基、烷氧基甲基或環氧基等交聯基而成的樹脂。另外,亦包含酚樹脂與多羥基苯乙烯的共聚聚合物。
此種樹脂為溶解於氫氧化四甲基銨、膽鹼、三乙基胺、二甲基胺基吡啶、單乙醇胺、二乙基胺基乙醇、氫氧化鈉、氫氧化鉀、碳酸鈉等鹼的水溶液中者。藉由含有該些鹼可溶性樹脂,可一邊保持耐熱性被膜的密合性或優異的感度,一邊賦予各鹼可溶性樹脂的特性。
作為較佳的酚樹脂,有酚醛清漆樹脂或甲階酚醛樹脂,可藉由利用福馬林等醛類使多種酚類單獨或該些多種的混合物進行縮聚而獲得。
作為構成酚醛清漆樹脂及甲階酚醛樹脂的酚類,例如可列舉:苯酚、對甲酚、間甲酚、鄰甲酚、2,3-二甲基苯酚、2,4-二甲基苯酚、2,5-二甲基苯酚、2,6-二甲基苯酚、3,4-二甲基苯酚、3,5-二甲基苯酚、2,3,4-三甲基苯酚、2,3,5-三甲基苯酚、3,4,5-三甲基苯酚、2,4,5-三甲基苯酚、亞甲基雙酚、亞甲基雙對甲酚、間苯二酚、鄰苯二酚、2-甲基間苯二酚、4-甲基間苯二酚、鄰氯苯酚、
間氯苯酚、對氯苯酚、2,3-二氯苯酚、間甲氧基苯酚、對甲氧基苯酚、對丁氧基苯酚、鄰乙基苯酚、間乙基苯酚、對乙基苯酚、2,3-二乙基苯酚、2,5-二乙基苯酚、對異丙基苯酚、α-萘酚、β-萘酚等,該些可單獨使用,或作為多種的混合物而使用。
另外,作為所述醛類,除了福馬林以外,亦可列舉:多聚甲醛、乙醛、苯甲醛、羥基苯甲醛、氯乙醛等,該些可單獨使用或作為多種的混合物而使用。
另外,本發明中所使用的酚樹脂亦可為藉由碳數1~20的烷基、氟烷基、烷氧基、酯基、硝基、氰基、氟原子、或氯原子對加成於芳香族環上的氫原子的1個~4個進行取代而成的結構等。
關於本發明中所使用的酚樹脂的重量平均分子量,使用凝膠滲透層析法(Gel Permeation Chromatography,GPC)並以聚苯乙烯換算計而較佳為處於2,000~50,000、較佳為3,000~30,000的範圍。於分子量為2,000以上的情況下,圖案形狀、解析度、顯影性、耐熱性優異,於分子量為50,000以下的情況下,可保持充分的感度。
作為較佳的多羥基苯乙烯,例如可列舉如下聚合物或共聚物,所述聚合物或共聚物是使利用公知的方法將對羥基苯乙烯、間羥基苯乙烯、鄰羥基苯乙烯、對異丙烯基苯酚、間異丙烯基苯酚、鄰異丙烯基苯酚等具有酚性羥基的芳香族乙烯基化合物單獨或兩種以上聚合而獲得的聚合物或共聚物、及利用的公知方
法將苯乙烯、鄰甲基苯乙烯、間甲基苯乙烯、對甲基苯乙烯等芳香族乙烯基化合物單獨或兩種以上聚合而獲得的聚合物或共聚物的一部分與烷氧基利用公知的方法進行加成反應而獲得。
另外,本發明中所使用的多羥基苯乙烯亦可為藉由碳數1~20的烷基、氟烷基、烷氧基、酯基、硝基、氰基、氟原子、或氯原子對加成於芳香族環上的氫原子的1個~4個進行取代而成的結構等。
關於本發明中所使用的多羥基苯乙烯的重量平均分子量,使用凝膠滲透層析法(GPC)並以聚苯乙烯換算計而較佳為3,000~60,000的範圍,更佳為3,000~25,000的範圍。於分子量為3,000以上的情況下,圖案形狀、解析度、顯影性、耐熱性優異,於分子量為60,000以下的情況下,可保持充分的感度。
關於該些酚樹脂、多羥基苯乙烯於蝕刻用罩幕抗蝕劑組成物中的含量,於蝕刻用罩幕抗蝕劑組成物中的樹脂整體100重量份中,較佳為5重量份~50重量份,更佳為10重量份~40重量份。若為50重量份以下,則可維持加熱處理後的耐熱性被膜的耐熱性或強度,若為10重量份以上,則可進一步提高樹脂膜的圖案形成性。
<其他成分>
本發明的蝕刻用罩幕抗蝕劑組成物亦可視需要含有矽烷偶合劑。藉由含有矽烷偶合劑,可於硬化膜形成時提高與基底基材的密合性。
作為矽烷偶合劑的具體例,可列舉:乙烯基三甲氧基矽烷、乙烯基三乙氧基矽烷、2-(3,4-環氧基環己基)乙基三甲氧基矽烷、3-縮水甘油氧基丙基三甲氧基矽烷、3-縮水甘油氧基丙基三乙氧基矽烷、對苯乙烯基三甲氧基矽烷、3-胺基丙基三甲氧基矽烷、3-胺基丙基三乙氧基矽烷、N-苯基-3-胺基丙基三甲氧基矽烷、3-巰基丙基甲基二甲氧基矽烷、3-巰基丙基三甲氧基矽烷、3-異氰酸酯丙基三乙氧基矽烷、4-羥基苯基三甲氧基矽烷、4-甲氧基苯基三甲氧基矽烷、4-乙氧基苯基三甲氧基矽烷等矽烷偶合劑等。可含有該些的兩種以上。
相對於蝕刻用罩幕抗蝕劑組成物中的樹脂整體100重量份,矽烷偶合劑的含量較佳為0.1重量份~10重量份。
更佳為0.2重量份~5重量份,進而佳為0.3重量份~3重量份。
本發明的蝕刻用罩幕抗蝕劑組成物可含有溶劑。作為溶劑,可列舉:N-甲基-2-吡咯啶酮、γ-丁內酯、N,N-二甲基甲醯胺、N,N-二甲基乙醯胺、二甲基亞碸等極性的非質子性溶媒,四氫呋喃、二噁烷、丙二醇單甲醚等醚類,丙酮、甲基乙基酮、二異丁酮、二丙酮醇等酮類,乙酸乙酯、丙二醇單甲醚乙酸酯、乳酸乙酯等酯類,甲苯、二甲苯等芳香族烴類等。可含有該些的兩種以上。
相對於蝕刻用罩幕抗蝕劑組成物中的樹脂整體100重量份,溶劑的含量較佳為50重量份以上,更佳為100重量份以上,
另外,較佳為5000重量份以下,更佳為3000重量份以下。
本發明的蝕刻用罩幕抗蝕劑組成物亦可含有界面活性劑。藉由含有界面活性劑,改善塗佈不均而可獲得均勻的塗佈膜。
較佳為使用氟系界面活性劑、或矽酮系界面活性劑。
作為氟系界面活性劑的具體例,可列舉包含以下化合物的氟系界面活性劑:1,1,2,2-四氟辛基(1,1,2,2-四氟丙基)醚、1,1,2,2-四氟辛基己基醚、八乙二醇二(1,1,2,2-四氟丁基)醚、六乙二醇(1,1,2,2,3,3-六氟戊基)醚、八丙二醇二(1,1,2,2-四氟丁基)醚、六丙二醇二(1,1,2,2,3,3-六氟戊基)醚、全氟十二烷基磺酸鈉、1,1,2,2,8,8,9,9,10,10-十氟十二烷、1,1,2,2,3,3-六氟癸烷、N-[3-(全氟辛烷磺醯胺)丙基]-N,N'-二甲基-N-羧基亞甲基銨甜菜鹼、全氟烷基磺醯胺丙基三甲基銨鹽、全氟烷基-N-乙基磺醯基甘胺酸鹽、磷酸雙(N-全氟辛基磺醯基-N-乙基胺基乙基)、單全氟烷基乙基磷酸酯等在末端、主鏈及側鏈的至少任一部位具有氟烷基或氟伸烷基的化合物。
另外,作為市售品,有:美佳法(Megafac)F142D、美佳法(Megafac)F172、美佳法(Megafac)F173、美佳法(Megafac)F183、美佳法(Megafac)F444、F477(以上為大日本油墨化學工業(股)製造),艾福拓(Eftop)EF301、艾福拓(Eftop)303、艾福拓(Eftop)352(新秋田化成(股)製造),弗拉德(Fluorad)FC-430、弗拉德(Fluorad)FC-431(住友3M(股)製造)),阿薩佳(Asahi Guard)AG710、沙福隆(Surflon)S-382、沙福隆
(Surflon)SC-101、沙福隆(Surflon)SC-102、沙福隆(Surflon)
SC-103、沙福隆(Surflon)SC-104、沙福隆(Surflon)SC-105、沙福隆(Surflon)SC-106(旭硝子(股)製造),BM-1000、BM-1100(裕商(股)製造),NBX-15、FTX-218、DFX-18(尼歐斯(Neos)(股)製造)等氟系界面活性劑。
作為矽酮系界面活性劑的市售品,可列舉:SH28PA、SH7PA、SH21PA、SH30PA、ST94PA(均為東麗.道康寧.矽酮(股)(Toray Dow Corning Silicone Co.,Ltd.)製造),BYK-333(日本畢克化學(BYK-Chemie Japan)(股)製造)等。
蝕刻用罩幕抗蝕劑組成物中,界面活性劑的含量通常設為0.0001重量%~1重量%。
本發明的蝕刻用罩幕抗蝕劑組成物亦可含有在用作曝光波長的紫外線區域具有吸收、且不會藉由該光而褪色的化合物。
藉由含有此種化合物,於對所獲得的正型感光性蝕刻用罩幕抗蝕劑組成物進行曝光而進行圖案形成時,吸收由曝光機照射的曝光波長,因此可防止由來自基板的反射光所引起的過度曝光或光暈,可提高顯影時的未曝光部的黏接性。
作為所述具有吸收特性的化合物,例如可列舉:香豆素衍生物、苯并三唑衍生物、羥基二苯甲酮衍生物、蒽醌衍生物、乙烷合萘衍生物等。香豆素衍生物可列舉:香豆素、香豆素-4(以上為商品名,日本西格瑪奧德里奇(Sigma-Aldrich Japan)(股)製造),4-羥基香豆素、7-羥基香豆素(以上為東京化成工業(股)
製造);苯并三唑衍生物可列舉:斯密索布(Sumisorb)200、斯密索布(Sumisorb)250、斯密索布(Sumisorb)320、斯密索布(Sumisorb)340、斯密索布(Sumisorb)350(以上為商品名,住友化學工業(股)製造);羥基二苯甲酮衍生物可列舉:斯密索布(Sumisorb)130、斯密索布(Sumisorb)140(以上為商品名,住友化學工業(股)製造),茲斯萊澤(Zislizer)M、茲斯萊澤(Zislizer)O(商品名,三協化成(股)製造),西索布(Seesorb)103(西普洛化成(Shipro Kasei)(股)製造);蒽醌衍生物可列舉:1-羥基蒽醌、2-羥基蒽醌、3-羥基蒽醌、1-羥基-2-甲氧基蒽醌、1,2-二羥基蒽醌、1,3-二羥基蒽醌、1,4-二羥基蒽醌、1,5-二羥基蒽醌、1,8-二羥基蒽醌、1,3-二羥基-3-甲基蒽醌、1,5-二羥基-3-甲基蒽醌、1,6-二羥基-3-甲基蒽醌、1,7-二羥基-3-甲基蒽醌、1,8-二羥基-3-甲基蒽醌、1,8-二羥基-2-甲基蒽醌、1,3-二羥基-2-甲氧基蒽醌、2,4-二羥基-1-甲氧基蒽醌、2,5-二羥基-1-甲氧基蒽醌、2,8-二羥基-1-甲氧基蒽醌、1,8-二羥基-3-甲氧基-6-甲基蒽醌、1,2,3-三羥基蒽醌、1,3,5-三羥基蒽醌、2-胺基蒽醌、2-胺基-1-硝基蒽醌、2,6-二胺基蒽醌、1-甲氧基蒽醌、2-甲氧基蒽醌、1,8-二甲氧基蒽醌、1-乙醯基胺基蒽醌、2-乙醯基胺基蒽醌、2-第三丁基蒽醌;乙烷合萘化合物可列舉:5-硝基乙烷合萘等。
繼而,本發明的蝕刻用罩幕抗蝕劑組成物亦可視需要而含有:交聯劑、交聯促進劑、增感劑、熱自由基產生劑、溶解促進劑、溶解抑制劑、穩定劑、消泡劑等添加劑。
<蝕刻用罩幕抗蝕劑組成物的製造方法>
對本發明的蝕刻用罩幕抗蝕劑組成物的製造方法進行說明。將聚醯亞胺或酚樹脂等樹脂成分、光酸產生劑、其他添加劑添加至溶媒中並使其溶解。作為順序,較佳為使樹脂成分溶解後,使其他成分溶解。溶解溫度為-5℃~60℃,較佳為10℃~50℃,更佳為20℃~40℃。視需要追加溶媒並進行稀釋而調整組成物的黏度。其後,於常溫下靜置1小時~24小時並進行脫泡,利用0.1μm~10μm的細孔徑的過濾器進行過濾而去除異物。
<經圖案加工的基板的製造方法>
使用本發明的蝕刻用罩幕抗蝕劑組成物的經圖案加工的基板的製造方法包括:設置所述蝕刻用罩幕抗蝕劑組成物的被膜的步驟;形成所述被膜的硬化圖案的步驟;以所述被膜的硬化圖案作為罩幕,藉由蝕刻而對基板進行圖案加工的步驟;以及將所述被膜的硬化圖案去除的步驟。
首先,利用旋塗法、狹縫塗佈法等公知的方法,將本發明的蝕刻用罩幕抗蝕劑組成物塗佈於基板上。
基板可使用:包含選自由鋁、矽、鈦、鉭、鎵、鍺、鐵、鎳、鋅、銦、硼、錳、磷、鈷及鋯所組成的群組中的至少一種元素的基板,或者該些形成於塗佈面上的基板等,但並不限定於該些。該些基板中,較佳為選自由藍寶石(Al2O3)、矽(Si)、氧化矽(SiO2)、氮化矽(SiN)、氮化鎵(GaN)、碳化矽(SiC)、砷化鎵(GaAs)、磷化銦(InP)、氮化鋁(AlN)、氮化鉭(TaN)、鉭
酸鋰(LiTaO3)、氮化硼(BN)、氮化鈦(TiN)、以及鈦酸鋇(BaTiO3)所組成的群組中的基板。
塗佈方法有:使用旋轉器的旋轉塗佈、噴霧塗佈、輥塗佈等方法。另外,塗佈膜厚根據塗佈方法、組成物的固體成分濃度、黏度等而不同,但通常較佳為乾燥後的膜厚為0.1μm~150μm。
為了提高矽晶圓等基板與蝕刻用罩幕抗蝕劑組成物的黏接性,亦可利用所述矽烷偶合劑對基板進行預處理。例如,將使矽烷偶合劑於異丙醇、乙醇、甲醇、水、四氫呋喃、丙二醇單甲醚乙酸酯、丙二醇單甲醚、乳酸乙酯、己二酸二乙酯等溶媒中溶解0.5重量%~20重量%而成的溶液,藉由旋塗、浸漬、噴霧塗佈、蒸氣處理等來進行表面處理。視情況,然後進行50℃~300℃為止的熱處理,進行基板與矽烷偶合劑的反應。
繼而,將塗佈有蝕刻用罩幕抗蝕劑組成物的基板加以乾燥而獲得蝕刻用罩幕抗蝕劑組成物被膜。乾燥較佳為使用烘箱、加熱板、紅外線等,於50℃~150℃的範圍內進行1分鐘~數小時。
繼而,通過具有所需的圖案的罩幕對該蝕刻用罩幕抗蝕劑組成物被膜照射化學射線,進行曝光。曝光中所使用的化學射線有紫外線、可見光線、電子束、X射線等,本發明中較佳為波長350nm以上且450nm以下的光,較佳為使用水銀燈的i射線(波長365nm)、h射線(波長405nm)、g射線(波長436nm)。
為了形成蝕刻用罩幕抗蝕劑組成物被膜的圖案,而於曝
光後使用顯影液去除曝光部。顯影液較佳為鹼性顯影液,較佳為氫氧化四甲基銨、二乙醇胺、二乙基胺基乙醇、氫氧化鈉、氫氧化鉀、碳酸鈉、碳酸鉀、三乙基胺、二乙基胺、甲基胺、二甲基胺、乙酸二甲基胺基乙酯、二甲基胺基乙醇、甲基丙烯酸二甲基胺基乙酯、環己基胺、乙二胺、六亞甲基二胺等顯示出鹼性的化合物的水溶液。另外,視情況,亦可於該些鹼性水溶液中單獨添加:N-甲基-2-吡咯啶酮、N,N-二甲基甲醯胺、N,N-二甲基乙醯胺、二甲基亞碸、γ-丁內酯、二甲基丙烯醯胺等極性溶媒,甲醇、乙醇、異丙醇等醇類,乳酸乙酯、丙二醇單甲醚乙酸酯等酯類,環戊酮、環己酮、異丁酮、甲基異丁酮等酮類等,或者可添加將數種組合而成者。顯影後較佳為利用水進行淋洗處理。此處,亦可將乙醇、異丙基醇等醇類,乳酸乙酯、丙二醇單甲醚乙酸酯等酯類等添加於水中來進行淋洗處理。
藉由將所獲得的蝕刻用罩幕抗蝕劑組成物被膜圖案進一步固化(cure),可獲得硬化圖案。例如,藉由利用加熱板、烘箱等加熱裝置,於100℃~450℃的範圍內固化30秒~2小時左右,來形成硬化圖案。較佳為120℃~250℃,更佳為180℃~230℃。
硬化圖案的剖面形狀不為矩形,較佳為曲面狀,特佳為半圓狀。藉由為半圓狀,光散射變大,可提高發光元件的光取出效率。
所謂此處所述的半圓狀,是指剖面形狀中的圖案高度為圖案底邊的長度以下且由凸型突起的曲線形成剖面形狀的狀態。
以所述由本發明的蝕刻用罩幕抗蝕劑組成物形成的硬化圖案作為罩幕並實施蝕刻處理,藉此可於基板上設置所需的凹凸圖案。
蝕刻方法有利用溶液的濕式蝕刻、利用氣體的乾式蝕刻等,但就所獲得的凹凸圖案的面內均勻性的觀點而言,較佳為使用乾式蝕刻。
關於乾式蝕刻處理中所使用的氣體,可使用三氯化硼(BCl3)、氯(Cl2)、四氟化碳(CF4)、三氟化甲烷(CHF3)、4-(二氟亞甲基)-2,3,3-三氟-1-(三氟甲基)環丁烯(C6F8)、六氟銻(SbF6)、氧(O2)、氬(Ar)等,自基板的蝕刻穩定性的觀點而言,較佳為使用氯、三氯化硼。
另外,為了提高基板的乾式蝕刻速度,乾式蝕刻時的溫度較佳為100℃~250℃,更佳為120℃~230℃,最佳為150℃~200℃。
蝕刻後的基板的凹凸圖案的剖面形狀不為矩形,較佳為曲面狀,特佳為半圓狀。藉由為半圓狀,光散射變大,可提高發光元件的光取出效率。
所謂此處所述的半圓狀,是指剖面形狀中的圖案高度為圖案底邊的長度以下且由凸型突起的曲線形成剖面形狀的狀態。
特別是藉由成為罩幕的硬化圖案的剖面形狀為半圓狀,蝕刻後的基板的凹凸圖案的剖面形狀亦可形成為半圓狀,因此較佳。
由本發明的蝕刻用罩幕抗蝕劑組成物形成的硬化圖案及乾式蝕刻處理後的抗蝕劑殘渣是使用抗蝕劑剝離液於乾式蝕刻後去除。
去除方法較佳為:利用噴淋、浸漬、覆液等方法,於常溫~100℃下,於抗蝕劑剝離液中浸漬5秒~24小時。
抗蝕劑剝離液可使用公知的抗蝕劑剝離液,具體例可列舉:剝離液104、剝離液105、剝離液106、SST-3(以上為商品名,東京應化工業(股)製造),EKC-265、EKC-270、EKC-270T(以上為商品名,杜邦(Dupont)(股)製造),N-300、N-321(以上為商品名,長瀨化成(Nagase ChemteX)(股)製造)等。
另外,於去除後,較佳為以水或有機溶媒進行淋洗,視需要,亦可利用加熱板、烘箱等加熱裝置,於50℃~150℃的範圍內進行乾燥烘烤。
<發光元件(二極體)的製造方法>
可使用本發明的蝕刻用罩幕抗蝕劑組成物於經加工的形成有凹凸圖案的基板的凹凸面上形成發光層,來製造發光二極體。
發光層可列舉選自由包含GaN或AlN的緩衝層、n型GaN層、InGaN發光層或者包含p型AlGaN的包層、以及p型GaN接觸層所組成的群組中的至少一層作為較佳例。
例如,將加工後的藍寶石基板安裝於有機金屬氣相沈積裝置(MOCVD裝置,Metal Organic Chemical Vapor Deposition)上,於氮氣主成分環境下,以1000度以上的高溫進行熱清洗
(thermal cleaning),使GaN低溫緩衝層、n-GaN層、InGaN層、
p-AlGaN層、p-GaN層依次成長。然後,藉由蝕刻使n-GaN露出,於n-GaN層、及p-GaN層上分別形成電極。藉由切割,對形成有電極的基板實施元件分離,藉此形成LED發光元件。
本發明的蝕刻用罩幕抗蝕劑組成物亦適合用作以所述n-GaN層的露出為目的的乾式蝕刻用光致抗蝕劑。
[實施例]
以下,列舉實施例,對本發明進一步進行具體說明,但本發明並不限定於該些實施例。再者,所使用的化合物中,使用略語者示於以下。
NMP:N-甲基-2-吡咯啶酮
GBL:γ-丁內酯
各評價是利用以下的方法來進行。
(1)醯亞胺基當量的算出
醯亞胺基當量是如以下般算出。將結構單元中的醯亞胺基數設為A(莫耳),將結構單元的分子量設為B(g)。
關於A、B,例如於為下述結構單元的情況下,分別為A=2、B=534。
另外,於為下述結構單元的情況下,為A=2、B=836。
醯亞胺基當量是由A/B表示的值。
(2)重量平均分子量
使用GPC(凝膠滲透層析法)裝置沃特斯(Waters)2690-996(日本沃特斯(Waters)(股)製造)並將展開溶媒設為N-甲基-2-吡咯啶酮來進行測定,進而以聚苯乙烯換算計來計算重量平均分子量(Mw)。
(3)預烘烤後抗蝕劑膜、抗蝕劑硬化圖案膜、乾式蝕刻前後的硬化圖案膜的膜厚
使用光干擾式膜厚計(大日本網屏(Dainippon Screen)(股份)製造的拉姆達艾斯(lambda ace)STM-602)並於折射率1.629下進行測定。
(4)感光感度
使用旋塗機(米卡薩(Mikasa)(股)製造的1H-360S),並以任意的轉數將蝕刻用罩幕抗蝕劑組成物旋塗於直徑為2英吋的單晶藍寶石晶圓上後,使用加熱板(亞速旺(AS ONE)(股)製造的HP-1SA),於120℃下預烘烤3分鐘,製作膜厚為3.0μm的蝕刻用罩幕抗蝕劑組成物被膜。
對於所製作的該組成物被膜,使用i射線步進機(尼康(Nikon)(股)公司製造的NSR-2009i9C),以0mJ/cm2~500mJ/cm2的曝光量,以20mJ/cm2的階差進行曝光。曝光中使用的網線是使用線與空間圖案中,獲得1、2、3、4、5、6、7、8、9、10、15、20、30、50、100μm者。
曝光後,使用自動顯影裝置(瀧澤產業(股)製造的AD-2000),以2.38質量%氫氧化四甲基銨水溶液進行60秒噴淋顯影,繼而以水淋洗30秒。將圖案顯影後3μm的線與空間圖案開口的曝光量作為感光感度。
(5)固化後硬化圖案的形狀
利用與(4)相同的方法進行至顯影為止,使用加熱板(亞速旺(AS ONE)(股)製造的HP-1SA),將該基板以既定的溫度、時間進行固化而進行硬化圖案形成。利用掃描電子顯微鏡(scanning electron microscope,SEM)觀察感光感度+20mJ/cm2的曝光量下的3μm的線圖案的剖面,若剖面為半圓狀,則為良,若並非如此,則為不良。
(6)耐乾式蝕刻性
利用與(5)相同的方法進行至硬化圖案的形成為止,使用乾式蝕刻裝置(莎姆克(Samco)(股)製造的RIE-200NL-101iPH),將該帶圖案的藍寶石基板於既定的溫度下,利用三氯化硼進行蝕刻。
當將乾式蝕刻前後的硬化圖案的膜厚分別設為T1、T2,且將藉由乾式蝕刻而蝕刻的藍寶石基板的深度設為T3時,算出蝕刻選擇比、(T1-T2)/T3,選擇比越高,設為越為高耐性。
(7)乾式蝕刻後的硬化圖案去除性
將乾式蝕刻後的硬化圖案以常溫浸漬於剝離液106(東京應化工業(股)製造,單乙醇胺:二甲基亞碸=70:30)中,然後以水進行30秒淋洗。然後,使用光學顯微鏡(尼康(Nikon)(股)製造的OPTISHOT300)來觀察基板上的蝕刻用罩幕抗蝕劑組成物被膜圖案有無殘留,為了去除圖案而必需的最低浸漬時間越短,設為越良好的去除性。
(合成例1)聚醯亞胺(PI-01)的合成
於乾燥氮氣流下,將15.9g(0.043莫耳)的2,2-雙(3-胺基-4-羥基苯基)六氟丙烷(中央玻璃(Central Glass)(股)製造,BAHF)、0.62g(0.0025莫耳)的1,3-雙(3-胺基丙基)四甲基二矽氧烷(SiDA)溶解於130g的NMP中。於其中,與50g的NMP一併添加15.5g(0.05莫耳)的3,3',4,4'-二苯基醚四羧酸二酐(馬納克(Manac)(股)製造,ODPA),於40℃下攪拌2小時。然後,添加1.09g
(0.01莫耳)的3-胺基苯酚(東京化成(股)製造),於40℃下
攪拌2小時。進而,於200℃下繼續攪拌6小時。攪拌結束後,將溶液投入至2L的水中,將聚合物固體的沈澱物過濾收集。進而以2L的水進行3次洗滌,將收集的聚合物固體於50℃的真空乾燥機中乾燥72小時,獲得聚醯亞胺(PI-01)。PI-01的醯亞胺基當量為0.0032莫耳/g,重量平均分子量為40000。
(合成例2)聚醯亞胺(PI-02)的合成
代替15.5g(0.05莫耳)的ODPA而添加14.7g(0.05莫耳)的2,2',3,3'-聯苯四羧酸二酐(東麗精細化學(Toray Fine Chemicals)(股)製造,i-BPDA),除此以外與合成例1同樣地進行而獲得聚醯亞胺(PI-02)。PI-02的醯亞胺基當量為0.0033莫耳/g,重量平均分子量為35000。
(合成例3)聚醯亞胺(PI-03)的合成
代替15.5g(0.05莫耳)的ODPA而添加10.9g(0.05莫耳)的均苯四甲酸酐(大賽璐(Daicel)化學(股)製造,PMDA),除此以外與合成例1同樣地進行而獲得聚醯亞胺(PI-03)。PI-03的醯亞胺基當量為0.0037莫耳/g,重量平均分子量為50000。
(合成例4)聚醯亞胺(PI-04)的合成
代替15.5g(0.05莫耳)的ODPA而添加13.4g(0.05莫耳)的1,2,5,6-萘四羧酸二酐(東京化成(股)製造),除此以外與合成例1同樣地進行而獲得聚醯亞胺(PI-04)。PI-04的醯亞胺基當量為0.0034莫耳/g,重量平均分子量為40000。
(合成例5)聚醯亞胺(PI-05)的合成
代替15.5g(0.05莫耳)的ODPA而添加26.0g(0.05莫耳)的2,2-雙[4-(3,4-二羧基苯氧基)苯基]丙烷二酐(東京化成(股)製造),除此以外與合成例1同樣地進行而獲得聚醯亞胺(PI-05)。
PI-05的醯亞胺基當量為0.0024莫耳/g,重量平均分子量為45000。
(合成例6)聚醯亞胺(PI-06)的合成
代替15.9g(0.043莫耳)的BAHF、1.09g(0.01莫耳)的3-胺基苯酚而添加17.4g(0.047莫耳)的BAHF、0.109g(0.001莫耳)的3-胺基苯酚,除此以外與合成例1同樣地進行而獲得聚醯亞胺(PI-06)。PI-06的醯亞胺基當量為0.0032莫耳/g,重量平均分子量為90000。
(合成例7)聚醯亞胺(PI-07)的合成
代替15.9g(0.043莫耳)的BAHF、1.09g(0.01莫耳)的3-胺基苯酚而添加11.1g(0.03莫耳)的BAHF、3.82g(0.035莫耳)的3-胺基苯酚,除此以外與合成例1同樣地進行而獲得聚醯亞胺(PI-07)。PI-07的醯亞胺基當量為0.0033莫耳/g,重量平均分子量為4000。
(合成例8)聚醯亞胺(PI-08)的合成
代替1.09g(0.01莫耳)的3-胺基苯酚而添加1.93g(0.01莫耳)的2-胺基蒽,除此以外與合成例1同樣地進行而獲得聚醯亞胺(PI-08)。PI-08的醯亞胺基當量為0.0032莫耳/g,重量平均分子量為41000。
(合成例9)聚醯亞胺(PI-09)的合成
代替1.09g(0.01莫耳)的3-胺基苯酚、15.5g(0.05莫耳)的ODPA而添加1.93g(0.01莫耳)的2-胺基蒽、14.7g(0.05莫耳)的2,2',3,3'-聯苯四羧酸二酐(東麗精細化學(Toray Fine Chemicals)(股)製造,i-BPDA),除此以外與合成例1同樣地進行而獲得聚醯亞胺(PI-09)。PI-09的醯亞胺基當量為0.0033莫耳/g,重量平均分子量為37000。
(合成例10)聚醯亞胺前驅物(PAE-01)的合成
於乾燥氮氣流下,將15.9g(0.043莫耳)的BAHF、0.62g(0.0025莫耳)的SiDA溶解於200g的NMP中。於其中,與50g的NMP一併添加15.5g(0.05莫耳)的ODPA,於40℃下攪拌2小時。然後,添加1.09g(0.01莫耳)的3-胺基苯酚,於40℃下攪拌2小時。進而,花10分鐘滴加將3.57g(0.03莫耳)的二甲基甲醯胺二甲基縮醛(三菱麗陽(股)製造,DFA)以5g的NMP稀釋而成的溶液,滴加後,於40℃下繼續攪拌2小時,繼而於100℃下繼續攪拌0.5小時。攪拌結束後,將溶液投入至2L的水中,將聚合物固體的沈澱物過濾收集。進而以2L的水進行3次洗滌,將收集的聚合物固體於50℃的真空乾燥機中乾燥72小時,獲得聚醯亞胺前驅物(PAE-01)。該聚醯亞胺前驅物的重量平均分子量為42000。
(合成例11)含羥基的二胺化合物(DA-01)的合成
將18.3g(0.05莫耳)的BAHF溶解於100mL的丙酮、17.4
g(0.3莫耳)的環氧丙烷(東京化成(股)製造)中,冷卻至-15℃。於其中滴加使20.4g(0.11莫耳)的3-硝基苯甲醯氯(東京化成(股)製造)溶解於100mL的丙酮中的溶液。滴加結束後,於-15℃下攪拌4小時,然後恢復至室溫。將析出的白色固體過濾分離,於50℃下進行真空乾燥。
將所獲得的30g白色固體加入至300mL的不鏽鋼高壓釜中,分散於250mL的甲基溶纖劑中,添加2g的5%鈀-碳(和光純藥工業(股)製造)。於其中,利用氣球來導入氫,於室溫下進行還原反應。約2小時後,確認氣球不再縮小而使反應結束。
反應結束後,進行過濾而去除作為觸媒的鈀化合物,利用旋轉蒸發器進行濃縮,獲得下述式所表示的含羥基的二胺化合物(DA-01)。
(合成例12)聚醯亞胺前驅物(PAE-02)的合成
於乾燥氮氣流下,將合成例11中獲得的25.7g(0.043莫耳)的含羥基的二胺化合物(DA-01)、0.62g(0.0025莫耳)的SiDA
溶解於200g的NMP中。於其中,與50g的NMP一併添加15.5g(0.05莫耳)的ODPA,於40℃下攪拌2小時。然後,添加1.17g(0.01莫耳)的4-乙炔基苯胺(東京化成(股)製造),於40℃下攪拌2小時。進而,花10分鐘滴加將3.57g(0.03莫耳)的DFA以5g的NMP稀釋而成的溶液,滴加後,於40℃下繼續攪拌2小時。攪拌結束後,將溶液投入至2L的水中,將聚合物固體的沈澱物過濾收集。進而以2L的水進行3次洗滌,將收集的聚合物固體於50℃的真空乾燥機中乾燥72小時,獲得聚醯亞胺前驅物(PAE-02)。該聚醯亞胺前驅物的重量平均分子量為45000。
(合成例13)萘醌二疊氮化合物(QD-01)的合成
於乾燥氮氣流下,使21.23g(0.05mol)的TrisP-PA(商品名,本州化學工業(股)製造)及37.62g(0.14mol)的4-萘醌二疊氮磺醯基醯氯溶解於450g的1,4-二噁烷中,設為室溫。於其中,以系統內不成為35℃以上的方式滴加與50g的1,4-二噁烷混合的15.58g(0.154mol)的三乙基胺。滴加後於30℃下攪拌2小時。將三乙基胺鹽過濾,使濾液投入至水中。然後,將析出的沈澱物過濾收集。使該沈澱物於真空乾燥機中進行乾燥,獲得下述結構的萘醌二疊氮化合物(QD-01)。
(合成例14)酚醛清漆樹脂(NV-01)的合成
於乾燥氮氣流下,添加57g(0.6莫耳)的間甲酚、38g(0.4莫耳)的對甲酚、75.5g(甲醛0.93莫耳)的37重量%甲醛水溶液、0.63g(0.005莫耳)的乙二酸二水合物、264g的甲基異丁酮後,浸漬於油浴中,一邊使反應液回流,一邊進行4小時縮聚反應。然後,花3小時使油浴的溫度升溫,然後,將燒瓶內的壓力減壓至30mmHg~50mmHg,去除揮發成分並進行溶解。將樹脂冷卻至室溫,獲得鹼可溶性的酚醛清漆樹脂(NV-01)的聚合物固體85g。
(實施例1)
將10g(100重量份)的合成例1中獲得的聚醯亞胺(PI-01)、2.0g(20重量份)的合成例9中獲得的萘醌二疊氮化合物(QD-01)、41.3g的作為溶劑的GBL混合、攪拌後,利用0.5μm的過濾器進行過濾來製備蝕刻用罩幕抗蝕劑組成物。對於該組成物,利用所述(1)~(7)的評價方法來實施評價。硬化圖案形成的固化條件(抗蝕劑硬化條件)為於160℃下進行5分鐘,乾式蝕刻時的溫度是設為150℃。將結果示於表1中。
(實施例2~實施例20、比較例1~比較例4)
以與實施例1相同的方式,製備蝕刻用罩幕抗蝕劑組成物,進行評價。將組成、抗蝕劑硬化條件、乾式蝕刻時的溫度、各評價結果示於表1中。再者,表1中的化合物PAG-01、PHH-01分別為下述結構的化合物。
Claims (16)
- 如申請專利範圍第1項所述的基板的製造方法,其中所述聚醯亞胺(A)的重量平均分子量為5000~80000。
- 如申請專利範圍第1項或第2項所述的基板的製造方法,其中所述(B)光酸產生劑包含醌二疊氮化合物及鎓鹽。
- 如申請專利範圍第1項或第2項所述的基板的製造方法,其中所述蝕刻用罩幕抗蝕劑組成物進而包含(C)選自通式(5)、通式(6)中的至少一種,
- 如申請專利範圍第1項或第2項所述的基板的製造方法,其中所述蝕刻用罩幕抗蝕劑組成物進而包含(D)選自酚樹 脂、多羥基苯乙烯中的至少一種。
- 如申請專利範圍第1項或第2項所述的基板的製造方法,其中所述基板包含選自由鋁、矽、鈦、鉭、鎵、鍺、鐵、 鎳、鋅、銦、硼、錳、磷、鈷及鋯所組成的群組中的至少一種元素。
- 如申請專利範圍第1項或第2項所述的基板的製造方法,其中所述基板為選自由藍寶石(Al2O3)、矽(Si)、氧化矽(SiO2)、氮化矽(SiN)、氮化鎵(GaN)、碳化矽(SiC)、砷化鎵(GaAs)、磷化銦(InP)、氮化鋁(AlN)、氮化鉭(TaN)、鉭酸鋰(LiTaO3)、氮化硼(BN)、氮化鈦(TiN)及鈦酸鋇(BaTiO3)所組成的群組中者。
- 如申請專利範圍第1項或第2項所述的基板的製造方法,其中對所述蝕刻用罩幕抗蝕劑組成物的被膜進行圖案加工的步驟包括使用波長為350nm以上且450nm以下的光進行圖案曝光的步驟、以及進行顯影的步驟。
- 如申請專利範圍第1項或第2項所述的基板的製造方法,其中所述蝕刻用罩幕抗蝕劑組成物的被膜的圖案的剖面形狀為半圓狀。
- 如申請專利範圍第1項或第2項所述的基板的製造方法,其中所述蝕刻為乾式蝕刻。
- 如申請專利範圍第13項所述的基板的製造方法,其中所述蝕刻所使用的蝕刻氣體包含選自氯、三氯化硼中的至少一種。
- 如申請專利範圍第13項所述的基板的製造方法,其中所述乾式蝕刻時的溫度為100℃~250℃。
- 一種發光元件的製造方法,其包括如下步驟:於利用如申請專利範圍第1項至第15項中任一項所述的方法所獲得的基板上,製膜選自由包含GaN或AlN的緩衝層、n型GaN層、InGaN發光層、p型AlGaN包層、p型GaN接觸層所組成的群組中的至少一層。
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