TWI583724B - 具有碸結構及胺結構之含有矽之阻劑底層膜形成組成物 - Google Patents
具有碸結構及胺結構之含有矽之阻劑底層膜形成組成物 Download PDFInfo
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- TWI583724B TWI583724B TW102121964A TW102121964A TWI583724B TW I583724 B TWI583724 B TW I583724B TW 102121964 A TW102121964 A TW 102121964A TW 102121964 A TW102121964 A TW 102121964A TW I583724 B TWI583724 B TW I583724B
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Classifications
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- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
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Description
本發明係關於新穎矽烷化合物。且本發明係關於使用於半導體裝置之製造的用以於基板與阻劑(例如光阻、電子束阻劑、EUV阻劑)之間形成底層膜之組成物。詳而言之,係關於用以於半導體裝置製造之微影術步驟中形成使用於光阻之底層的底層膜之微影術用阻劑底層膜形成組成物。又,係關於使用了該底層膜形成組成物之阻劑圖型之形成方法。
自以往的半導體裝置製造中,係進行使用了光阻之微影術的微細加工。前述微細加工係為於矽晶圓等半導體基板上形成光阻之薄膜,於其上透過描繪有半導體裝置之圖型的遮罩圖型照射紫外線等之活性光線,並顯影,以所得之光阻圖型作為保護膜對基板蝕刻處理,藉以於基板表面形成對應於前述圖型之微細凹凸的加工法。
近年來,半導體裝置之高積體度化有所進展,所使用之活性光線亦有從KrF準分子雷射(248nm)朝向ArF準分子雷射(193nm)、EUV光(13.5nm)之短波長化的傾向。伴隨於此,活性光線自半導體基板之反射的影響係變成大的問題。
因此,近年來的半導體裝置的製造中,以抗反射效果為始,為了達成各種效果,係成為在半導體基板與光阻之間配置阻劑底層膜。
例如,作為半導體基板與光阻之間的底層膜,係進行使用已知作為含有矽等金屬元素的硬遮罩之膜(例如參照專利文獻1)。此時,阻劑與硬遮罩,其構成成分有很大的不同,因此藉由乾蝕刻去除該等的速度,係大幅依賴乾蝕刻所使用之氣體種類。再者,藉由適當地選擇氣體種類,可在不伴隨光阻膜厚之大幅減少之下,藉由乾蝕刻去除硬遮罩。如此地,雖進行了阻劑底層膜用之組成物的探討,但由其所要求之特性的多樣性等,尚期望阻劑底層膜用之新材料的開發。
又,由別的觀點來看,亦有將基板表面改質的方法。例如,揭示有使用具有碸基之矽烷偶合劑,將曝光後之表面變化為親水性的方法(參照專利文獻2)。
又,揭示有具有磺醯胺基之含有矽之阻劑底層膜(參照專利文獻3、4)。
[先前技術文獻]
[專利文獻]
[專利文獻1]國際公開WO2011-033965
[專利文獻2]日本特開2005-112732號公報
[專利文獻3]日本特開2009-244722號公報
[專利文獻4]國際公開WO2011-033965
本發明之目的,係提供可進行利用了矩形阻劑圖型之微細的基板加工,且可使用於半導體裝置製造之微影術用阻劑底層膜形成組成物。詳言之,係提供用以形成可使用作為硬遮罩之阻劑底層膜之微影術用阻劑底層膜形成組成物。又,係提供用以形成可使用作為抗反射膜之阻劑底層膜之微影術用阻劑底層膜形成組成物。又,係提供不引起與阻劑之互混,相較於阻劑具有大的乾蝕刻速度之微影術用阻劑底層膜及用以形成該底層膜之阻劑底層膜形成組成物。又,本發明之目的係提供可使用於該等之微影術用阻劑底層膜形成組成物的新穎化合物。
本發明之第1觀點,係關於以下述式(1-a)或以式(1-b)表示之矽烷化合物
(式(1-a)中,R1、R3、及R4當中之至少1個基,表示碳原子數1至10之伸烷基的末端鍵結有-Si(X)3基之基,剩餘之基表示氫原子、碳原子數1至10之烷基、或碳原子數6至40之芳基,R2表示碳原子數1至10之伸烷基、或碳原子數6至40之伸芳基。惟上述X表示烷氧基、醯氧基、或鹵素原子。
式(1-b)中,R6、R7、R9、及R10當中之至少1個基,表示碳原子數1至10之伸烷基之末端鍵結有-Si(X)3基之基,剩餘之基表示氫原子、碳原子數1至10之烷基、或碳原子數6至40之芳基,R5及R8表示碳原子數1至10之伸烷基、或碳原子數6至40之伸芳基。惟上述X表示烷氧基、醯氧基、或鹵素原子);
第2觀點,係關於一種微影術用阻劑底層膜形成組成物,其係至少含有水解性有機矽烷、其水解物及其水解縮合物當中之至少1種作為矽烷,且該矽烷包含如請求項1記載之以式(1-a)或以式(1-b)表示之矽烷化合物;
第3觀點,係如第2觀點之阻劑底層膜形成組成物,
其中上述以式(1-a)表示之矽烷化合物係以下述式(2):
(式(2)中,R1及R4表示氫原子、碳原子數1至10之烷基、或碳原子數6至40之芳基,R2表示碳原子數1至10之伸烷基、或碳原子數6至40之伸芳基,R11表示碳原子數1至10之伸烷基,X表示烷氧基、醯氧基、或鹵素原子)表示之矽烷化合物;第4觀點,係如請求項2或請求項3之微影術用阻劑底層膜形成組成物,其中前述矽烷係包含:由以式(3):【化3】R21 aSi(R22)4-a 式(3)
(式(3)中,R21為烷基、芳基、芳烷基、鹵化烷基、鹵化芳基、鹵化芳烷基、烯基、或環氧基、丙烯醯基、甲基丙烯醯基、巰基、烷氧基芳基、醯氧基氫芳基、三聚異氰酸酯基、羥基、環狀胺基、或具有氰基之有機基、或該等之組合,且係藉由Si-C鍵與矽原子鍵結者,R22表示烷氧基、醯氧基、或鹵素原子,a表示0至3之整數)表示之有機矽化合物、及以式(4):
【化4】〔R31 cSi(R32)3-c〕2Yb 式(4)
(式(4)中,R31表示烷基,R32表示烷氧基、醯氧基、或鹵素原子,Y表示伸烷基或伸芳基,b表示0或1之整數,c表示0或1之整數)表示之有機矽化合物所構成群組中選出之至少1種有機矽化合物與上述式(1-a)或以式(1-b)表示之矽烷化合物之組合;該等之水解物;及該等之水解縮合物當中之至少1種;第5觀點,係如第2觀點至第4觀點中任一者之組成物,其係含有以上述式(1-a)或以式(1-b)表示之矽烷化合物之水解縮合物、及以式(1-a)或以式(1-b)表示之矽烷化合物與以式(3)表示之有機矽化合物之水解縮合物當中至少1種作為聚合物;第6觀點,係如第2觀點至第5觀點中任一者之組成物,其係進一步含有酸;第7觀點,係如第2觀點至第6觀點中任一者之組成物,其係進一步含有水;第8觀點,係關於一種阻劑底層膜,其係藉由將第2觀點至第7觀點中任一者之阻劑底層膜形成組成物塗佈於半導體基板上並燒成而得到;第9觀點,係關於一種半導體裝置之製造方法,其係包含將如第2觀點至第7觀點中任一者之阻劑底層膜形成組成物塗佈於半導體基板上並燒成而形成阻劑底層膜之步驟、於前述阻劑底層膜之上塗佈阻劑用組成物而形成阻劑
膜之步驟、使前述阻劑膜曝光之步驟、於曝光後將阻劑膜顯影而得到經圖型化之阻劑膜的步驟、依照該經圖型化之阻劑膜的圖型來蝕刻阻劑底層膜之步驟、以及依照阻劑膜及阻劑底層膜之圖型來加工半導體基板之步驟;第10觀點,係關於一種半導體裝置之製造方法,其係包含於半導體基板上形成有機底層膜之步驟、於其上塗佈如第2觀點至第7觀點中任一者之阻劑底層膜形成組成物並燒成而形成阻劑底層膜之步驟、於前述阻劑底層膜之上塗佈阻劑用組成物而形成阻劑膜之步驟、使前述阻劑膜曝光之步驟、於曝光後將前述阻劑膜顯影而得到經圖型化之阻劑膜的步驟、依照該經圖型化之阻劑膜的圖型來蝕刻阻劑底層膜之步驟、依照該經圖型化之阻劑底層膜的圖型來蝕刻有機底層膜之步驟、及依照該經圖型化之有機底層膜的圖型來加工半導體基板之步驟。
本發明之阻劑底層膜形成組成物,因以式(1-a)或以式(1-b)表示之矽烷化合物為具有碸基及胺基者,故由該阻劑底層膜形成組成物形成之阻劑底層膜,可改善經圖型化之阻劑膜的截面形狀成為腳化形狀。
又,本發明之阻劑底層膜形成組成物,因式(1-a)或以式(1-b)表示之矽烷化合物為可藉由水解性基水解或部分水解,進行縮合反應而形成聚有機矽氧烷結構者,故於半導體裝置之製造中可發揮作為硬遮罩及抗反射膜之功能,且
可形成不易引起與阻劑之互混的阻劑底層膜。
[圖1]圖1為顯示實施例中得到之以式(1-1)表示之化合物(惟,X表示乙氧基)的NMR光譜之圖。
[圖2]圖2為顯示實施例中得到之以式(1-2)表示之化合物(惟,X表示乙氧基)的NMR光譜之圖。
本發明中,係於基板上藉由塗佈法形成阻劑底層膜,或隔著基板上之有機底層膜於其上藉由塗佈法形成阻劑底層膜,於該阻劑底層膜上形成阻劑膜(例如光阻、電子束阻劑、EUV阻劑)。然後,藉由曝光與顯影形成阻劑圖型,使用該阻劑圖型乾蝕刻阻劑底層膜來進行圖型之轉印,藉由該圖型來加工基板、或藉由蝕刻而將有機底層膜進行圖型轉印,藉由該有機底層膜進行基板之加工。
在形成微細的圖型的情況,為了防止圖型倒塌,有使阻劑膜厚變薄之傾向。因阻劑之薄膜化,用以將圖型轉印於存在於其底層之膜的乾蝕刻,若非蝕刻速度較上層之膜更高,則無法進行圖型轉印。本發明中,係於基板上隔著有機底層膜,或不隔著有機底層膜,依序於其上被覆本案之阻劑底層膜(含有無機系矽系化合物),且於其上被覆阻劑膜(有機阻劑膜)。有機系成分之膜與無機系成分之膜,
隨著蝕刻氣體的選擇而乾蝕刻速度大幅相異,有機系成分之膜以氧系氣體使乾蝕刻速度變高、無機系成分之膜係以含有鹵素之氣體而使乾蝕刻速度變高。
例如形成阻劑圖型,且將存在於其底層之本願阻劑底層膜以含有鹵素之氣體乾蝕刻而將圖型轉印於阻劑底層膜,並以經轉印於該阻劑底層膜之圖型,使用含有鹵素之氣體進行基板加工。或者,使用經圖型轉印之阻劑底層膜,將其底層之有機底層膜以氧系氣體乾蝕刻,進行圖型轉印於有機底層膜,以該經圖型轉印之有機底層膜,使用含有鹵素之氣體進行基板加工。
本發明中,該阻劑底層膜係發揮作為硬遮罩之功能,上述式(1)、(2)之結構中的烷氧基或醯氧基、鹵素原子等之水解性基係水解或部分水解,之後藉由矽醇基之縮合反應,形成聚矽氧烷結構之聚合物。此聚有機矽氧烷結構係具有作為硬遮罩之充分的功能。
此外,聚有機矽氧烷結構(中間膜),於存在於其下之有機底層膜的蝕刻、或基板之加工(蝕刻),係有效於作為硬遮罩。亦即,係對於基板加工時或有機底層膜之氧系乾蝕刻氣體具有充分之耐乾蝕刻性者。
本發明之阻劑底層膜係具備提高對該等上層阻劑之乾蝕刻速度、與基板加工時等之耐乾蝕刻性者。
本發明之阻劑底層膜形成組成物所得之阻劑底層膜,藉由含有:含有包含碸基與吸光基之有機基的矽烷化合物、其水解物、其水解縮合物,曝光與顯影後之阻劑圖型形
狀會成為矩形。藉此可進行微細圖型之基板加工。
例如專利文獻記載之使用了具有磺醯胺基之矽烷化合物的阻劑底層膜而得之阻劑圖型雖有容易腳化之傾向,但使用了具有本發明之碸結構與胺基結構之矽烷化合物的阻劑底層膜,可改善阻劑圖型之腳化傾向。
本發明係關於以式(1-a)或以式(1-b)表示之矽烷化合物。
此外,本發明係關於一種微影術用阻劑底層膜形成組成物,其係含有水解性有機矽烷、其水解物、及其水解縮合物當中之至少1種作為矽烷,且該矽烷為以式(1-a)或以式(1-b)表示之矽烷化合物。
矽烷全體中,以式(1-a)或式(1-b)表示之矽烷之比例,能夠以未達50莫耳%、例如0.5至30莫耳%、0.5至25莫耳%、0.5至15莫耳%、或0.5至10莫耳%之比例含有。
本發明之阻劑底層膜形成組成物,係含有以式(1-a)或以式(1-b)表示之矽烷化合物之水解性有機矽烷、其水解物、或其水解縮合物;及溶劑。此外可含有作為任意成分之酸、水、醇、硬化觸媒、酸產生劑、其他有機聚合物、吸光性化合物、及界面活性劑等。
又,本發明中,可合併使用以式(1-a)表示之矽烷化合物與以式(1-b)表示之矽烷化合物,本發明之阻劑底層膜形成組成物,可含有以式(1-a)表示之矽烷化合物、以式(1-b)表示之矽烷化合物、以式(1-a)表示之矽烷化合物之水解物
、以式(1-b)表示之矽烷化合物之水解物、以式(1-a)表示之矽烷化合物之水解縮合物、以式(1-b)表示之矽烷化合物之水解縮合物及以式(1-a)表示之矽烷化合物與以式(1-b)表示之矽烷化合物之水解縮合物當中之1種或2種以上。
本發明之阻劑底層膜形成組成物中之固體成分,例如為0.1至50質量%、或0.1至30質量%、0.1至25質量%。此處固體成分意指由阻劑底層膜形成組成物之全部成分中去除溶劑成分後者。
固體成分中所佔之水解性有機矽烷、其水解物、及其水解縮合物之比例,為20質量%以上,例如為50至100質量%、60至100質量%、70至100質量%。
本發明中所用之水解性有機矽烷係具有以式(1-a)或式(1-b)表示之結構。
以式(1-a)表示之矽烷化合物之例子,可舉例以式(2)表示之矽烷化合物。
式(1)中,R1、R3、及R4當中之至少1個基,係表示碳原子數1至10之伸烷基之末端鍵結有-Si(X)3基之基,剩餘之基表示氫原子、碳原子數1至10之烷基、或碳原子數6至40之芳基,R2表示碳原子數1至10之伸烷基、或碳原子數6至40之伸芳基。惟上述X表示烷氧基、醯氧基、或鹵素原子。
式(2)中,R6、R7、R9、及R10當中之至少1個基,表示碳原子數1至10之伸烷基之末端鍵結有-Si(X)3基之基,剩餘之基表示氫原子、碳原子數1至10之烷基、或碳
原子數6至40之芳基,R5及R8表示碳原子數1至10之伸烷基、或碳原子數6至40之伸芳基。惟上述X表示烷氧基、醯氧基、或鹵素原子。
上述碳原子數1至10之烷基,可列舉甲基、乙基、n-丙基、i-丙基、環丙基、n-丁基、i-丁基、s-丁基、t-丁基、環丁基、1-甲基-環丙基、2-甲基-環丙基、n-戊基、1-甲基-n-丁基、2-甲基-n-丁基、3-甲基-n-丁基、1,1-二甲基-n-丙基、1,2-二甲基-n-丙基、2,2-二甲基-n-丙基、1-乙基-n-丙基、環戊基、1-甲基-環丁基、2-甲基-環丁基、3-甲基-環丁基、1,2-二甲基-環丙基、2,3-二甲基-環丙基、1-乙基-環丙基、2-乙基-環丙基、n-己基、1-甲基-n-戊基、2-甲基-n-戊基、3-甲基-n-戊基、4-甲基-n-戊基、1,1-二甲基-n-丁基、1,2-二甲基-n-丁基、1,3-二甲基-n-丁基、2,2-二甲基-n-丁基、2,3-二甲基-n-丁基、3,3-二甲基-n-丁基、1-乙基-n-丁基、2-乙基-n-丁基、1,1,2-三甲基-n-丙基、1,2,2-三甲基-n-丙基、1-乙基-1-甲基-n-丙基、1-乙基-2-甲基-n-丙基、環己基、1-甲基-環戊基、2-甲基-環戊基、3-甲基-環戊基、1-乙基-環丁基、2-乙基-環丁基、3-乙基-環丁基、1,2-二甲基-環丁基、1,3-二甲基-環丁基、2,2-二甲基-環丁基、2,3-二甲基-環丁基、2,4-二甲基-環丁基、3,3-二甲基-環丁基、1-n-丙基-環丙基、2-n-丙基-環丙基、1-i-丙基-環丙基、2-i-丙基-環丙基、1,2,2-三甲基-環丙基、1,2,3-三甲基-環丙基、2,2,3-三甲基-環丙基、1-乙基-2-甲基-環丙基、2-乙基-1-甲基-環丙基、2-乙基-2-
甲基-環丙基及2-乙基-3-甲基-環丙基等。其中較佳可使用甲基、乙基、n-丙基。
又,碳原子數1至10之伸烷基,可列舉對應於上述烷基之伸烷基。而較佳亦可使用亞甲基、伸乙基、伸丙基。
碳原子數6至40之芳基,可列舉苯基、o-甲基苯基、m-甲基苯基、p-甲基苯基、o-氯苯基、m-氯苯基、p-氯苯基、o-氟苯基、p-氟苯基、o-甲氧基苯基、p-甲氧基苯基、p-硝基苯基、p-氰基苯基、α-萘基、β-萘基、o-聯苯基、m-聯苯基、p-聯苯基、1-蒽基、2-蒽基、9-蒽基、1-菲基、2-菲基、3-菲基、4-菲基及9-菲基。
其中較佳可使用苯基。
又,碳原子數6至40之伸芳基,可列舉對應於上述芳基之伸芳基。而較佳可使用伸苯基。
上述水解性矽烷之水解基可列舉烷氧基、醯氧基、及鹵素原子。
烷氧基可列舉具有碳原子數1至20之直鏈、分支、環狀之烷基部分的烷氧基,可列舉例如甲氧基、乙氧基、n-丙氧基、i-丙氧基、n-丁氧基、i-丁氧基、s-丁氧基、t-丁氧基、n-戊氧基、1-甲基-n-丁氧基、2-甲基-n-丁氧基、3-甲基-n-丁氧基、1,1-二甲基-n-丙氧基、1,2-二甲基-n-丙氧基、2,2-二甲基-n-丙氧基、1-乙基-n-丙氧基、n-己氧基、1-甲基-n-戊氧基、2-甲基-n-戊氧基、3-甲基-n-戊氧基等。
碳原子數2至20之醯氧基,可列舉例如甲基羰氧基、乙基羰氧基、n-丙基羰氧基、i-丙基羰氧基、n-丁基羰氧基、i-丁基羰氧基、s-丁基羰氧基、t-丁基羰氧基、n-戊基羰氧基、1-甲基-n-丁基羰氧基、2-甲基-n-丁基羰氧基、3-甲基-n-丁基羰氧基、1,1-二甲基-n-丙基羰氧基等。
鹵素原子可列舉氟、氯、溴、碘等。
以式(1-a)表示之矽烷化合物、以式(1-b)表示之矽烷化合物、及式(2)表示之矽烷化合物(水解性有機矽烷)亦可使胺化合物與碸化合物反應而合成。
以式(1-a)表示之矽烷化合物、以式(1-b)表示之矽烷化合物、及式(2)表示之矽烷化合物(水解性有機矽烷)例如可舉例如以下。下述式中,X表示上述烷氧基、上述醯氧基、或上述鹵素原子。
本發明中,可包含由以式(3)表示之有機矽化合物(水解性有機矽烷)及以式(4)表示之有機矽化合物(水解性有機矽烷)所構成群組中選出之至少1種有機矽化合物、與上述以式(1-a)或以式(1-b)表示之矽烷化合物(水解性有機矽烷)之組合;該等之水解物;及該等之水解縮合物當中之至少1種。
又,本發明中,可使用上述以式(1-a)或以式(1-b)表示
之矽烷化合物(水解性有機矽烷)之水解縮合物、及以式(1-a)或以式(1-b)表示之矽烷化合物(水解性有機矽烷)與以式(3)表示之有機矽化合物(水解性有機矽烷)之水解縮合物當中之至少1種。
進一步地,本發明中可合併使用以式(1-a)或以式(1-b)表示之矽烷化合物(水解性有機矽烷)、及以式(3)表示之有機矽化合物(水解性有機矽烷)。可合併使用以式(1-a)或以式(1-b)表示之矽烷化合物(水解性有機矽烷)、其水解物、及其水解縮合物當中之至少1種;與以式(3)表示之有機矽化合物、其水解物、及其水解縮合物當中之至少1種。
又,本發明之阻劑底層膜形成組成物,可合併使用:以式(1-a)表示之矽烷化合物、以式(1-b)表示之矽烷化合物、以式(1-a)表示之矽烷化合物之水解物、以式(1-b)表示之矽烷化合物之水解物、以式(1-a)表示之矽烷化合物之水解縮合物、以式(1-b)表示之矽烷化合物之水解縮合物、以式(1-a)表示之矽烷化合物與以式(1-b)表示之矽烷化合物之水解縮合物當中之至少1種;以及
以式(3)表示之有機矽化合物、其水解物、其水解縮合物、以式(1-a)表示之矽烷化合物與以式(3)表示之有機矽化合物之水解縮合物、以式(1-b)表示之矽烷化合物與以式(3)表示之有機矽化合物之水解縮合物、及以式(1-a)表示之矽烷化合物與以式(1-b)表示之矽烷化合物與以式(3)表示之有機矽化合物之水解縮合物當中之至少1種。
上述之以式(1-a)或以式(1-b)表示之矽烷化合物(水解
性有機矽烷)、與以式(3)表示之有機矽化合物之比例,以莫耳比計可於1:0至1:200之範圍使用。為了得到良好之阻劑形狀,以式(1-a)或以式(1-b)表示之矽烷化合物(水解性有機矽烷)、與以式(3)表示之有機矽化合物之比例,以莫耳比計可在1:199至1:2之範圍使用。
該等較佳係作為水解縮合物(聚有機矽氧烷之聚合物)來使用;較佳係使用以式(1-a)或以式(1-b)表示之矽烷化合物(水解性有機矽烷)與以式(3)表示之有機矽化合物(水解性有機矽烷)之水解縮合物(聚有機矽氧烷之聚合物)。
以式(3)表示之有機矽化合物(水解性有機矽烷)中之R1為烷基、芳基、芳烷基、鹵化烷基、鹵化芳基、鹵化芳烷基、烯基、或環氧基、丙烯醯基、甲基丙烯醯基、巰基、烷氧基芳基、醯氧基氫芳基、三聚異氰酸酯基、羥基、環狀胺基、或具有氰基之有機基、或該等之組合,且係藉由Si-C鍵與矽原子鍵結者,R2表示烷氧基、醯氧基、或鹵素原子,a表示0至3之整數。
R1、及R2表示之烷基、芳基、芳烷基、鹵化烷基、鹵化芳基、鹵化芳烷基、烯基、或環氧基、丙烯醯基、甲基丙烯醯基、巰基、烷氧基芳基、醯氧基氫芳基、三聚異氰酸酯基、羥基、環狀胺基、或具有氰基之有機基,進而水解性基中所含之烷氧基、醯氧基、或鹵素原子,可舉例上述式(1-a)及式(1-b)中所記載者。
以式(3)表示之有機矽化合物(水解性有機矽烷)可列舉例如四甲氧基矽烷、四氯矽烷、四乙醯氧基矽烷
、四乙氧基矽烷、四n-丙氧基矽烷、四異丙氧基矽烷、四n-丁氧基矽烷、四乙醯氧基矽烷、甲基三甲氧基矽烷、甲基三乙氧基矽烷、甲基三氯矽烷、甲基三乙醯氧基矽烷、甲基三丙氧基矽烷、甲基三乙醯氧基矽烷、甲基三丁氧基矽烷、甲基三丙氧基矽烷、甲基三戊氧基矽烷、甲基三苯氧基矽烷、甲基三苄氧基矽烷、甲基三苯乙基氧基矽烷、環氧丙氧基甲基三甲氧基矽烷、環氧丙氧基甲基三乙氧基矽烷、α-環氧丙氧基乙基三甲氧基矽烷、α-環氧丙氧基乙基三乙氧基矽烷、β-環氧丙氧基乙基三甲氧基矽烷、β-環氧丙氧基乙基三乙氧基矽烷、α-環氧丙氧基丙基三甲氧基矽烷、α-環氧丙氧基丙基三乙氧基矽烷、β-環氧丙氧基丙基三甲氧基矽烷、β-環氧丙氧基丙基三乙氧基矽烷、γ-環氧丙氧基丙基三甲氧基矽烷、γ-環氧丙氧基丙基三乙氧基矽烷、γ-環氧丙氧基丙基三丙氧基矽烷、γ-環氧丙氧基丙基三丁氧基矽烷、γ-環氧丙氧基丙基三苯氧基矽烷、α-環氧丙氧基丁基三甲氧基矽烷、α-環氧丙氧基丁基三乙氧基矽烷、β-環氧丙氧基丁基三乙氧基矽烷、γ-環氧丙氧基丁基三甲氧基矽烷、γ-環氧丙氧基丁基三乙氧基矽烷、δ-環氧丙氧基丁基三甲氧基矽烷、δ-環氧丙氧基丁基三乙氧基矽烷、(3,4-環氧基環己基)甲基三甲氧基矽烷、(3,4-環氧基環己基)甲基三乙氧基矽烷、β-(3,4-環氧基環己基)乙基三甲氧基矽烷、β-(3,4-環氧基環己基)乙基三乙氧基矽烷、β-(3,4-環氧基環己基)乙基三丙氧基矽烷、β-(3,4-環氧基環己基)乙基三丁氧基矽烷、β-(3,4-環氧基環己基)乙基
三苯氧基矽烷、γ-(3,4-環氧基環己基)丙基三甲氧基矽烷、γ-(3,4-環氧基環己基)丙基三乙氧基矽烷、δ-(3,4-環氧基環己基)丁基三甲氧基矽烷、δ-(3,4-環氧基環己基)丁基三乙氧基矽烷、環氧丙氧基甲基甲基二甲氧基矽烷、環氧丙氧基甲基甲基二乙氧基矽烷、α-環氧丙氧基乙基甲基二甲氧基矽烷、α-環氧丙氧基乙基甲基二乙氧基矽烷、β-環氧丙氧基乙基甲基二甲氧基矽烷、β-環氧丙氧基乙基乙基二甲氧基矽烷、α-環氧丙氧基丙基甲基二甲氧基矽烷、α-環氧丙氧基丙基甲基二乙氧基矽烷、β-環氧丙氧基丙基甲基二甲氧基矽烷、β-環氧丙氧基丙基乙基二甲氧基矽烷、γ-環氧丙氧基丙基甲基二甲氧基矽烷、γ-環氧丙氧基丙基甲基二乙氧基矽烷、γ-環氧丙氧基丙基甲基二丙氧基矽烷、γ-環氧丙氧基丙基甲基二丁氧基矽烷、γ-環氧丙氧基丙基甲基二苯氧基矽烷、γ-環氧丙氧基丙基乙基二甲氧基矽烷、γ-環氧丙氧基丙基乙基二乙氧基矽烷、γ-環氧丙氧基丙基乙烯基二甲氧基矽烷、γ-環氧丙氧基丙基乙烯基二乙氧基矽烷、乙基三甲氧基矽烷、乙基三乙氧基矽烷、乙烯基三甲氧基矽烷、乙烯基三氯矽烷、乙烯基三乙醯氧基矽烷、乙烯基三乙氧基矽烷、乙烯基三乙醯氧基矽烷、苯基三甲氧基矽烷、苯基三氯矽烷、苯基三乙醯氧基矽烷、苯基三乙氧基矽烷、苯基三乙醯氧基矽烷、γ-氯丙基三甲氧基矽烷、γ-氯丙基三乙氧基矽烷、γ-氯丙基三乙醯氧基矽烷、3、3、3-三氟丙基三甲氧基矽烷、γ-甲基丙烯醯氧基丙基三甲氧基矽烷、γ-巰基丙基三甲氧基矽烷、γ-巰基丙基
三乙氧基矽烷、β-氰基乙基三乙氧基矽烷、氯甲基三甲氧基矽烷、氯甲基三乙氧基矽烷、二甲基二甲氧基矽烷、苯基甲基二甲氧基矽烷、二甲基二乙氧基矽烷、苯基甲基二乙氧基矽烷、γ-氯丙基甲基二甲氧基矽烷、γ-氯丙基甲基二乙氧基矽烷、二甲基二乙醯氧基矽烷、γ-甲基丙烯醯氧基丙基甲基二甲氧基矽烷、γ-甲基丙烯醯氧基丙基甲基二乙氧基矽烷、γ-巰基丙基甲基二甲氧基矽烷、γ-巰基甲基二乙氧基矽烷、甲基乙烯基二甲氧基矽烷、甲基乙烯基二乙氧基矽烷、苯基碸基胺基丙基三乙氧基矽烷、甲基碸基胺基丙基三乙氧基矽烷、苯基碸基胺基丙基三甲氧基矽烷、甲基碸基胺基丙基三甲氧基矽烷等。
特別較佳為四甲氧基矽烷、四乙氧基矽烷等之四烷氧基矽烷;與苯基三甲氧基矽烷、苯基三乙氧基矽烷等之苯基三烷氧基矽烷的組合。又更佳為於該等組合中再組合甲基三甲氧基矽烷、甲基三乙氧基矽烷等之烷基三烷氧基矽烷。
上述以式(3)表示之有機矽化合物(水解性有機矽烷)亦可舉例以下之結構。結構中之R22與式(3)中之R22表示同樣意義。
以式(4)表示之有機矽化合物(水解性有機矽烷)之R31表示烷基,R32表示烷氧基、醯氧基、或鹵素原子,Y表示伸烷基或伸芳基,b表示0或1之整數,c表示0或1之整數。
上述烷基、烷氧基、醯氧基、或鹵素原子,可使用式(1-a)及式(1-b)中舉例者。又,伸烷基、伸芳基可舉例對應於上述烷基、及芳基之2價有機基。
以式(4)表示之有機矽化合物(水解性有機矽烷),可列舉例如亞甲基雙三甲氧基矽烷、亞甲基雙三氯矽烷、亞甲基雙三乙醯氧基矽烷、伸乙基雙三乙氧基矽烷、伸乙基雙
三氯矽烷、伸乙基雙三乙醯氧基矽烷、伸丙基雙三乙氧基矽烷、伸丁基雙三甲氧基矽烷、伸苯基雙三甲氧基矽烷、伸苯基雙三乙氧基矽烷、伸苯基雙甲基二乙氧基矽烷、伸苯基雙甲基二甲氧基矽烷、伸萘基雙三甲氧基矽烷、雙三甲氧基二矽烷、雙三乙氧基二矽烷、雙乙基二乙氧基二矽烷、雙甲基二甲氧基二矽烷等。
以式(1-a)或以(1-b)表示之矽烷化合物(水解性有機矽烷)與以式(3)表示之有機矽化合物(水解性有機矽烷)之水解縮合物的具體例,係如以下舉例。
以式(1-a)或以式(1-b)表示之矽烷化合物(水解性有機矽烷)之水解縮合物(聚有機矽氧烷)、或以式(1-a)或以式(1-b)表示之矽烷化合物(水解性有機矽烷)與以式(3)表示之有機矽化合物及以式(4)表示之有機矽化合物中之至少1種的水解縮合物(聚有機矽氧烷),可作為重量平均分子量1000至1000000、或1000至100000之縮合物而得到。該等之分子量係為以GPC分析之聚苯乙烯換算所得之分子量。
GPC之測定條件,可使用例如GPC裝置(商品名HLC-8220GPC、TOSOH股份有限公司製)、GPC管柱(商品名ShodexKF803L、KF802、KF801、昭和電工製)、管柱溫度40℃、溶離液(溶出溶劑)為四氫呋喃、流量(流速)為1.0ml/min、標準試樣為聚苯乙烯(昭和電工股份有限公司製)來進行。
烷氧基矽烷基、醯氧基矽烷基、或鹵化矽烷基之水解,每1莫耳水解性基,係使用0.5至100莫耳、較佳為1至10莫耳的水。
又,可使用每1莫耳水解性基,為0.001至10莫耳、較佳為0.001至1莫耳之水解觸媒。
進行水解與縮合時的反應溫度,通常係20至80℃。
水解可為完全地進行水解、亦可為部分水解。亦即,水解縮合物中亦可殘存水解物或單體。
水解而縮合時,可使用觸媒。
水解觸媒可列舉金屬螯合化合物、有機酸、無機酸、
有機鹼、無機鹼。
作為水解觸媒之金屬螯合化合物,可列舉例如三乙氧基.單(乙醯丙酮)鈦、三-n-丙氧基.單(乙醯丙酮)鈦、三-i-丙氧基.單(乙醯丙酮)鈦、三-n-丁氧基.單(乙醯丙酮)鈦、三-sec-丁氧基.單(乙醯丙酮)鈦、三-t-丁氧基.單(乙醯丙酮)鈦、二乙氧基.雙(乙醯丙酮)鈦、二-n-丙氧基.雙(乙醯丙酮)鈦、二-i-丙氧基.雙(乙醯丙酮)鈦、二-n-丁氧基.雙(乙醯丙酮)鈦、二-sec-丁氧基.雙(乙醯丙酮)鈦、二-t-丁氧基.雙(乙醯丙酮)鈦、單乙氧基.參(乙醯丙酮)鈦、單-n-丙氧基.參(乙醯丙酮)鈦、單-i-丙氧基.參(乙醯丙酮)鈦、單-n-丁氧基.參(乙醯丙酮)鈦、單-sec-丁氧基.參(乙醯丙酮)鈦、單-t-丁氧基.參(乙醯丙酮)鈦、肆(乙醯丙酮)鈦、三乙氧基.單(乙基乙醯乙酸酯)鈦、三-n-丙氧基.單(乙基乙醯乙酸酯)鈦、三-i-丙氧基.單(乙基乙醯乙酸酯)鈦、三-n-丁氧基.單(乙基乙醯乙酸酯)鈦、三-sec-丁氧基.單(乙基乙醯乙酸酯)鈦、三-t-丁氧基.單(乙基乙醯乙酸酯)鈦、二乙氧基.雙(乙基乙醯乙酸酯)鈦、二-n-丙氧基.雙(乙基乙醯乙酸酯)鈦、二-i-丙氧基.雙(乙基乙醯乙酸酯)鈦、二-n-丁氧基.雙(乙基乙醯乙酸酯)鈦、二-sec-丁氧基.雙(乙基乙醯乙酸酯)鈦、二-t-丁氧基.雙(乙基乙醯乙酸酯)鈦、單乙氧基.參(乙基乙醯乙酸酯)鈦、單-n-丙氧基.參(乙基乙醯乙酸酯)鈦、單-i-丙氧基.參(乙基乙醯乙酸酯)鈦、單-n-丁氧基.參(乙基乙醯乙酸酯)鈦、單-sec-丁氧基.參(乙基乙醯乙酸酯)鈦、單-t-丁氧基.參(乙基乙醯乙酸酯)鈦
、肆(乙基乙醯乙酸酯)鈦、單(乙醯丙酮)參(乙基乙醯乙酸酯)鈦、雙(乙醯丙酮)雙(乙基乙醯乙酸酯)鈦、參(乙醯丙酮)單(乙基乙醯乙酸酯)鈦、等之鈦螯合化合物;三乙氧基.單(乙醯丙酮)鋯、三-n-丙氧基.單(乙醯丙酮)鋯、三-i-丙氧基.單(乙醯丙酮)鋯、三-n-丁氧基.單(乙醯丙酮)鋯、三-sec-丁氧基.單(乙醯丙酮)鋯、三-t-丁氧基.單(乙醯丙酮)鋯、二乙氧基.雙(乙醯丙酮)鋯、二-n-丙氧基.雙(乙醯丙酮)鋯、二-i-丙氧基.雙(乙醯丙酮)鋯、二-n-丁氧基.雙(乙醯丙酮)鋯、二-sec-丁氧基.雙(乙醯丙酮)鋯、二-t-丁氧基.雙(乙醯丙酮)鋯、單乙氧基.參(乙醯丙酮)鋯、單-n-丙氧基.參(乙醯丙酮)鋯、單-i-丙氧基.參(乙醯丙酮)鋯、單-n-丁氧基.參(乙醯丙酮)鋯、單-sec-丁氧基.參(乙醯丙酮)鋯、單-t-丁氧基.參(乙醯丙酮)鋯、肆(乙醯丙酮)鋯、三乙氧基.單(乙基乙醯乙酸酯)鋯、三-n-丙氧基.單(乙基乙醯乙酸酯)鋯、三-i-丙氧基.單(乙基乙醯乙酸酯)鋯、三-n-丁氧基.單(乙基乙醯乙酸酯)鋯、三-sec-丁氧基.單(乙基乙醯乙酸酯)鋯、三-t-丁氧基.單(乙基乙醯乙酸酯)鋯、二乙氧基.雙(乙基乙醯乙酸酯)鋯、二-n-丙氧基.雙(乙基乙醯乙酸酯)鋯、二-i-丙氧基.雙(乙基乙醯乙酸酯)鋯、二-n-丁氧基.雙(乙基乙醯乙酸酯)鋯、二-sec-丁氧基.雙(乙基乙醯乙酸酯)鋯、二-t-丁氧基.雙(乙基乙醯乙酸酯)鋯、單乙氧基.參(乙基乙醯乙酸酯)鋯、單-n-丙氧基.參(乙基乙醯乙酸酯)鋯、單-i-丙氧基.參(乙基乙醯乙酸酯)鋯、單-n-丁氧基.參(乙基乙醯乙酸酯)鋯、單-sec-丁氧基.參(乙基乙醯乙酸酯)
鋯、單-t-丁氧基.參(乙基乙醯乙酸酯)鋯、肆(乙基乙醯乙酸酯)鋯、單(乙醯丙酮)參(乙基乙醯乙酸酯)鋯、雙(乙醯丙酮)雙(乙基乙醯乙酸酯)鋯、參(乙醯丙酮)單(乙基乙醯乙酸酯)鋯、等之鋯螯合化合物;參(乙醯丙酮)鋁、參(乙基乙醯乙酸酯)鋁等之鋁螯合化合物等。
作為水解觸媒之有機酸,可列舉例如乙酸、丙酸、丁酸、戊酸、己酸、庚酸、辛酸、壬酸、癸酸、草酸、馬來酸、甲基丙二酸、己二酸、癸二酸、没食子酸、丁酸、蜜臘酸、花生四烯酸、莽草酸、2-乙基己酸、油酸、硬脂酸、亞麻油酸、次亞麻油酸、水楊酸、安息香酸、p-胺基安息香酸、p-甲苯磺酸、苯磺酸、單氯乙酸、二氯乙酸、三氯乙酸、三氟乙酸、甲酸、丙二酸、磺酸、鄰苯二甲酸、富馬酸、檸檬酸、酒石酸等。
作為水解觸媒之無機酸,可列舉例如鹽酸、硝酸、硫酸、氫氟酸、磷酸等。
作為水解觸媒之有機鹼,可列舉例如吡啶、吡咯、哌嗪、吡咯啶、哌啶、甲吡啶、三甲基胺、三乙基胺、單乙醇胺、二乙醇胺、二甲基單乙醇胺、單甲基二乙醇胺、三乙醇胺、二氮雜雙環辛烷、二氮雜雙環壬烷、二氮雜雙環十一烯、氫氧化四甲基銨等。無機鹼可列舉例如氨、氫氧化鈉、氫氧化鉀、氫氧化鋇、氫氧化鈣等。該等觸媒當中,較佳為金屬螯合化合物、有機酸、無機酸,該等可1種或者2種以上同時使用。
水解所用之有機溶劑,可列舉例如n-戊烷、i-
戊烷、n-己烷、i-己烷、n-庚烷、i-庚烷、2,2,4-三甲基戊烷、n-辛烷、i-辛烷、環己烷、甲基環己烷等之脂肪族碳化氫系溶劑;苯、甲苯、二甲苯、乙基苯、三甲基苯、甲基乙基苯、n-丙基苯、i-丙基苯、二乙基苯、i-丁基苯、三乙基苯、二-i-丙基苯、n-戊基萘、三甲基苯等之芳香族碳化氫系溶劑;甲醇、乙醇、n-丙醇、i-丙醇、n-丁醇、i-丁醇、sec-丁醇、t-丁醇、n-戊醇、i-戊醇、2-甲基丁醇、sec-戊醇、t-戊醇、3-甲氧基丁醇、n-己醇、2-甲基戊醇、sec-己醇、2-乙基丁醇、sec-庚醇、庚醇-3、n-辛醇、2-乙基己醇、sec-辛醇、n-壬醇、2,6-二甲基庚醇-4、n-癸醇、sec-十一醇、三甲基壬醇、sec-四癸醇、sec-十七醇、酚、環己醇、甲基環己醇、3,3,5-三甲基環己醇、苄基醇、苯基甲基甲醇、二丙酮醇、甲酚等之單元醇系溶劑;乙二醇、丙二醇、1,3-丁二醇、戊二醇-2,4、2-甲基戊二醇-2,4、己二醇-2,5、庚二醇-2,4、2-乙基己二醇-1,3、二乙二醇、二丙二醇、三乙二醇、三丙二醇、甘油等之多元醇系溶劑;丙酮、甲基乙基酮、甲基-n-丙基酮、甲基-n-丁基酮、二乙基酮、甲基-i-丁基酮、甲基-n-戊基酮、乙基-n-丁基酮、甲基-n-己基酮、二-i-丁基酮、三甲基壬酮、環己酮、甲基環己酮、2,4-戊烷二酮、丙酮基丙酮、二丙酮醇、苯乙酮、葑酮等之酮系溶劑;乙基醚、i-丙基醚、n-丁基醚、n-己基醚、2-乙基己基醚、環氧乙烷、1,2-環氧丙烷、二氧雜環戊烷、4-甲基二氧雜環戊烷、二噁烷、二甲基二噁烷、乙二醇單甲基醚、乙二醇單乙基醚、乙二醇二乙
基醚、乙二醇單-n-丁基醚、乙二醇單-n-己基醚、乙二醇單苯基醚、乙二醇單-2-乙基丁基醚、乙二醇二丁基醚、二乙二醇單甲基醚、二乙二醇單乙基醚、二乙二醇二乙基醚、二乙二醇單-n-丁基醚、二乙二醇二-n-丁基醚、二乙二醇單-n-己基醚、乙氧基三甘醇、四乙二醇二-n-丁基醚、丙二醇單甲基醚、丙二醇單乙基醚、丙二醇單丙基醚、丙二醇單丁基醚、二丙二醇單甲基醚、二丙二醇單乙基醚、二丙二醇單丙基醚、二丙二醇單丁基醚、三丙二醇單甲基醚、四氫呋喃、2-甲基四氫呋喃等之醚系溶劑;二乙基碳酸酯、乙酸甲酯、乙酸乙酯、γ-丁內酯、γ-戊內酯、乙酸n-丙酯、乙酸i-丙酯、乙酸n-丁酯、乙酸i-丁酯、乙酸sec-丁酯、乙酸n-戊酯、乙酸sec-戊酯、乙酸3-甲氧基丁酯、乙酸甲基戊酯、乙酸2-乙基丁酯、乙酸2-乙基己酯、乙酸苄酯、乙酸環己酯、乙酸甲基環己酯、乙酸n-壬酯、乙醯乙酸甲酯、乙醯乙酸乙酯、乙酸乙二醇單甲基醚、乙酸乙二醇單乙基醚、乙酸二乙二醇單甲基醚、乙酸二乙二醇單乙基醚、乙酸二乙二醇單-n-丁基醚、乙酸丙二醇單甲基醚、乙酸丙二醇單乙基醚、乙酸丙二醇單丙基醚、乙酸丙二醇單丁基醚、乙酸二丙二醇單甲基醚、乙酸二丙二醇單乙基醚、二乙酸二醇、乙酸甲氧基三甘醇、丙酸乙酯、丙酸n-丁酯、丙酸i-戊酯、草酸二乙酯、草酸二-n-丁酯、乳酸甲酯、乳酸乙酯、乳酸n-丁酯、乳酸n-戊酯、丙二酸二乙酯、鄰苯二甲酸二甲酯、鄰苯二甲酸二乙酯等之酯系溶劑;N-甲基甲醯胺、N,N-二甲基甲醯胺、N,N-
二乙基甲醯胺、乙醯胺、N-甲基乙醯胺、N,N-二甲基乙醯胺、N-甲基丙醯胺、N-甲基吡咯啶酮等之含氮系溶劑;硫化二甲基、硫化二乙基、噻吩、四氫噻吩、二甲基亞碸、環丁碸、1,3-丙烷磺內酯等之含硫系溶劑等。該等溶劑可使用1種、或2種以上之組合。
特別是丙酮、甲基乙基酮、甲基-n-丙基酮、甲基-n-丁基酮、二乙基酮、甲基-i-丁基酮、甲基-n-戊基酮、乙基-n-丁基酮、甲基-n-己基酮、二-i-丁基酮、三甲基壬酮、環己酮、甲基環己酮、2,4-戊烷二酮、丙酮基丙酮、二丙酮醇、苯乙酮、葑酮(1,1,3-三甲基-2-降莰烯)等之酮系溶劑,以溶液保存安定性之觀點而言較佳。
於溶劑中使用觸媒將水解性有機矽烷水解並縮合,所得之水解縮合物(聚合物)可藉由減壓蒸餾等,將副生成物之醇或所使用之水解觸媒或水同時去除。又,可藉由中和或離子交換來去除水解所用之酸或鹼觸媒。此外本發明之微影術用阻劑底層膜形成組成物中,為了安定化,含有其水解縮合物之阻劑底層膜形成組成物可添加酸(例如有機酸)、水、醇、或該等之組合。
上述有機酸可列舉例如草酸、丙二酸、甲基丙二酸、琥珀酸、馬來酸、蘋果酸、酒石酸、鄰苯二甲酸、檸檬酸、戊二酸、檸檬酸、乳酸、水楊酸等。其中尤以草酸、馬來酸等較佳。所添加之有機酸,相對於縮合物(聚有機矽氧烷)100質量份,為0.5至5.0質量份。又,所添加之水可使用純水、超純水、離子交換水等,其添加量相對於阻
劑底層膜形成組成物100質量份,可為1至20質量份。
又,所添加之醇較佳為藉由塗佈後之加熱而容易飛散者,可列舉例如甲醇、乙醇、丙醇、異丙醇、丁醇等。所添加之醇,相對於阻劑底層膜形成組成物100質量份,可為1至20質量份。
又,作為添加劑,可添加雙酚S、或雙酚S衍生物。雙酚S、或雙酚S衍生物,相對於聚有機矽氧烷100質量份,係0.01至20質量份、或0.01至10質量份、或0.01至5質量份。
較佳之雙酚S、或雙酚S衍生物係如以下所舉例。
本發明之微影術用底層膜形成組成物,於上述成分以外,亦可依照需要含有有機聚合物化合物、光酸產生劑及界面活性劑等。
藉由使用有機聚合物化合物,可調整由本發明之微影
術用底層膜形成組成物所形成之阻劑底層膜的乾蝕刻速度(每單位時間之膜厚減少量)、衰減係數及折射率等。
作為有機聚合物化合物並無特殊限制,可使用各種有機聚合物。可使用縮聚合聚合物及加成聚合聚合物等。可使用聚酯、聚苯乙烯、聚醯亞胺、丙烯酸系聚合物、甲基丙烯酸系聚合物、聚乙烯基醚、酚酚醛清漆、萘酚酚醛清漆、聚醚、聚醯胺、聚碳酸酯等之加成聚合聚合物及縮聚合聚合物。較佳為使用發揮作為吸光部位之功能的具有苯環、萘環、蒽環、三嗪環、喹啉環、及喹噁啉環等之芳香環結構之有機聚合物。
作為如此之有機聚合物化合物,可列舉例如含有丙烯酸苄酯、甲基丙烯酸苄酯、丙烯酸苯酯、丙烯酸萘酯、甲基丙烯酸蒽酯、甲基丙烯酸蒽基甲酯、苯乙烯、羥基苯乙烯、苄基乙烯基醚及N-苯基馬來醯亞胺等之加成聚合性單體作為其結構單位的加成聚合聚合物、或酚酚醛清漆及萘酚酚醛清漆等之縮聚合聚合物。
使用加成聚合聚合物作為有機聚合物化合物時,其聚合物化合物可為均聚物亦可為共聚物。加成聚合聚合物之製造係使用加成聚合性單體。作為如此之加成聚合性單體可列舉丙烯酸、甲基丙烯酸、丙烯酸酯化合物、甲基丙烯酸酯化合物、丙烯醯胺化合物、甲基丙烯醯胺化合物、乙烯基化合物、苯乙烯化合物、馬來醯亞胺化合物、馬來酸酐、丙烯腈等。
丙烯酸酯化合物可列舉丙烯酸甲酯、丙烯酸
乙酯、丙烯酸正己酯、丙烯酸異丙酯、丙烯酸環己酯、丙烯酸苄酯、丙烯酸苯酯、丙烯酸蒽基甲酯、丙烯酸2-羥基乙酯、丙烯酸3-氯-2-羥基丙酯、丙烯酸2-羥基丙酯、丙烯酸2,2,2-三氟乙酯、丙烯酸2,2,2-三氯乙酯、丙烯酸2-溴乙酯、丙烯酸4-羥基丁酯、丙烯酸2-甲氧基乙酯、丙烯酸四氫糠酯、5-丙烯醯氧基-6-羥基降莰烯-2-羧酸-6-內酯、3-丙烯醯氧基丙基三乙氧基矽烷及丙烯酸環氧丙酯等。
甲基丙烯酸酯化合物可列舉甲基丙烯酸甲酯、甲基丙烯酸乙酯、甲基丙烯酸正己酯、甲基丙烯酸異丙酯、甲基丙烯酸環己酯、甲基丙烯酸苄酯、甲基丙烯酸苯酯、甲基丙烯酸蒽基甲酯、甲基丙烯酸2-羥基乙酯、甲基丙烯酸2-羥基丙酯、甲基丙烯酸2,2,2-三氟乙酯、甲基丙烯酸2,2,2-三氯乙酯、甲基丙烯酸2-溴乙酯、甲基丙烯酸4-羥基丁酯、甲基丙烯酸2-甲氧基乙酯、甲基丙烯酸四氫糠酯、5-甲基丙烯醯氧基-6-羥基降莰烯-2-羧酸-6-內酯、3-甲基丙烯醯氧基丙基三乙氧基矽烷、甲基丙烯酸環氧丙酯、甲基丙烯酸2-苯基乙酯、甲基丙烯酸羥基苯酯及甲基丙烯酸溴苯酯等。
丙烯醯胺化合物,可列舉丙烯醯胺、N-甲基丙烯醯胺、N-乙基丙烯醯胺、N-苄基丙烯醯胺、N-苯基丙烯醯胺、N,N-二甲基丙烯醯胺及N-蒽基丙烯醯胺等。
甲基丙烯醯胺化合物,可列舉甲基丙烯醯胺、N-甲基甲基丙烯醯胺、N-乙基甲基丙烯醯胺、N-苄基甲基丙烯醯
胺、N-苯基甲基丙烯醯胺、N,N-二甲基甲基丙烯醯胺及N-蒽基丙烯醯胺等。
乙烯基化合物,可列舉乙烯基醇、2-羥基乙基乙烯基醚、甲基乙烯基醚、乙基乙烯基醚、苄基乙烯基醚、乙烯基乙酸、乙烯基三甲氧基矽烷、2-氯乙基乙烯基醚、2-甲氧基乙基乙烯基醚、乙烯基萘及乙烯基蒽等。
苯乙烯化合物,可列舉苯乙烯、羥基苯乙烯、氯苯乙烯、溴苯乙烯、甲氧基苯乙烯、氰基苯乙烯及乙醯基苯乙烯等。
馬來醯亞胺化合物,可列舉馬來醯亞胺、N-甲基馬來醯亞胺、N-苯基馬來醯亞胺、N-環己基馬來醯亞胺、N-苄基馬來醯亞胺及N-羥基乙基馬來醯亞胺等。
使用縮聚合聚合物作為聚合物時,作為如此之聚合物,可列舉例如二醇化合物與二羧酸化合物之縮聚合聚合物。二醇化合物可列舉二乙二醇、六甲二醇、丁二醇等。二羧酸化合物可列舉琥珀酸、己二酸、對苯二甲酸、馬來酸酐等。又,可列舉例如聚苯均四醯亞胺、聚(對苯二甲醯對苯二胺)、聚對苯二甲酸丁二酯、聚對苯二甲酸乙二酯等之聚酯、聚醯胺、聚醯亞胺。
有機聚合物化合物中含有羥基時,此羥基可與聚有機矽氧烷形成交聯反應。
作為有機聚合物化合物,可使用例如重量平均分子量為1000至1000000、或3000至300000、或5000至200000、或10000至100000之聚合物化合物。
有機聚合物化合物可僅使用一種、或可組合二種以上使用。
使用有機聚合物化合物時,其比例,相對於縮合物(聚有機矽氧烷)100質量份,為1至200質量份、或5至100質量份、或10至50質量份、或20至30質量份。
本發明之阻劑底層膜形成組成物中可含有酸產生劑。
酸產生劑可列舉熱酸產生劑或光酸產生劑。
光酸產生劑係於阻劑曝光時產生酸。因此,可調整底層膜之酸性度。此係為用以使底層膜之酸性度與上層阻劑之酸性度配合的其一方法。又,藉由調整底層膜之酸性度,可調整形成於上層之阻劑的圖型形狀。
本發明之阻劑底層膜形成組成物中所含之光酸產生劑,可列舉鎓鹽化合物、磺醯亞胺化合物、及二碸基重氮甲烷化合物等。
鎓鹽化合物可列舉二苯基錪鎓六氟磷酸、二苯基錪鎓三氟甲烷磺酸、二苯基錪鎓九氟正丁烷磺酸、二苯基錪鎓全氟正辛烷磺酸、二苯基錪鎓樟腦磺酸、雙(4-tert-丁基苯基)錪鎓樟腦磺酸及雙(4-tert-丁基苯基)錪鎓三氟甲烷磺酸等之錪鎓鹽化合物、及三苯基鋶六氟銻酸、三苯基鋶九氟正丁烷磺酸、三苯基鋶樟腦磺酸及三苯基鋶三氟甲烷磺酸等之鋶鹽化合物等。
磺醯亞胺化合物可列舉例如N-(三氟甲烷碸基氧基)琥珀醯亞胺、N-(九氟正丁烷碸基氧基)琥珀醯亞胺、N-(樟腦碸基氧基)琥珀醯亞胺及N-(三氟甲烷碸基氧基)萘醯亞胺
等。
二碸基重氮甲烷化合物可列舉例如、雙(三氟甲基碸基)重氮甲烷、雙(環己基碸基)重氮甲烷、雙(苯基碸基)重氮甲烷、雙(p-甲苯碸基)重氮甲烷、雙(2,4-二甲基苯碸基)重氮甲烷、及甲基碸基-p-甲苯碸基重氮甲烷等。
光酸產生劑可僅使用一種,或可組合二種以上使用。
使用光酸產生劑時,其比例,相對於縮合物(聚有機矽氧烷)100質量份,為0.01至5質量份、或0.1至3質量份、或0.5至1質量份。
界面活性劑係有效於將本發明之微影術用阻劑底層膜形成組成物塗佈於基板時,抑制針孔及條痕等之發生。
本發明之阻劑底層膜形成組成物中所含之界面活性劑,可列舉例如、聚氧乙烯月桂基醚、聚氧乙烯硬脂基醚、聚氧乙烯鯨蠟基醚、聚氧乙烯油基醚等之聚氧乙烯烷基醚類、聚氧乙烯辛基酚醚、聚氧乙烯壬基酚醚等之聚氧乙烯烷基烯丙基醚類、聚氧乙烯.聚氧丙烯嵌段共聚物類、山梨醇酐單月桂酸酯、山梨醇酐單棕櫚酸酯、山梨醇酐單硬脂酸酯、山梨醇酐單油酸酯、山梨醇酐三油酸酯、山梨醇酐三硬脂酸酯等之山梨醇酐脂肪酸酯類、聚氧乙烯山梨醇酐單月桂酸酯、聚氧乙烯山梨醇酐單棕櫚酸酯、聚氧乙烯山梨醇酐單硬脂酸酯、聚氧乙烯山梨醇酐三油酸酯、聚氧乙烯山梨醇酐三硬脂酸酯等之聚氧乙烯山梨醇酐脂肪酸酯類等之非離子系界面活性劑、商品名EFTOP
EF301、EF303、EF352((股)Tokem Products製)、商品名Megaface F171、F173、R-08、R-30(大日本油墨化學工業(股)製)、Fluorad FC430、FC431(住友3M(股)製)、商品名Asahiguard AG710、Surflon S-382、SC101、SC102、SC103、SC104、SC105、SC106(旭硝子(股)製)等之氟系界面活性劑、及有機矽氧烷聚合物KP341(信越化學工業(股)製)等。該等界面活性劑可單獨使用,亦可以二種以上之組合來使用。使用界面活性劑時,其比例,相對於縮合物(聚有機矽氧烷)100質量份,為0.0001至5質量份、或0.001至1質量份、或0.01至0.5質量份。
又,本發明之阻劑底層膜形成組成物中,可添加流變性調整劑及接著輔助劑等。流變性調整劑,係有效於提高底層膜形成組成物之流動性。接著輔助劑,係有效於提高半導體基板或阻劑與底層膜之密合性。
使用於本發明之阻劑底層膜形成組成物的溶劑,只要係可溶解前述固體成分之溶劑,則可無特殊限制地使用。作為如此溶劑,可列舉例如甲基賽璐索芙乙酸酯、乙基賽璐索芙乙酸酯、丙二醇、丙二醇單甲基醚、丙二醇單乙基醚、甲基異丁基甲醇、丙二醇單丁基醚、丙二醇單甲基醚乙酸酯、丙二醇單乙基醚乙酸酯、丙二醇單丙基醚乙酸酯、丙二醇單丁基醚乙酸酯、甲苯、二甲苯、甲基乙基酮、環戊酮、環己酮、2-羥基丙酸乙酯、2-羥基-2-甲基丙酸乙酯、乙氧基乙酸乙酯、羥基乙酸乙酯、2-羥基-3-甲基丁酸甲酯、3-甲氧基丙酸甲酯、3-甲氧基丙酸乙酯、3-乙氧基
丙酸乙酯、3-乙氧基丙酸甲酯、丙酮酸甲酯、丙酮酸乙酯、乙二醇單甲基醚、乙二醇單乙基醚、乙二醇單丙基醚、乙二醇單丁基醚、乙二醇單甲基醚乙酸酯、乙二醇單乙基醚乙酸酯、乙二醇單丙基醚乙酸酯、乙二醇單丁基醚乙酸酯、二乙二醇二甲基醚、二乙二醇二乙基醚、二乙二醇二丙基醚、二乙二醇二丁基醚丙二醇單甲基醚、丙二醇二甲基醚、丙二醇二乙基醚、丙二醇二丙基醚、丙二醇二丁基醚、乳酸乙酯、乳酸丙酯、乳酸異丙酯、乳酸丁酯、乳酸異丁酯、甲酸甲酯、甲酸乙酯、甲酸丙酯、甲酸異丙酯、甲酸丁酯、甲酸異丁酯、甲酸戊酯、甲酸異戊酯、乙酸甲酯、乙酸乙酯、乙酸戊酯、乙酸異戊酯、乙酸己酯、丙酸甲酯、丙酸乙酯、丙酸丙酯、丙酸異丙酯、丙酸丁酯、丙酸異丁酯、丁酸甲酯、丁酸乙酯、丁酸丙酯、丁酸異丙酯、丁酸丁酯、丁酸異丁酯、羥基乙酸乙酯、2-羥基-2-甲基丙酸乙酯、3-甲氧基-2-甲基丙酸甲酯、2-羥基-3-甲基丁酸甲酯、甲氧基乙酸乙酯、乙氧基乙酸乙酯、3-甲氧基丙酸甲酯、3-乙氧基丙酸乙酯、3-甲氧基丙酸乙酯、3-甲氧基丁基乙酸酯、3-甲氧基丙基乙酸酯、3-甲基-3-甲氧基丁基乙酸酯、3-甲基-3-甲氧基丁基丙酸酯、3-甲基-3-甲氧基丁基丁酸酯、乙醯乙酸甲酯、甲苯、二甲苯、甲基乙基酮、甲基丙基酮、甲基丁基酮、2-庚酮、3-庚酮、4-庚酮、環己酮、N、N-二甲基甲醯胺、N-甲基乙醯胺、N,N-二甲基乙醯胺、N-甲基吡咯啶酮、4-甲基-2-戊醇、及γ-丁內酯等。該等溶劑可單獨使用、或以二種以上之組合來使
用。
以下,說明本發明之阻劑底層膜形成組成物之使用。
於半導體裝置之製造所使用的基板(例如、矽晶圓基板、矽/二氧化矽被覆基板、氮化矽基板、玻璃基板、ITO基板、聚醯亞胺基板、及低介電率材料(low-k材料)被覆基板等)之上,藉由旋轉器、塗佈器等之適當的塗佈方法塗佈本發明之阻劑底層膜形成組成物,之後,藉由燒成而形成阻劑底層膜。燒成之條件,係於燒成溫度80℃至250℃、燒成時間0.3至60分鐘當中適當選擇。較佳為燒成溫度150℃至250℃、燒成時間0.5至2分鐘。此處,所形成之底層膜的膜厚,例如為10至1000nm、或20至500nm、或50至300nm、或100至200nm。
接著在其阻劑底層膜之上,形成例如光阻之層。光阻之層的形成,可藉由周知方法,亦即光阻組成物溶液之對底層膜上的塗佈及燒成來進行。光阻之膜厚例如為50至10000nm、或100至2000nm、或200至1000nm。
本發明中,於基板上使有機底層膜成膜後,可於其上使本發明之阻劑底層膜成膜,進一步於其上被覆光阻。藉此,光阻之圖型寬度變窄,即使為了防止圖型倒塌而薄薄地被覆光阻的情況時,亦可藉由選擇適切的蝕刻氣體而進行基板之加工。例如,以對光阻具有充分快的蝕刻速度之氟系氣體作為蝕刻氣體,可對本發明之阻劑底層膜加工,又以對本發明之阻劑底層膜具有充分快的蝕刻速
度之氧系氣體作為蝕刻氣體,可進行有機底層膜之加工,再者以對有機底層膜具有充分快的蝕刻速度之氟系氣體作為蝕刻氣體,可進行基板之加工。
形成於本發明之阻劑底層膜之上的光阻,只要係對曝光所使用的光感光者則無特殊限定。負型光阻及正型光阻均可使用。係有由酚醛清漆樹脂與1,2-萘醌二疊氮磺酸酯所構成之正型光阻;由具有因為酸而分解而使鹼溶解速度上昇之基的黏結劑與光酸產生劑所構成之化學增幅型光阻;由因為酸而分解而使光阻之鹼溶解速度上昇的低分子化合物、鹼可溶性黏結劑與光酸產生劑所構成之化學增幅型光阻;及由具有因為酸而分解而使鹼溶解速度上昇之基的黏結劑、因為酸而分解而使光阻之鹼溶解速度上昇的低分子化合物與光酸產生劑所構成之化學增幅型光阻等。可列舉例如Shipley公司製商品名APEX-E、住友化學工業(股)製商品名PAR710、及信越化學工業(股)製商品名SEPR430等。又,可列舉例如Proc.SPIE,Vol.3999,330-334(2000)、Proc.SPIE,Vol.3999,357-364(2000)、或Proc.SPIE,Vol.3999,365-374(2000)記載之含氟原子聚合物系光阻。
接著,通過指定之遮罩進行曝光。曝光可使用KrF準分子雷射(波長248nm)、ArF準分子雷射(波長193nm)及F2準分子雷射(波長157nm)等。曝光後,亦可依需要進行曝光後加熱(post exposure bake)。曝光後加熱係以由加熱溫度70℃至150℃、加熱時間0.3至10分鐘適
當選擇之條件來進行。
又,本發明中作為阻劑,可使用電子束微影術用阻劑、或EUV微影術用阻劑以取代光阻。作為電子束阻劑,負型、正型均可使用。係有由酸產生劑與具有因為酸而分解而使鹼溶解速度變化之基的黏結劑所構成之化學增幅型阻劑;由鹼可溶性黏結劑、酸產生劑與因為酸而分解而使阻劑之鹼溶解速度變化的低分子化合物所構成之化學增幅型阻劑;由酸產生劑、具有因為酸而分解而使鹼溶解速度變化之基的黏結劑與因為酸而分解而使阻劑之鹼溶解速度變化的低分子化合物所構成之化學增幅型阻劑;由具有因為電子束而分解而使鹼溶解速度變化之基的黏結劑所構成之非化學增幅型阻劑;由具有因為電子束而切斷而使鹼溶解速度變化之部位的黏結劑所構成之非化學增幅型阻劑等。使用該等之電子束阻劑時,亦能夠與將照射源作為電子束而使用光阻的情況同樣地形成阻劑圖型。
又,可使用甲基丙烯酸酯樹脂系阻劑作為EUV阻劑。
接著,藉由顯影液(例如鹼顯影液)來進行顯影。藉此,例如使用正型光阻的情況時,經曝光之部分的光阻被去除,而形成光阻之圖型。
顯影液可列舉氫氧化鉀、氫氧化鈉等之鹼金屬氫氧化物之水溶液;氫氧化四甲基銨、氫氧化四乙基銨、膽鹼等之氫氧化四級銨之水溶液;乙醇胺、丙基胺、乙二胺等之胺水溶液等之鹼性水溶液為例。進一步地,亦可於該等顯影液中添加界面活性劑等。顯影條件係由溫度5至50℃、
時間10至600秒之中適當選擇。
又,本發明中可使用有機溶劑作為顯影液。曝光後藉由顯影液(溶劑)進行顯影。藉此,例如使用正型光阻時,未曝光之部分的光阻會被去除,而形成光阻之圖型。
顯影液可列舉例如乙酸甲酯、乙酸丁酯、乙酸乙酯、乙酸異丙酯、乙酸戊酯、乙酸異戊酯、甲氧基乙酸乙酯、乙氧基乙酸乙酯、丙二醇單甲基醚乙酸酯、乙二醇單乙基醚乙酸酯、乙二醇單丙基醚乙酸酯、乙二醇單丁基醚乙酸酯、乙二醇單苯基醚乙酸酯、二乙二醇單甲基醚乙酸酯、二乙二醇單丙基醚乙酸酯、二乙二醇單乙基醚乙酸酯、二乙二醇單苯基醚乙酸酯、二乙二醇單丁基醚乙酸酯、二乙二醇單乙基醚乙酸酯、乙酸2-甲氧基丁酯、乙酸3-甲氧基丁酯、乙酸4-甲氧基丁酯、乙酸3-甲基-3-甲氧基丁酯、乙酸3-乙基-3-甲氧基丁酯、丙二醇單甲基醚乙酸酯、丙二醇單乙基醚乙酸酯、丙二醇單丙基醚乙酸酯、乙酸2-乙氧基丁酯、乙酸4-乙氧基丁酯、乙酸4-丙氧基丁酯、乙酸2-甲氧基戊酯、乙酸3-甲氧基戊酯、乙酸4-甲氧基戊酯、乙酸2-甲基-3-甲氧基戊酯、乙酸3-甲基-3-甲氧基戊酯、乙酸3-甲基-4-甲氧基戊酯、乙酸4-甲基-4-甲氧基戊酯、丙二醇二乙酸酯、甲酸甲酯、甲酸乙酯、甲酸丁酯、甲酸丙酯、乳酸乙酯、乳酸丁酯、乳酸丙酯、碳酸乙酯、碳酸丙酯、碳酸丁酯、丙酮酸甲酯、丙酮酸乙酯、丙酮酸丙酯、丙酮酸丁酯、乙醯乙酸甲酯、乙醯乙酸乙酯、丙酸甲酯、丙酸乙酯、丙酸丙酯、丙酸異丙酯、2-羥
基丙酸甲酯、2-羥基丙酸乙酯、丙酸甲基-3-甲氧酯、丙酸乙基-3-甲氧酯、丙酸乙基-3-乙氧酯、丙酸丙基-3-甲氧酯等為例。進一步地,亦可於該等顯影液中添加界面活性劑等。顯影之條件係由溫度5至50℃、時間10至600秒當中適當選擇。
然後,以如此方式形成之光阻(上層)的圖型作為保護膜,進行本發明之阻劑底層膜(中間層)的去除,接著以由經圖型化之光阻及本發明之阻劑底層膜(中間層)所構成之膜為保護膜,進行有機底層膜(底層)的去除。最後,以經圖型化之本發明之阻劑底層膜(中間層)及有機底層膜(底層)為保護膜,進行半導體基板之加工。
首先,藉由乾蝕刻去除經去除光阻之部分的本發明之阻劑底層膜(中間層),使半導體基板露出。本發明之阻劑底層膜之乾蝕刻可使用四氟甲烷(CF4)、全氟環丁烷(C4F8)、全氟丙烷(C3F8)、三氟甲烷、一氧化碳、氬、氧、氮、六氟化硫、二氟甲烷、三氟化氮及三氟化氯、氯、三氯硼烷及二氯硼烷等之氣體。阻劑底層膜之乾蝕刻較佳為使用鹵素系氣體。鹵素系氣體之乾蝕刻中,基本上由有機物質所構成的光阻係難以被去除。相對於此,含有多量矽原子之本發明之阻劑底層膜,會被鹵素系氣體快速去除。因此,可抑制伴隨阻劑底層膜之乾蝕刻的光阻膜厚減少。而結果能夠以薄膜的型態來使用光阻。阻劑底層膜之乾蝕刻較佳係以氟系氣體進行,氟系氣體可列舉例如四氟甲烷(CF4)、全氟環丁烷(C4F8)、全氟丙烷(C3F8)、三氟甲烷、
及二氟甲烷(CH2F2)等。
之後,以由經圖型化之光阻及本發明之阻劑底層膜所構成的膜為保護膜,進行有機底層膜的去除。有機底層膜(底層)較佳為藉由氧系氣體之乾蝕刻來進行。其係因含有多量矽原子之本發明之阻劑底層膜,以氧系氣體之乾蝕刻難以去除之故。
最後,進行半導體基板之加工。半導體基板之加工較佳為藉由氟系氣體之乾蝕刻來進行。
氟系氣體可列舉例如四氟甲烷(CF4)、全氟環丁烷(C4F8)、全氟丙烷(C3F8)、三氟甲烷、及二氟甲烷(CH2F2)等。
又,於本發明之阻劑底層膜之上層,於光阻形成前可形成有機系之抗反射膜。於其所使用之抗反射膜組成物並無特殊限制,可由至今為止微影術製程中慣用者當中任意選擇來使用,又,可藉由慣用之方法、例如以旋轉器、塗佈器之塗佈及燒成,來進行抗反射膜的形成。
又,塗佈有本發明之阻劑底層膜形成組成物之基板,於其表面可具有以CVD法等形成之有機系或無機系的抗反射膜、亦可於其上形成本發明之底層膜。
又,由本發明之阻劑底層膜形成組成物所形成之阻劑底層膜,隨著微影術製程中使用之光的波長不同,有時具有對其光之吸收。再者,如此情況時,可發揮作為具有防止來自基板之反射光的效果之抗反射膜的功能。進一步地,本發明之底層膜,亦可作為用以防止基板與光
阻之相互作用之層、具有防止光阻所用之材料或對光阻曝光時生成之物質對基板之不良作用的功能之層、具有防止加熱燒成時由基板生成之物質對上層光阻之擴散的功能之層、及用以減少半導體基板介電體層所致之光阻層的毒化效果之障蔽層等來使用。
又,由阻劑底層膜形成組成物所形成之阻劑底層膜,係適用於形成有雙重金屬鑲嵌製程所用之通孔的基板,可作為可將孔洞無空隙地填充之埋入材來使用。又,亦可作為用以使具有凹凸之半導體基板的表面平坦化之平坦化材來使用。
又,作為EUV阻劑之底層膜,除了作為硬遮罩之功能以外,於以下目的亦可使用。可使用上述阻劑底層膜形成組成物,作為可在不與EUV阻劑互混之下,防止EUV曝光(波長13.5nm)時所不佳的曝光光、例如上述UV或DUV(ArF光、KrF光)之來自基板或界面的反射之EUV阻劑的底層抗反射膜。於EUV阻劑之底層可有效率地防止反射。作為EUV阻劑底層膜使用時,製程可與光阻用底層膜同樣方式進行。
[實施例]
(原料單體合成1)
於100ml茄型燒瓶中,置入N-甲基胺基丙基三乙氧基矽烷10.00g(0.05mol)、三乙基胺6.54g(0.06mol)、N,N-
二甲基甲醯胺33.1g,一邊以磁攪拌器攪拌,同時滴入2-氯乙基苯基碸10.59g(0.05mol)、N,N-二甲基甲醯胺21.2g之混合溶劑,滴入結束後於70℃加熱,反應4小時。藉由過濾以去除因反應而生成之三乙基胺鹽酸鹽,以蒸發器將濾液去除溶劑後,以乙酸乙酯、水進行分液。將有機層以硫酸鎂進行脫水處理後,進行過濾,以蒸發器去除乙酸乙酯,得到粗生成物。藉由將粗生成物減壓蒸餾,得到目標物之化合物1(式(1-1)、X為乙氧基)。
1H-NMR(500MHz):0.47ppm(t、2H)、1.30ppm(quint、2H)、2.02ppm(s、3H)、2.20ppm(t、2H)、2.61ppm(t、2H)、3.43~3.49(m、11H)、7.64~7.93ppm(m、5H)
(原料單體合成2)
於100ml茄型燒瓶中,置入N-甲基烯丙基胺5.00g(0.067mol)、4-氟苯基甲基碸9.80g(0.056mol)、碳酸鉀7.77g(0.056mol)、N-甲基吡咯啶酮10.0g,於60℃加熱並反應8日。將反應液以乙酸乙酯、水進行分液後,以蒸發器去除乙酸乙酯,得到中間體1之粗生成物。
於50ml茄型燒瓶中,置入1.50g(0.006mol)之中間體1、三乙氧基矽烷1.18g(0.007mol)、鉑觸媒PI-Pt 0.08g、甲苯15g,進行加熱回流反應6小時。以過濾去除鉑觸媒PI-Pt,以蒸發器去除甲苯,得到粗生成物。藉由將粗生成物減壓蒸餾,得到目標物之化合物2(式(1-2)、X為乙氧基)。
1H-NMR(500MHz):0.58ppm(t、2H)、1.14ppm(t、9H)、1.58ppm(quint、2H)、2.98ppm(s、3H)、3.06ppm(s、3H)、3.40(t、2H)、3.75ppm(q、6H)、6.78~6.80ppm(m、2H)、7.61~7.63ppm(m、2H)
(合成例1)
將15.42g(70mol%)之四乙氧基矽烷、4.71g(25mol%)之甲基三乙氧基矽烷、1.05g(5mol%)之苯基三甲氧基矽烷、31.77g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.01mol/l之鹽酸7.05g滴入混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單甲基醚乙酸酯21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單甲基醚乙酸酯溶液。添加丙二醇單乙基醚,作為丙二醇單甲基醚乙酸酯/丙二醇單乙基醚20/80之溶劑比率,係調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(E-1)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1600。
(合成例2)
將14.72g(70mol%)之四乙氧基矽烷、4.50g(25mol%)之甲基三乙氧基矽烷、2.09g(5mol%)之3-(三乙氧基矽烷基丙基)二烯丙基三聚異氰酸酯、31.96g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.01mol/l之鹽酸6.73g滴入於混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單甲基醚乙酸酯21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單甲基醚乙酸酯溶液。添加丙二醇單乙基醚,作為丙二醇單甲基醚乙酸酯/丙二醇單乙基醚20/80之溶劑比率,係調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(E-2)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1700。
(合成例3)
將15.36g(70mol%)之四乙氧基矽烷、4.60g(24.5mol%)之甲基三乙氧基矽烷、1.04g(5mol%)之苯基三甲氧基矽烷、0.19g(0.5mol%)之化合物1、31.79g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.02mol/l之鹽酸7.02g滴入於混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單乙基醚21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單乙基醚溶液。添加丙二醇單乙基醚,調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(A-1)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1700。
(合成例4)
將14.66g(70mol%)之四乙氧基矽烷、4.39g(24.5mol%)之甲基三乙氧基矽烷、2.08g(5mol%)之3-(三乙氧基矽烷基丙基)二烯丙基三聚異氰酸酯、0.18g(0.5mol%)之化合物1、31.79g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.02mol/l之鹽酸6.70g滴入於混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單
乙基醚21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單乙基醚溶液。添加丙二醇單乙基醚,調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(A-2)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1800。
(合成例5)
將15.20g(70mol%)之四乙氧基矽烷、3.72g(20mol%)之甲基三乙氧基矽烷、1.03g(5mol%)之苯基三甲氧基矽烷、1.26g(5mol%)之(4-甲氧基苄基)三甲氧基矽烷、31.83g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.01mol/l之鹽酸6.95g滴入於混合溶液。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單甲基醚乙酸酯21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單甲基醚乙酸酯溶液。添加丙二醇單乙基醚,調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(E-3)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1600。
(合成例6)
將14.53g(70mol%)之四乙氧基矽烷、3.55g(20mol%)之甲基三乙氧基矽烷、2.06g(5mol%)之3-(三乙氧基矽烷基丙基)二烯丙基三聚異氰酸酯、1.21g(5mol%)之(4-甲氧基苄基)三甲氧基矽烷、32.02g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.01mol/l之鹽酸6.64g滴入混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單甲基醚乙酸酯21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單甲基醚乙酸酯溶液。添加丙二醇單乙基醚,調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(E-4)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1600。
(合成例7)
將15.14g(70mol%)之四乙氧基矽烷、3.61g(19.5mol%)之甲基三乙氧基矽烷、1.03g(5mol%)之苯基三甲氧基矽烷、1.26g(5mol%)之(4-甲氧基苄基)三甲氧基矽烷、0.19g(0.5mol%)之化合物1、31、85g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.02mol/l之鹽酸6.92g滴入混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單乙基醚21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單乙基醚溶液。添加丙二醇單乙基醚,調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(A-3)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1700。
(合成例8)
將14.47g(70mol%)之四乙氧基矽烷、3.45g(19.5mol%)之甲基三乙氧基矽烷、2.05g(5mol%)之3-(三乙氧基矽烷基丙基)二烯丙基三聚異氰酸酯、1.20g(5mol%)之(4-甲氧基苄基)三甲氧基矽烷、0.18g(0.5mol%)之化合物1、32.03g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.02mol/l之鹽酸6.62g滴入於混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單乙基醚21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單乙基醚溶液。添加丙二醇單乙基醚,調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(A-4)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1800。
(比較合成例1)
將15.40g(70mol%)之四乙氧基矽烷、4.61g(24.5mol%)之甲基三乙氧基矽烷、1.05g(5mol%)之苯基三甲氧基矽烷、0.12g(0.5mol%)之N-(3-三乙氧基矽烷基丙基)-4,5-二氫咪唑、31.78g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.02mol/l之鹽酸7.04g滴入於混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶
液冷卻至室溫,於反應溶液中添加丙二醇單乙基醚21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單乙基醚溶液。添加丙二醇單乙基醚,調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(E-5)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1700。
(比較合成例2)
將15.39g(70mol%)之四乙氧基矽烷、4.70g(25mol%)之甲基三乙氧基矽烷、0.94g(4.5mol%)之苯基三甲氧基矽烷、0.15g(0.5mol%)之4-甲基碸基甲基苯基三甲氧基矽烷、31.78g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.02mol/l之鹽酸7.04g滴入於混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單乙基醚21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單乙基醚溶液。添加丙二醇單乙基醚,調整至以
140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(E-6)之聚合物為主成分,存在有水解物與單體。聚合物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1600。
(比較合成例3)
將15.37g(70mol%)之四乙氧基矽烷、4.70g(25mol%)之甲基三乙氧基矽烷、0.94g(4.5mol%)之苯基三甲氧基矽烷、0.19g(0.5mol%)之3-(N-三乙氧基矽烷基)丙基苯磺醯胺、31.79g之丙酮置入100ml之燒瓶,將混合溶液一邊以磁攪拌器攪拌,同時將0.02mol/l之鹽酸7.02g滴入混合溶液中。添加後,將燒瓶移至調整為85℃之油浴,加溫回流下反應240分鐘。之後,將反應溶液冷卻至室溫,於反應溶液中添加丙二醇單乙基醚21g,將反應副生物之乙醇、水、鹽酸減壓餾除,濃縮而得到水解縮合物(聚合物)丙二醇單乙基醚溶液。添加丙二醇單乙基醚,調整至以140℃中之固體剩餘物換算,為15重量百分比。生成物係以式(E-7)之聚合物為主成分,存在有水解物與單體。聚合
物之以GPC所得之重量平均分子量,以聚苯乙烯換算,為Mw1700。
(阻劑底層膜之調製)
將上述合成例1至合成例8中得到之含有矽之聚合物、酸、硬化觸媒、添加劑、溶劑、水,以表1所示比例混合,藉由以0.1μm之氟樹脂製濾膜過濾,分別調製阻劑底層膜形成用組成物之溶液。
表1中,馬來酸略稱為MA、N-(3-三乙氧基矽烷基丙基)-4,5-二氫咪唑略稱為IMIDTEOS、雙酚S略稱為BPS、丙二醇單甲基醚乙酸酯略稱為PGMEA、丙二醇單乙基醚略稱為PGEE。水係使用超純水。各添加量係以質量份表示。聚合物之添加量並非聚合物溶液之質量,而係聚合物之質量。
[表1]
(耐溶劑性試驗)
將實施例1至實施例14及比較例1至比較例7之阻劑底層膜形成組成物,以旋轉塗佈法分別塗佈於矽晶圓上,於240℃之加熱板上燒成1分鐘,形成阻劑底層膜。之後,浸漬於使用於頂塗佈阻劑組成物之溶劑的丙二醇單甲基醚乙酸酯(PGMEA)1分鐘,浸漬前後的阻劑底層膜之膜厚變化為1nm以下時則判斷為「良好(○)」,膜厚變化在其以上時則判斷為「不良(×)」。所得之結果如表2所示。
(光學定數測定)
將實施例1至14、比較例1至7中調製之含有Si之阻劑底層膜形成組成物,使用旋轉器分別塗佈於矽晶圓上
。於加熱板上200℃加熱1分鐘,形成含有Si之阻劑底層膜(膜厚0.05μm)。然後,將該等阻劑底層膜使用分光橢圓偏光計(J.A.Woollam公司製、VUV-VASE VU-302),測定於波長193nm之折射率(n值)及光學吸光係數(k值,亦稱為衰減係數)。
(乾蝕刻速度之測定)
乾蝕刻速度之測定所用之蝕刻器及蝕刻氣體係使用以下者。
ES401(日本Scientific製):CF4
RIE-10NR(Samco製):O2
將實施例1至14、比較例1至7中調製之含有Si之阻劑底層膜形成組成物的溶液,使用旋轉器塗佈於矽晶圓上。於加熱板上240℃加熱1分鐘,分別形成含有Si之阻劑底層膜(膜厚0.08μm(以CF4氣體的蝕刻速度測定用)、0.05μm(以O2氣體的蝕刻速度測定用)。又,同樣地將下述記載之有機底層膜形成組成物使用旋轉器於矽晶圓上形成塗膜。作為蝕刻氣體,使用O2氣體測定乾蝕刻速度,進行與實施例1至實施例14、比較例1至比較例7之含有Si之阻劑底層膜的乾蝕刻速度之比較。
對丙二醇單甲基醚乙酸酯(PGMEA)之溶劑耐性、於193nm波長之折射率n、於193nm波長之光學吸收係數k、以氟系氣體(CF4氣體)之蝕刻率(蝕刻速度:nm/分)、氧系氣體(O2氣體)耐性,係以(本願阻劑底層膜)/(有機底層膜)
之蝕刻率比來顯示。
(有機阻劑底層膜之調製)
在氮下,於100mL四口燒瓶中添加咔唑(6.69g、0.040mol、東京化成工業(股)製)、9-茀酮(7.28g、0.040mol、東京化成工業(股)製)、對甲苯磺酸一水合物(0.76g、0.0040mol、東京化成工業(股)製),饋入1,4-二噁烷(6.69g、關東化學(股)製),攪拌,昇溫至100℃並溶解
而開始聚合。24小時後放冷至60℃後,添加氯仿(34g、關東化學(股)製)稀釋,對甲醇(168g、關東化學(股)製)再沈澱。將所得之沈澱物過濾,以減壓乾燥機80℃乾燥24小時,得到目標之聚合物(式(F-1)、以下略稱為PCzFL)9.37g。
PCzFL之1H-NMR之測定結果係如以下所示。
1H-NMR(400MHz,DMSO-d6):δ7.03-7.55(br,12H),δ7.61-8.10(br,4H),δ11.18(br,1H)
PCzFL之GPC之以聚苯乙烯換算所測定的重量平均分子量Mw為2800、多分散度Mw/Mn為1.77。
於所得到之樹脂20g中,混合作為交聯劑之四甲氧基甲基乙炔脲(三井Cytec(股)製、商品名Powderlink 1174)3.0g、作為觸媒之吡啶鎓對甲苯磺酸酯0.30g、作為界面活性劑之Megaface R-30(大日本油墨化學(股)製、商品名)0.06g,溶解於丙二醇單甲基醚乙酸酯88g作為溶液。之後,使用孔徑0.10μm之聚乙烯製微濾膜過濾,進一步地使用孔徑0.05μm之聚乙烯製微濾膜過濾,調製多層膜之微影術製程所用之有機阻劑底層膜形成組成物的溶液。
(阻劑圖型化評估)
將上述式中所得之有機底層膜(A層)形成組成物塗佈於矽晶圓上,於加熱板上240℃烘烤60秒,得到膜厚200nm之有機底層膜(A層)。於其上塗佈實施例1至實施例10、比較例1至比較例7得到之含有Si之阻劑底層膜(B層)形成組成物,於加熱板上240℃烘烤45秒,得到含有Si之阻劑底層膜(B層)。含有Si之阻劑底層膜(B層)之膜厚為45nm。
(以鹼顯影液之顯影.PTD)
於B層之上藉由旋轉器分別塗佈市售之光阻溶液(JSR(股)製、商品名AR2772),於加熱板上110℃烘烤60秒,形成膜厚120nm之光阻膜(C層)。阻劑之圖型化係使用NIKON公司製ArF曝光機S-307E(波長193nm、NA、σ:0.85、0.93/0.85(Dipole)液浸液:水)進行。標的係通過以顯影後形成光阻之線寬及其線間寬度為0.065μm之所謂線寬與線距(稠密線)的方式所設定之遮罩以進行曝光。
之後,於加熱板上110℃烘烤60秒,冷卻後,於60秒單槳(single paddle)式步驟,以2.38質量%濃度之氫氧化四甲基銨水溶液(顯影液)顯影。關於所得之光阻圖型,將未發生大的圖型剝離或底切、線底部之膨大(腳化)者評估為良好。
(以有機溶劑之顯影.NTD)
於B層之上藉由旋轉器分別塗佈市售之光阻溶液(富士軟片(股)製、商品名FAiRS-9521NT05),於加熱板上100℃加熱1分鐘,形成膜厚85nm之光阻膜(C層)。
接著,使用(股)Nikon製NSR-S307E掃描器(波長193nm、NA、σ:0.85、0.93/0.85),分別通過以顯影後形成光阻之線寬及其線間之寬度為0.065μm、亦即0.065μm之線寬與線距(L/S)=1/1之稠密線的方式所設定的遮罩、及以顯影後形成光阻之線寬及其線間之寬度為0.060μm、亦即0.060μm之線寬與線距(L/S)=1/1的稠密線的方式所設
定的遮罩進行曝光。之後,於加熱板上100℃烘烤60秒,冷卻後,使用乙酸丁酯(溶劑顯影液)顯影60秒,於阻劑底層膜(B層)上形成負型之圖型。
關於所得之光阻圖型,將未發生大的圖型剝離或底切、線底部之膨大(腳化)者評估為良好。
[產業上之可利用性]
可利用作為用以形成可使用作為硬遮罩之阻劑底層膜的微影術用阻劑底層膜形成組成物。此外,不引起與頂塗佈阻劑之互混。氟系之蝕刻氣體中,相較於阻劑具有大的乾蝕刻速度,可將阻劑圖型轉印至本案阻劑底層膜,且氧系蝕刻氣體中,顯示蝕刻耐性,可將阻劑圖型轉印至有機底層膜。如此地,提供用以形成能夠以矩形圖型加工基板之阻劑底層膜的阻劑底層膜形成組成物。
Claims (9)
- 一種組成物,其包含:作為矽烷之水解性有機矽烷、該水解性有機矽烷之水解物、該水解性有機矽烷之水解縮合物、或其等之組合,其中該水解性有機矽烷包含下列的組合:選自由式(1-a)的矽烷化合物及式(1-b)的矽烷化合物組成的群組之至少一種矽烷化合物:
- 一種微影術用阻劑底層膜形成組成物,其包含:作為矽烷之水解性有機矽烷、該水解性有機矽烷之水解物、該水解性有機矽烷之水解縮合物、或其等之組合,其中該水解性有機矽烷包含下列的組合:選自由式(1-a)的矽烷化合物及式(1-b)的矽烷化合物組成的群組之至少一種矽烷化合物:
- 如申請專利範圍第2項之阻劑底層膜形成組成物,其中上述以式(1-a)表示之矽烷化合物為以下述式(2)表示之矽烷化合物:
- 如申請專利範圍第2項之阻劑底層膜形成組成物,其含有至少一種上述以式(1-a)或式(1-b)表示之矽烷化合物與以式(3)表示之有機矽化合物之水解縮合物作為聚合物。
- 如申請專利範圍第2項之阻劑底層膜形成組成物,其進一步含有酸。
- 如申請專利範圍第2項之阻劑底層膜形成組成物,其進一步含有水。
- 一種阻劑底層膜,其係藉由將如申請專利範圍第2項之阻劑底層膜形成組成物塗佈於半導體基板上並燒成該組成物而得到。
- 一種半導體裝置之製造方法,其包含:將如申請專利範圍第2項之阻劑底層膜形成組成物塗佈於半導體基板上並燒成該組成物而形成阻劑底層膜之步驟;於前述阻劑底層膜之上塗佈阻劑用組成物而形成阻劑膜之步驟;使前述阻劑膜曝光之步驟;於曝光後將該阻劑膜顯影而得到經圖型化之阻劑膜的步驟;依照該經圖型化之阻劑膜的圖型來蝕刻該阻劑底層膜之步驟;以及依照該阻劑膜及該阻劑底層膜之圖型來加工半導體基板之步驟。
- 一種半導體裝置之製造方法,其包含:於半導體基板上形成有機底層膜之步驟;於該有機底層膜上塗佈如申請專利範圍第2項之阻劑底層膜形成組成物並燒成該組成物而形成阻劑底層膜之步驟;於前述阻劑底層膜之上塗佈阻劑用組成物而形成阻劑膜之步驟;使前述阻劑膜曝光之步驟; 於曝光後將前述阻劑膜顯影而得到經圖型化之阻劑膜的步驟;依照該經圖型化之阻劑膜的圖型來蝕刻該阻劑底層膜之步驟;依照該經圖型化之阻劑底層膜的圖型來蝕刻該有機底層膜之步驟;及依照該經圖型化之有機底層膜的圖型來加工半導體基板之步驟。
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