JPWO2008111134A1 - 表面疎水化膜、表面疎水化膜形成材料、配線層、半導体装置および半導体装置の製造方法 - Google Patents
表面疎水化膜、表面疎水化膜形成材料、配線層、半導体装置および半導体装置の製造方法 Download PDFInfo
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- JPWO2008111134A1 JPWO2008111134A1 JP2009503777A JP2009503777A JPWO2008111134A1 JP WO2008111134 A1 JPWO2008111134 A1 JP WO2008111134A1 JP 2009503777 A JP2009503777 A JP 2009503777A JP 2009503777 A JP2009503777 A JP 2009503777A JP WO2008111134 A1 JPWO2008111134 A1 JP WO2008111134A1
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- insulating film
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- C—CHEMISTRY; METALLURGY
- 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
- C09D183/00—Coating compositions based on macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon, with or without sulfur, nitrogen, oxygen, or carbon only; Coating compositions based on derivatives of such polymers
- C09D183/04—Polysiloxanes
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- C—CHEMISTRY; METALLURGY
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- H01L21/02216—Forming insulating materials on a substrate characterised by the type of layer, e.g. type of material, porous/non-porous, pre-cursors, mixtures or laminates the layer being characterised by the precursor material for deposition the precursor containing a compound comprising Si the compound comprising silicon and oxygen the compound being a molecule comprising at least one silicon-oxygen bond and the compound having hydrogen or an organic group attached to the silicon or oxygen, e.g. a siloxane
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- H01L21/31—Treatment of semiconductor bodies using processes or apparatus not provided for in groups H01L21/20 - H01L21/26 to form insulating layers thereon, e.g. for masking or by using photolithographic techniques; After treatment of these layers; Selection of materials for these layers
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- H01L21/71—Manufacture of specific parts of devices defined in group H01L21/70
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Abstract
Description
R1Si(OR8)3・・・・・式(2)
R2R3Si(OR9)2・・・式(3)
R4R5R6SiOR10・・・式(4)
(式1〜4中のR1〜R10は、互いに独立に、水素または、それぞれ置換基を有していてもよい、炭素数1〜20のアルキル基、炭素数2〜20のアルケニル基、アルキニル基、アルキルカルボニル基、アルケニルアルキル基およびアルキニルアルキル基ならびに炭素数6〜20のアリール基からなる群から選ばれた基を含む基である。前記の少なくとも一つ含まれた化合物中に、R1〜R6のいずれかが含まれる場合には、その少なくとも一つが、硫黄原子、リン原子および窒素原子からなる群から選ばれた少なくとも一つの原子を含む。)
本発明の他の一態様によれば、上記の表面疎水化膜形成材料を用いて作製された、上記の表面疎水化膜が提供される。
X1Si(OR12)3・・・・式(6)
X2X3Si(OR13)2・・・式(7)
X4X5X6SiOR14・・・式(8)
(式(5)〜(8)中、X1〜X6は、互いに独立に、水素原子、フッ素原子、または、それぞれ置換基を有していてもよい、炭素数1〜8のアルキル基、フッ素置換アルキル基、アリール基およびビニル基からなる群から選ばれた基を含む基である。R11〜R14は互いに独立に、それぞれ置換基を有していてもよい、炭素数1〜20のアルキル基、炭素数2〜20のアルケニル基、アルキニル基、アルキルカルボニル基、アルケニルアルキル基およびアルキニルアルキル基ならびに炭素数6〜20のアリール基からなる群から選ばれた基を含む基である。)
本発明の他の態様によれば、上記の表面疎水化膜を含んでなる配線層や、半導体装置、上記の表面疎水化膜形成材料を用いて作製された配線層や半導体装置、上記の製造法を用いて製造された半導体装置等が提供される。
2 素子間分離膜
3 サイドウォール絶縁膜
4 ゲート電極
5a ソース拡散層
5b ドレイン拡散層
6 層間絶縁膜
7 ストッパ膜
8 TiN
9 導体プラグ
10 低誘電率被膜(配線分離絶縁膜)
11 TEOS−SiO2膜
12 表面疎水化膜
13 SiOC膜
14 SiN膜
15 低誘電率絶縁膜
16 TEOS−SiO2膜
17 Cu層
18 Cu層
19 キャップ層
20 表面疎水化膜
21 コンタクトホール
22 配線溝
23 シード層
24 配線層
25 ビア
26 配線溝
27 シード層
28 ビア
29 配線層
30 ビア穴
31 絶縁膜
32 TiNバリアメタル層
33 コンタクトホール
34 パッシベーション膜
35 電極パッド
111 配線
112 バリアメタル層
113 表面疎水化膜
114 絶縁膜
X1Si(OR12)3・・・・式(6)
X2X3Si(OR13)2・・式(7)
X4X5X6SiOR14・・・式(8)
(式(5)〜(8)中、X1〜X6は、互いに独立に、水素原子、フッ素原子、または、それぞれ置換基を有していてもよい、炭素数1〜8のアルキル基、フッ素置換アルキル基、アリール基およびビニル基からなる群から選ばれた基を含む基である。R11〜R14は互いに独立に、それぞれ置換基を有していてもよい、炭素数1〜20のアルキル基、炭素数2〜20のアルケニル基、アルキニル基、アルキルカルボニル基、アルケニルアルキル基およびアルキニルアルキル基ならびに炭素数6〜20のアリール基からなる群から選ばれた基を含む基である。)
このようにして得られる低誘電率膜は同等の誘電率を持つ他の低誘電率膜と比較して機械的強度・絶縁性・信頼性に優れていることが多く、絶縁性・信頼性のより高い配線層(LSI配線層等)の形成に寄与し得る。
R1Si(OR8)3・・・・・式(2)
R2R3Si(OR9)2・・・式(3)
R4R5R6SiOR10・・・式(4)
(式1〜4中のR1〜R10は、互いに独立に、水素または、それぞれ置換基を有していてもよい、炭素数1〜20のアルキル基、炭素数2〜20のアルケニル基、アルキニル基、アルキルカルボニル基、アルケニルアルキル基およびアルキニルアルキル基ならびに炭素数6〜20のアリール基からなる群から選ばれた基を含む基である。前記の少なくとも一つ含まれた化合物中に、R1〜R6のいずれかが含まれる場合には、その少なくとも一つが、硫黄原子、リン原子および窒素原子からなる群から選ばれた少なくとも一つの原子を含む。)
これらの剤は、容易に、加水分解物、縮合物およびそれらの混合物に変性することができる。このため、これらの剤や、加水分解物、縮合物およびそれらの混合物を使用することにより、上記効果を与える表面疎水化膜を容易に作製することができる。
H2N(CH2)(CH2)(CH2)Si(OCH3)3
H2N(CH2)(CH2)(CH2)Si(OH)3
H2N(CH2)(CH2)Si(OC2H5)3
H2N(CH2)(CH2)Si(OCH3)3
H2N(CH2)(CH2)Si(OH)3
H2N(CH2)Si(OC2H5)3
H2N(CH2)Si(OCH3)3
H2N(CH2)Si(OH)3
H3C(NH)(CH2)(CH2)(CH2)Si(OCH3)3
H3C(NH)(CH2)(CH2)(CH2)Si(CH3)(OCH3)2
(H3C)2N(CH2)(CH2)(CH2)Si(CH3)(OC2H5)2
(H3C)2N(CH2)(CH2)(CH2)Si(OC2H5)3
(C6H5)HN(CH2)(CH2)(CH2)Si(OCH3)3
(C6H5)(H3CO)2SiO(CH2)(CH2)N(C5H10)
OCN(CH2)(CH2)(CH2)Si(OC2H5)3
HCoC(CH2)(CO)(NH)(CH2)(CH2)(CH2)Si(OC2H5)3
(H3C)3CO(CO)(NH)(CH2)(CH2)(CH2)Si(OC2H5)3
H2N(CO)(NH)(CH2)(CH2)(CH2)Si(OC2H5)3
H2N(CO)(NH)(CH2)(CH2)(CH2)Si(OCH3)3
(H5C2O)2(PO)(CH2)(CH2)Si(OC2H5)3
(C6H5)2P(CH2)(CH2)Si(CH3)2OC2H5
(C6H5)2P(CH2)(CH2)Si(OC2H5)3
(C6H5)2P(CH2)(CH2)Si(OCH3)3
(C6H5)2P(CH2)(CH2)Si(OH)3
(C6H5)2P(CH2)Si(OC2H5)3
(C6H5)2P(CH2)Si(OCH3)3
(C6H5)2P(CH2)Si(OH)3
(H3C)(PO2−Na+)O(CH2)(CH2)(CH2)Si(OH)3
HS(CH2)Si(OC2H5)3
HS(CH2)Si(CH3)(OC2H5)2
HS(CH2)Si(CH3)2OC2H5
HS(CH2)Si(OCH3)3
HS(CH2)Si(CH3)(OCH3)2
HS(CH2)Si(CH3)2OCH3
HS(CH2)(CH2)Si(OC2H5)3
HS(CH2)(CH2)Si(CH3)(OC2H5)2
HS(CH2)(CH2)Si(CH3)2OC2H5
HS(CH2)(CH2)Si(OCH3)3
HS(CH2)(CH2)Si(CH3)(OCH3)2
HS(CH2)(CH2)Si(CH3)2OCH3
HS(CH2)(CH2)(CH2)Si(OC2H5)3
HS(CH2)(CH2)(CH2)Si(CH3)(OC2H5)2
HS(CH2)(CH2)(CH2)Si(CH3)2OC2H5
HS(CH2)(CH2)(CH2)Si(OCH3)3
HS(CH2)(CH2)(CH2)Si(CH3)(OCH3)2
HS(CH2)(CH2)(CH2)Si(CH3)2OCH3
なお、(6)〜(8)のX1〜X6に硫黄原子、リン原子および/または窒素原子が含まれる場合も、上記(2)〜(4)のR1〜R6についての上記説明と同様に考えることができる。
(I)半導体装置の配線溝やビア孔をエッチングで形成する工程
(II)次いで、表面疎水化膜を形成する工程
(III)次いで、バリアメタル層を形成する工程
を含むように用いると、実際半導体装置の製造に好適に応用でき、効果的である。具体的には、配線との密着強度を向上させると共に、エッチングによる配線溝側壁の絶縁膜表面または絶縁膜中の水分を低減することができ、配線間のリーク電流量がより少なく、またより信頼性の高いLSI配線層を形成可能になる。
低誘電率絶縁膜を形成するため、まず、
テトラエトキシシラン 20.8g(0.1mol)
メチルトリエトキシシラン 17.8g(0.1mol)
グリシドキシプロピルトリメトキシシラン 23.6g(0.1mol)
メチルイソブチルケトン 39.6g
の組成比の溶液200mLを反応容器に仕込み、1%のテトラメチルアンモニウムハイドロキサイド水溶液を16.2g(0.9mol)を10分間滴下し、滴下終了後2時間の熟成反応を行った。次いで、硫酸マグネシウム5gを添加して過剰の水分を除去した後、熟成反応により生成したエタノールをロータリーエバポレータにより反応溶液が50mLになるまで除去し、次いで、得られた反応溶液にメチルイソブチルケトンを20mL添加し、比誘電率2.5の塗布型低誘電率絶縁材料前躯体塗布溶液を作製した。
図1〜10に本発明に係る多層配線実施例の作製法を示す。まず、素子間分離膜2で分離され、ソース拡散層5aとドレイン拡散層5bとサイドウォール絶縁膜3とを有するゲート電極4を形成したトランンジスタ層を形成したシリコンウェハ1(ステップ1)に、層間絶縁膜6(リンガラス)およびストッパ膜7を形成し(ステップ2)、電極取り出し用のコンタクトホール21を形成した(ステップ3)。
例2において、表面疎水化層12、20を例1のサンプル6を用いて作製し、他は全く同様にして3層配線を形成した。試作した多層配線を用いて電流密度を1MA/cm2としてビアのEM測定を行ったところ、500時間経過しても不良の発生はなかった。
例2において、表面疎水化層12、20を例1のサンプル7を用いて作製し、他は全く同様にして3層配線を形成した。試作した多層配線を用いて電流密度を1MA/cm2としてビアのEM測定を行ったところ、500時間経過しても不良の発生はなかった。
例2において、表面疎水化膜12、20を形成せず、他は全く同様にして3層配線を形成した。試作した多層配線を用いて電流密度を1MA/cm2としてビアのEM測定を行ったところ、不良の発生までの経過時間のメジアンは40時間であった。
Claims (12)
- 絶縁膜と接触した、当該接触時の当該絶縁膜よりも疎水性の大きい表面疎水化膜であって、その反対側の面で配線とも接触し、硫黄原子、リン原子および窒素原子からなる群から選ばれた少なくとも一つの原子を含む表面疎水化膜を形成する材料。
- 前記表面疎水化膜形成材料が、平均分子量が1000以下である条件と、1分子内に含まれるケイ素原子の数が20以下である条件との少なくともいずれか一つを満たすケイ素化合物を含有してなるものである、請求項1に記載の表面疎水化膜形成材料。
- 前記ケイ素化合物が、オルガノシラン、オルガノシランの加水分解物および縮合物ならびにそれらの混合物からなる群から選ばれたものである、請求項2に記載の表面疎水化膜形成材料。
- 前記オルガノシランを加水分解して得られる生成物中に含まれる成分と同一物質である溶媒を含む、請求項3に記載の表面疎水化膜形成材料。
- 前記オルガノシランが、下記(2)〜(4)のいずれかの式で表される化合物を少なくとも一つ含み、オプションで下記(1)の式で表される化合物を含む、請求項3または4に記載の表面疎水化膜形成材料。
Si(OR7)4・・・・・・式(1)
R1Si(OR8)3・・・・・式(2)
R2R3Si(OR9)2・・・式(3)
R4R5R6SiOR10・・・式(4)
(式1〜4中のR1〜R10は、互いに独立に、水素または、それぞれ置換基を有していてもよい、炭素数1〜20のアルキル基、炭素数2〜20のアルケニル基、アルキニル基、アルキルカルボニル基、アルケニルアルキル基およびアルキニルアルキル基ならびに炭素数6〜20のアリール基からなる群から選ばれた基を含む基である。前記の少なくとも一つ含まれた化合物中に、R1〜R6のいずれかが含まれる場合には、その少なくとも一つが、硫黄原子、リン原子および窒素原子からなる群から選ばれた少なくとも一つの原子を含む。) - 少なくとも絶縁膜と配線とを含んでなる多層配線構造であって、前記絶縁膜と前記配線層の間に請求項1〜5のいずれかに記載の表面疎水化膜形成材料を用いて作製された表面疎水化膜を有する多層配線構造。
- 少なくとも絶縁膜と配線層とトランジスタとを含んでなる半導体装置であって、前記絶縁膜と前記配線層の間に請求項1〜5のいずれかに記載の表面疎水化膜形成材料を用いて作製された表面疎水化膜を有する半導体装置。
- 半導体装置上の絶縁膜に接して請求項1〜5のいずれかに記載の表面疎水化膜形成材料を塗布することと、
その後当該塗布された膜を80℃〜500℃で0.5〜180分間加熱して表面疎水化膜を形成することと
を含む半導体装置の製造方法。 - 前記絶縁膜に表面疎水化膜形成材料を塗布する前に、エッチングまたは化学的機械研磨を行う、請求項8に記載の半導体装置の製造方法。
- 前記絶縁膜が層間絶縁膜と層間絶縁膜の保護膜との少なくともいずれか一方である、請求項9に記載の半導体装置の製造方法。
- 前記絶縁膜が、下記式(5)〜(8)で表されるオルガノシランを単独または組み合わせ、テトラアルキルアンモニウムハイドロオキサイドの存在下、加水分解して得られるケイ素化合物を含む液状組成物を、被加工基材上に塗布し、当該被加工基材上に塗布された液状組成物からなる被膜を80℃以上350℃以下の温度で加熱処理し、当該加熱処理により加熱された被膜を350℃より高く450℃以下の温度で焼成することを含んでなる処理により得られたものである、請求項8〜10のいずれかに記載の半導体装置の製造方法。
Si(OR11)4・・・・・・式(5)
X1Si(OR12)3・・・・式(6)
X2X3Si(OR13)2・・・式(7)
X4X5X6SiOR14・・・式(8)
(式(5)〜(8)中、X1〜X6は、互いに独立に、水素原子、フッ素原子または、それぞれ置換基を有していてもよい、炭素数1〜8のアルキル基、フッ素置換アルキル基、アリール基およびビニル基からなる群から選ばれた基を含む基である。R11〜R14は互いに独立に、それぞれ置換基を有していてもよい、炭素数1〜20のアルキル基、炭素数2〜20のアルケニル基、アルキニル基、アルキルカルボニル基、アルケニルアルキル基およびアルキニルアルキル基ならびに炭素数6〜20のアリール基からなる群から選ばれた基を含む基である。) - 前記絶縁膜が比誘電率2.7以下である、請求項8〜11のいずれかに記載の半導体装置の製造方法。
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