JP2009170439A - ゲート絶縁膜の形成方法 - Google Patents
ゲート絶縁膜の形成方法 Download PDFInfo
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- JP2009170439A JP2009170439A JP2008003336A JP2008003336A JP2009170439A JP 2009170439 A JP2009170439 A JP 2009170439A JP 2008003336 A JP2008003336 A JP 2008003336A JP 2008003336 A JP2008003336 A JP 2008003336A JP 2009170439 A JP2009170439 A JP 2009170439A
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- Prior art keywords
- precursor
- forming
- film
- gate insulating
- semiconductor substrate
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- 238000000034 method Methods 0.000 title claims description 101
- 238000009413 insulation Methods 0.000 title abstract 3
- 239000002243 precursor Substances 0.000 claims abstract description 121
- 239000007800 oxidant agent Substances 0.000 claims abstract description 87
- 238000001179 sorption measurement Methods 0.000 claims abstract description 73
- 229910052914 metal silicate Inorganic materials 0.000 claims abstract description 64
- 229910044991 metal oxide Inorganic materials 0.000 claims abstract description 59
- 150000004706 metal oxides Chemical class 0.000 claims abstract description 59
- 239000000203 mixture Substances 0.000 claims abstract description 44
- 238000006243 chemical reaction Methods 0.000 claims abstract description 25
- 229910052751 metal Inorganic materials 0.000 claims abstract description 19
- 239000002184 metal Substances 0.000 claims abstract description 19
- 239000004065 semiconductor Substances 0.000 claims description 64
- 239000000758 substrate Substances 0.000 claims description 62
- 230000001590 oxidative effect Effects 0.000 claims description 43
- 239000001301 oxygen Substances 0.000 claims description 41
- 229910052760 oxygen Inorganic materials 0.000 claims description 41
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 39
- 238000000231 atomic layer deposition Methods 0.000 claims description 31
- 229910052735 hafnium Inorganic materials 0.000 claims description 30
- 238000010926 purge Methods 0.000 claims description 26
- 229910052710 silicon Inorganic materials 0.000 claims description 25
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 23
- 229910052814 silicon oxide Inorganic materials 0.000 claims description 23
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical group [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 claims description 20
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 claims description 19
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical group [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 claims description 17
- 229920006395 saturated elastomer Polymers 0.000 claims description 14
- 238000005229 chemical vapour deposition Methods 0.000 claims description 13
- 239000010703 silicon Substances 0.000 claims description 13
- 229910003902 SiCl 4 Inorganic materials 0.000 claims description 8
- 230000008569 process Effects 0.000 claims description 8
- 229910000449 hafnium oxide Inorganic materials 0.000 claims description 7
- WIHZLLGSGQNAGK-UHFFFAOYSA-N hafnium(4+);oxygen(2-) Chemical compound [O-2].[O-2].[Hf+4] WIHZLLGSGQNAGK-UHFFFAOYSA-N 0.000 claims description 7
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 claims description 6
- PDPJQWYGJJBYLF-UHFFFAOYSA-J hafnium tetrachloride Chemical group Cl[Hf](Cl)(Cl)Cl PDPJQWYGJJBYLF-UHFFFAOYSA-J 0.000 claims description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 5
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 claims description 4
- 238000010438 heat treatment Methods 0.000 claims description 4
- 238000002156 mixing Methods 0.000 claims description 4
- VXEGSRKPIUDPQT-UHFFFAOYSA-N 4-[4-(4-methoxyphenyl)piperazin-1-yl]aniline Chemical group C1=CC(OC)=CC=C1N1CCN(C=2C=CC(N)=CC=2)CC1 VXEGSRKPIUDPQT-UHFFFAOYSA-N 0.000 claims description 3
- XLYOFNOQVPJJNP-ZSJDYOACSA-N Heavy water Chemical compound [2H]O[2H] XLYOFNOQVPJJNP-ZSJDYOACSA-N 0.000 claims description 3
- VZVQQBDFMNEUHK-UHFFFAOYSA-N [La].[Hf] Chemical compound [La].[Hf] VZVQQBDFMNEUHK-UHFFFAOYSA-N 0.000 claims description 3
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims description 3
- 239000005049 silicon tetrachloride Substances 0.000 claims description 3
- 229910001928 zirconium oxide Inorganic materials 0.000 claims description 3
- 229960001730 nitrous oxide Drugs 0.000 claims description 2
- 235000013842 nitrous oxide Nutrition 0.000 claims description 2
- 230000007704 transition Effects 0.000 claims description 2
- 229910004129 HfSiO Inorganic materials 0.000 claims 1
- 230000008021 deposition Effects 0.000 abstract description 16
- 238000009738 saturating Methods 0.000 abstract description 2
- 239000010408 film Substances 0.000 description 278
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 31
- 239000007789 gas Substances 0.000 description 21
- 229910004298 SiO 2 Inorganic materials 0.000 description 17
- 238000000151 deposition Methods 0.000 description 17
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 16
- 229910052757 nitrogen Inorganic materials 0.000 description 15
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 11
- 238000007254 oxidation reaction Methods 0.000 description 9
- 230000007423 decrease Effects 0.000 description 8
- 229910003839 Hf—Si Inorganic materials 0.000 description 7
- 235000012431 wafers Nutrition 0.000 description 7
- 206010021143 Hypoxia Diseases 0.000 description 6
- 230000004048 modification Effects 0.000 description 6
- 238000012986 modification Methods 0.000 description 6
- 239000002994 raw material Substances 0.000 description 6
- 238000010586 diagram Methods 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 239000003990 capacitor Substances 0.000 description 2
- 230000008878 coupling Effects 0.000 description 2
- 238000010168 coupling process Methods 0.000 description 2
- 238000005859 coupling reaction Methods 0.000 description 2
- 230000002950 deficient Effects 0.000 description 2
- 230000001419 dependent effect Effects 0.000 description 2
- 238000004453 electron probe microanalysis Methods 0.000 description 2
- CJNBYAVZURUTKZ-UHFFFAOYSA-N hafnium(iv) oxide Chemical compound O=[Hf]=O CJNBYAVZURUTKZ-UHFFFAOYSA-N 0.000 description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 229910021420 polycrystalline silicon Inorganic materials 0.000 description 2
- 230000009257 reactivity Effects 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 239000012686 silicon precursor Substances 0.000 description 2
- AUTKBRQEGLGPHE-UHFFFAOYSA-N CC[Hf](C)(N)(CC)(CC)CC Chemical compound CC[Hf](C)(N)(CC)(CC)CC AUTKBRQEGLGPHE-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 238000000137 annealing Methods 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 229940079593 drug Drugs 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000001941 electron spectroscopy Methods 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 230000001678 irradiating effect Effects 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- 238000005121 nitriding Methods 0.000 description 1
- 229910002059 quaternary alloy Inorganic materials 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
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- H01L29/40—Electrodes ; Multistep manufacturing processes therefor
- H01L29/43—Electrodes ; Multistep manufacturing processes therefor characterised by the materials of which they are formed
- H01L29/49—Metal-insulator-semiconductor electrodes, e.g. gates of MOSFET
- H01L29/51—Insulating materials associated therewith
- H01L29/517—Insulating materials associated therewith the insulating material comprising a metallic compound, e.g. metal oxide, metal silicate
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- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
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- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
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- C—CHEMISTRY; METALLURGY
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- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/44—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating
- C23C16/455—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating characterised by the method used for introducing gases into reaction chamber or for modifying gas flows in reaction chamber
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Abstract
【解決手段】高誘電体金属シリケートからなるゲート絶縁膜の形成において、金属等を含む前駆体の暴露時間には、表面吸着反応により成膜レートが飽和する時間を用い、酸化剤の暴露時間には、金属酸化膜の組成が化学量論値の97%以上となる時間を用いてALD堆積を行う。
【選択図】図1
Description
前駆体をパージする工程(b)と、
吸着層を酸化剤に暴露して、吸着層を酸化することにより、吸着層から金属酸化膜を形成する工程(c)と、
酸化剤をパージする工程(d)とを備え、
工程(a)、工程(b)、工程(c)及び工程(d)とを1サイクルとして少なくとも1回実行して、金属酸化膜における原子層レベルの少なくとも1層分を形成することにより、高誘電体金属酸化物を形成し、
工程(a)において、半導体基板の前駆体への暴露時間は、1サイクルで堆積される金属酸化膜の1層の厚さが飽和する時間で決定し、
工程(c)において、吸着層の酸化剤への暴露時間は、金属酸化膜における酸素の含有量が化学量論により決定される組成の97%以上となる時間で決定することを特徴とする。
本発明の第1の実施形態について図面を参照しながら説明する。
以下、本発明の第2の実施形態について図面を参照しながら説明する。
2 界面層
3A Hf吸着層
3B 酸化ハフニウム(HfO2)膜
4A Si吸着層
4B 酸化シリコン(SiO2)膜
5A Hf−Si吸着層
5B ハフニウムシリケート(HfSiO)膜
Claims (12)
- 半導体基板の上に、高誘電体金属シリケートからなるゲート絶縁膜を形成するゲート絶縁膜の形成方法であって、
前記半導体基板を500℃以下の温度で且つ所定の圧力下に保持した状態で、前記高誘電体金属シリケートを構成する金属元素を含む第1の前駆体に前記半導体基板を暴露することにより、前記半導体基板の上に前記第1の前駆体からなる第1の吸着層を形成する工程(a)と、
前記第1の前駆体をパージする工程(b)と、
前記第1の吸着層を酸化剤に暴露して、前記第1の吸着層を酸化することにより、前記第1の吸着層から金属酸化膜を形成する工程(c)と、
前記酸化剤をパージする工程(d)と、
前記工程(d)よりも後に、シリコンを含む第2の前駆体に前記金属酸化膜を暴露することにより、前記金属酸化膜の上に前記第2の前駆体からなる第2の吸着層を形成する工程(e)と、
前記第2の前駆体をパージする工程(f)と、
前記第2の吸着層を前記酸化剤に暴露して、前記第2の吸着層を酸化することにより、前記第2の吸着層からシリコン酸化膜を形成する工程(g)と、
前記酸化剤をパージする工程(h)とを備え、
前記工程(a)、工程(b)、工程(c)及び工程(d)とを1サイクルとして少なくとも1回実行して、前記金属酸化膜における原子層レベルの少なくとも1層分を形成し、且つ、前記工程(e)、工程(f)、工程(g)及び工程(h)とを1サイクルとして少なくとも1回実行して前記シリコン酸化膜における原子層レベルの少なくとも1層分を形成することにより、前記高誘電体金属シリケートを形成し、
前記工程(a)において、前記半導体基板の前記第1の前駆体への暴露時間は、前記1サイクルで堆積される前記金属酸化膜の1層の厚さが飽和する時間で決定し、
前記工程(c)において、前記第1の吸着層の前記酸化剤への暴露時間は、前記金属酸化膜における酸素の含有量が化学量論により決定される組成の97%以上となる時間で決定し、
前記工程(e)において、前記金属酸化膜の前記第2の前駆体への暴露時間は、前記1サイクルで堆積される前記シリコン酸化膜の1層の厚さが飽和する時間で決定し、
前記工程(g)において、前記第2の吸着層の前記酸化剤への暴露時間は、前記シリコン酸化膜における酸素の含有量が化学量論により決定される組成の97%以上となる時間で決定することを特徴とするゲート絶縁膜の形成方法。 - 前記工程(c)及び工程(g)における前記酸化剤への暴露時間は、前記半導体基板当たり5秒以上であって、且つ、前記工程(c)における暴露時間及び前記工程(g)における暴露時間のうち、時間が長い工程に暴露時間を合わせることを特徴とする請求項1に記載のゲート絶縁膜形成方法。
- 半導体基板の上に、高誘電体金属酸化物からなるゲート絶縁膜を形成するゲート絶縁膜の形成方法であって、
前記半導体基板を500℃以下の温度で且つ所定の圧力下に保持した状態で、前記高誘電体金属酸化物を構成する金属元素を含む前駆体に前記半導体基板を暴露することにより、前記半導体基板の上に前記前駆体からなる吸着層を形成する工程(a)と、
前記前駆体をパージする工程(b)と、
前記吸着層を酸化剤に暴露して、前記吸着層を酸化することにより、前記吸着層から金属酸化膜を形成する工程(c)と、
前記酸化剤をパージする工程(d)とを備え、
前記工程(a)、工程(b)、工程(c)及び工程(d)とを1サイクルとして少なくとも1回実行して、前記金属酸化膜における原子層レベルの少なくとも1層分を形成することにより、前記高誘電体金属酸化物を形成し、
前記工程(a)において、前記半導体基板の前記前駆体への暴露時間は、前記1サイクルで堆積される前記金属酸化膜の1層の厚さが飽和する時間で決定し、
前記工程(c)において、前記吸着層の前記酸化剤への暴露時間は、前記金属酸化膜における酸素の含有量が化学量論により決定される組成の97%以上となる時間で決定することを特徴とするゲート絶縁膜の形成方法。 - 前記金属酸化膜は、酸化ハフニウム又は酸化ジルコニウムからなることを特徴とする請求項3に記載のゲート絶縁膜の形成方法。
- 前記前駆体は、四塩化ハフニウム(HfCl4)、テトラキスエチルメチルアミノハフニウム(TEMAH)又はテトラキスジメチルアミノハフニウム(TDMAH)であることを特徴とする請求項3に記載のゲート絶縁膜の形成方法。
- 半導体基板の上に、高誘電体金属シリケートからなるゲート絶縁膜を形成するゲート絶縁膜の形成方法であって、
前記半導体基板を500℃以下の温度で且つ所定の圧力下に保持した状態で、前記高誘電体金属シリケートを構成する、金属元素を含む第1の前駆体とシリコンを含む第2の前駆体とに、前記高誘電体金属シリケートの組成比に合わせた混合比で前記半導体基板を暴露することにより、前記半導体基板の上に前記第1の前駆体及び第2の前駆体からなり、前記組成比と対応した組成比を持つ吸着層を形成する工程(a)と、
前記第1の前駆体及び第2の前駆体をパージする工程(b)と、
前記吸着層を酸化剤に暴露して、前記吸着層を酸化することにより、前記吸着層から金属シリケート膜を形成する工程(c)と、
前記酸化剤をパージする工程(d)とを備え、
前記工程(a)、工程(b)及び工程(c)とを1サイクルとして少なくとも1回実行して、前記金属シリケート膜における原子層レベルの少なくとも1層分を形成することにより、前記高誘電体金属シリケートを形成し、
前記工程(a)において、前記半導体基板の前記第1の前駆体及び第2の前駆体への暴露時間は、前記高誘電体金属シリケートを構成する金属の酸化膜とシリコンの酸化膜とを独立に堆積した場合の、前記1サイクルで堆積される1層分の厚さが飽和する時間のうちのいずれか長い方の時間とし、
前記工程(c)において、前記吸着層の前記酸化剤への暴露時間は、前記高誘電体金属シリケートを構成する金属の酸化膜とシリコンの酸化膜とを独立に堆積した場合の、前記金属の酸化膜における酸素の含有量及びシリコンの酸化膜における酸素の含有量がそれぞれ化学量論により決定される組成の97%以上となる時間のうちのいずれか長い方の時間とすることを特徴とするゲート絶縁膜の形成方法。 - 前記高誘電体金属シリケートは、ハフニウムシリケート(HfSiO)又はハフニウムランタンシリケート(HfLaSiO)であることを特徴とする請求項1又は6に記載のゲート絶縁膜の形成方法。
- 前記酸化剤は、オゾン(O3)、水蒸気(H2O)、重水(D2O)又は一酸化二窒素(N2O)又は酸素ラジカルであることを特徴とする請求項1〜7のいずれか1項に記載のゲート絶縁膜の形成方法。
- 前記第1の前駆体は、四塩化ハフニウム(HfCl4)、テトラキスエチルメチルアミノハフニウム(TEMAH)又はテトラキスジメチルアミノハフニウム(TDMAH)であり、
前記第2の前駆体は、四塩化シリコン(SiCl4)、トリジメチルアミノシリコン(TDMAS)又はテトラエチルオルソシリケート(TEOS)であることを特徴とする請求項1又は6に記載のゲート絶縁膜の形成方法。 - 前記第1の前駆体及び第2の前駆体は、酸素を含むことを特徴とする請求項6に記載のゲート絶縁膜の形成方法。
- 前記酸化剤に暴露する工程において、
前記半導体基板に対する加熱温度は、原子層堆積(ALD)反応又は該原子層堆積(ALD)反応から化学気相堆積(CVD)反応に遷移するまでの温度であり、
前記所定の圧力は、前記半導体基板における面内均一性が悪化する直前までの圧力であることを特徴とする請求項1、3及び6のいずれか1項に記載のゲート絶縁膜の形成方法。 - 前記酸化剤に暴露する工程において、
前記半導体基板に対する加熱温度は、300℃以上で且つ化学気相堆積(CVD)反応が主体とならない温度であり、
前記所定の圧力は、1.33×102Pa以上且つ3.99×102Pa以下であることを特徴とする請求項1、3及び6のいずれか1項に記載のゲート絶縁膜の形成方法。
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Cited By (7)
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JP2011155243A (ja) * | 2009-10-23 | 2011-08-11 | Air Products & Chemicals Inc | 第四族金属含有フィルムの堆積方法 |
WO2012014447A1 (ja) * | 2010-07-27 | 2012-02-02 | パナソニック株式会社 | 不揮発性記憶装置の製造方法 |
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JP2015217566A (ja) * | 2014-05-15 | 2015-12-07 | 東京応化工業株式会社 | 積層体の製造方法および積層体 |
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JP2011155243A (ja) * | 2009-10-23 | 2011-08-11 | Air Products & Chemicals Inc | 第四族金属含有フィルムの堆積方法 |
JP2012256926A (ja) * | 2009-10-23 | 2012-12-27 | Air Products & Chemicals Inc | 第四族金属含有フィルムの堆積方法 |
US8952188B2 (en) | 2009-10-23 | 2015-02-10 | Air Products And Chemicals, Inc. | Group 4 metal precursors for metal-containing films |
KR101584100B1 (ko) | 2009-10-29 | 2016-01-13 | 삼성전자주식회사 | 금속 실리케이트 막의 형성 방법 및 이를 이용한 반도체 소자의 형성 방법 |
WO2012014447A1 (ja) * | 2010-07-27 | 2012-02-02 | パナソニック株式会社 | 不揮発性記憶装置の製造方法 |
JP5436674B2 (ja) * | 2010-07-27 | 2014-03-05 | パナソニック株式会社 | 不揮発性記憶装置の製造方法 |
US9355846B2 (en) | 2012-03-16 | 2016-05-31 | Kabushiki Kaisha Toshiba | Non-uniform silicon dioxide and air gap for separating memory cells |
JP2015217566A (ja) * | 2014-05-15 | 2015-12-07 | 東京応化工業株式会社 | 積層体の製造方法および積層体 |
US10707073B2 (en) | 2017-09-05 | 2020-07-07 | Asm Ip Holding B.V. | Film forming method and patterning method |
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