JP6086071B2 - 熱電変換素子およびその製造方法 - Google Patents
熱電変換素子およびその製造方法 Download PDFInfo
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- 238000006243 chemical reaction Methods 0.000 title claims description 30
- 238000004519 manufacturing process Methods 0.000 title claims description 5
- 239000010409 thin film Substances 0.000 claims description 140
- 239000000758 substrate Substances 0.000 claims description 44
- 238000010438 heat treatment Methods 0.000 claims description 42
- 238000001816 cooling Methods 0.000 claims description 23
- 239000013078 crystal Substances 0.000 claims description 21
- 229910052758 niobium Inorganic materials 0.000 claims description 17
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 10
- 229910052760 oxygen Inorganic materials 0.000 claims description 10
- 239000001301 oxygen Substances 0.000 claims description 10
- 150000001875 compounds Chemical class 0.000 claims description 8
- 239000011159 matrix material Substances 0.000 claims description 6
- VEALVRVVWBQVSL-UHFFFAOYSA-N strontium titanate Chemical group [Sr+2].[O-][Ti]([O-])=O VEALVRVVWBQVSL-UHFFFAOYSA-N 0.000 claims description 4
- 206010021143 Hypoxia Diseases 0.000 claims description 3
- 229910002367 SrTiO Inorganic materials 0.000 claims description 3
- 239000010955 niobium Substances 0.000 claims 3
- 239000012535 impurity Substances 0.000 claims 2
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims 1
- 239000010408 film Substances 0.000 description 35
- 238000004544 sputter deposition Methods 0.000 description 15
- 229910052746 lanthanum Inorganic materials 0.000 description 14
- 229910052751 metal Inorganic materials 0.000 description 7
- 239000002184 metal Substances 0.000 description 7
- 230000010355 oscillation Effects 0.000 description 7
- 230000005540 biological transmission Effects 0.000 description 5
- 238000005259 measurement Methods 0.000 description 5
- 238000000034 method Methods 0.000 description 5
- 238000001000 micrograph Methods 0.000 description 5
- 229910052712 strontium Inorganic materials 0.000 description 5
- 238000009826 distribution Methods 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 239000000969 carrier Substances 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 239000002019 doping agent Substances 0.000 description 3
- 238000009616 inductively coupled plasma Methods 0.000 description 3
- 239000002918 waste heat Substances 0.000 description 3
- 230000005678 Seebeck effect Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 238000004611 spectroscopical analysis Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 230000005355 Hall effect Effects 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 238000003917 TEM image Methods 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 230000010365 information processing Effects 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- -1 lanthanum aluminate Chemical class 0.000 description 1
- 238000001755 magnetron sputter deposition Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000005240 physical vapour deposition Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 238000001552 radio frequency sputter deposition Methods 0.000 description 1
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
- 229910052714 tellurium Inorganic materials 0.000 description 1
- PORWMNRCUJJQNO-UHFFFAOYSA-N tellurium atom Chemical compound [Te] PORWMNRCUJJQNO-UHFFFAOYSA-N 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
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- H10N10/80—Constructional details
- H10N10/85—Thermoelectric active materials
- H10N10/851—Thermoelectric active materials comprising inorganic compositions
- H10N10/854—Thermoelectric active materials comprising inorganic compositions comprising only metals
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/46—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates
- C04B35/462—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates
- C04B35/465—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates based on alkaline earth metal titanates
- C04B35/47—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates based on alkaline earth metal titanates based on strontium titanates
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- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
- C23C14/08—Oxides
- C23C14/088—Oxides of the type ABO3 with A representing alkali, alkaline earth metal or Pb and B representing a refractory or rare earth metal
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- H10N10/10—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects
- H10N10/17—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects characterised by the structure or configuration of the cell or thermocouple forming the device
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
- H10N10/80—Constructional details
- H10N10/85—Thermoelectric active materials
- H10N10/851—Thermoelectric active materials comprising inorganic compositions
- H10N10/855—Thermoelectric active materials comprising inorganic compositions comprising compounds containing boron, carbon, oxygen or nitrogen
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
- C04B2235/3227—Lanthanum oxide or oxide-forming salts thereof
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- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
- C04B2235/74—Physical characteristics
- C04B2235/78—Grain sizes and shapes, product microstructures, e.g. acicular grains, equiaxed grains, platelet-structures
- C04B2235/787—Oriented grains
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Materials Engineering (AREA)
- Ceramic Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Inorganic Chemistry (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Structural Engineering (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
- Physical Vapour Deposition (AREA)
- Physical Deposition Of Substances That Are Components Of Semiconductor Devices (AREA)
- Compositions Of Oxide Ceramics (AREA)
Description
11 真空容器
11A 排気ポート
11B プラズマガス導入ポート
12 ターゲット
12A ターゲット保持台
12B 高周波電源
12D ドーパント金属片
13 被処理基板
13A 基板保持台
22,22A.22B 第1電極
23F La,NbドープSTO薄膜
23F1,23F2,23F3,23F4 La,NbドープSTO薄膜パタ―ン
24 第2電極
41,42 加熱/冷却部
41A〜41D,42A〜42D 突起
図1は、第1の実施形態においてSTO薄膜を形成するのに使われるスパッタ装置10の構成を示す図である。なお本実施形態におけるSTO薄膜の形成は、図1のスパッタ装置10を使ったスパッタ法に限定されるものではなく、他のPVD法、例えばパルスレーザ堆積法などにより形成することも可能である。
図4には、前記STO薄膜23FにおいてLaのドープを行わず、Nbのドープのみを行った比較対照例を示すが、この場合には、STO薄膜の電気伝導度σが半分以下に低減しているのがわかる。これはB席のみにドープを行った結果、ABO3で表されるペロブスカイト型化合物の化学量論組成に対しA席とB席の間で原子数の均衡が崩れて欠陥が発生し、かかる欠陥によりキャリアが相殺されていることを示唆している。
図12Aおよび図12Bは、それぞれ第2の実施形態による熱電変換装置40の構成を示す断面図および平面図を示す。ただし図12Bは図12Aの平面図中、線A−A'に沿った断面を示している。
Claims (3)
- STO基板と、
前記STO基板上に形成され、ペロブスカイト構造の化合物よりなる薄膜と、
前記STO基板上に設けられ、前記薄膜の上面に第1の領域においてコンタクトする第1の電極と、
前記薄膜の上面に前記第1の領域から離間した第2の領域においてコンタクトする第2の電極と、
前記薄膜を、前記第1の領域において加熱または冷却する第1の加熱または冷却部と、
前記薄膜を、前記第2の領域において加熱または冷却する第2の加熱または冷却部と、
を含み、
前記第2の加熱または冷却部は、前記第1の加熱または冷却部が前記薄膜の前記第1の領域を加熱する場合に前記薄膜の前記第2の領域を冷却し、
前記第2の加熱または冷却部は、前記第1の加熱または冷却部が前記薄膜の前記第1の領域を冷却する場合に前記薄膜の前記第2の領域を加熱し、
前記薄膜中には、前記ペロブスカイト構造の化合物を構成する結晶中に、前記結晶とは異なる結晶方位の領域が複数形成されており、
前記薄膜は(001)面方位のSrTiO3の薄膜であり、前記複数の領域は、(031)面方位を有するドメインであって、
前記薄膜は、Nbを25原子%の割合で含むことを特徴とする熱電変換素子。 - 前記薄膜は酸素欠損を含み、1020cm−3〜1022cm−3の範囲のキャリア濃度を有していることを特徴とする請求項1記載の熱電変換素子。
- STO基板上に形成され、ペロブスカイト構造の化合物よりなる薄膜を形成する工程と、
前記薄膜の上面に、第1の領域において第1の電極を形成する工程と、
前記薄膜の上面に、前記第1の領域から離間した第2の領域において第2の電極を形成する工程と、
前記第1の領域に加熱または冷却部を形成する工程と、
前記第2の領域に冷却または加熱部を形成する工程と、
を含み、
前記薄膜を形成する工程は、前記薄膜を構成する前記ペロブスカイト構造の化合物の結晶中に、前記結晶のマトリクスとは結晶方位の異なる領域が複数形成されるような濃度で、不純物元素をドープする工程を含み、
前記薄膜は(001)面方位のSrTiO3の薄膜であり、前記複数の領域は、(031)面方位を有するドメインであって、
前記ペロブスカイト構造の化合物は酸素欠損を含むチタン酸ストロンチウムであり、前記不純物元素はNb(ニオブ)であり、25原子%の濃度でドープされることを特徴とする熱電変換素子の製造方法。
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WO2016129082A1 (ja) * | 2015-02-12 | 2016-08-18 | 株式会社日立製作所 | 薄膜熱電変換モジュールおよびその製造方法 |
JP7473112B2 (ja) | 2020-11-17 | 2024-04-23 | 国立大学法人東北大学 | 圧電体薄膜、圧電体薄膜の製造装置、圧電体薄膜の製造方法、および、疲労推定システム |
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JP3999300B2 (ja) * | 1997-02-07 | 2007-10-31 | Tdk株式会社 | 強誘電体薄膜およびその製造方法 |
WO2008109564A1 (en) * | 2007-03-02 | 2008-09-12 | The Regents Of The University Of California | Complex oxides useful for thermoelectric energy conversion |
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JPWO2011065185A1 (ja) * | 2009-11-27 | 2013-04-11 | 富士通株式会社 | 熱電変換モジュール及びその製造方法 |
JP2011243824A (ja) * | 2010-05-20 | 2011-12-01 | Panasonic Corp | 異方的熱電材料とこれを用いた放射検出器および発電デバイス |
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US9508912B2 (en) | 2016-11-29 |
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US20140338717A1 (en) | 2014-11-20 |
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