JP2018049970A - 光電変換素子 - Google Patents
光電変換素子 Download PDFInfo
- Publication number
- JP2018049970A JP2018049970A JP2016185215A JP2016185215A JP2018049970A JP 2018049970 A JP2018049970 A JP 2018049970A JP 2016185215 A JP2016185215 A JP 2016185215A JP 2016185215 A JP2016185215 A JP 2016185215A JP 2018049970 A JP2018049970 A JP 2018049970A
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- Prior art keywords
- photoelectric conversion
- electrode
- layer
- conversion element
- polishing
- Prior art date
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- JFBZPFYRPYOZCQ-UHFFFAOYSA-N [Li].[Al] Chemical compound [Li].[Al] JFBZPFYRPYOZCQ-UHFFFAOYSA-N 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 239000003570 air Substances 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 150000001299 aldehydes Chemical class 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 150000001340 alkali metals Chemical class 0.000 description 1
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- 125000003342 alkenyl group Chemical group 0.000 description 1
- 150000001347 alkyl bromides Chemical class 0.000 description 1
- 125000000217 alkyl group Chemical group 0.000 description 1
- 150000001351 alkyl iodides Chemical class 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- SNAAJJQQZSMGQD-UHFFFAOYSA-N aluminum magnesium Chemical compound [Mg].[Al] SNAAJJQQZSMGQD-UHFFFAOYSA-N 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 125000006615 aromatic heterocyclic group Chemical group 0.000 description 1
- 125000002029 aromatic hydrocarbon group Chemical group 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 125000005605 benzo group Chemical group 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 229910021418 black silicon Inorganic materials 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- GMYSDEOJMBLAKZ-UHFFFAOYSA-N calcium indium Chemical compound [Ca].[In] GMYSDEOJMBLAKZ-UHFFFAOYSA-N 0.000 description 1
- 125000004432 carbon atom Chemical group C* 0.000 description 1
- UBAZGMLMVVQSCD-UHFFFAOYSA-N carbon dioxide;molecular oxygen Chemical compound O=O.O=C=O UBAZGMLMVVQSCD-UHFFFAOYSA-N 0.000 description 1
- 125000002915 carbonyl group Chemical group [*:2]C([*:1])=O 0.000 description 1
- 150000001735 carboxylic acids Chemical class 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 125000001309 chloro group Chemical group Cl* 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- BQVVSSAWECGTRN-UHFFFAOYSA-L copper;dithiocyanate Chemical compound [Cu+2].[S-]C#N.[S-]C#N BQVVSSAWECGTRN-UHFFFAOYSA-L 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 125000004093 cyano group Chemical group *C#N 0.000 description 1
- 230000009849 deactivation Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000032798 delamination Effects 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 229910052805 deuterium Inorganic materials 0.000 description 1
- 150000008049 diazo compounds Chemical class 0.000 description 1
- UIJLKECZHOSSHF-UHFFFAOYSA-N diphenyl-bis(4-pyridin-3-ylphenyl)silane Chemical compound C1=CC=CC=C1[Si](C=1C=CC(=CC=1)C=1C=NC=CC=1)(C=1C=CC(=CC=1)C=1C=NC=CC=1)C1=CC=CC=C1 UIJLKECZHOSSHF-UHFFFAOYSA-N 0.000 description 1
- 229910001651 emery Inorganic materials 0.000 description 1
- 125000005678 ethenylene group Chemical group [H]C([*:1])=C([H])[*:2] 0.000 description 1
- 125000001301 ethoxy group Chemical group [H]C([H])([H])C([H])([H])O* 0.000 description 1
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- RMBPEFMHABBEKP-UHFFFAOYSA-N fluorene Chemical compound C1=CC=C2C3=C[CH]C=CC3=CC2=C1 RMBPEFMHABBEKP-UHFFFAOYSA-N 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 125000001153 fluoro group Chemical group F* 0.000 description 1
- 125000005843 halogen group Chemical group 0.000 description 1
- 229910052734 helium Inorganic materials 0.000 description 1
- 239000001307 helium Substances 0.000 description 1
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 1
- ZMZDMBWJUHKJPS-UHFFFAOYSA-N hydrogen thiocyanate Natural products SC#N ZMZDMBWJUHKJPS-UHFFFAOYSA-N 0.000 description 1
- 230000003301 hydrolyzing effect Effects 0.000 description 1
- ZZLONYJSCSHJMR-UHFFFAOYSA-N hydron 2,2,2-trifluoroethanamine iodide Chemical compound [I-].FC(C[NH3+])(F)F ZZLONYJSCSHJMR-UHFFFAOYSA-N 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 150000003949 imides Chemical class 0.000 description 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- LHJOPRPDWDXEIY-UHFFFAOYSA-N indium lithium Chemical compound [Li].[In] LHJOPRPDWDXEIY-UHFFFAOYSA-N 0.000 description 1
- 229910003437 indium oxide Inorganic materials 0.000 description 1
- YZASAXHKAQYPEH-UHFFFAOYSA-N indium silver Chemical compound [Ag].[In] YZASAXHKAQYPEH-UHFFFAOYSA-N 0.000 description 1
- PJXISJQVUVHSOJ-UHFFFAOYSA-N indium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[In+3].[In+3] PJXISJQVUVHSOJ-UHFFFAOYSA-N 0.000 description 1
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 description 1
- 229910052809 inorganic oxide Inorganic materials 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 229910052744 lithium Inorganic materials 0.000 description 1
- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 1
- GCICAPWZNUIIDV-UHFFFAOYSA-N lithium magnesium Chemical compound [Li].[Mg] GCICAPWZNUIIDV-UHFFFAOYSA-N 0.000 description 1
- SJCKRGFTWFGHGZ-UHFFFAOYSA-N magnesium silver Chemical compound [Mg].[Ag] SJCKRGFTWFGHGZ-UHFFFAOYSA-N 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- 125000000956 methoxy group Chemical group [H]C([H])([H])O* 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- 239000012046 mixed solvent Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- DCZNSJVFOQPSRV-UHFFFAOYSA-N n,n-diphenyl-4-[4-(n-phenylanilino)phenyl]aniline Chemical class C1=CC=CC=C1N(C=1C=CC(=CC=1)C=1C=CC(=CC=1)N(C=1C=CC=CC=1)C=1C=CC=CC=1)C1=CC=CC=C1 DCZNSJVFOQPSRV-UHFFFAOYSA-N 0.000 description 1
- 125000001624 naphthyl group Chemical group 0.000 description 1
- 229910052754 neon Inorganic materials 0.000 description 1
- GKAOGPIIYCISHV-UHFFFAOYSA-N neon atom Chemical compound [Ne] GKAOGPIIYCISHV-UHFFFAOYSA-N 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- 239000010955 niobium Substances 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 229910000484 niobium oxide Inorganic materials 0.000 description 1
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 description 1
- 230000006911 nucleation Effects 0.000 description 1
- 238000010899 nucleation Methods 0.000 description 1
- NIHNNTQXNPWCJQ-UHFFFAOYSA-N o-biphenylenemethane Natural products C1=CC=C2CC3=CC=CC=C3C2=C1 NIHNNTQXNPWCJQ-UHFFFAOYSA-N 0.000 description 1
- 125000001741 organic sulfur group Chemical group 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 238000005192 partition Methods 0.000 description 1
- 230000000149 penetrating effect Effects 0.000 description 1
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 1
- 150000003009 phosphonic acids Chemical class 0.000 description 1
- 150000003014 phosphoric acid esters Chemical class 0.000 description 1
- IEQIEDJGQAUEQZ-UHFFFAOYSA-N phthalocyanine Chemical class N1C(N=C2C3=CC=CC=C3C(N=C3C4=CC=CC=C4C(=N4)N3)=N2)=C(C=CC=C2)C2=C1N=C1C2=CC=CC=C2C4=N1 IEQIEDJGQAUEQZ-UHFFFAOYSA-N 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 229920003023 plastic Polymers 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
- 229920003227 poly(N-vinyl carbazole) Polymers 0.000 description 1
- 229920000553 poly(phenylenevinylene) Polymers 0.000 description 1
- 229920000548 poly(silane) polymer Polymers 0.000 description 1
- 229920002647 polyamide Polymers 0.000 description 1
- 229920002312 polyamide-imide Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 239000011112 polyethylene naphthalate Substances 0.000 description 1
- 229920001721 polyimide Polymers 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 229920006254 polymer film Polymers 0.000 description 1
- 239000002861 polymer material Substances 0.000 description 1
- 229920001296 polysiloxane Polymers 0.000 description 1
- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 150000004032 porphyrins Chemical class 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000007639 printing Methods 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 150000003219 pyrazolines Chemical class 0.000 description 1
- 125000004076 pyridyl group Chemical group 0.000 description 1
- 229910052701 rubidium Inorganic materials 0.000 description 1
- 229910052711 selenium Inorganic materials 0.000 description 1
- 239000011669 selenium Substances 0.000 description 1
- 229910000077 silane Inorganic materials 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011780 sodium chloride Substances 0.000 description 1
- 238000003980 solgel method Methods 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- PJANXHGTPQOBST-UHFFFAOYSA-N stilbene Chemical class C=1C=CC=CC=1C=CC1=CC=CC=C1 PJANXHGTPQOBST-UHFFFAOYSA-N 0.000 description 1
- 230000007847 structural defect Effects 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
- VJYJJHQEVLEOFL-UHFFFAOYSA-N thieno[3,2-b]thiophene Chemical class S1C=CC2=C1C=CS2 VJYJJHQEVLEOFL-UHFFFAOYSA-N 0.000 description 1
- 150000003577 thiophenes Chemical class 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 238000002834 transmittance Methods 0.000 description 1
- 238000000870 ultraviolet spectroscopy Methods 0.000 description 1
- 229930195735 unsaturated hydrocarbon Natural products 0.000 description 1
- 238000007738 vacuum evaporation Methods 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 1
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 1
- 229910052724 xenon Inorganic materials 0.000 description 1
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
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Abstract
Description
ガラス基板の上に第1の電極としてITO膜を形成した。このITO膜の上に、PEDOTを含む下地層を形成した。下地層は正孔輸送層としても機能する。PEDOT:PSSはHIL1.1を5000rpmでスピンコートした後、140℃で10分間乾燥した。次に、ヨウ化メチルアンモニウムとヨウ化鉛から成るペロブスカイトの前駆体を含む塗布層を形成した。ペロブスカイト型化合物の前駆体を含む塗布液はヨウ化メチルアンモニウムとヨウ化鉛をDMFに溶解させて調製した。このとき、ヨウ化メチルアンモニウムは200mg/ml、ヨウ化鉛は578mg/mlになるように調整した。この溶液を下地層の上に500rpmでスピンコートした。
実施例1と同様の工程で研磨および熱処理まで実施した変換効率9.1%のサンプルと、研磨を行わなかった変換効率7.1%のサンプルに対しIV測定とXRD測定を行った。
なお、XRD測定のサンプルは光電変換素子とは別に作製した。BCPとAgの成膜は行わずに実施例1と同じ製造工程を実施した。得られた光電変換素子のIV特性を図21に示し、X線回折パターンを図22に示し、図22の一部の拡大図を図23および図24に示す。図23および図24から研磨を行うことによってペロブスカイト型化合物の(004)の回折ピークを有することがわかる。この回折ピークは、単結晶のXRDでは検出されるが、素子では検出されにくい。研磨を行うと、ペロブスカイト型化合物の結晶構造が一度歪むが、熱処理等で再配列させることによって、成膜過程の影響を排除した理想的な結晶構造が形成されるためだと考えられる。このとき、(220)の回折ピークの最大強度に対する(004)の回折ピークの最大強度の比は0.18であった。この強度が高いほど、より一層良質の結晶が得られているといえる。
研磨の方向を変えて熱処理の効果を比較した。研磨の条件以外は実施例1と同様に作業を行い、研磨ローラの回転軸が塗布層の表面に対して垂直である条件と、平行である条件とを比較した。それぞれのIV特性を図25および図26に示す。図25は、熱処理前のサンプルのIV特性を示す図であり、図26は熱処理後のサンプルのIV特性を示す図である。図25からわかるように熱処理前は垂直条件の方が高い変換効率だが、熱処理後は平行条件の方が高い変換効率を有する。図26では、平行条件の変換効率が熱処理前の垂直条件の変換効率を上回った。垂直条件では、剥離したペロブスカイト型化合物が正常なペロブスカイト型化合物に傷を付けてしまったり、塗布層に加わる負荷の方向が一定方向ではないため、熱処理によるイオンの再配列効果が得られにくかったためだと考えられる。平行条件であれば、ガスブロー等のクリーニング装置と組み合わせれば、剥離したペロブスカイト型化合物を研磨面から排除することも可能であり、さらに、塗布層に加わる面方向の負荷も一定方向に揃えられ、再配列効果が得られ易かったと考えられる。
塗布液中の前駆体濃度を変えて熱処理の効果を比較した。前駆体の濃度以外は実施例1と同様の工程を行った。それぞれIV特性を図27ないし図29に示す。図27ないし図29からわかるように、前駆体の濃度が1640mg/ml、1770mg/mlまで増やしても熱処理による効果が表れている。しかし、前駆体の濃度が2020mg/mlでは熱処理を行っても変換効率は向上せず、IVカーブも明確ではなくなった。前駆体の濃度が高くなると、ペロブスカイト型化合物の結晶粒径も大きくなるため、研磨したときに中間層まで貫通するピンホールが発生しやすくなるためだと考えられる。
研磨を行わない以外は、実施例1と同様の作業で素子を作製し、70℃での熱処理の前後のIV特性の比較を行った。図30に示すIV特性からわかるように、熱処理前後でIV特性を構成する各パラメータが変化するが、変換効率はほとんど変化しないことがわかる。
Claims (14)
- 第1の電極と、
第2の電極と、
前記第1の電極および前記第2の電極に接し、ペロブスカイト型化合物を含む活性層を備える光電変換層と、
を具備し、
X線回折測定により得られる前記活性層のX線回折パターンは、前記ペロブスカイト型化合物の(004)面に起因する第1の回折ピークと、前記ペロブスカイト型化合物の(220)面に起因する第2の回折ピークと、を有し、
前記第2の回折ピークの最大強度に対する前記第1の回折ピークの最大強度の比は、0.18以上である、光電変換素子。 - 前記ペロブスカイト型化合物は、一般式:ABX3で表され、
前記Aは、1級アンモニウムイオンであり、
前記Bは、2価の金属イオンであり、
前記Xは、ハロゲンイオンである、請求項1に記載の光電変換素子。 - 前記光電変換層は、
前記第1の電極と前記活性層との間に設けられた中間層をさらに有し、
前記中間層は、有機材料を含む、請求項1または請求項2に記載の光電変換素子。 - 前記中間層は、ポリエチレンジオキシチオフェンを含む、請求項3に記載の光電変換素子。
- 前記中間層は、ポリエチレンジオキシチオフェンとポリスチレンスルホン酸とを含む、請求項3または請求項4に記載の光電変換素子。
- 前記光電変換層は、
前記第2の電極と前記活性層との間に設けられた第2の中間層をさらに有する、請求項1ないし請求項5のいずれか一項に記載の光電変換素子。 - 第1の電極と、
第2の電極と、
前記第1の電極および前記第2の電極に接し、ペロブスカイト型化合物を含む活性層を備える光電変換層と、
を具備する光電変換素子の製造方法であって、
前記ペロブスカイト型化合物を含む被処理体の表面を研磨する工程と、
前記研磨する工程の後に前記被処理体に対して熱処理を行う工程と、を具備する、光電変換素子の製造方法。 - 前記研磨する工程の前に前記ペロブスカイト型化合物の前駆体を含む塗布液を前記被処理体の表面に塗布して塗布層を形成する工程と、
前記塗布層を形成する工程と前記研磨する工程との間に前記塗布層にガスを吹き付けて前記ペロブスカイト型化合物を形成する工程と、をさらに具備する、請求項7に記載の光電変換素子の製造方法。 - 前記塗布液中の前記前駆体の濃度は、1770mg/ml以下である、請求項8に記載の光電変換素子の製造方法。
- 前記塗布層を形成する工程の前に前記被処理体上に中間層を形成する工程をさらに具備する、請求項8または請求項9に記載の光電変換素子の製造方法。
- 前記ペロブスカイト型化合物を形成する工程と前記研磨する工程との間に前記塗布層上に第2の中間層を形成する工程をさらに具備する、請求項8ないし請求項10のいずれか一項に記載の光電変換素子の製造方法。
- 第1の電極と、
第2の電極と、
前記第1の電極および前記第2の電極に接し、ペロブスカイト型化合物を含む活性層を備える光電変換層と、
を具備する光電変換素子の製造装置であって、
前記ペロブスカイト型化合物を含む被処理体を支持するための支持面を有する支持体と、
回転軸と、前記回転軸を中心に回転して前記被処理体の表面を研磨するための研磨面と、を備える研磨ローラと、
前記被処理体の表面が前記回転軸と平行に前記研磨面に接するように、前記研磨ローラおよび前記被処理体の少なくとも一つを移動させるための移動機構と、を具備する、光電変換素子の製造装置。 - 前記被処理体の表面に前記ペロブスカイト型化合物の前駆体を含む塗布液を塗布して塗布層を形成するための塗布機構と、
前記塗布層にガスを吹き付けて前記ペロブスカイト型化合物を形成するためのガス供給機構と、をさらに具備する、請求項12に記載の光電変換素子の製造装置。 - 前記移動機構は、前記回転軸と平行な第2の回転軸と前記被処理体を支持するための第2の支持面とを有する第2の支持体を有し、前記研磨ローラよりも遅い回転速度で前記第2の支持体を回転させて前記被処理体を移動させる、請求項12または請求項13に記載の光電変換素子の製造装置。
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