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WO1999031741A1 - Contacts en composes metalliques pour des composants organiques et leur procede de fabrication - Google Patents

Contacts en composes metalliques pour des composants organiques et leur procede de fabrication Download PDF

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Publication number
WO1999031741A1
WO1999031741A1 PCT/IB1997/001565 IB9701565W WO9931741A1 WO 1999031741 A1 WO1999031741 A1 WO 1999031741A1 IB 9701565 W IB9701565 W IB 9701565W WO 9931741 A1 WO9931741 A1 WO 9931741A1
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WO
WIPO (PCT)
Prior art keywords
cathode
electroluminescent device
organic electroluminescent
organic
metallic compound
Prior art date
Application number
PCT/IB1997/001565
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English (en)
Inventor
Edward W. Kiewra
Peter Roentgen
Paul F. Seidler
Original Assignee
International Business Machines Corporation
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by International Business Machines Corporation filed Critical International Business Machines Corporation
Priority to PCT/IB1997/001565 priority Critical patent/WO1999031741A1/fr
Publication of WO1999031741A1 publication Critical patent/WO1999031741A1/fr

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Classifications

    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K59/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic light-emitting element covered by group H10K50/00
    • H10K59/80—Constructional details
    • H10K59/805—Electrodes
    • H10K59/8052—Cathodes
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K2102/00—Constructional details relating to the organic devices covered by this subclass
    • H10K2102/301—Details of OLEDs
    • H10K2102/302—Details of OLEDs of OLED structures
    • H10K2102/3023—Direction of light emission
    • H10K2102/3026—Top emission

Definitions

  • the present invention concerns a new class of contact materials used as electrodes for organic devices, such as organic light emitting diodes (OLEDs), organic displays and the like.
  • organic devices such as organic light emitting diodes (OLEDs), organic displays and the like.
  • OLEDs are an emerging technology with potential applications as discrete light emitting devices, or as the active element of light emitting arrays or displays, such as flat-panel displays.
  • OLEDs are devices in which a stack of organic layers is sandwiched between two electrodes. At least one of these electrodes must be transparent in order for light - which is generated in the active region of the organic stack - to escape.
  • OLEDs emit light which is generated by organic electroluminescence (EL).
  • EL organic electroluminescence
  • Organic EL at low efficiency was observed many years ago in metal/organic/metal structures as, for example, reported in Pope et al., Journal Chem. Phys., Vol. 38, 1963, pp. 2024, and in "Recombination Radiation in Anthracene Crystals", Helfrich et al., Physical Review Letters, Vol. 14, No. 7, 1965, pp. 229-231.
  • Recent developments have been spurred largely by two reports of high efficiency organic EL. These are C.W. Tang et al., "Organic electroluminescent diodes", Applied Physics Letters, Vol. 51, No. 12, 1987, pp.
  • OLED structures suitable for opaque substrates are highly desirable.
  • substrates other than the conventional glass substrates are highly desirable.
  • OLEDs could be fabricated on silicon, this would permit the use of an integrated active-matrix drive scheme. In such a structure light must be emitted through the uppermost layers of the device rather than through the substrate.
  • One possible solution would be to build OLEDs by depositing the layers in the opposite order, which means a structure would be obtained with the transparent ITO anode deposited on top. This has proved difficult because of the harsh conditions under which the ITO is deposited, as reported by Zilan Shen et al. in "Three-Color, Tunable, Organic Light-Emitting Devices", Science, Vol. 276, 27 June 1997, pp. 2009-2011.
  • GaN Gallium Nitride
  • nd-WBS wide-bandgap semiconductor
  • the wide bandgap also leads to a favorable alignment of either the conduction band or valance band, or both, with the lowest unoccupied molecular orbitals (LUMO) or highest occupied molecular orbital (HOMO), respectively, of the organic material into which charge is to be injected.
  • LUMO lowest unoccupied molecular orbitals
  • HOMO highest occupied molecular orbital
  • Electrode materials With multilayer device architectures now well understood and commonly used, a major performance limitation of OLEDs is the lack of ideal contact electrodes.
  • the main figure of merit for electrode materials is the position of their bands relative to those of the organic materials.
  • the electrode should be chemically inert and capable of forming a dense uniform film to ensure uniform injection and to effectively encapsulate the OLED.
  • TiN for example, is used in semiconductor technology on n-type silicon to form low barrier Schottky diodes, as described by M. Wittmer et al., in "Applications of TiN Thin Films in Silicon Device Technology", Thin Solid Films, Vol. 93, p. 397, 1982.
  • TiN is also used in photo voltaic cells as an intermediate layer, as described in US patent 4,485,265, for example.
  • TiN is employed in photo voltaic cells because it is less expensive and more abundant than other transition metals.
  • the TiN is formed using chemical vapor deposition techniques at temperatures above 400°C.
  • Metallic compound or compound metal in the present context means any carbide, nitride, or boride of the early transition metals, lanthanides, and alkaline earths (group IIA), any mixture of these metallic compounds, or mixed carbides, nitrides and borides.
  • the term early transition metal in the present context is meant to cover any elements of groups IIIB, IVB, VB, and VIB of the periodic table of elements.
  • One example of such a metallic compound is titanium nitride (TiN).
  • Metallic compounds are not meant to cover any alloys of elements that are already metals. These metallic compounds make up a whole new class of low-workfunction, semi-transparent, conducting materials very well suited as cathodes for organic devices.
  • the inventive approach capitalizes primarily on the inventor's finding that these metallic compounds are very well suited for efficiently injecting electrons into the organic layers of an OLED.
  • the injection efficiency is correlated with the band lineup of metallic compounds and organics, a property which has been investigated and analyzed for the first time by the inventors. It has been found that the bands of the metallic compounds line up well at the compound-metal/organic interface. Experiments have revealed that the fermi energy of the metallic compounds is high enough to allow efficient injection of electrons.
  • the metallic compounds also serve as a barrier to diffusion
  • the metallic compounds are metals and not nd-WBS semiconductors as the GaN proposed in the co-pending international patent application PCT/IB96/00780.
  • the metallic compounds can be used to make semi-transparent cathode OLEDs, a distinct advantage over the normally used opaque, low-workfunction elemental metals and alloys (class 1 metals) for fabricating OLED devices on silicon, where light must be extracted through the top of the device.
  • semi-transparency can also be achieved with layers of class 1 metals if they would be made thin enough. The problem, however, would be that these layers have to be made so thin that they do not have sufficient conductivity anymore. Such layers may not form a continuous film any longer and they may therefore lose their bulk properties.
  • a single or multilayer OLED structure having a metallic compound cathode directly in contact with the corresponding organic layer, and a conventional opposite contact electrode (anode) is envisioned.
  • an additional layer or stack of layers of transparent conducting metal oxide is deposited on top of the compound metal in order to provide for improved lateral conductivity.
  • metallic compounds due to its inherent simplicity it is less expensive than the class 1 metals or class 2 nd-WBSs.
  • the stability to atmospheric exposure is also an advantage of the metallic compounds.
  • Class 1 metals and alloys in contrast, tend to be highly reactive with respect to water and oxygen.
  • a transparent cathode in accordance with the present invention adds flexibility in the choice of anode designs, e.g. the anode can be opaque.
  • a metallic compound cathode is chemically inert and thermally stable and therefore has no undesirable solid state interactions with the organic layers with which it is in contact or close proximity;
  • a metallic compound is an outstanding encapsulant and mechanical protectant material for OLEDs
  • a metallic compound can be deposited at conditions required for OLED formation (e.g. low temperature, minimum damage to the growth surface) in a conductive state;
  • a metallic compound has high infrared reflectivity, providing for protection of the organic compounds during deposition.
  • Fig. 1 is a schematic cross section of an organic light emitting diode, according to the present invention.
  • Fig. 2 is a schematic cross section of another organic light emitting diode, according to the present invention.
  • Fig. 3 is a schematic cross section of an organic light emitting array or display, according to the present invention.
  • metallic compounds or compound metals is meant to cover carbides, nitrides, and borides of the early transistion metals, lanthanides, and alkaline earths (group II A).
  • early transition metal in the present context is meant to cover any elements of groups IIIB, IVB, VB, and VIB of the periodic table of elements.
  • metallic compounds examples include CaB 6 , LaB 6 , TiC, HfC, TaC, TiN, ZrN, HfN, any mixture of these metallic compounds, or mixed carbides, nitrides and borides such as TiC ⁇ N y , for example.
  • TiN which serves as an example out of the class of the metallic compounds.
  • a first embodiment of the present invention is described in connection with Figure 1.
  • a schematic cross-section of an organic light emitting diode 10 is shown in this Figure.
  • This diode 10 is formed on a substrate 11.
  • This substrate 11 may be a silicon substrate for example. Any other substrate can be chosen.
  • An anode 12 is formed on said substrate 11. ITO is well suited for this purpose.
  • ITO is well suited for this purpose.
  • This organic stack 13 at least comprises an organic layer in which electroluminescence takes place if an appropriate voltage is applied.
  • Such an organic layer is usually referred to as an electroluminescent layer or emissive layer (EML).
  • EML electroluminescent layer
  • a TiN cathode 14 is situated on top of the organic stack 13.
  • the thickness of the TiN cathode layer 14 is chosen to provide as high a transmittance as possible. Well suited is a thickness of 100 nm or less. In the present embodiment the TiN cathode is 50 nm thick. While bulk TiN is opaque and has a gold color, thin films of TiN can be prepared with transmittances well suited for OLED applications. A TiN layer of less than 50nm thickness has a transmittance above 50% in the wavelength range from 400 to 700nms. Exemplary details of the first embodiment are given in the following table (PPV means poly (p-phenylenevinylene)) . Laver No. Material Thickness present example substrate 11 silicon 0.1mm-5mm 1mm anode 12 ITO 10-2000nm 50 nm organic stack 13 PPV 10-lOOOnm 200 nm cathode 14 TiN 5-100 nm 50 nm
  • the first embodiment is a cathode-up structure where light is emitted through the cathode 14 into the half-space above the device 10, as indicated in Figure 1.
  • an additional layer or stack of layers of transparent conducting metal oxide, such as ITO, could be deposited on top of the compound metal cathode.
  • ITO transparent conducting metal oxide
  • the stability, resistance to diffusion, and infrared reflectivity (heat mirror behavior) of the compound metal cathode protects the rest of the OLED structure 10 from the metal oxide deposition process if such an additional layer is deposited.
  • the outstanding characteristics of the compound metal cathode furthermore provide for excellent protection of the OLED structure during the compound metal deposition.
  • the organic stack comprises several layers. Note that the layered structure of the organic stack is not shown in Figure 1.
  • the shown device 20 is an anode-up device. From the substrate 21 up, listed in the order of deposition, is a glass/ITO/TiN/ETL/EML/HTL Metal OLED structure. A low barrier to electron injection is obtained when employing a compound metal cathode 24.1 on an ITO layer 24.2.
  • the conventional ITO anode can be replaced by a high work function metal since the anode 22 no longer serves as the transparent contact.
  • light is emitted from the active region within the organic stack 23 through the metallic compound cathode 24.1 and ITO 24.2 and substrate 21.
  • the organic stack 23 comprises an electron transport layer (ETL), an electroluminescent layer (EML), and a hole transport layer (HTL).
  • ETL electron transport layer
  • EML electroluminescent layer
  • HTL hole transport layer
  • Alq3 means tris(8-hydroxyquinolate)aluminum
  • TPD means
  • HTL TPD 5-500nm 50 nm anode 22 Au 10-2000nm 100 nm
  • the substrate could be fabricated to contain active Si devices, such as for example an active matrix, drivers, memory and so forth.
  • active Si devices such as for example an active matrix, drivers, memory and so forth.
  • An OLED, OLED array or an OLED display may either by grown directly on such a Si substrate carrying Si devices, or it may be fabricated separately and mounted onto the Si substrate later.
  • a problem is the Si metallization. Cathode metals traditionally used in
  • OLEDs i.e. class 1 materials
  • OLEDs are not stable under most Si processing conditions or in air.
  • Another problem is that a transparent top contact is needed because Si is not a transparent substrate.
  • the present invention offers a solution to these problems.
  • the disclosed metallic compound-based cathode permits a stable, low voltage contact to be formed on top of an organic stack situated on a silicon substrate.
  • the inventive metallic compound-based cathodes are compatible with OLED on silicon technology.
  • This display comprises a Si substrate 31 which has integrated circuits comprising active and/or passive devices such as memory cells, drivers, capacitors, transistor etc. (these devices are not shown in Figure 3).
  • stable OLED anodes 32 e.g. ITO, Au, Pt, Ni, Cr
  • These anodes, together with the cathode layer 34 drive the organic stack 33 when a voltage is applied.
  • the organic stack 33 is deposited in the cathode-up geometry on the patterned anodes 32 and Si substrate 31.
  • a metallic compound cathode layer 34 is provided. It is to be noted that no details of the organic stack are shown for sake of simplicity.
  • the cross-section of Figure 3 shows two adjacent OLEDs. These OLEDs may emit any color including blue or white.
  • the substrate 31 may be an Al-metallized Si chip on which the Al contacts are suitably modified to act as an anode.
  • This Al-metallized Si chip serves as substrate for two OLEDs. These two OLEDs may be part of an OLED array or display.
  • One such OLED comprises (from the bottom to the top):
  • an organic stack 33 comprising an HTL, an organic doped or undoped active region (EML), and an ETL, and
  • the cathode layer 34 is shown as a continuos layer in Figure 3. Likewise, this cathode layer 34 may be patterned.
  • the organic stack 33 of the present devices may - in addition to charge transport layers if needed at all - either comprise:
  • EML organic emission layer
  • Such a stack may also comprise inorganic, e.g. LiF, barrier layers.
  • TiN and the other compound metals can be deposited by a variety of techniques, including vacuum evaporation, E-beam evaporation, reactive sputtering, glow discharges, and chemical vapor deposition (CVD). It has been determined that the deposition on an OLED layer structure requires temperatures below 200°C. Even better suited are temperatures below 100°C. The higher temperature CVD processes are thus not well suited if TiN goes on top of the organic. Vacuum evaporation, E-beam evaporation, reactive sputtering, and glow discharges process, however, are well suited for the formation of compound metal cathodes on organic structures. TiN and the other compound metals have been proven to be compatible with organic manufacturing technology, if deposited at low enough temperatures.
  • the compound metal is deposited prior to the organic layers, and harsher conditions may be used.
  • TiN can be deposited by CVD at temperatures above 200° C, for example, directly onto the Si substrate to form cathodes on the metal contacts.
  • the preferred method for deposition of TiN cathodes is radio frequency (rf) reactive magnetron sputtering. Direct current (DC) reactive magnetron sputtering is also possible.
  • rf radio frequency
  • DC direct current
  • a mixture of Ar and N 2 is introduced into the sputter chamber, the ratio of which is chosen to give the desired conductivity and transparency properties in the deposited film.
  • Total chamber pressure, sputtering power, and target-to-substrate distance are additional, system-dependent parameters which must be optimized to give the desired film characteristics and minimize any damage to the substrate or organic films due, for example, to bombardment by ions or neutral species. If necessary, the substrate is cooled to avoid overheating during film deposition, but often this is not required.
  • Electron transport/Emitting materials
  • 8-hydroxyquinoline metal complexes such as Znq 2 , Beq 2 , Mgq 2 , ZnMq 2 , BeMq 2 , BAlq, and AlPrq 3 , for example. These materials can be used as ETL or emission layer.
  • electron transporting materials are electron-deficient nitrogen-containing systems, for example oxadiazoles like PBD (and many derivatives), and triazoles, for example TAZ (1,2,4-triazole).
  • DPS6T didecyl sexithiophene
  • 2D6T bis-triisopropylsilyl sexithiophene
  • Azomethin-zinc complexes pyrazine (e.g. BNVP), strylanthracene derivatives (e.g. BSA-1, BSA-2), non-planar distyrylarylene derivatives, for example DPVBi (see C. Hosokawa and T.
  • cyano-substituted polymers such as cyano PPV (PPV means poly(p-phenylenevinylene)) and cyano PPV derivatives.
  • PPV poly(p-phenylenevinylene)
  • cyano PPV derivatives cyano PPV derivatives.
  • Anthracene pyridine derivatives (e.g. ATP), Azomethin-zinc complexes, pyrazine (e.g. BNVP), strylanthracene derivatives (e.g. BSA-1, BSA-2), Coronene, Coumarin, DCM compounds (DCM1, DCM2), distyryl arylene derivatives (DSA), alkyl-substituted distyrylbenzene derivatives (DSB), benzimidazole derivatives (e.g. NBI), naphthostyrylamine derivatives (e.g. NSD), oxadiazole derivatives (e.g.
  • MEH-PPV poly(2-methoxy)-5-(2'ethylhexoxy)- 1 ,4-phenylene-vinylene), poly(2,4-bis(cholestanoxyl)-l,4-phenylene-vinylene) (BCHA-PPV), and segmented PPVs (see for example: E. Staring in International Symposium on Inorganic and Organic Electroluminescence, 1994, Hamamatsu, 48, and T. Oshino et al. in Sumitomo Chemicals, 1995 monthly report).
  • the following materials are suited as hole injection layers and hole transport layers.
  • Materials containing aromatic amino groups like tetraphenyldiaminodiphenyl (TPD-1, TPD-2, or TAD) and NPB (see C. Tang, SID Meeting San Diego, 1996, and C. Adachi et al. Applied Physics Letters, Vol. 66, p. 2679, 1995), TPA, NIPC, TPM, DEH (for the abbreviations see for example: P. Borsenberger and D.S. Weiss, Organic Photoreceptors for Imaging Systems, Marcel Dekker, 1993).
  • aromatic groups can also be incorporated in polymers, starburst (for example: TCTA, m-MTDATA, see Y. Kuwabara et al., Advanced Materials, 6, p. 677, 1994, Y. Shirota et al., Applied Physics Letters, Vol. 65, p. 807, 1994) and spiro compounds.
  • NSD quinacridone
  • P3MT poly(3-methylthiophene)
  • PT polythiophene
  • PTCDA 3,4,9, 10-perylenetetracarboxylic dianhydride
  • PPV poly(2-methoxyl,5-(2'ethyl-hexoxy)- 1 ,4-phenylene-vinylene
  • PVK poly(9-vinylcarbazole)
  • HPT discotic liquid crystal materials
  • blend (i.e. guest-host) systems containing active groups in a polymeric binder are also possible.
  • the concepts employed in the design of organic materials for OLED applications are to a large extent derived from the extensive existing experience in organic photoreceptors. A brief overview of some organic materials used in the fabrication of organic photoreceptors is found in the above mentioned publication of P. Brosenberger and D.S. Weiss, and in Tel tech, Technology Dossier Service, Organic Electroluminescence (1995), as well as in the primary literature.
  • inorganic barrier materials are LiF, CaO, MgO and so forth.
  • OLEDs have been demonstrated using polymeric, oligomeric and small organic molecules. The devices formed from each type of molecules are similar in function, although the deposition of the layers varies widely. The present invention is equally valid in all forms described above for organic light emitting devices based on polymers and oligomers, or small molecules.
  • Evaporation can be performed in a Bell jar type chamber with independently controlled resistive and electron-beam heating of sources. It can also be performed in a Molecular Beam Deposition System incorporating multiple effusion cells and sputter sources. In these cases, the metallic compound deposition can occur in the same chamber, a vacuum connected chamber, or even a separate chamber if some atmospheric contamination is tolerable.
  • Oligomeric and polymeric organics can also be deposited by evaporation of their monomeric components with later polymerization via heating or plasma excitation at the substrate. It is therefore possible to copolymerize or create mixtures by co-evaporation.
  • polymer containing devices are made by dissolving the polymer in a solvent and spreading it over the substrate either by spin coating or the doctor blade technique. After coating the substrate, the solvent is removed by evaporation or otherwise. This method allows the fabrication of well defined multilayer organic stacks, provided that the respective solvents for each subsequent layer do not dissolve previously deposited layers.
  • hybrid devices containing both polymeric and evaporated small organic molecules are possible.
  • the polymer film is generally deposited first, since evaporated small molecule layers cannot withstand much solvent processing.
  • inventive metallic compound cathodes are fully compatible with polymeric, oligomeric, and small-molecule OLED designs, or any hybrid design thereof.

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Abstract

Composant organique électroluminescent comprenant un substrat, une anode, une cathode et un empilement organique pris en sandwich entre l'anode et la cathode. La cathode de ce composant organique électroluminescent est constituée par un composé métallique consistant en carbure, nitrure ou borure d'un métal de transition précoce, de lanthanides ou d'un métal alcalino-terreux (groupe IIA du tableau périodique des éléments).
PCT/IB1997/001565 1997-12-15 1997-12-15 Contacts en composes metalliques pour des composants organiques et leur procede de fabrication WO1999031741A1 (fr)

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6316786B1 (en) 1998-08-29 2001-11-13 International Business Machines Corporation Organic opto-electronic devices
WO2002063698A1 (fr) * 2001-02-07 2002-08-15 Consiglio Nazionale Delle Ricerche Encapsulation de protection pour dispositifs electroluminescents organiques
US7843125B2 (en) 2004-01-26 2010-11-30 Cambridge Display Technology Limited Organic light emitting diode
WO2012053972A1 (fr) * 2010-10-20 2012-04-26 Empire Technology Development Llc Anodes d'hexaborure de calcium pour cellules électrochimiques
JPWO2013128504A1 (ja) * 2012-03-02 2015-07-30 株式会社Ｊｏｌｅｄ 有機ｅｌ素子とその製造方法、および金属酸化物膜の成膜方法

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JPH02234394A (ja) * 1989-03-08 1990-09-17 Idemitsu Kosan Co Ltd 有機エレクトロルミネッセンス素子用電極及びこれを用いた有機エレクトロルミネッセンス素子
JPH06310280A (ja) * 1993-04-20 1994-11-04 Fuji Xerox Co Ltd 有機発光素子用電極及びこれを用いた有機発光素子、並びに有機発光素子の製造方法
EP0729191A2 (fr) * 1995-02-23 1996-08-28 Eastman Kodak Company Injecteur conducteur d'électrons pour des diodes émettrices de lumière
WO1997047050A1 (fr) * 1996-06-05 1997-12-11 International Business Machines Corporation Semi-conducteurs non degeneres a bande interdite large et/ou electrodes de contact pour dispositifs organiques electroluminescents

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JPH02234394A (ja) * 1989-03-08 1990-09-17 Idemitsu Kosan Co Ltd 有機エレクトロルミネッセンス素子用電極及びこれを用いた有機エレクトロルミネッセンス素子
JPH06310280A (ja) * 1993-04-20 1994-11-04 Fuji Xerox Co Ltd 有機発光素子用電極及びこれを用いた有機発光素子、並びに有機発光素子の製造方法
EP0729191A2 (fr) * 1995-02-23 1996-08-28 Eastman Kodak Company Injecteur conducteur d'électrons pour des diodes émettrices de lumière
WO1997047050A1 (fr) * 1996-06-05 1997-12-11 International Business Machines Corporation Semi-conducteurs non degeneres a bande interdite large et/ou electrodes de contact pour dispositifs organiques electroluminescents

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PATENT ABSTRACTS OF JAPAN vol. 095, no. 002 31 March 1995 (1995-03-31) *

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6316786B1 (en) 1998-08-29 2001-11-13 International Business Machines Corporation Organic opto-electronic devices
WO2002063698A1 (fr) * 2001-02-07 2002-08-15 Consiglio Nazionale Delle Ricerche Encapsulation de protection pour dispositifs electroluminescents organiques
US7843125B2 (en) 2004-01-26 2010-11-30 Cambridge Display Technology Limited Organic light emitting diode
WO2012053972A1 (fr) * 2010-10-20 2012-04-26 Empire Technology Development Llc Anodes d'hexaborure de calcium pour cellules électrochimiques
US8435312B2 (en) 2010-10-20 2013-05-07 Empire Technology Development Llc Calcium hexaboride anodes for electrochemical cells
JPWO2013128504A1 (ja) * 2012-03-02 2015-07-30 株式会社Ｊｏｌｅｄ 有機ｅｌ素子とその製造方法、および金属酸化物膜の成膜方法

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