JP7410596B2 - エレクトロルミネセンス素子の製造方法、エレクトロルミネセンス素子、および表示装置 - Google Patents
エレクトロルミネセンス素子の製造方法、エレクトロルミネセンス素子、および表示装置 Download PDFInfo
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- JP7410596B2 JP7410596B2 JP2022532499A JP2022532499A JP7410596B2 JP 7410596 B2 JP7410596 B2 JP 7410596B2 JP 2022532499 A JP2022532499 A JP 2022532499A JP 2022532499 A JP2022532499 A JP 2022532499A JP 7410596 B2 JP7410596 B2 JP 7410596B2
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- 238000012360 testing method Methods 0.000 description 1
- 125000001544 thienyl group Chemical group 0.000 description 1
- HLLICFJUWSZHRJ-UHFFFAOYSA-N tioxidazole Chemical compound CCCOC1=CC=C2N=C(NC(=O)OC)SC2=C1 HLLICFJUWSZHRJ-UHFFFAOYSA-N 0.000 description 1
- 238000010023 transfer printing Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 238000002834 transmittance Methods 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 238000007740 vapor deposition Methods 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- TYHJXGDMRRJCRY-UHFFFAOYSA-N zinc indium(3+) oxygen(2-) tin(4+) Chemical compound [O-2].[Zn+2].[Sn+4].[In+3] TYHJXGDMRRJCRY-UHFFFAOYSA-N 0.000 description 1
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Description
1.EL素子の構造
EL素子の構造は光の出射方向に基づいて、基板を通して光を出射するボトムエミッション型と、基板とは反対側に光を出射するトップエミッション型に分類される。また、EL素子の構造は製造工程における積層順に基づいて、基板側から陽極、正孔輸送層、発光層、電子輸送層、陰極の順に積層された順積み構造と、その逆の順に積層された逆積み構造に分類される。本実施形態に係るEL素子は、逆積み構造に分類され、ボトムエミッション型及びトップエミッション型の双方に適用することができる。
図1は、本発明の一実施形態に係るEL素子200aの断面構造を示す。図1に示すEL素子200aは、ボトムエミッション型であり、逆積み構造を有する。すなわち、EL素子200aは、基板100側から、第1電極102、第1絶縁層104、電子輸送層106(第1電子輸送層106a、第2電子輸送層106b)、発光層112、第3電極118が積層された構造を有する。
図2は、トップエミッション型のEL素子200bを示す。トップエミッション型のEL素子200bは、第3電極118と第1電極102の構成が異なる他は、図1に示すボトムエミッション型のEL素子200aと構造は同じである。EL素子200bがトップエミッション型である場合、第1電極102は、光反射面が形成されるように金属膜で形成され、第3電極118は発光層112から放射される光が透過するように透明導電膜で形成される。第2電極108は発光領域の外側に配置されるため、構造及び構成材料を特段変更する必要がない。第3電極118の上層には、通常、薄膜封止層としてプラズマCVD(Chemical Vapor Deposition)法又はスパッタリング法で作製された窒化シリコン膜(Si3N4膜)、酸化シリコン膜(SiO2膜)、酸化アルミニウム膜(Al2O3膜)などが形成されるが、この図では省略する。
2-1.第1電極(キャリア注入量制御電極)
第1電極102は、金属材料、導電性を有する金属酸化物材料、金属窒化物材料又は金属酸窒化物材料を用いて形成される。金属材料としては、アルミニウム(Al)、銀(Ag)、チタン(Ti)、モリブデン(Mo)、タンタル(Ta)等の金属材料、又はこれらの金属を用いた合金材料や積層金属で形成される。金属酸化物材料としては、例えば、酸化インジウム錫(In2O3・SnO2:ITO)、酸化インジウム亜鉛(In2O3・ZnO:IZO)、酸化錫(SnO2)、酸化亜鉛(ZnO)を用いることができる。さらに、金属酸化物材料として、ニオブ(Nb)をドープした酸化チタン(TiOx:Nb)等を用いることができる。金属窒化物材料としては、窒化チタン(TiNx)、窒化ジルコニウム(ZrNx)等を用いることができる。金属酸窒化物材料としては、酸窒化チタン(TiOxNy)、酸窒化タンタル(TaOxNy)、酸窒化ジルコニウム(ZrOxNy)、酸窒化ハフニウム(HfOxNy)等を用いることができる。これらの金属酸化物材料、金属窒化物材料、金属酸窒化物材料に対して、導電性を向上させる微量の金属元素が添加されていてもよい。例えば、タンタル(Ta)がドープされた酸化チタン(TiOx:Ta)を用いてもよい。
第1絶縁層104は、無機絶縁材料を用いて形成される。無機絶縁材料としては、酸化シリコン、窒化シリコン、酸窒化シリコン、酸化アルミニウム等を選択することができる。第1絶縁層104は、プラズマCVD(Chemical Vapor Deposition)法、スパッタリング法等を用いて形成される。第1絶縁層104は、50nm~900nm、好ましくは100nm~600nmの膜厚で形成される。第1絶縁層104の膜厚を上記範囲とすることで、第1電極102によって生成される電界を電子輸送層106に作用させることができ、バイアス電圧を高くした場合においてもトンネル効果によって第1電極102から電子輸送層106にトンネル電流が流れることを防止することができる。
本実施形態において、第2絶縁層120は、極性を有する有機絶縁材料で形成される。第2絶縁層120は、例えば、直鎖系フッ素有機材料が用いられてもよい。直鎖系フッ素有機材料としては、例えば、フルオロアルキルシラン(FAS)系材料が用いられる。フルオロアルキルシラン(FAS)系材料としては、例えば、H,1H,2H,2H-ペルフルオロデシルトリクロロシラン(FDTS)、トリデカフルオロ-1,1,2,2-テトラヒドロオクチルトリクロロシラン(FOTS)等が用いられる。
電子輸送層106は、第2電極108から注入されるキャリア(電子)を、EL素子200の発光領域の面内に輸送するために、電子移動度が高い材料で形成されることが好ましい。また、電子輸送層106は、ボトムエミッション型の場合、発光層よりも光出射側に配置されるので、良好な可視光透光性を有する材料で形成されることが好ましい。また、第1電子輸送層106aと第2電子輸送層106bとの間でキャリア濃度を異ならせるために、キャリア濃度の制御が容易である材料で形成されることが好ましい。
EL素子の陰極材料としては、従来、アルミニウム・リチウム合金(AlLi)、マグネシウム・銀合金(MgAg)等の材料が用いられている。しかし、これらの材料は、大気中の酸素や水分の影響を受けて劣化しやすく、取扱が困難な材料である。また、これらの材料は金属又はアルカリ金属であり、透光性を持たせるためには薄膜化して半透過膜とする必要がある。しかし、陰極を薄膜化するとシート抵抗が高くなってしまうことが問題となる。電極の抵抗はEL素子の中で直列抵抗成分として作用するので、陰極の薄膜化は駆動電圧を高め、消費電力を増加させる要因となる。さらに、EL素子の発光領域の面内で、発光強度(輝度)の不均一性の原因ともなる。
EL素子において、電子注入層は、陰極から電子輸送材料へ電子を注入するためのエネルギー障壁を小さくするために用いられる。本実施形態に係るEL素子200は、酸化物半導体で形成される電子輸送層106から発光層112へ電子が注入されやすくするために、電子注入層110が設けられることが好ましい。電子注入層110は、電子輸送層106と発光層112との間に設けられる。図1および図2に示すように、電子注入層110は、表示領域全面に形成されることが歩留まり向上と信頼性向上のためには重要である。
発光層112はエレクトロルミネセンス材料を用いて形成される。エレクトロルミネセンス材料としては、例えば、蛍光を発光する蛍光性化合物材料、燐光を発光する燐光性化合物材料、又は熱活性化遅延蛍光材料(Thermally activated delayed fluorescence:TADF)を用いることができる。
正孔輸送層114は、正孔輸送性を有する材料を用いて形成される。正孔輸送層114は、例えば、アリールアミン系化合物、カルバゾール基を含むアミン化合物、およびフルオレン誘導体を含むアミン化合物などであっても良い。正孔輸送層114は、例えば、4,4’-ビス[N-(ナフチル)-N-フェニル-アミノ]ビフェニル(α-NPD)、N,N’-ビス(3-メチルフェニル)-(1,1’-ビフェニル)-4,4’-ジアミン(TPD)、2-TNATA、4,4’,4”-トリス(N-(3-メチルフェニル)N-フェニルアミノ)トリフェニルアミン(MTDATA)、4,4’-N,N’-ジカルバゾールビフェニル(CBP)、4,4’-ビス[N-(9,9-ジメチルフルオレン-2-イル)-N-フェニルアミノ]ビフェニル(DFLDPBi)、4,4’-ビス[N-(スピロ-9,9’-ビフルオレン-2-イル)-N―フェニルアミノ]ビフェニル(BSPB)、スピロ-NPD、スピロ-TPD、スピロ-TAD、TNB等の有機材料が用いられる。
正孔注入層116は、有機層に対して正孔注入性の高い物質を含む。正孔注入性の高い物質としては、モリブデン酸化物やバナジウム酸化物、ルテニウム酸化物、タングステン酸化物、マンガン酸化物等の金属酸化物を用いることができる。また、フタロシアニン(H2Pc)、銅(II)フタロシアニン(略称:CuPc)、バナジルフタロシアニン(VOPc)、4,4’,4’’-トリス(N,N-ジフェニルアミノ)トリフェニルアミン(TDATA)、4,4’,4’’-トリス[N-(3-メチルフェニル)-N-フェニルアミノ]トリフェニルアミン(MTDATA)、4,4’-ビス[N-(4-ジフェニルアミノフェニル)-N-フェニルアミノ]ビフェニル(DPAB)、4,4’-ビス(N-{4-[N’-(3-メチルフェニル)-N’-フェニルアミノ]フェニル}-N-フェニルアミノ)ビフェニル(DNTPD)、1,3,5-トリス[N-(4-ジフェニルアミノフェニル)-N-フェニルアミノ]ベンゼン(DPA3B)、3-[N-(9-フェニルカルバゾール-3-イル)-N-フェニルアミノ]-9-フェニルカルバゾール(PCzPCA1)、3,6-ビス[N-(9-フェニルカルバゾール-3-イル)-N-フェニルアミノ]-9-フェニルカルバゾール(PCzPCA2)、3-[N-(1-ナフチル)-N-(9-フェニルカルバゾール-3-イル)アミノ]-9-フェニルカルバゾール(PCzPCN1)、2,3,6,7,10,11-ヘキサシアノ-1,4,5,8,9,12-ヘキサアザトリフェニレン(HAT-CN)等の有機化合物を用いることができる。
第3電極118としては、仕事関数の大きい(具体的には4.0eV以上)金属、合金、導電性化合物で作製される。第3電極118には、例えば、酸化インジウム錫(ITO)、酸化インジウム亜鉛(IZO)、酸化タングステン及び酸化亜鉛を含有した酸化インジウム(IWZO)などが用いられる。これらの導電性金属酸化物材料が用いられる第3電極118は、真空蒸着法、スパッタリング法により作製される。
配線111は、アルミニウム(Al)、銅(Cu)等の導電率の高い金属材料が用いられる。例えば、配線111は、アルミニウム合金、銅合金、または銀合金を用いて作製される。アルミニウム合金としては、アルミニウム・ネオジム合金(Al-Nd)、アルミニウム・チタン合金(Al-Ti)、アルミニウム・シリコン合金(Al-Si)、アルミニウム・ネオジム・ニッケル合金(Al-Nd-Ni)、アルミニウム・カーボン・ニッケル合金(Al-C-Ni)、銅・ニッケル合金(Cu-Ni)等を適用することができる。このような金属材料を用いれば、耐熱性を有すると共に、配線抵抗を低減することができる。また、Mo/Al/Mo、Mo/Cu/Moなどの3層積層構造の電極も有効である。すなわち、上述する金属材料をモリブデン(Mo)、ジルコニウム(Zr)、チタン(Ti)、またはこれらの合金材料を含む酸化防止層で挟んだ3層積層構造を適用することもできる。
図3、図4、及び図5を参照して、本実施形態に係るEL素子の動作を説明する。なお、本節で示すEL素子200は、模式的な構造を示す。
図3は、本実施形態に係るEL素子200の構成を模式的に示す。図3は、EL素子200を構成する部材として、第2電極108、電子輸送層106、電子注入層110、発光層112、正孔輸送層114、正孔注入層116、第3電極118、第1絶縁層104、及び第1電極102が設けられた構造を示す。
EL素子が発光するには、陽極から正孔が注入され、陰極から電子が注入される必要がある。そして、EL素子の電流効率(発光効率)を高めるには、陽極から発光層に輸送される正孔の量と陰極から発光層に輸送される電子の量とが一致するようにバランスをとる必要がある(以下、「キャリアバランス」ともいう)。EL素子は、キャリアバランスをとることで電流効率を高めることができる。
本発明の一実施形態に係るEL素子の作製方法の一例を、図7、図8、及び図9を参照して説明する。以下においては、図1に示すボトムエミッション型のEL素子200aの作製方法について説明する。
本実施形態は、本発明の一実施形態に係るEL素子で画素が構成された表示装置(EL表示装置)の一例について説明する。
図13及び図14は、第1実施形態で示すEL素子に対し、陰極の構成が異なるEL素子を示す。以下の説明においては、第1実施形態と相違する部分について説明し、共通する部分については説明を省略する。
図15は、第1実施形態で示すEL素子に対し、第1電極がなく陰極の構成が異なるEL素子を示す。以下の説明においては、第1実施形態と相違する部分について説明し、共通する部分については説明を省略する。
第1実施形態で示すEL素子に対し、陰極の構成が異なるEL素子について示す。以下の説明においては、第1実施形態と相違する部分について説明し、共通する部分については説明を省略する。
本実施形態は、第1実施形態で示すEL素子に対し、陰極の構成が異なるEL素子について示す。以下の説明においては、第1実施形態と相違する部分について説明し、共通する部分については説明を省略する。
本実施形態に係るEL素子200gで画素が構成された表示装置(EL表示装置)の一例について説明する。以下の説明においては、第2実施形態と相違する部分について説明し、共通する部分については説明を省略する。
本実施形態に係るEL素子200hで画素が構成された表示装置(EL表示装置)の一例について説明する。以下の説明においては、第2実施形態と相違する部分について説明し、共通する部分については説明を省略する。
Claims (13)
- 基板上に第1電極を形成し、
前記第1電極と接する第1電子輸送層を形成し、
前記第1電極と重なる領域に開口部を有する第1絶縁層を形成し、
前記開口部に、有機2族金属化合物と有機3族金属化合物とが有機溶媒に溶解されている組成物を塗布し、塗布後に溶媒を除去して金属酸化物半導体からなる第2電子輸送層を形成し、
前記第2電子輸送層と重なり、エレクトロルミネセンス材料を含む発光層を形成し、
前記発光層と重なる領域に、第2電極を形成すること、を含むエレクトロルミネセンス素子の製造方法。 - 基板上に第1電極を形成し、
前記第1電極と接する第1電子輸送層を形成し、
前記第1電極と重なる領域に開口部を有する第1絶縁層を形成し、
前記開口部に、2価のZn及びMg、3価のIn及びGa、並びに4価のSnからなる群から選択される少なくとも1つをドーピングした無機酸塩と第1アミドと溶媒とを含む組成物を塗布し、塗布後に溶媒を除去して無機透明酸化物半導体からなる第2電子輸送層を形成し、
前記第2電子輸送層と重なり、エレクトロルミネセンス材料を含む発光層を形成し、
前記発光層と重なる領域に、第2電極を形成すること、を含むエレクトロルミネセンス素子の製造方法。 - 前記第1電極は陰極であり、
前記第2電極は陽極であり、
前記エレクトロルミネセンス素子は逆積み構造である請求項1または2に記載の製造方法。 - 第1電極と、
前記第1電極と対向する領域を有する第2電極と、
前記第1電極と前記第2電極との間の第1絶縁層と、
前記第1電極と電気的に接続する電子輸送層と、
前記電子輸送層と前記第2電極との間のエレクトロルミネセンス材料を含む発光層と、
を有し、
前記第1絶縁層は開口部を有し、
前記開口部において、前記第2電極、前記発光層、前記電子輸送層、及び前記第1電極が重なる重畳領域を有し、
前記電子輸送層は、前記第1電極と接する第1電子輸送層と、前記開口部に配置され、前記第1電子輸送層と接する第2電子輸送層と、を有し、
前記第2電子輸送層は無機透明酸化物半導体からなり、前記開口部の中心部に比べ端部の膜厚が大きく、前記開口部の側面に接し、前記側面に沿ってせり上がり、前記第1絶縁層の前記開口部を超えず、前記端部は前記開口部内に配置されているエレクトロルミネセンス素子。 - 前記第2電子輸送層は、50nm以上2000nm以下の範囲の膜厚で設けられる、請求項4に記載のエレクトロルミネセンス素子。
- 前記第1電子輸送層の電子移動度は、前記第2電子輸送層の電子移動度より高い、請求項4に記載のエレクトロルミネセンス素子。
- 前記第1電子輸送層のキャリア濃度は、前記第2電子輸送層のキャリア濃度より高い、請求項6に記載のエレクトロルミネセンス素子。
- 前記第1電子輸送層のバンドギャップは3.0eV以上であり、前記第2電子輸送層のバンドギャップは3.0eV以上である、請求項6に記載のエレクトロルミネセンス素子。
- 前記第1電子輸送層及び前記第2電子輸送層は酸化物半導体を含み、かつ前記第1電子輸送層の厚みより前記第2電子輸送層の厚みの方が大きい、請求項6に記載のエレクトロルミネセンス素子。
- 前記第1電子輸送層は、酸化スズ及び酸化インジウムと、酸化ガリウム、酸化タングステン、酸化アルミニウム及び酸化シリコンから選ばれた少なくとも一種を含み、
前記第2電子輸送層は、酸化亜鉛と、酸化シリコン、酸化マグネシウム、酸化インジウム、酸化アルミニウム及び酸化ガリウムから選ばれた少なくとも一種を含む、請求項9に記載のエレクトロルミネセンス素子。 - 前記第2電子輸送層の比抵抗値は、10 2Ω・cm~10 6Ω・cmの範囲である、請求項9に記載のエレクトロルミネセンス素子。
- 前記第2電子輸送層の仕事関数の値は3.8eV以下である、請求項4に記載のエレクトロルミネセンス素子。
- 基板上に、請求項4乃至12のいずれか一項に記載のエレクトロルミネセンス素子と、前記エレクトロルミネセンス素子と接続される駆動トランジスタと、を含む画素を有し、
前記駆動トランジスタは、
酸化物半導体層と、
前記酸化物半導体層の下に配置される第1絶縁層と、
前記酸化物半導体層と重なる領域を有し、前記第1絶縁層を介して前記酸化物半導体層の前記基板側に配置された第1ゲート電極と、
前記酸化物半導体層及び前記第1ゲート電極と重なる領域を有し、前記酸化物半導体層の前記基板側とは反対に配置された第2ゲート電極と、を有し、
前記第1電極は前記酸化物半導体層と電気的に接続することを特徴とする表示装置。
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