JP2019054142A - 光電変換素子、その製造方法、およびその製造装置 - Google Patents
光電変換素子、その製造方法、およびその製造装置 Download PDFInfo
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- JP2019054142A JP2019054142A JP2017178161A JP2017178161A JP2019054142A JP 2019054142 A JP2019054142 A JP 2019054142A JP 2017178161 A JP2017178161 A JP 2017178161A JP 2017178161 A JP2017178161 A JP 2017178161A JP 2019054142 A JP2019054142 A JP 2019054142A
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Images
Classifications
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- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/20—Light-sensitive devices
- H01G9/2022—Light-sensitive devices characterized by he counter electrode
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/0029—Processes of manufacture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/20—Light-sensitive devices
- H01G9/2068—Panels or arrays of photoelectrochemical cells, e.g. photovoltaic modules based on photoelectrochemical cells
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/20—Light-sensitive devices
- H01G9/2095—Light-sensitive devices comprising a flexible sustrate
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/20—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising organic-organic junctions, e.g. donor-acceptor junctions
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/80—Constructional details
- H10K30/81—Electrodes
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
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Abstract
Description
ペロブスカイト太陽電池を塗布法で製造する方法として、ロール・トゥー・ロール法が挙げられる。ロール・トゥー・ロール法では、塗布された基板がロールによって搬送されるため、基板は柔軟性を有する必要がある。
ここで、ペロブスカイト太陽電池は製造工程において欠陥が発生しやすいことが知られている。欠陥とは、太陽電池において、局所的に透明電極と対向電極間の距離が短くなる箇所であり、透明電極と対向電極が直接接触する場合も該当する。この箇所では、ペロブスカイト層の膜厚が薄いので、目視観察で透過率が高いことがわかる。そのため、ピンホールと呼ばれることもある。
基板と、
透明電極と、
活性層と、
対向電極と
をこの順に積層した構造を有しており、かつ対向電極側の面に凹部を有しており、
前記凹部が対向電極を貫通しており、
前記凹部の前記対向電極部分における開口面積が、前記活性層部分における開口面積より大きく、
かつ前記凹部の底部に、前記対向電極に由来する導電性部分が露出していないことを特徴とするものである。
基板と、
透明電極と、
塗布法により形成された活性層と、
対向電極と
をこの順に積層した構造を有する積層構造体を形成させ、
前記積層構造体を形成させた後、前記対向電極の表面の、発生した欠陥の直上部分に粘着性部材を押圧し、その後、前記欠陥およびその周囲部分を前記粘着部材と共に剥離することを含むことを特徴とするものである。
図1は、第1実施形態による光電変換素子1の模式断面図である。以下、簡単のために光電変換素子を単に素子ということがある。本実施形態による素子は、基板11と、透明電極12と、第1中間層13と、光電変換層14と、第2中間層15と、対向電極16、封止層17とをこの順に備えている。このうち、第1中間層13および第2中間層15は必要に応じて設けられる層である。透明電極は基板上に設けられ、第1中間層は透明電極上に設けられている。光電変換層は第1中間層上に設けられており、例えばペロブスカイト化合物を含む光電変換層である。第2中間送層は光電変換層上に設けられ、対向電極は第2中間層上に設けられる。そして、対向電極16を貫通し、光電変換層14に及ぶ凹部10が形成されている。さらに、封止層17は対向電極上に設けられている。以下、本実施形態による素子を構成する各部材について詳細に説明する。
基板11は、他の構成部材を支持するためのものである。基板の材料は、従来知られている光電変換素子に用いられるものから任意に選択することができる。ただし、実施形態による光電変換素子が有効に作用するように、入射光がこの基板を通過して光電変換層まで届く必要があるので、透明性が高い材料であることが好ましい。
透明電極の材料としては、導電性の金属酸化物膜、半透明の金属薄膜等が挙げられる。
具体的には、酸化インジウム、酸化亜鉛、酸化スズ、およびそれらの複合体である酸化インジウムスズ(ITO)、フッ素ドープ酸化スズ(FTO)、またはインジウム、亜鉛、およびオキサイド等からなる導電性ガラスを用いて作製された酸化スズ膜等が用いられる。
特に、ITOが好ましい。ITOは電極の材料として、高い光透過率、低いシート抵抗、および小さな表面粗さを有するものであることが知られている。
第1中間層13および第2中間層15は、必要に応じて設けられる層である。これらは、例えば正孔輸送層または電子輸送層として機能するものである。光電変換層の構造などによって、それぞれが適切に設置される。例えば、第1中間層が正孔輸送層である場合、第1中間層13は、光電変換層14で生成された電子をブロックし、正孔を選択的にかつ効率的に透明電極12に輸送する機能等を有する。このとき、第2中間層は電子輸送層とされ、第2中間層15は、光電変換層14で生成された正孔をブロックし、電子を選択的にかつ効率的に対向電極16に輸送する機能等を有する。
実施形態による素子において、活性層14は、光電変換機能を有するものであれば特に限定されない。入射光により起電力が発生するもの(光電変換層)であっても、電圧印加によって発光するもの(発光層)であってもよい。しかしながら、柔軟性を有する素子を形成させるために、ペロブスカイト系化合物または有機材料の少なくともいずれかを含むものが好ましい。
まず、光電変換層14として、ペロブスカイト系化合物を用いた場合を説明する。実施形態による素子は、活性層としてペロブスカイト系化合物を含むことが好ましい。
ペロブスカイト系化合物を含む光電変換層14は、後述するペロブスカイト材料溶液を用いて、塗布成膜法により形成させることができる。ペロブスカイト材料溶液は、溶媒と、溶媒中に溶解または分散されたペロブスカイト結晶粒子とを含む。典型的なペロブスカイト結晶粒子は、下記の式(1)で表される組成を有し、3次元結晶構造を持つものである。
組成式:ABX3 ・・・(1)
式(1)において、Aはアミン化合物の1価陽イオンであり、Bは金属元素の2価陽イオンであり、Xはハロゲン元素の1価陰イオンである。
t=(Aイオン半径+Xイオン半径)/{21/2×(Bイオン半径+Xイオン半径)}・・・(2)
次に、光電変換層14として、有機材料からなるヘテロ接合構造またはバルクヘテロ接合構造である場合を説明する。
対向電極16は、導電性を有し、必要に応じて光透過性を有する材料により構成される。対向電極16の構成材料としては、例えば銀、金、アルミニウム、銅、チタン、白金、ニッケル、コバルト、鉄、マンガン、タングステン、ジルコニウム、スズ、亜鉛、インジウム、クロム、リチウム、ナトリウム、カリウム、ルビジウム、セシウム、カルシウム、マグネシウム、バリウム、サマリウム、テルビウムのような金属、それらを含む合金、ITOやインジウム−亜鉛酸化物(IZO)のような導電性金属酸化物、PEDOT:PSSのような導電性高分子、あるいはグラフェン、カーボンナノチューブ、カーボンペーストのような炭素材料等が挙げられる。対向電極16は、用いられる材料に応じて適当な方法、例えば真空蒸着法やスパッタ法のような真空成膜法、ゾルゲル法、塗布法等により形成される。
実施形態による素子は、必要に応じて、封止層を有する事ができる。封止層17は、光電変換素子に耐久性を付与する保護膜として機能する。封止層17は光電変換素子の光吸収を妨げないために、可視光(波長360nm〜830nm)を透過させることが望ましい。例えば、可視光の透過率は上限に制限は無いが、60%以上が望ましい。封止層17の厚みは特に制限は無いが、通常1μm以上である。
実施形態による光電変換素子1は、上記の各層を積層した構造を有する。そして、対向電極側の面に凹部10を有していることを特徴としている。この凹部は、対向電極16を貫通して開口部分を形成している。そして、図1においては、凹部は第2中間層15も貫通し、活性層14に及んでいる。
発光素子、特に有機電界発光素子(以下、OLEDと称することがある)は、照明やディスプレイのバックライトへの応用のための開発が進められている。
図6は、実施形態に係る有機電界発光素子6を示す断面図である。図6に示されたOLEDは、基板61上に陽極(透明電極)62、正孔輸送層63、活性層(発光層)64、電子輸送層65、電子注入層66、陰極(対向電極)67、および封止層68が積層された構造を有する。ここで正孔輸送層63は第1の中間層に、電子輸送層65および電子注入層66は、第2の中間層に相当するものであり、必要に応じて形成される。
基板としては、第1の実施形態において説明したものと同様のものを用いることができる。なお、OLEDにおいては発光層からの光を効率良く取り出すために、基板表面に、例えば凹凸構造を有する膜(凹凸構造膜)を設けることができる。適切な構造を付与することによって、外界(空気)と凹凸構造膜の屈折率差が連続的に変化することで、光取り出し効率が改善する。また、また、凹凸構造膜を構成する材料の屈折率を、基板の屈折率に近いものを選ぶことによって、さらに光取り出し効率が改善する。
陽極62は、正孔輸送層63または発光層64に正孔を注入する。発光層から放射される光は、基板61側から取り出されるので、陽極は透明性が高いことが好ましい。このような理由から選択される透明または半透明の電極材料としては、導電性の金属酸化物膜や半透明の金属薄膜等が挙げられる。具体的には第1の実施形態において説明したものとおなじものを用いることができる。
正孔輸送層63は、陽極62と発光層64との間に任意に配置される。
正孔輸送層63は、陽極62から正孔を受け取り、発光層側へ輸送する機能を有する層である。正孔輸送層63の材料としては、例えば、導電性インクであるPEDOT:PSSのようなポリチオフェン系ポリマーを使用することができるが、これに限定されない。
発光層64の材料としては、OLEDに用いられる材料から任意に選択することができる。この材料は、蛍光材料であっても燐光材料であってもよく、また低分子材料であっても高分子材料であってもよい。具体的には以下のものを挙げることができる。
青色発光材料:
4,4’−ビス(9−エチル−3−カルバゾビニレン)−1,1’−ビフェニル)BCzVBi)、
ビス(3,5−ジフルオロ−2−(2−ピリジル)フェニル−(2−カルボキシピリジル)イリジウム(III)(Firpic)、
ビス(2,4−ジフルオロフェニルピリジナト)テトラキシ(1−ピラゾリル)ボレート イリジウム(III)(FIr6)、
緑色発光材料:
トリス(8−キノリノラト)アルミニウム(Alq3)、
2,3,6,7−テトラヒドロ−1,1,7,7,−テトラメチル−1H,5H,11H−10−(2−ベンゾチアゾリル)キノリジノ−[9,9a,1gh]クマリン(C545T)、
トリス(2−フェニルピリジナト)イリジウム(III)(Ir(ppy)3)、
赤色発光材料:
4−(ジシアノメチレン)−2−メチル−6−(4’−ジメチルアミノスチリル)−4H−ピラン(DCM1)、
4−(ジシアノメチレン)−2−tert−ブチル−6−(1,1,7,7−テトラメチルジュロリジン−4−イル−ビニル)−4H−ピラン(DCJTB)、
2,3,7,8,12,13,17,18−オクタエチル−21H,23H−ポルフィリン白金(II)(PtOEP)
なお、発光材料はこれらに限定されず、その他のものから任意に選択することができる。
電子輸送層65は、必要に応じて、発光層64の上に形成される。電子輸送層65は、電子注入層66から電子を受け取り、発光層64へ輸送する機能を有する層である。電子輸送層65の材料としては、例えば、トリス(2,4,6−トリメチル−3−(ピリジン−3−イル)フェニル)ボラン(3TPYMB]、トリス(8−キノリノラト)アルミニウム錯体(Alq3)、バソフェナントロリン(BPhen)等を使用することができるが、これらに限定されない。
電子注入層66は、必要に応じて、電子輸送層65の上に形成される。電子注入層66は、陰極67から電子を受け取り、電子輸送層65または発光層64へ注入する機能を有する層である。
陰極67は、発光層64(または電子輸送層65もしくは電子注入層66)の上に形成される。陰極67の機能は、発光層64(または電子輸送層65もしくは電子注入層66)に電子を注入することである。
実施形態による発光素子は、必要に応じて封止層68を有する。封止層68は、発光素子に耐久性を付与する保護膜として機能する。この封止層を形成するための材料は、実施形態1に例示したものと同じものを用いることができる。
実施形態にかかる発光素子は、陰極側に凹部を有し、その構造は第1の実施形態において説明したものと同様である。陰極67を貫通する凹部は、発光層64、または正孔輸送層63に及ぶ。そして、陽極62と陰極67の間の短絡を抑制し、発光層に効率よく電圧が印加され、高い発光効率で発光を得ることができる。
実施形態に係る光電変換素子は任意の方法で製造することができるが、一般的に知られている製造方法によって素子を製造し、その後に発生した欠陥を処理することで製造することが好ましい。以下、光電変換素子が太陽電池である場合に、欠陥の処理をテープ法によって行う素子の製造方法を説明する。
欠陥に対する処理は、太陽電池であっても発光素子であっても同様に行うことができる。ここではペロブスカイト太陽電池を例に説明する。
任意の方法で透明電極81、活性層82、および対向電極83を積層した素子8を形成させる。このような素子には、一般的に活性層中に欠陥72が散在している。この素子について、欠陥位置特定機構、例えばCCDカメラ85を用いて欠陥72の位置を特定する(図8(A))。
実施例1では、ペロブスカイト太陽電池の場合を例に説明する。用いた太陽電池は、以下の構成を有するものである。
基板: PEN、
透明電極: ITO
第1中間層(正孔輸送層): PEDOT:PSS
活性層(光電変換層): ペロブスカイト系化合物
第2中間層(電子輸送層): 60PCBM
対向電極: Au
実施例2では、有機薄膜太陽電池の場合を例に挙げて説明する。用いた太陽電池は、以下の構成を有するものである。
基板: PEN
透明電極: ITO
第1中間層(正孔輸送層): PEDOT:PSS
活性層(光電変換層): PTB7−Thと70PCBMの混合物
第2中間層(電子輸送層): LiF
対向電極: Ag
クロロベンゼン:1,8−ジヨードオクタン=97Vol%:3Vol%の混合溶媒1mLに、PTB7−Thを8mgと70PCBMを12mg加えて有機薄膜材料溶液を作製した。この溶液をスピンコート法で塗布し、乾燥させて、光電変換層を形成した。
スピンコートの条件は、回転数が700rpmで30秒間とした。
実施例3では、OLEDの場合を例に説明する。用いたOLEDは、以下の構成を有するものである。
基板: PEN
陽極: ITO
正孔輸送層: PEDOT:PSS
発光層: Alq3
電子注入層: LiF
対向電極: Al
素子の外観を観察したところ、目視で確認できるサイズの欠陥が存在していることが分かった。実施例1と同様に、欠陥部の処理を行ったところ、4V印加時に輝度2000(cd/m2)に改善した。
10 凹部
11 基板
12 透明電極
13 第1中間層
14 光電変換層
15 第2中間層
16 対向電極
17 封止層
6 有機電界発光素子
60 凹部
61 基板
62 陽極
63 正孔輸送層
64 活性層
65 電子輸送層
66 電子注入層
67 陰極
68 封止層
71 発電領域
72 欠陥
8 素子
81 透明電極
82 活性層
83 対向電極
85 CCDカメラ
86 粘着部材
87 支持部材
Claims (15)
- 基板と、
透明電極と、
活性層と、
対向電極と
をこの順に積層した構造を有しており、かつ対向電極側の面に凹部を有しており、
前記凹部が対向電極を貫通しており、
前記凹部の前記対向電極部分における開口面積が、前記活性層部分における開口面積より大きく、
かつ前記凹部の底部に、前記対向電極に由来する導電性部分が露出していないことを特徴とする、光電変換素子。 - 前記凹部の底面に前記基板が露出していない、請求項1に記載の素子。
- 前記凹部の底面に、前記透明電極が露出している、請求項1または2に記載の素子。
- 活性層と透明電極の間、または活性層と対向電極の間に中間層を有する、請求項1〜3のいずれか1項に記載の素子。
- 前記対向電極部分における開口面積が、4mm2以下である、請求項1〜4のいずれか1項に記載の素子。
- 前記基板が、柔軟性を有する有機材料からなる、請求項1〜5のいずれか1項に記載の素子。
- 前機有機材料が、ポリエチレンナフタレート、ポリエチレンテレフタレート、ポリエチレン、ポリイミド、ポリアミド、ポリアミドイミド、ポリエステル、ポリシクロオレフィン、および液晶ポリマーからなる群から選択される、請求項6に記載の素子。
- 前記活性層が、ペロブスカイト化合物を含む、請求項1〜7のいずれか1項に記載の素子。
- 前記活性層は、有機材料からなるヘテロ接合構造またはバルクヘテロ接合構造を有する、請求項1〜8のいずれか1項に記載の素子。
- 前記対向電極の上に、さらに封止層を有する、請求項1〜9のいずれか1項に記載の素子。
- 前記封止層が前記凹部の内部に嵌入している、請求項1〜10のいずれか1項に記載の素子。
- 光電池、発光素子、光センサ、光ダイオード、および光メモリからなる群から選択される、請求項1〜11のいずれか1項に記載の素子。
- 請求項1〜11のいずれか1項に記載の素子が複数配列されたことを特徴とする、光電池モジュール。
- 基板と、
透明電極と、
塗布法により形成された活性層と、
対向電極と
をこの順に積層した構造を有する積層構造体を形成させ、
前記積層構造体を形成させた後、
(a)前記対向電極の表面の、発生した欠陥の直上部分に粘着性部材を押圧し、その後、前記欠陥およびその周囲部分を前記粘着部材と共に剥離すること、または
(b)前記対向電極の表面の、発生した欠陥をその周囲部分と共に吸引除去すること
を含むことを特徴とする、光電素子の製造方法。 - 請求項1〜12のいずれか1項に記載の素子の製造装置、または請求項13に記載の光電池モジュールの製造装置であって、欠陥の位置を特定する欠陥位置特定機構と、前記欠陥を除去する欠陥除去機構とを備えていることを特徴とする装置。
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US11335871B2 (en) | 2018-09-18 | 2022-05-17 | Kabushiki Kaisha Toshiba | Photoelectric conversion device and manufacturing method thereof |
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CN116234338A (zh) * | 2023-04-27 | 2023-06-06 | 广东爱旭科技有限公司 | 太阳能电池 |
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KR20200141767A (ko) * | 2019-06-11 | 2020-12-21 | 엘지디스플레이 주식회사 | 전자장치 |
ES2954469T3 (es) * | 2019-08-23 | 2023-11-22 | Saule Spolka Akcyjna | Un dispositivo fotovoltaico y un método para la preparación del mismo |
CN113130759B (zh) * | 2021-03-05 | 2022-08-16 | 华南理工大学 | 一种快速去除卤化物钙钛矿薄膜表面缺陷的方法及其在钙钛矿太阳能电池中的应用 |
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US10950391B2 (en) | 2021-03-16 |
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