CN103594632B - Composite transparent electrode and organic solar cell including same - Google Patents
Composite transparent electrode and organic solar cell including same Download PDFInfo
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- CN103594632B CN103594632B CN201310547707.XA CN201310547707A CN103594632B CN 103594632 B CN103594632 B CN 103594632B CN 201310547707 A CN201310547707 A CN 201310547707A CN 103594632 B CN103594632 B CN 103594632B
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- 239000002131 composite material Substances 0.000 title claims abstract description 25
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 67
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 66
- 239000004411 aluminium Substances 0.000 claims abstract description 64
- 238000000034 method Methods 0.000 claims abstract description 30
- 239000011521 glass Substances 0.000 claims abstract description 24
- 239000000463 material Substances 0.000 claims abstract description 23
- 239000000758 substrate Substances 0.000 claims abstract description 20
- 238000000151 deposition Methods 0.000 claims abstract description 4
- 239000010410 layer Substances 0.000 claims description 46
- 238000004528 spin coating Methods 0.000 claims description 30
- 238000002360 preparation method Methods 0.000 claims description 28
- 229920000301 poly(3-hexylthiophene-2,5-diyl) polymer Polymers 0.000 claims description 24
- 239000002904 solvent Substances 0.000 claims description 23
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 20
- MCEWYIDBDVPMES-UHFFFAOYSA-N [60]pcbm Chemical compound C123C(C4=C5C6=C7C8=C9C%10=C%11C%12=C%13C%14=C%15C%16=C%17C%18=C(C=%19C=%20C%18=C%18C%16=C%13C%13=C%11C9=C9C7=C(C=%20C9=C%13%18)C(C7=%19)=C96)C6=C%11C%17=C%15C%13=C%15C%14=C%12C%12=C%10C%10=C85)=C9C7=C6C2=C%11C%13=C2C%15=C%12C%10=C4C23C1(CCCC(=O)OC)C1=CC=CC=C1 MCEWYIDBDVPMES-UHFFFAOYSA-N 0.000 claims description 16
- 238000001771 vacuum deposition Methods 0.000 claims description 16
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 12
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 12
- 238000001035 drying Methods 0.000 claims description 12
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- 238000005374 membrane filtration Methods 0.000 claims description 12
- 238000010438 heat treatment Methods 0.000 claims description 11
- 238000003760 magnetic stirring Methods 0.000 claims description 11
- 229910052757 nitrogen Inorganic materials 0.000 claims description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 7
- 239000011247 coating layer Substances 0.000 claims description 6
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- 238000001704 evaporation Methods 0.000 claims description 5
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- 239000011368 organic material Substances 0.000 claims description 4
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- 229910052724 xenon Inorganic materials 0.000 description 14
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 14
- 238000002156 mixing Methods 0.000 description 9
- JKQOBWVOAYFWKG-UHFFFAOYSA-N molybdenum trioxide Inorganic materials O=[Mo](=O)=O JKQOBWVOAYFWKG-UHFFFAOYSA-N 0.000 description 9
- 229920000144 PEDOT:PSS Polymers 0.000 description 6
- 239000010409 thin film Substances 0.000 description 6
- 230000005540 biological transmission Effects 0.000 description 5
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- 238000002835 absorbance Methods 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
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- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- 238000013086 organic photovoltaic Methods 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 238000005406 washing Methods 0.000 description 2
- LLYXJBROWQDVMI-UHFFFAOYSA-N 2-chloro-4-nitrotoluene Chemical compound CC1=CC=C([N+]([O-])=O)C=C1Cl LLYXJBROWQDVMI-UHFFFAOYSA-N 0.000 description 1
- AGBXYHCHUYARJY-UHFFFAOYSA-N 2-phenylethenesulfonic acid Chemical compound OS(=O)(=O)C=CC1=CC=CC=C1 AGBXYHCHUYARJY-UHFFFAOYSA-N 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- 229920001609 Poly(3,4-ethylenedioxythiophene) Polymers 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- 229910003087 TiOx Inorganic materials 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
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- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910000024 caesium carbonate Inorganic materials 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000005229 chemical vapour deposition Methods 0.000 description 1
- 238000005034 decoration Methods 0.000 description 1
- 238000002242 deionisation method Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005485 electric heating Methods 0.000 description 1
- 238000005566 electron beam evaporation Methods 0.000 description 1
- 239000000686 essence Substances 0.000 description 1
- 238000005530 etching Methods 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 229910021389 graphene Inorganic materials 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- MRNHPUHPBOKKQT-UHFFFAOYSA-N indium;tin;hydrate Chemical compound O.[In].[Sn] MRNHPUHPBOKKQT-UHFFFAOYSA-N 0.000 description 1
- 238000001755 magnetron sputter deposition Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000002715 modification method Methods 0.000 description 1
- 229920000867 polyelectrolyte Polymers 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 238000005118 spray pyrolysis Methods 0.000 description 1
- 230000003746 surface roughness Effects 0.000 description 1
- 238000004381 surface treatment Methods 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 229930192474 thiophene Natural products 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
Classifications
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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
- H10K30/82—Transparent electrodes, e.g. indium tin oxide [ITO] electrodes
-
- 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
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/549—Organic PV cells
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- Physics & Mathematics (AREA)
- Electromagnetism (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Photovoltaic Devices (AREA)
Abstract
The invention discloses an AZO composite transparent electrode which is decorated by an ultra-thin aluminium film and an organic solar cell which is manufactured by the transparent electrode. In high vacuum, a thin film deposition technology is used for depositing a layer of ultra-thin aluminium film on an AZO substrate, so that the work function of AZO conducting glass is adjusted, and the AZO substrate is made to be a negative electrode for collecting electrons. The thickness of the ultra-thin aluminium film is about 0.5-5nm. According to the composite transparent electrode and the organic solar cell including the composite transparent electrode, AZO is used for replacing traditional conducting glass ITO, the cost of the devices is lowered, and meanwhile an ultra-thin aluminium film electrode decorating layer is used so that complex electrode decorating materials can be avoided. The process is relatively simple, and mass production can be achieved easily.
Description
Technical field
The invention belongs to organic photovoltaic devices field is and in particular to a kind of AZO composite transparent electrode modified of ultra-thin aluminium film
And the transconfiguration organic solar batteries prepared by this transparency electrode.
Background technology
Tin indium oxide（ITO）It is organic solar batteries transparent electrode material widely used at present.But it is as market
The continuous expansion of demand, the global provisioning shortage of indium, people are continuously searching for replace ITO as the material of transparency electrode
Material, such as CNT, Graphene, metal-oxide etc..ZnO doping the 3rd major element（Al, Ga）Have been investigated as
The transparent conductive oxide of low cost.ZnO is a kind of width gap（3.3eV）N-type semiconductor, can by laser pulse sink
The method preparation such as long-pending, chemical vapor deposition, spray pyrolysis and magnetron sputtering.ZnO doping Al（AZO）There is higher conductance
Rate, near-infrared and visible region transmitance are higher, therefore show good application prospect in organic solar batteries.
Transparent hearth electrode that the organic solar batteries of traditional structure comprise a hole collection and electronics are collected
Top electrode.Hearth electrode is generally by poly- 3,4- ethylene oxide,1,2-epoxyethane thiophene：Poly-（P styrene sulfonic acid）Root anion（PEDOT:PSS）Thin film is repaiied
Decorations.Due to PEDOT:PSS itself has stronger acidity, understands etching conductive oxide surface so as to surface roughness increases,
Series resistance is led to increase, device efficiency reduces.Additionally, traditional structure device adopts the metal of low work content as top electrode, pole
It easily aoxidizes, and reduces the stability of device.The appearance of transconfiguration device solves the problems, such as above.Transconfiguration device
It is critical only that to set up a low work content can promote electronics collect hearth electrode.The method generally adopting is that hearth electrode is entered
Row is modified so as to become the negative electrode collecting electronics.At present, the cathodic modification method improving electronics collection is mainly in electrically conducting transparent
Deposited semiconductor metal-oxide on substrate, such as ZnO, TiOx.In some document reports, also someone adopts ultra-thin insulating barrier
（As Cs2CO3, PEO）To modify ITO with conjugated polyelectrolytes to reduce its work content.However, the modification of negative electrode can make device prepare
Process complications, increased the preparation cost of device, are unfavorable for realizing industrialization.Reduce device preparation cost further, simplify
Preparation technology, improves the stability of device, is the key of organic photovoltaic devices industrialization.
Content of the invention
In consideration of it, it is an object of the invention to provide a kind of AZO composite transparent electrode of ultra-thin aluminium film modification, it is not only
Relatively costly ITO electrode is replaced using AZO, ultra-thin aluminium film modification process is simple simultaneously, low cost.
For realizing above goal of the invention, the present invention employs the following technical solutions：
In one embodiment it is proposed that a kind of method preparing the AZO composite transparent electrode that ultra-thin aluminium film is modified, including
Following steps：
（1）AZO transparent conducting glass is used successively acetone, ethanol, deionized water are cleaned by ultrasonic, nitrogen is placed in electricity after drying up
Dry in hot blast drying baker；
(2) described AZO glass is put in vacuum coating equipment, using the aluminium wire more than 99.999% for the purity as evaporation source,
To cavity evacuation, when vacuum reaches 2 × below 10-4Pa, ultra-thin aluminium film is deposited with the speed of 0.3A/s；
Wherein, the thickness of aluminium film is monitored by thickness monitoring instrument, and the thickness adjusting aluminium film is to change AZO composite transparent electrode
Work function so as to and organic material level-density parameter.
In another embodiment it is proposed that a kind of AZO composite transparent electricity modified by ultra-thin aluminium film prepared by said method
Pole, described composite transparent electrode is made up of substrate of glass, AZO conductive film and ultra-thin aluminium film.
In another embodiment it is proposed that a kind of prepare the organic of the AZO composite transparent electrode comprising that ultra-thin aluminium film is modified
The method of solar cell device, comprises the following steps：
（1）Active layer material is dissolved in 1 milliliter of o-dichlorohenzene solvent, 60 DEG C of stirrings on magnetic stirring apparatuss fully, make
It is completely dissolved, using front with 0.22 micron of filtration membrane filtration；
（2）The ultra-thin aluminium film of predetermined thickness is deposited on AZO transparent conducting glass, afterwards directly spin coating according to the method described above
Active layer, adopts sol evenning machine to rotate 30s with 600 revs/min of rotating speed, puts into solvent anneal in culture dish afterwards until active layer
Thin film becomes dry, and measures active layer thickness with surface profiler；
（3）The substrate of active for spin coating layer is placed on warm table, 150 DEG C of heating anneals ten minutes, makes Donor acceptor
Material forms and is effectively separated；
（4）It is deposited with MoO successively in vacuum coating equipment3With Al electrode, thickness respectively 25nm and 100nm, final preparation
Going out device architecture is the ultra-thin aluminium film/active layer/MoO of AZO/3The solar cell device of/Al.
Compared with prior art, the technique effect of the present invention is embodied in：
（1）AZO transparency electrode of the present invention can be bought in market, also can prepare laboratory, wide material sources.
（2）Ultra-thin aluminium film method of modifying process is simple proposed by the invention, can prepare, no after AZO deposition immediately
Need any surface treatment, easily realize volume to volume and continuously produce, transconfiguration device is prepared with this electrode simultaneously, it is to avoid adopt
With complicated electrode modification layer, simplify device preparation technology.
（3）AZO composite transparent electrode in the present invention can change its work function by adjusting the thickness of ultra-thin aluminium film, from
And make itself and organic material level-density parameter, advantageously promote transmission and the collection of electronics.
（4）Transconfiguration organic solar batteries are prepared for hearth electrode with AZO composite transparent electrode proposed by the present invention, keeps away
Exempt from using acid PEDOT:PSS and the metal of low work content, improve the stability of device.
Brief description
Fig. 1 is the structural representation of the AZO composite transparent electrode that ultra-thin aluminium film of the present invention is modified.
Fig. 2 is the organic solar batteries of preparation in embodiment 2-7 and comparative example 1 in 100mW/cm2Xenon lamp irradiates lower survey
The photovoltaic property curve obtaining.
Fig. 3 is the transmission of the AZO thin film in the AZO laminated film and comparative example 1 that in embodiment 2-7, ultra-thin aluminium film is modified
Rate.
Fig. 4 is embodiment 8 and comparative example 2, and in 3, the organic solar batteries of preparation are in 100mW/cm2Xenon lamp irradiates lower survey
The photovoltaic property curve obtaining.
Specific embodiment
The organic solar batteries device coordinating accompanying drawing and its specific embodiment to this combination electrode below and comprising this electrode
Part elaborates.It should be appreciated that such description is only used for illustrating the purpose of the present invention, rather than limit.
Referring to Fig. 1, this combination electrode specifically includes substrate of glass 1, AZO conductive film 2 and ultra-thin aluminium film decorative layer 3.
The present invention is modified to AZO transparency electrode using ultra-thin aluminium film, adjusts its work content, and wherein ultra-thin aluminium film can be splashed by magnetic control
Penetrate, electron beam evaporation, the preparation of the method such as thermal evaporation.The following detailed description of the concrete reality preparing this combination electrode with thermal evaporation techniques
Apply example, to be better understood from present invention.
Embodiment 1：Thermal evaporation techniques prepare the AZO composite transparent electrode that ultra-thin aluminium film is modified
AZO transparent conducting glass employed in the present embodiment is to be bought by Shenzhen Jing Weite Science and Technology Ltd..To purchase
The AZO glass bought is placed in beaker, uses acetone, ethanol, deionized water to be cleaned by ultrasonic successively, nitrogen is placed in electric heating air blast after drying up
Dry stand-by in drying baker.AZO glass is put in vacuum coating equipment, using the aluminium wire more than 99.999% for the purity as evaporation
Source, to cavity evacuation, when vacuum reaches 2 × 10-4During below Pa, ultra-thin aluminium film is deposited with the speed of 0.3A/s.Aluminium film
Thickness is monitored by thickness monitoring instrument.Change the work function of AZO composite transparent electrode by adjusting the thickness of ultra-thin aluminium film, make
Itself and organic material level-density parameter.In this specific embodiment, the THICKNESS CONTROL of ultra-thin aluminium film is 0.5～5nm.In addition, in aluminum
Before film deposition, AZO substrate need not any be surface-treated, and such as oxygen plasma is processed, UV ozone is processed etc..
In the examples below, the invention still further relates to the AZO composite transparent electrode modified using described ultra-thin aluminium film is the bottom of as
Electrode（Negative electrode）Prepare transconfiguration organic solar batteries device.Described organic solar batteries include composite transparent electrode,
Photoactive layer and top electrode.Wherein, the active layer material that embodiment 2-7 adopts is P3HT:PCBM, the work that embodiment 8 adopts
Property layer material be P3HT:ICBA.It should also be appreciated by one skilled in the art that various unit types are only shown used in embodiment
Example, is not intended to limit the present invention.
Embodiment 2：Organic solar batteries device is prepared with the AZO that the ultra-thin aluminium film of 0.5nm is modified
The polymer solar battery that the present invention provides specifically includes composite transparent electrode, photoactive layer and top electrode,
Its preparation method is as follows：By 20 milligrams of P3HT（Laboratory synthesizes）With 16 milligrams of PCBM（Version and science and technology）It is dissolved in 1 milliliter after mixing
In o-dichlorohenzene solvent, on magnetic stirring apparatuss, 60 DEG C are stirred fully so as to be completely dissolved, using front with 0.22 micron of filtration
Membrane filtration.According to the method in embodiment 1, the ultra-thin aluminium film of 0.5nm is deposited on AZO transparent conducting glass, directly spin coating is lived afterwards
Property layer.Using sol evenning machine（KW-4A）Low speed spin coating, rotates 30s with 600 revs/min of rotating speed, puts into solvent in culture dish afterwards
Until active layer film becomes dry, thickness is measured with TENCOR ALFA-STEP-500 surface profiler, and thickness is about for annealing
200nm.The substrate of active for spin coating layer is placed on warm table, 150 DEG C of heating anneals ten minutes, makes Donor acceptor material shape
Become effectively to be separated.It is deposited with MoO afterwards successively in vacuum coating equipment3With Al electrode, thickness respectively 25nm and 100nm.
Finally preparing device architecture is AZO/Al（0.5nm）/P3HT:PCBM/MoO3The solar cell device of/Al.This was prepared
Cheng Jun completes in nitrogen environment.The photovoltaic property curve of device is to be recorded by a keithley2400 digital sourcemeter.AM1.5
Sunlight by 300W xenon arc lamp solar simulator provide, by a silicon substrate reference cell, it is corrected, makes light
It is by force 100mW/cm2.Organic solar batteries device in the present embodiment is in 100mW/cm2Performance parameter under xenon lamp irradiation is such as
Shown in Fig. 2 and Biao 1.
Embodiment 3：Organic solar batteries device is prepared with the AZO that the ultra-thin aluminium film of 1nm is modified
By 20 milligrams of P3HT（Laboratory synthesizes）With 16 milligrams of PCBM（Version and science and technology）It is dissolved in 1 milliliter of o-dichlorohenzene after mixing
In solvent, on magnetic stirring apparatuss, 60 DEG C are stirred fully so as to be completely dissolved, using front with 0.22 micron of filtration membrane filtration.
According to the method in embodiment 1, the ultra-thin aluminium film of 1nm is deposited on AZO transparent conducting glass, afterwards direct spin coating active layer.Using
Sol evenning machine（KW-4A）Low speed spin coating, rotates 30s with 600 revs/min of rotating speed, put into solvent anneal in culture dish afterwards until
Active layer film becomes dry, and thickness is measured with TENCOR ALFA-STEP-500 surface profiler, and thickness is about 200nm.To revolve
The substrate scribbling active layer is placed on warm table, 150 DEG C of heating anneals ten minutes, makes Donor acceptor material form effective phase
Separate.It is deposited with MoO afterwards successively in vacuum coating equipment3With Al electrode, thickness respectively 25nm and 100nm.Finally prepare
Device architecture is AZO/Al（1nm）/P3HT:PCBM/MoO3The solar cell device of/Al.This preparation process is all in nitrogen ring
Complete in border.Organic solar batteries device in the present embodiment is in 100mW/cm2Xenon lamp irradiate lower performance parameter such as Fig. 2 with
Shown in table 1.
Embodiment 4：Organic solar batteries device is prepared with the AZO that the ultra-thin aluminium film of 1.5nm is modified
By 20 milligrams of P3HT（Laboratory synthesizes）With 16 milligrams of PCBM（Version and science and technology）It is dissolved in 1 milliliter of o-dichlorohenzene after mixing
In solvent, on magnetic stirring apparatuss, 60 DEG C are stirred fully so as to be completely dissolved, using front with 0.22 micron of filtration membrane filtration.
According to the method in embodiment 1, the ultra-thin aluminium film of 1.5nm is deposited on AZO transparent conducting glass, afterwards direct spin coating active layer.Adopt
Use sol evenning machine（KW-4A）Low speed spin coating, rotates 30s with 600 revs/min of rotating speed, puts into solvent anneal in culture dish afterwards straight
Become dry to active layer film, thickness is measured with TENCOR ALFA-STEP-500 surface profiler, and thickness is about 200nm.Will
The substrate of the active layer of spin coating is placed on warm table, 150 DEG C of heating anneals ten minutes, so that Donor acceptor material is formed effectively
It is separated.It is deposited with MoO afterwards successively in vacuum coating equipment3With Al electrode, thickness respectively 25nm and 100nm.Final preparation
Going out device architecture is AZO/Al（1.5nm）/P3HT:PCBM/MoO3The solar cell device of/Al.This preparation process is all in nitrogen
Compression ring completes in border.Organic solar batteries device in the present embodiment is in 100mW/cm2Performance parameter under xenon lamp irradiation is such as
Shown in Fig. 2 and Biao 1.
Embodiment 5：Organic solar batteries device is prepared with the AZO that the ultra-thin aluminium film of 2nm is modified
By 20 milligrams of P3HT（Laboratory synthesizes）With 16 milligrams of PCBM（Version and science and technology）It is dissolved in 1 milliliter of o-dichlorohenzene after mixing
In solvent, on magnetic stirring apparatuss, 60 DEG C are stirred fully so as to be completely dissolved, using front with 0.22 micron of filtration membrane filtration.
According to the method in embodiment 1, the ultra-thin aluminium film of 2nm is deposited on AZO transparent conducting glass, afterwards direct spin coating active layer.Using
Sol evenning machine（KW-4A）Low speed spin coating, rotates 30s with 600 revs/min of rotating speed, put into solvent anneal in culture dish afterwards until
Active layer film becomes dry, and thickness is measured with TENCOR ALFA-STEP-500 surface profiler, and thickness is about 200nm.To revolve
The substrate scribbling active layer is placed on warm table, 150 DEG C of heating anneals ten minutes, makes Donor acceptor material form effective phase
Separate.It is deposited with MoO afterwards successively in vacuum coating equipment3With Al electrode, thickness respectively 25nm and 100nm.Finally prepare
Device architecture is AZO/Al（2nm）/P3HT:PCBM/MoO3The solar cell device of/Al.This preparation process is all in nitrogen ring
Complete in border.Organic solar batteries device in the present embodiment is in 100mW/cm2Performance parameter such as Fig. 2 under xenon lamp irradiation
With shown in table 1.
Embodiment 6：Organic solar batteries device is prepared with the AZO that the ultra-thin aluminium film of 2.5nm is modified
By 20 milligrams of P3HT（Laboratory synthesizes）With 16 milligrams of PCBM（Version and science and technology）It is dissolved in 1 milliliter of o-dichlorohenzene after mixing
In solvent, on magnetic stirring apparatuss, 60 DEG C are stirred fully so as to be completely dissolved, using front with 0.22 micron of filtration membrane filtration.
According to the method in embodiment 1, the ultra-thin aluminium film of 2.5nm is deposited on AZO transparent conducting glass, afterwards direct spin coating active layer.Adopt
Use sol evenning machine（KW-4A）Low speed spin coating, rotates 30s with 600 revs/min of rotating speed, puts into solvent anneal in culture dish afterwards straight
Become dry to active layer film, thickness is measured with TENCOR ALFA-STEP-500 surface profiler, and thickness is about 200nm.Will
The substrate of the active layer of spin coating is placed on warm table, 150 DEG C of heating anneals ten minutes, so that Donor acceptor material is formed effectively
It is separated.It is deposited with MoO afterwards successively in vacuum coating equipment3With Al electrode, thickness respectively 25nm and 100nm.Final preparation
Going out device architecture is AZO/Al（2.5nm）/P3HT:PCBM/MoO3The solar cell device of/Al.This preparation process is all in nitrogen
Compression ring completes in border.Organic solar batteries device in the present embodiment is in 100mW/cm2Performance parameter under xenon lamp irradiation is such as
Shown in Fig. 2 and Biao 1.
Embodiment 7：Organic solar batteries device is prepared with the AZO that the ultra-thin aluminium film of 3nm is modified
By 20 milligrams of P3HT（Laboratory synthesizes）With 16 milligrams of PCBM（Version and science and technology）It is dissolved in 1 milliliter of o-dichlorohenzene after mixing
In solvent, on magnetic stirring apparatuss, 60 DEG C are stirred fully so as to be completely dissolved, using front with 0.22 micron of filtration membrane filtration.
According to the method in embodiment 1, the ultra-thin aluminium film of 3nm is deposited on AZO transparent conducting glass, afterwards direct spin coating active layer.Using
Sol evenning machine（KW-4A）Low speed spin coating, rotates 30s with 600 revs/min of rotating speed, put into solvent anneal in culture dish afterwards until
Active layer film becomes dry, and thickness is measured with TENCOR ALFA-STEP-500 surface profiler, and thickness is about 200nm.To revolve
The substrate scribbling active layer is placed on warm table, 150 DEG C of heating anneals ten minutes, makes Donor acceptor material form effective phase
Separate.It is deposited with MoO afterwards successively in vacuum coating equipment3With Al electrode, thickness respectively 25nm and 100nm.Finally prepare
Device architecture is AZO/Al（3nm）/P3HT:PCBM/MoO3The solar cell device of/Al.This preparation process is all in nitrogen ring
Complete in border.Organic solar batteries device in the present embodiment is in 100mW/cm2Xenon lamp irradiate lower performance parameter such as Fig. 2 with
Shown in table 1.
Comparative example 1：Organic solar batteries are prepared for hearth electrode with AZO
The AZO glass of purchase is placed in beaker, uses acetone, ethanol, deionized water to be cleaned by ultrasonic, after nitrogen dries up successively
Be placed in electric drying oven with forced convection dry stand-by.By 20 milligrams of P3HT（Laboratory synthesizes）With 16 milligrams of PCBM（Version and science and technology）Mixed
Be dissolved in after conjunction in 1 milliliter of o-dichlorohenzene solvent, on magnetic stirring apparatuss 60 DEG C of stirrings fully so as to be completely dissolved, using front with
0.22 micron of filtration membrane filtration.Spin coating active layer material on the AZO electro-conductive glass dried.Using sol evenning machine（KW-4A）Low
Fast spin coating, rotates 30s with 600 revs/min of rotating speed, puts into solvent anneal in culture dish afterwards until thin film becomes dry, thickness is used
TENCOR ALFA-STEP-500 surface profiler measures, and thickness is about 200nm.The substrate of active for spin coating layer is placed on
On warm table, 150 DEG C of heating anneals ten minutes, so that Donor acceptor material is formed and be effectively separated.Afterwards in vacuum coating equipment
In be deposited with MoO successively3With Al electrode, thickness respectively 25nm and 100nm.Finally preparing device architecture is AZO/P3HT:
PCBM/MoO3The solar cell device of/Al.This preparation process all completes in nitrogen environment.In this comparative example organic too
Sun energy battery device is in 100mW/cm2Performance parameter under xenon lamp irradiation is as shown in Figure 2 and Table 1.
Fig. 2 is the organic solar batteries of preparation in embodiment 2-7 and comparative example 1 in 100mW/cm2Xenon lamp irradiates lower survey
The photovoltaic property curve obtaining, its corresponding device parameters is as shown in table 1.Found out by Fig. 2, after adding ultra-thin aluminium film, the opening of device
Road voltage, short circuit current and fill factor, curve factor are all greatly improved, so that the energy conversion efficiency of device is improved by 0.52%
To 3% about.When aluminium film thickness is 0.5nm, the efficiency of device has reached maximum 3.34%, afterwards with aluminium film thickness
Increase, device efficiency reduction by a small margin, when thickness is for 3nm, the efficiency of device remains at 3% about.
The performance parameter of the organic solar batteries of table 1 embodiment 2-7 and comparative example 1 preparation
Fig. 3 is the transmission of the AZO thin film in the AZO laminated film and comparative example 1 that in embodiment 2-7, ultra-thin aluminium film is modified
Rate.Shown by figure, with the increase of ultra-thin aluminium film thickness, the absorbance of laminated film is gradually lowered, but in long wave length direction
Absorbance is still more than 90%.
Embodiment 8 active layer is P3HT:The preparation of the organic solar batteries device of ICBA
Concrete preparation method is as follows：By 17 milligrams of P3HT（Laboratory synthesizes）With 17 milligrams of ICBA（Version and science and technology）After mixing
It is dissolved in 1 milliliter of o-dichlorohenzene solvent, on magnetic stirring apparatuss, 60 DEG C are stirred fully so as to be completely dissolved, using front with 0.22
The filtration membrane filtration of micron.According to the method in embodiment 1,0.5nm is deposited on AZO transparency electrode（Optimal thickness）Ultra-thin
Aluminium film, direct spin coating active layer afterwards.Using sol evenning machine（KW-4A）Low speed spin coating, rotates 30s with 600 revs/min of rotating speed,
Put into solvent anneal in culture dish afterwards until active layer film becomes dry, thickness TENCOR ALFA-STEP-500 surface profile
Instrument measures, and thickness is about 220nm.The substrate of active for spin coating layer is placed on warm table, 150 DEG C of heating anneals are very
Clock, makes Donor acceptor material be formed and is effectively separated.It is deposited with MoO afterwards successively in vacuum coating equipment3With Al electrode, thickness
It is respectively 25nm and 100nm.Organic solar batteries device in the present embodiment is in 100mW/cm2Performance under xenon lamp irradiates is joined
Number is as shown in Fig. 4 and Biao 2.
Comparative example 2 comparative device ITO/PEDOT:PSS/P3HT:The preparation of ICBA/Al
Comparative example 2 be with ITO as hearth electrode, PEDOT:The formal structure organic solar that PSS is prepared for hole transmission layer
Battery, its concrete preparation process is as follows：Ito glass is placed in beaker, uses organic washing agent, acetone, ethanol, deionization successively
Water be cleaned by ultrasonic, nitrogen be placed in after drying up dry in electric drying oven with forced convection stand-by.Using front, oxygen plasma is carried out to ITO
Process 5min.Using PEDOT:PSS hole transmission layer（Purchased from Baytron company）ITO surface is modified, uses sol evenning machine
（KW-4A）High speed spin coating, rotating speed is 2500 revs/min, and thickness is measured with TENCOR ALFA-STEP-500 surface profiler, thick
Degree is about 40nm.Afterwards substrate is put into 120 DEG C of annealing 30min in electric drying oven with forced convection, with eliminating water post bake.By 17 milligrams
P3HT（Laboratory synthesizes）With 17 milligrams of ICBA（Version and science and technology）It is dissolved in after mixing in 1 milliliter of o-dichlorohenzene solvent, stir in magnetic force
Mix on device 60 DEG C of stirrings fully so as to be completely dissolved, using front with 0.22 micron of filtration membrane filtration.In PEDOT:PSS modifies
ITO surface spin coating active layer material, using sol evenning machine（KW-4A）Low speed spin coating, rotates 2 points with 600 revs/min of rotating speed
Clock, thickness is about 200nm.Evaporating Al electrode in vacuum coating equipment afterwards, thickness is 100nm.The device preparing is entered
Row after annealing, places it on warm table, and 150 DEG C are heated 10 minutes, so that Donor acceptor material is formed and are effectively separated.This
Organic solar batteries device in comparative example is in 100mW/cm2Performance parameter under xenon lamp irradiation is as shown in Fig. 4 and Biao 2.
Comparative example 3 comparative device ITO/Al/P3HT:ICBA/MoO3The preparation of/Al
Comparative example 3 is the transconfiguration organic solar batteries that the ITO being modified with ultra-thin aluminium film is prepared for hearth electrode, its tool
Production procedure is as follows：Ito glass is placed in beaker, uses organic washing agent, acetone, ethanol, deionized water ultrasonic clear successively
Wash, nitrogen be placed in after drying up dry in electric drying oven with forced convection stand-by.Ito glass is put in vacuum coating equipment, big with purity
Aluminium wire in 99.999% as evaporation source, to cavity evacuation, when vacuum reaches 2 × below 10-4Pa, with 0.3A/s
Speed be deposited with 0.5nm ultra-thin aluminium film.By 17 milligrams of P3HT (laboratory synthesis) and 17 milligrams of ICBA (version and science and technology) mixing
After be dissolved in 1 milliliter of o-dichlorohenzene solvent, on magnetic stirring apparatuss 60 DEG C of stirrings fully so as to be completely dissolved, using front with
0.22 micron of filtration membrane filtration.The ITO surface spin coating active layer modified in aluminium film using sol evenning machine (KW-4A), with 600 turns/
The rotating speed rotation 30s of minute, puts into solvent anneal in culture dish afterwards until thin film becomes dry, thickness TENCOR ALFA-
STEP-500 surface profiler measures, and thickness is about 220nm.The substrate of active for spin coating layer is placed on warm table, 150
DEG C heating anneal ten minutes, makes Donor acceptor material be formed and is effectively separated.It is deposited with successively in vacuum coating equipment afterwards
MoO3With Al electrode, thickness respectively 25nm and 100nm.Organic solar batteries device in this comparative example is in 100mW/cm2Xenon
Performance parameter under light irradiation is as shown in Fig. 4 and Biao 2.
Shown by Fig. 4, comparative example 1 is the formal structure organic solar batteries with ITO as hearth electrode, its efficiency only has
3.67%, and the transconfiguration device of the ITO preparation that comparative example 2 is modified with ultra-thin aluminium film, efficiency has reached 3.99%, has mainly returned
Because in the raising of open-circuit voltage（0.76V has been brought up to by 0.71V）.After using AZO replacement ITO as hearth electrode, embodiment 8
In device open-circuit voltage to be maintained at 0.76V constant, and short circuit current and fill factor, curve factor improve, and final efficiency reaches
4.38%.
The performance parameter of the organic solar batteries of table 2 embodiment 8 and comparative example 2,3 preparation
The foregoing is only presently preferred embodiments of the present invention, not in order to limit the present invention, all essences in the present invention
Any modification, equivalent and improvement made within god and principle etc., should be included within the scope of the present invention.
Claims (4)
1. a kind of method preparing the organic solar batteries device of AZO composite transparent electrode comprising ultra-thin aluminium film modification, bag
Include following steps：
(1) active layer material is dissolved in 1 milliliter of o-dichlorohenzene solvent, on magnetic stirring apparatuss, 60 DEG C of stirrings are fully so as to complete
CL, using front with 0.22 micron of filtration membrane filtration；
(2) deposit on AZO transparent conducting glass according to the method preparing the AZO composite transparent electrode that ultra-thin aluminium film is modified and make a reservation for
Thickness is the ultra-thin aluminium film of 0.5～5nm, afterwards direct spin coating active layer, adopts sol evenning machine to rotate with 600 revs/min of rotating speed
30s, puts into solvent anneal in culture dish afterwards until active layer film becomes dry, measures active layer thickness with surface profiler；
Wherein, the described method preparing the AZO composite transparent electrode that ultra-thin aluminium film is modified comprises the following steps：(A) AZO is transparent
Electro-conductive glass uses acetone, ethanol, deionized water to be cleaned by ultrasonic successively, and nitrogen is placed in after drying up in electric drying oven with forced convection and dries；
(B) described AZO transparent conducting glass is put in vacuum coating equipment, using the aluminium wire more than 99.999% for the purity as evaporation source,
To cavity evacuation, when vacuum reaches 2 × 10-4During below Pa, ultra-thin aluminium film is deposited with the speed of 0.3A/s；Wherein, in aluminum
Before film deposition, AZO substrate is processed without other surfaces, and the thickness of aluminium film is monitored by thickness monitoring instrument, adjusts the thickness of aluminium film
Degree with change the work function of AZO composite transparent electrode so as to and organic material level-density parameter；
(3) substrate of active for spin coating layer is placed on warm table, 150 DEG C of heating anneals ten minutes, makes Donor acceptor material
Formed and be effectively separated；
(4) it is deposited with MoO in vacuum coating equipment successively3With Al electrode, thickness respectively 25nm and 100nm, finally prepare device
Structure is the ultra-thin aluminium film/active layer/MoO of AZO/3The solar cell device of/Al.
2. the method preparing organic solar batteries device according to claim 1, wherein, described active layer material is 20
Measuring active layer thickness with surface profiler in milligram P3HT and 16 milligram of PCBM, and, described step (2) is 200nm.
3. the method preparing organic solar batteries device according to claim 2, wherein, described active layer material is 17
Measuring active layer thickness with surface profiler in milligram P3HT and 17 milligram of ICBA, and, described step (2) is 220nm.
4. a kind of organic solar batteries device of method preparation any one of claim 1-3, including hearth electrode, work
Property layer and top electrode, wherein, hearth electrode is the AZO composite transparent electrode that described ultra-thin aluminium film is modified.
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| CN103137881A (en) * | 2011-11-22 | 2013-06-05 | 海洋王照明科技股份有限公司 | Organic electroluminescent device and production method thereof |
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| Efficient and ultraviolet durable inverted organic solar cells based on an aluminum-doped zinc oxide transparent cathode;Hanxiao Liu，et al.;《Applied Physics Letters》;20130725;第103卷(第4期);page 043309-1-4 * |
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