CN101521261B - Novel organic solar cell producing free carriers based on interface recombination - Google Patents
Novel organic solar cell producing free carriers based on interface recombination Download PDFInfo
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Abstract
The invention provides a novel organic solar cell producing free carriers based on interface recombination, which comprises the following functional layers according to connection sequence: a transparent anode, anode buffer layer materials added according to requirements, an organic cavity transmission layer connected with the anode (connected with an anode buffer layer in case that the anode buffer layer exists), an organic electron transmission layer connected with an cathode (connected with a cathode buffer layer in case that the cathode buffer layer exists), cathode buffer layer materials added according to requirements and the cathode. Completely differing from a P-N section type solar cell which obtains free carriers by interface split, the invention produces the free carriers by theexciton recombination on the interface and has higher energy transfer efficiency, wherein the organic semiconductor material can be micromolecule or polymer.
Description
Technical field
The present invention relates to organic electro-optic device, be specially adapted to organic solar batteries.
Background technology
Solar cell is that the transform light energy with solar radiation is the device of electric energy.Solar cell is used for providing electric energy to load as electric light, computer etc.Also relate to apparatus for storing electrical energy in actual applications, could not have to provide electric energy continuously to load under the sunlit situation like this.Solar cell can produce photovoltaic response under the situation of illumination.Photovoltage is open circuit voltage (V under the situation of open circuit outside
OC), the electric current that obtains under the situation of short circuit is short circuit current (I outside
SC).Under loaded situation, the power output of solar cell equals the voltage landing (V) in the load and the product of the electric current (I) by load, and it is less than the product of open circuit voltage and short circuit current.The peak power output and the V of definition solar cell
OCI
SCRatio be fill factor, curve factor.
As its name suggests, organic solar batteries is exactly the solar cell that adopts the organic semiconducting materials preparation.At present the energy conversion efficiency of the best organic solar batteries of report is about 5%, the energy conversion efficiency of the organic solar batteries of lamination about 7%.The free carrier of these organic solar batteries is to obtain by the fractionation of exciton on the interface of forming for body (electron donor) and acceptor (electron acceptor) material.When illumination is mapped on the organic semiconducting materials, can form free carrier usually in the organic semiconductor, but form electron-hole pair (exciton) earlier.Utilize organic material to obtain photoelectric current these are split by the exciton that optical excitation obtains, otherwise these excitons will be sent out by radiation or radiationless mode de excitation.Interface with two kinds of organic materials (giving body and acceptor) of different level structures is considered to split the place of exciton, this by giving body (P-type material, the main charge carrier of material is the hole) and acceptor (n type material, the main charge carrier of material is an electronics) interface and the P/N in the inorganic solar cell that form save similar, such as the interface of CuPc (CuPc) and fullerene (C60) formation, as shown in Figure 1.In this structure, give the sub-occupied orbital of best result (HOMO) of body (CuPc) and minimum molecule not the energy of occupied orbital (LUMO) all than the HOMO and the LUMO height of corresponding acceptor (C60).Exciton is finished like this in the fractionation that the donor-receiver interface goes out: the electronics in the CuPc exciton stays the hole at the HOMO of CuPc in the LUMO of C60 injection, perhaps the hole in the C60 exciton stays electronics at the LUMO of C60 when the HOMO of CuPc injects.Why can produce such exciton split process is because the energy summation of free carrier (electronics among hole among the HOMO of CuPc and the LUMO of C60) is littler than the exciton energy summation before not splitting.Obtain useful electric current, these free carriers must be collected by electrode, and promptly anode is collected the hole, and negative electrode is collected electronics.In fact, exciton is at the interface except existing the above-mentioned split process of passing through to produce the free carrier, the possible approach that also has the charge carrier that gains freedom: the hole-recombination in electronics in the CuPc exciton and the C60 exciton stays hole and electronics freely freely respectively in CuPc and C60.But because the split process of exciton at the donor-receiver interface have overwhelming advantage, the process by the compound generation free carrier in interface has been left in the basket.
Summary of the invention
The present invention proposes a kind of interface that is different from and splits the novel organic solar cell that obtains free carrier, and it is by the compound free carrier that produces in interface.
Will produce measurable free carrier by the interface is compound, at first must suppress to split the quantity that produces free carrier by the interface as far as possible, this target can realize by careful selection combination organic semiconducting materials.Secondly, the free carrier by the compound acquisition in interface must reach as early as possible to be collected by electrode, otherwise produce between the free carrier compound will make measure infeasible.Because the generation of free carrier realizes that by the interface is compound therefore two kinds of materials at selected formation interface must have good absorption and the overlapping of absorption spectrum arranged in the visible region.
The present invention just is based on above consideration, has realized utilizing the compound free carrier that produces in interface, thereby has proposed a kind of novel organic solar cell based on the compound generation free carrier in interface, comprises following functional layer by the order of connection:
Transparent anode
The anode buffer layer material of Jia Ruing as required
The organic cavity transmission layer of (then linking to each other with this resilient coating if any anode buffer layer) links to each other with anode
The organic electron transport layer of (then linking to each other with this resilient coating if any cathode buffer layer) links to each other with negative electrode
The cathode cushioning layer material of Jia Ruing as required
Negative electrode
The HOMO of described organic cavity transmission layer and LUMO are lower than the HOMO and the LUMO of organic electron transport layer; Described anode work function is bigger than negative electrode work function.
Described cathode buffer layer is between organic electron transport layer and negative electrode, and anode buffer layer is between organic cavity transmission layer and anode.
Described hole transmission layer is F16ZnPc (perfluorinated hexadecafluoro-phthalocyanineatozinc), F16CuPc (perfluorinated hexadecafluoro-phthalocyaninatocopper), CuPc (Copper phthalocyanine) or ZnPc (Zincphthalocyanine); Described electron transfer layer is C60, PTCBI (3,4,9,10-perylenetetracarboxylic bis-benzimidazole) or pentacene.The thickness of organic cavity transmission layer and organic electron transport layer is suitable with its exciton diffusion length, in 10 nanometers between 100 nanometers.
Described cathode buffer layer is Alq3 (tris-8-hydroxy-quinolinato aluminum), PTCBI, BCP (bathocuproine) or CuPc, thickness in 1 nanometer between 10 nanometers.。Described anode buffer layer is NPB (N, N'-Bis (naphthalene-1-yl)-N, N'-bis (phenyl) benzidine) or TPD (triphenylamine dimer), thickness in 1 nanometer between 10 nanometers.
The organic solar batteries that the present invention proposes is different from fully in the P-N nodal pattern organic solar batteries and obtains free carrier by the interface fractionation, adopt a kind of brand-new operation principle, by compound the produce free carrier of exciton at the interface, have the higher-energy conversion efficiency, organic semiconducting materials wherein can be that micromolecule also can be a polymer.
Description of drawings
The structure of Fig. 1, conventional P-N nodal pattern organic solar batteries and energy level are arranged.
The structure of Fig. 2 N, novel N-N type organic solar batteries and energy level are arranged (containing cathode buffer layer).The production process of free carrier is in this battery: produce exciton by absorbing light in F16ZnPc and C60, exciton is diffused into the interface that is formed by F16ZnPc and C60, electronics in F16ZnPc exciton at the interface and the hole-recombination in the C60 exciton have discharged hole in the F16ZnPc exciton and the electronics in the C60 exciton makes them become free carrier, and these free carriers are collected by the electrode at two ends by diffusion and drift.
The structure of Fig. 2 P, novel P-P type organic solar batteries and energy level are arranged (containing cathode buffer layer).The production process of free carrier is in this battery: produce exciton by absorbing light in CuPc and pentacene, exciton is diffused into the interface that is formed by CuPc and pentacene, electronics in CuPc exciton at the interface and the hole-recombination in the pentacene exciton have discharged hole in the CuPc exciton and the electronics in the pentacene exciton makes them become free carrier, and these free carriers are collected by the electrode at two ends by diffusion and drift.
Fig. 3, the current-voltage curve of novel N-N organic solar batteries under illumination and dark attitude.
Fig. 4, the current-voltage curve of novel P-P organic solar batteries under illumination and dark attitude.
Fig. 5, quantum efficiency under light bias voltage and the unglazed bias voltage is being arranged at the N-N type novel organic solar cell that measures under 11 hertz the chopper frequencies.Measuring sequence is to measure the first time that does not have the light bias voltage, the ruddiness bias voltage is arranged, the green glow bias voltage is arranged and do not have measure the second time of light bias voltage.Do not have the measurement of light bias voltage to compare with the first time, do not have the second time quantum efficiency that the meter of light bias voltage has revealed a little to descend, this shows that device has the decay of a little in whole measuring process.Can find out clearly that in 400-530 nano waveband scope, quantum efficiency has bigger increase under the situation that the ruddiness bias voltage is arranged, and does not change substantially under the situation of green glow bias voltage.In addition, also measured quantum efficiency at wavelength under greater than the situation of 800 nanometers.
The F16ZnPc uv-visible absorption spectra of the C60 of 48 nanometers and 25 nanometers on Fig. 6, the calcirm-fluoride substrate.At the 400-530 nano waveband, the absorption of F16ZnPc is very little, and at same wave band C
60Absorption then bigger.
Fig. 7 a, has the novel organic solar cell level structure of anode buffer layer.
Fig. 7 b, has a novel organic solar cell level structure of anode buffer layer and cathode buffer layer simultaneously.
Embodiment
Fig. 2 N and 2P are depicted as the example of this organic solar batteries, and Fig. 3 has enumerated the correlated results of these example devices to Fig. 5.
Fig. 2 N and Fig. 2 P have provided based on compound structure and the energy level Rankine-Hugoniot relations that obtains the novel organic solar cell of free carrier in the employing interface of above-mentioned consideration.Here the material that links to each other with anode is called as hole transmission layer, and the material that links to each other with negative electrode then that links to each other with resilient coating is called as electron transfer layer.Obviously, under the energy level arranging situation shown in Fig. 2 N and Fig. 2 P, exciton is impossible in the fractionation at the interface of hole transmission layer and electron transfer layer formation.Do anode such as in Fig. 2 N, adopting tin indium oxide (ITO), F16ZnPc (a kind of n section bar material, its HOMO and LUMO be respectively-6.9eV and-5.2eV) do hole transmission layer, C60 (a kind of n section bar material, its HOMO and LUMO be respectively-6.2eV and-4.5eV) do electron transfer layer, cathode buffer layer is Alq3, and negative electrode is silver-colored Ag.The example of another one P-P type of the present invention is Fig. 2 P, adopt ITO to do anode, CuPc (a kind of P-type material, its HOMO and LUMO be respectively-5.2eV and-3.5eV) do hole transmission layer, pentacene (a kind of P-type material, its HOMO and LUMO be respectively-4.9eV and-3.0eV) do electron transfer layer, cathode buffer layer is Alq3, negative electrode is aluminium Al.
In Fig. 2 N and 2P, absorbed by hole transmission layer and electron transfer layer behind the light transmission ito glass, produce exciton (process among Fig. 2 N and the 2P is a)) in the both sides, interface of hole transmission layer and electron transfer layer formation.These excitons reach interface (the process b among Fig. 2 N and the 2P) by diffusion process).At the electronics of hole transmission layer one side with produce compoundly in the hole of electron transfer layer one side, the electronics of the hole of hole transmission layer one side and electron transfer layer one side discharged becomes free carrier (the process c among Fig. 2 N and the 2P) in these excitons).These freely hole and electronics under the effect of the internal electric field of setting up by the work function difference of two electrodes by diffusion and drift respectively and e) by anode and negative electrode collected (the process d among Fig. 2 N and the 2P)).Therefore in this class novel organic solar cell, half electric charge in the exciton is used to produce free carrier, and half is then compound disappearance the at the interface in addition.Traditional P-N nodal pattern organic solar batteries is then different, and exciton splits the generation free carrier makes the whole electric charges in the exciton all be used to produce free carrier.In fact in traditional P-N nodal pattern organic solar batteries, process by the compound charge carrier that gains freedom in interface also is same the existence, but, therefore can't in this quasi-tradition battery, observe free carrier by the compound generation in interface because that the effect that the interface splits is far longer than the interface is compound.
Our example solar cell shown in Fig. 2 N and the 2P of on the ito glass substrate that cleans up, growing.ITO thickness approximately
About 13 Ω of square resistance/square.Vacuum is about 1 * 10 during the evaporation organic material
-6Pa, the vacuum when evaporation negative electrode silver and aluminium is about 1 * 10
-5Pa.The ITO substrate is a room temperature during growth, and the growth rate of CuPc (Aldrich, 99%), C60 (Aldrich, 99.5%), F16ZnPc (Aldrich, 95%, purify through distillation once), pentacene (Aldrich, 99%) approximately
Alq3 (Aldrich, 99.95%) growth rate is about
The growth rate of silver and aluminium (Aldrich, 99.99%) approximately
The effective area of the battery for preparing is 4mm
2Measurement is to carry out under the solar simulator that Newport (Oriel) company produces.The I-V curve is measured with Keithley 2400.All measurements are all carried out under atmospheric environment.
The thickness of N-N type and P-P type device architecture and corresponding each layer is respectively: ITO/F16ZnPc (20nm)/C60 (55nm)/Alq3 (5nm)/Ag and ITO/CuPc (20nm)/pentacene (30nm)/Alq3 (5nm)/Al.The I-V curve of this device under the situation of illumination and unglazed photograph as shown in Figure 3 and Figure 4.When measuring quantum efficiency, the frequency of chopper is 11 hertz.All measuring under the situation of light bias voltage the light bias voltage being arranged and do not have respectively of quantum efficiency.
Fig. 3 is the current-voltage curve of novel N-N organic solar batteries.At 100mW/cm
2The irradiation of simulated solar under obtained open circuit voltage and 0.25mA/cm with respect to the 510mV of silver electrode
2Short circuit current.Because the hole collected by ITO, electronics is collected by silver electrode, from the level structure of Fig. 2 as can be seen, this battery free carrier compound rather than interface splits and obtains by the interface.When adding between the filter disc of sample and AM1.5G 560 nanometers by filter disc filter below 560 nanometers have a high-octane simulated solar after, this device still has 0.13mA/cm
2Short circuit current.Adopt still to have obtained bigger photoelectric current later on by filter disc and show that direct ionization is not the approach of charge carrier that gains freedom, be cut off filter disc and filtered because can produce the high-energy photons of direct ionization.Quantum efficiency measurement result among Fig. 5 shows that also free carrier does not derive from ionization process, because wavelength still has contribution to photoelectric current greater than the light (energy is 1.55 electron-volts) of 800 nanometers.
Fig. 4 is the current-voltage curve of novel P-P organic solar batteries under illumination and dark attitude.At 100mW/cm
2The irradiation of simulated solar under obtained open circuit voltage and 9.3 μ A/cm with respect to the 912mV of aluminium electrode
2Short circuit current.Because the hole collected by ITO, electronics is collected by the aluminium electrode, from the level structure of Fig. 2 as can be seen, this battery free carrier compound rather than interface splits and obtains by the interface.
In the battery of cascaded structure, also be that half electric charge in the exciton is used to produce photoelectric current.Different with series-connected cell, battery of the present invention directly falls in the compound charge recombination with half by exciton at the interface, and earlier exciton is split in secondary battery in series-connected cell, and half electric charge wherein is compound in the junction of two secondary batteries then.In series-connected cell, obtain bigger photoelectric current, the photoelectric current that just needs each secondary battery to produce is wanted quite.Therefore the present invention has converted the coupling of photoelectric current at both sides, interface exciton number coupling.Fig. 5 is the N-N type novel organic solar cell represented of Fig. 2 N to be had the light bias voltage and not to have quantum efficiency measurement result under the light bias condition.Can find out clearly that the contribution of photoelectric current derives from two kinds of n type materials.Under the situation of light bias voltage, it is corresponding that this device has shown the spectrum different with conventional P-N nodal pattern organic solar batteries: under the situation that the ruddiness bias voltage is arranged, bigger increase has appearred in the quantum efficiency of 400-530 nano waveband.And in conventional P-N nodal pattern battery, the light bias voltage makes the quantum efficiency of whole wave band measure reduction.According to the process of the compound generation free carrier in previously described interface, the measurement of the quantum efficiency of this device depends on fully that under the situation that does not have the light bias voltage incident monochromatic light is compound at the exciton and the interface subsequently of F16ZnPc and C60 generation.At the 300-400 nano waveband, because there are bigger absorption (referring to Fig. 6) in F16ZnPc and C60, therefore produced more exciton in the both sides, interface of F16ZnPc and C60 formation, the free carrier of the compound generation of more exciton has also just been arranged, therefore bigger in the quantum efficiency of this wave band.Therefore and at the 400-530 nano waveband, the absorption of the absorptance F16ZnPc of C60 is a lot of by force, and the exciton number in the both sides, interface that F16ZnPc and C60 form is unbalanced, thus photoelectric current just quantum efficiency is just smaller.Under the situation of ruddiness bias voltage, F16ZnPc is because the effect of ruddiness can just produce a large amount of excitons at the monochromatic light pre-irradiation, therefore the exciton that produces in C60 of monochromatic light has been increased greatly by compound chance, thereby has produced the increase in the quantum efficiency of 400-530 wave band.If the light bias voltage can not bring better exciton number balance and compounding machine to increase, quantum efficiency just can not obtain increasing so.From Fig. 5, can find, when the green glow that adopts 532 nanometers as the light bias voltage, because F16ZnPc is very weak so do not increase the balance of exciton in the both sides, interface in the absorption of this wavelength, the existence of green glow bias voltage so quantum efficiency not have yet and obtain increase.
Fig. 7 a and Fig. 7 b are respectively the novel organic solar cell level structures that has the novel organic solar cell level structure of anode buffer layer and have anode buffer layer and cathode buffer layer simultaneously.According to the analysis of the novel organic solar cell of Fig. 2 N and Fig. 2 P-structure and experimental measurements as can be known, thereby the battery with Fig. 7 a and Fig. 7 b structure also can reach and utilizes equally that the interface exciton is compound to produce the purpose that free carrier is realized opto-electronic conversion.
Claims (8)
1. based on the novel organic solar cell of the compound generation free carrier in interface, it is characterized in that comprising following functional layer by the order of connection:
Transparent anode
The organic cavity transmission layer that links to each other with anode
The organic electron transport layer that links to each other with negative electrode
Negative electrode
Sub-occupied orbital HOMO of the best result of described organic cavity transmission layer and minimum molecule not occupied orbital LUMO are all lower than the HOMO and the LUMO of organic electron transport layer; Described anode work function is bigger than negative electrode work function.
2. organic solar batteries according to claim 1 is characterized in that, is connected with anode buffer layer between described anode and organic cavity transmission layer.
3. organic solar batteries according to claim 1 is characterized in that, is connected by cathode buffer layer between described negative electrode and organic electron transport layer organic electron transport layer.
4. according to claim 1,2 or 3 described organic solar batteries, it is characterized in that the material of described organic cavity transmission layer adopts F16ZnPc, F16CuPc, CuPc or ZnPc; The material of described organic electron transport layer adopts C60, PTCBI or pentacene; The thickness of organic cavity transmission layer and organic electron transport layer is suitable with its exciton diffusion length, in 10 nanometers between 100 nanometers.
5. organic solar batteries according to claim 3 is characterized in that described cathode cushioning layer material adopts Alq3, PTCBI, BCP or CuPc, thickness in 1 nanometer between 10 nanometers.
6. organic solar batteries according to claim 2 is characterized in that described anode buffer layer material adopts NPB, TPD or metal oxide, thickness in 1 nanometer between 10 nanometers.
7. organic solar batteries according to claim 4 is characterized in that, described hole transmission layer and electron transfer layer are by the hierarchy of physical vapour deposition (PVD) or pass through hole transport and the electron transport material that the spin coating technique spin coating mixes.
8. the laminated organic solar cell that utilizes claim 1,2 or 3 described organic solar batteries to form is characterized in that, wherein has at least a secondary organic solar batteries to satisfy situation in the claim 1.
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| CN101877386A (en) * | 2010-06-04 | 2010-11-03 | 北京大学 | Universal solar battery based on mesoscopic optical structure |
| CN101882664B (en) * | 2010-06-13 | 2011-11-23 | 西南大学 | Organic solar cell with monolayer organic material as functional layer |
| KR101415822B1 (en) | 2010-06-29 | 2014-07-09 | 코오롱인더스트리 주식회사 | Polymer solar cell and method for manufacturing the same |
| JP2013058562A (en) * | 2011-09-07 | 2013-03-28 | Semiconductor Energy Lab Co Ltd | Photoelectric conversion device |
| CN103872247A (en) * | 2014-03-19 | 2014-06-18 | 太原理工大学 | Organic small-molecule photovoltaic device based on three-terminal electrode structure |
| CN104916781A (en) * | 2015-05-18 | 2015-09-16 | 中国华能集团清洁能源技术研究院有限公司 | Wideband solar cell adopting resonance energy transfer layer |
| CN105098079A (en) * | 2015-07-13 | 2015-11-25 | 电子科技大学 | Organic thin-film solar cell based on dual cathode buffer layers and preparation method of organic thin-film solar cell |
| CN106981574B (en) * | 2017-04-18 | 2019-07-05 | 浙江蓝绿新材料科技有限公司 | A kind of long-life perovskite photovoltaic cell and preparation method thereof |
| CN108258125B (en) * | 2018-01-30 | 2021-07-16 | 遵义师范学院 | Method for improving performance of novel organic solar cell of interface recombination generated current carrier |
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