CN103474576A - Organic solar cell and manufacturing method thereof - Google Patents
Organic solar cell and manufacturing method thereof Download PDFInfo
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- CN103474576A CN103474576A CN2013104637758A CN201310463775A CN103474576A CN 103474576 A CN103474576 A CN 103474576A CN 2013104637758 A CN2013104637758 A CN 2013104637758A CN 201310463775 A CN201310463775 A CN 201310463775A CN 103474576 A CN103474576 A CN 103474576A
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Abstract
The invention discloses an organic solar cell and a manufacturing method of the organic solar cell. The organic solar cell comprises a substrate, a first electrode, a first charge transferring layer, an optical activity layer, a second charge transferring layer and a second electrode, wherein the first electrode, the first charge transferring layer, the optical activity layer, the second charge transferring layer and the second electrode are sequentially located on one surface of the substrate, an antireflection layer is arranged on the other surface of the substrate and is provided with a first nanometer concave-convex structure, and the refractive index of the first nanometer concave-convex structure changes in a gradient mode in the incident light direction. The organic solar cell effectively improves photoelectric conversion efficiency, has a self-cleaning effect at the same time, and is simple in manufacturing process and suitable for large-scale industrial popularization and application.
Description
Technical field
The present invention relates to technical field of solar batteries, be specifically related to a kind of organic solar batteries and preparation method thereof.
Background technology
Along with constantly exhausting and environmental pollution day by day serious of main energy sources-fossil fuel (coal, oil, natural gas etc.), energy problem has become one of major issue that society faces.Thereby the sight of impelling the researcher turns to clean regenerative resource.Solar energy is because its " inexhaustible, nexhaustible " is a kind of " green " energy truly, and becomes the energy strategy of countries in the world government sustainable development.The solar cell used at present, mainly rely on the inorganic material such as silicon or rare metal alloy to make.
And organic solar batteries is the novel solar battery grown up the nineties in 20th century, it usings organic semiconductor as the active material of realizing opto-electronic conversion.Compare with inorganic solar cell, have that cost is low, thin thickness, quality is light, manufacturing process is simple, can make the outstanding advantages such as large area flexible device, thereby day by day caused people's concern.But simultaneously, the photoelectric conversion efficiency of organic solar batteries fails to surpass 10% always, therefore vast researcher is devoted to seek new method always and is improved its efficiency.And the method that improves the organic solar photoelectric conversion efficiency can be divided into the exploitation of two large class (1) new materials and the optimize and improve of application (2) structure generally.For structure optimization and improvement, fall into light technology (light trapping) and day by day cause people's attention.The main direction of studying that falls at present the light technology is aspect following three:
(1) anti-reflection structure realizes that light is anti-reflection;
(2) nanostructure realizes the surface plasma bulk effect;
(3) photonic crystal is realized Wave guide resonance.
In the sunken light Fabrication of nanostructures of organic solar batteries, nanometer embossing is one of the most frequently used technology.Nanometer embossing can be subdivided into the hard stamping technique of nanometer (Hard nanoimprint lithography; H-NIL) and the soft stamping technique of nanometer (Soft nanoimprint lithography; S-NIL).
2012, Dian Chen etc. delivered the paper (referring to the non-patent literature 1 of following explanation) of the application in organic solar batteries about hard nanometer embossing on ACSNANO.It is stay in place form that the utilization of this group has periodically anodised aluminium (AAO) sheet of nano-pore structure, prepares the periodicity P3HT nano-pillar that diameter is about 30nm on the P3HT film by hard stamping technique.PCBM and the electrode deposition on the P3HT film has completed the preparation of polymer-polymer nanocomposite structure heterojunction organic solar batteries device subsequently, and has obtained 2.4% device efficiency (referring to the non-patent literature 1 of following explanation).
Aspect the device antireflective film, Fang Jiao equals to have delivered related article in 2012 on Microelectronic Engineering.This group utilizes AAO for stay in place form, on the inorganic solar cell surface that scribbles ultra-violet curing glue, by hard nanometer embossing, has prepared the nanometer antireflection structure.The existence of antireflective film greatly reduces the incident light reflectivity of device, thus the raising of going up largely the efficiency of device (referring to the non-patent literature 2 of following explanation).
But hard nanometer embossing is based on the stamping technique of the hard templates such as quartz, glass, silicon chip, the use of rigid template in the organic material moulding process can cause air to be wrapped in the hole of template and substrate, thereby causes the structure dimension heterogeneity obtained in substrate; And rigid template generally has larger surface energy due to it, therefore can cause the damage of substrate film pattern in knockout course.In a word, the use of rigid template greatly reduces the fidelity of stamping structure.
2012, the PDMS that the use such as Jingbi You have the nanometer grating structure is stay in place form, by soft nanometer embossing toward copying nano optical grating construction on the PTB7:PC71BM active layer, the evaporation of silver electrode on graphical active layer obtained the back electrode with optical grating construction subsequently, this organic solar batteries with graphical back electrode has very strong back electrode scattering and surface plasma resonance to incident light, so its performance is than planar device tool have greatly improved (referring to the non-patent literature 3 of following explanation).
The Chinese patent that application number is 201110068868.1 discloses a kind of solar cell, this solar cell is in manufacturing process, prepare the metal nanometer thin film that one deck is comprised of the metal nano chain between back electrode of solar cell and photovoltaic layer, incident light is through light anode and photovoltaic layer, by local on metal nano chain surface, and the surface plasma excimer transmission mode of formation lateral transport, therefore the effective propagation path of incident light at photovoltaic layer increased substantially, thereby improve the absorption efficiency of solar cell to incident light, can significantly improve the photoelectric conversion efficiency of solar cell.But the shortcoming of this technology is: directly contact between metal nanometer thin film and photovoltaic layer, easily affect the electrical properties such as solar cell device resistance, open circuit voltage, fill factor, curve factor.
The Chinese invention patent that application number is 201110252280.1 discloses a kind of preparation method of the porous pyramid-type silicon surface light trapping structure for solar cell, after cleaning silicon chip, adopt alkaline etching to prepare the pyramid structure surface, and then make porous pyramid surface light trapping structure in conjunction with the method for noble metal nano particles catalysis etching, the silicon face porous pyramid-type light trapping structure of preparing by the method, dropped to 3.3% level at 300nm to its average reflectance in the spectral region of 1000nm, for the efficiency that improves silicon solar cell provides new technological means.But the shortcoming of this technology is: but its preparation method only is confined to silicon solar cell, is unsuitable for the making of organic solar batteries.
The Chinese invention patent that application number is 201210231569.X discloses in electron transfer layer and/or hole transmission layer and has been provided with metal nanoparticle, strengthened the absorption of light by the surface plasma bulk effect of metal nanoparticle, the photoelectric current of device is increased, thereby improved the electricity conversion of organic solar batteries device.But the shortcoming of this technology is: due to randomness and the uncontrollability of the distribution of metal nanoparticle, thus the unsteadiness that causes efficiency to improve, and the surface plasma bulk effect strengthens DeGrain near ultraviolet and visible light wave range.
The Chinese invention patent that application number is 201210257338.6 discloses a kind of organic thin film solar cell, by a plurality of battery cells compact arrangement on a plane, formed, battery cell be shaped as positive three face cones, positive four sides cone or positive six face cones, the medial surface of cone is sensitive surface, and each medial surface all comprises a battery unit.This technology has increased assembly to the absorbing of light, but the shortcoming of this technology is: cell inside is without light trapping structure, and the cone structure of monomer ABSORPTION AND SCATTERING light fully, has a light leak problem.
Reference listing:
Non-patent literature 1
1.Dian?Chen,Wei?Zhao,and?Thomas?P.Russell.,P3HT?Nanopillars?for?Organic?Photovoltaic?Devices?Nanoimprinted?by?AAO?Templates.ACSNano.2012,6(2),1479-1485.
Non-patent literature 2
2.Fang?Jiao,Qiyu?Huang,Wangchun?Ren.,Enhanced?performance?for?solar?cells?with?moth-eye?structure?fabricated?by?UV?nanoimprint?lithography.Microelectronic?Engineering2013,10(3),126–130.
Non-patent literature 3
3.Jingbi?You,Xuanhua?Li,Feng-xian?Xie,et?al.,Surface?Plasmon?and?Scattering-Enhanced?Low-Bandgap?Polymer?Solar?Cell?by?a?Metal?Grating?Back?Electrode.Advanced?Energy?Materials2012.
What approach the most with technical solution of the present invention is that of the applicant's association request people is in first to file, the Chinese invention patent that application number is 201310033982.X, this patent discloses a kind of organic solar batteries and preparation method thereof, this solar cell comprises substrate, and be positioned at successively described suprabasil the first electrode, the first transport layer, active layer, the second transport layer and the second electrode, wherein, the first transport layer is provided with the nano concavo-convex structure, in this nano concavo-convex structure of at least part of infiltration of photoactive layer, make the complementary structure of this photoactive layer in the formation of the interface place with described the first transport layer and described nano concavo-convex structure, although the light trapping structure of this patent can effectively increase the absorption to light in ultraviolet in infrared wide spectral range, thereby improve the conversion efficiency of organic solar batteries, but because solar cell still can be subject to the material of substrate own, exist the reason such as transmittancy restriction can not the incident light of all angles be absorbed fully, cause photoelectric conversion efficiency to improve limited.
Therefore, need to seek new technical scheme and further improve the organic solar batteries photoelectric conversion efficiency.
Summary of the invention
In view of this, the object of the present invention is to provide a kind of organic solar batteries and preparation method thereof, effectively improve the photoelectric conversion efficiency of organic solar batteries, have self_cleaning effect simultaneously, and manufacture craft is simple, applicable scale production is applied.
To achieve these goals, technical scheme provided by the invention is as follows:
A kind of organic solar batteries, the first electrode, the first charge transport layer, photoactive layer, the second charge transport layer and the second electrode that comprise substrate and be positioned at successively described substrate one surface, wherein, another surface of described substrate is provided with antireflection layer, has the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on described antireflection layer.
Preferably, interface between described the first charge transport layer and described photoactive layer is provided with the first light trapping structure, this first light trapping structure comprises the second nano concavo-convex structure be arranged on described the first charge transport layer, with be arranged on described photoactive layer and with the complementary structure of described the second nano concavo-convex structure, wherein, the refractive index of described the second nano concavo-convex structure changes in gradient along the incident light direction.
Preferably, interface between described the second charge transport layer and described photoactive layer is provided with the second light trapping structure, this second light trapping structure comprises the 3rd nano concavo-convex structure be arranged on described photoactive layer, with be arranged on described the second charge transport layer and with the complementary structure of described the 3rd nano concavo-convex structure, wherein, the refractive index of described the 3rd nano concavo-convex structure changes in gradient along the incident light direction.
Preferably, interface between described the second charge transport layer and described the second electrode is provided with the 3rd light trapping structure, the 3rd light trapping structure comprises the 4th nano concavo-convex structure be arranged on described the second charge transport layer, with be arranged on described the second electrode and with the complementary structure of described the 4th nano concavo-convex structure, wherein, the refractive index of described the 4th nano concavo-convex structure changes in gradient along the incident light direction.
Preferably, described the first charge transport layer is electron transfer layer or hole transmission layer, and, when described the first charge transport layer is electron transfer layer, described the second charge transport layer is hole transmission layer; When described the first charge transport layer is hole transmission layer, described the second charge transport layer is electron transfer layer.
Preferably, the material of described the first charge transport layer or the second transport layer is selected from any one in transition metal oxide, cesium fluoride, high molecular polymer;
Described nano concavo-convex structure is aperiodicity, quasi periodicity or periodic concaveconvex structure, and the column that is shaped as one dimension or two dimension of this nano concavo-convex structure, parabolic shape, taper or stepped in any one;
Described photoactive layer is the bulk heterojunction layer formed by donor material and acceptor material blend, or becomes respectively film formed duplex heterojunction layer for donor material with acceptor material, or the little molecule heterojunction layer formed for evaporation;
The material of described the first electrode is selected from any one in tin indium oxide, tin oxide or fluorine doped tin oxide; The material layer of described the second electrode is selected from any one in aluminium, silver, calcium, copper, gold, platinum.
Preferably, a kind of manufacture method of organic solar batteries as above, wherein, its operating procedure comprises:
A10), the material layer that is colloidal state or half colloidal state in substrate one surface-coated;
B10), described material layer carried out to the soft imprint process of nanometer process, obtain antireflection layer, there is the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on described antireflection layer;
C10), make successively the first electrode, the first charge transport layer, photoactive layer, the second charge transport layer, the second electrode on another surface of described substrate;
D10), complete the making of organic solar batteries.
Preferably, the material of described material layer is selected from any one in zinc oxide, titanium dioxide, ultraviolet cured adhesive, dimethione, polystyrene acrylic acid, PFPE.
Preferably, a kind of manufacture method of organic solar batteries as above, wherein, its operating procedure comprises:
A20), make successively the first electrode on substrate one surface, be the first charge transport layer of colloidal state or half colloidal state, and be the material layer of colloidal state or half colloidal state in another surface-coated of described substrate;
B20), described material layer and described the first charge transport layer are carried out to the soft imprint process processing of nanometer simultaneously, obtain respectively the second nano concavo-convex structure that antireflection layer and its refractive index change in gradient along the incident light direction, there is the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on described antireflection layer;
C20), make photoactive layer on described the first charge transport layer, at least part of infiltration of described photoactive layer is to described the second nano concavo-convex structure, the complementary structure of formation and the second nano concavo-convex structure, make on the interface between the first charge transport layer and photoactive layer and form the first light trapping structure;
D20), make successively the second charge transport layer, the second electrode on described photoactive layer;
E20), complete the making of organic solar batteries.
Preferably, the soft imprint process of described nanometer specifically comprises:
S1 '), by any one technique in laser direct-writing or holography or electron beam deposition or evaporation sputter or chemical synthesis or self-assembling method, prepare the nano concavo-convex structure in substrate, form respectively the first impression block and the second impression block;
S2 '), the nano concavo-convex structure in the first impression block and the second impression block is transferred to respectively on soft material to corresponding first making ide Renhe the second impression die that forms;
Adopt first making ide Renhe the second impression die described material layer and described the first charge transport layer to be impressed, solidify simultaneously, the nano concavo-convex structure in first making ide Renhe the second impression die is transferred to respectively on material layer and the first charge transport layer S3 '), respectively;
S4 '), the demoulding, form respectively the second nano concavo-convex structure that antireflection layer and its refractive index change in gradient along the incident light direction on substrate and the first charge transport layer, there is the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on described antireflection layer.
The present invention has by arranging at substrate surface on this antireflection layer of antireflection layer the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction, make incident light enter organic solar batteries by this antireflection layer, because the first nano concavo-convex structure makes the most of light that are scattered through repeatedly reflecting and enter substrate, thereby effectively strengthen the light transmittance of substrate, and then effectively improve the photoelectric conversion efficiency of organic solar batteries, because also making organic solar batteries of the present invention, this antireflection layer there is hydrophobic surface simultaneously, thereby acquisition self_cleaning effect, contribute to alleviate its cleaning in the BIPV application, guarantee useful life of the present invention and service behaviour simultaneously.The present invention further optimally, in order further effectively to improve the photoelectric conversion efficiency of organic solar batteries, interface between the first charge transport layer of the present invention and photoactive layer is provided with the first light trapping structure, this first light trapping structure comprises the second nano concavo-convex structure be arranged on the first charge transport layer, with be arranged on photoactive layer, and the complementary structure with the second nano concavo-convex structure, wherein, the refractive index of the second nano concavo-convex structure changes in gradient along the incident light direction, effectively increase the light absorption of photoactive layer, thereby further effectively raising photoelectric conversion efficiency of the present invention.
The present invention further specifically optimally, adopt soft nano-imprint process to prepare the nano concavo-convex structure, effectively guaranteed to copy the high fidelity of transfer process, realize that a step impression is shaped simultaneously, wherein, the impression die can be repeatedly used, and when reducing costs, has high production application and is worth; Impression block can pass through the methods such as electron beam lithography, laser direct-writing, photoetching, holography, chemical synthesis and obtain, and has very high flexibility, and can be repeatedly used equally; Therefore impressed under room temperature and normal pressure, do not needed coolingly after having impressed, saved time, improved production efficiency;
The present invention further especially optimally, material layer and the first charge transport layer that is positioned at substrate surface carried out to the soft imprint process processing of nanometer simultaneously, obtain respectively antireflection layer and the second nano concavo-convex structure, realizing the maximized while of organic solar batteries electricity conversion, greatly improved soft imprint process treatment effeciency, so decrease fabrication cycle of the present invention.
The accompanying drawing explanation
In order to be illustrated more clearly in the embodiment of the present invention or technical scheme of the prior art, below will the accompanying drawing of required use in embodiment or description of the Prior Art be briefly described, apparently, the accompanying drawing the following describes is only some embodiment that put down in writing in the present invention, for those of ordinary skills, under the prerequisite of not paying creative work, can also obtain according to these accompanying drawings other accompanying drawing.
Accompanying drawing 1 is the structural representation of organic solar batteries under the specific embodiment of the invention;
Accompanying drawing 3 is nano concavo-convex structure of the present invention action principle figure for light;
Accompanying drawing 4 is fabrication processing figure of a kind of execution mode of Fig. 1;
Accompanying drawing 5 is fabrication processing figure of the another kind of execution mode of Fig. 1;
Accompanying drawing 6 is Fig. 5 structural representations when impression;
Accompanying drawing 7 is the structural representations after Fig. 6 completes impression;
Accompanying drawing 8 is voltage-to-current density curve comparison diagrams of the specific embodiment of the invention and prior art;
Accompanying drawing 9 is external quantum efficiency curve comparison diagrams of the specific embodiment of the invention and prior art;
Accompanying drawing 10 is contact angle resolution charts of the specific embodiment of the invention.
Embodiment
The embodiment of the invention discloses a kind of organic solar batteries, the first electrode, the first charge transport layer, photoactive layer, the second charge transport layer and the second electrode that comprise substrate and be positioned at successively substrate one surface, wherein, another surface of substrate is provided with antireflection layer, has the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on antireflection layer.
The embodiment of the invention discloses a kind of manufacture method of organic solar batteries as above, wherein, its operating procedure comprises:
A10), the material layer that is colloidal state or half colloidal state in substrate one surface-coated;
B10), material layer carried out to the soft imprint process of nanometer process, obtain antireflection layer, there is the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on antireflection layer;
C10), make successively the first electrode, the first charge transport layer, photoactive layer, the second charge transport layer, the second electrode on another surface of substrate;
D10), complete the making of organic solar batteries.
The embodiment of the present invention has by arranging at substrate surface on this antireflection layer of antireflection layer the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction, make incident light enter organic solar batteries by this antireflection layer, because the first nano concavo-convex structure makes the most of light that are scattered through repeatedly reflecting and enter substrate, thereby effectively strengthen the light transmittance of substrate, and then effectively improve the photoelectric conversion efficiency of organic solar batteries, because also making the organic solar batteries of the embodiment of the present invention, this antireflection layer there is hydrophobic surface simultaneously, thereby acquisition self_cleaning effect, contribute to alleviate its cleaning in the BIPV application, guarantee useful life and the service behaviour of the embodiment of the present invention simultaneously.The embodiment of the present invention further optimally, in order further effectively to improve the photoelectric conversion efficiency of organic solar batteries, the first charge transport layer of the embodiment of the present invention and the interface between photoactive layer are provided with the first light trapping structure, this first light trapping structure comprises the second nano concavo-convex structure be arranged on the first charge transport layer, with be arranged on photoactive layer, and the complementary structure with the second nano concavo-convex structure, wherein, the refractive index of the second nano concavo-convex structure changes in gradient along the incident light direction, effectively increase the light absorption of photoactive layer, thereby the further photoelectric conversion efficiency that effectively improves the embodiment of the present invention.
The embodiment of the present invention further specifically optimally, adopt soft nano-imprint process to prepare the nano concavo-convex structure, effectively guaranteed to copy the high fidelity of transfer process, realize that a step impression is shaped simultaneously, wherein, the impression die can be repeatedly used, and when reducing costs, has high production application and is worth; Impression block can pass through the methods such as electron beam lithography, laser direct-writing, photoetching, holography, chemical synthesis and obtain, and has very high flexibility, and can be repeatedly used equally; Therefore impressed under room temperature and normal pressure, do not needed coolingly after having impressed, saved time, improved production efficiency;
The embodiment of the present invention further especially optimally, material layer and the first charge transport layer that is positioned at substrate surface carried out to the soft imprint process processing of nanometer simultaneously, obtain respectively antireflection layer and the second nano concavo-convex structure, realizing the maximized while of organic solar batteries electricity conversion, greatly improved soft imprint process treatment effeciency, so decrease the fabrication cycle of the embodiment of the present invention.
In order to make those skilled in the art person understand better the technical scheme in the present invention, below in conjunction with the accompanying drawing in the embodiment of the present invention, technical scheme in the embodiment of the present invention is clearly and completely described, obviously, described embodiment is only the present invention's part embodiment, rather than whole embodiment.Embodiment based in the present invention, those of ordinary skills, not making under the creative work prerequisite the every other embodiment obtained, should belong to the scope of protection of the invention.
Shown in Figure 1, a kind of organic solar batteries 100, comprise substrate 110, and the first electrode 120 that is positioned at successively substrate 110 1 surfaces, the first charge transport layer 130, photoactive layer 140, the second charge transport layer 150 and the second electrode 160, wherein, substrate 110 another surfaces are provided with antireflection layer 170, there is the first nano concavo-convex structure 171 that its refractive index changes in gradient along the incident light direction on antireflection layer 170, because the first nano concavo-convex structure 171 makes the most of light that are scattered through repeatedly reflecting and enter substrate 110, thereby effectively strengthen the light transmittance of substrate 110, and then effectively improve the photoelectric conversion efficiency of organic solar batteries 100, because also making the organic solar batteries 110 of the embodiment of the present invention, this antireflection layer 170 there is hydrophobic surface simultaneously, thereby acquisition self_cleaning effect, contribute to alleviate its cleaning in the BIPV application, guarantee useful life and the service behaviour of the embodiment of the present invention simultaneously.
In order effectively to increase the light absorption of photoactive layer 140, preferably, in the present embodiment, interface between the first charge transport layer 130 and photoactive layer 140 is provided with the first light trapping structure 181, this first light trapping structure 181 comprises the second nano concavo-convex structure (scheming unmarked) be arranged on the first charge transport layer 130, with be arranged on photoactive layer 140 and with the complementary structure (scheming unmarked) of the second nano concavo-convex structure, wherein, the refractive index of the second nano concavo-convex structure changes in gradient along the incident light direction.
In order further effectively to increase the light absorption of photoactive layer 140, preferably, in the present embodiment, interface between the second charge transport layer 150 and photoactive layer 140 is provided with the second light trapping structure 182, this second light trapping structure 182 comprises the 3rd nano concavo-convex structure (scheming unmarked) be arranged on photoactive layer 140, with be arranged on the second charge transport layer 150 and with the complementary structure (scheming unmarked) of the 3rd nano concavo-convex structure, wherein, the refractive index of the 3rd nano concavo-convex structure changes in gradient along the incident light direction.
In order further effectively to increase the light absorption of photoactive layer, preferably, in the present embodiment, interface between the second charge transport layer 150 and the second electrode 160 is provided with the 3rd light trapping structure 183, the 3rd light trapping structure 183 comprises the 4th nano concavo-convex structure (scheming unmarked) be arranged on the second charge transport layer 150, with be arranged on the second electrode 160 and with the complementary structure of the 4th nano concavo-convex structure, wherein, the refractive index of the 4th nano concavo-convex structure changes in gradient along the incident light direction.
In one embodiment, the first charge transport layer 130 is electron transfer layer, and the second charge transport layer 150 is hole transmission layer; In another embodiment, the first charge transport layer 130 is hole transmission layer, and the second charge transport layer 150 is electron transfer layer.
Further particularly, the material of the first charge transport layer 130 or the second transport layer 150 is selected from any one in transition metal oxide (zinc oxide, titanium oxide, molybdenum oxide etc.), cesium fluoride, high molecular polymer;
Shown in Figure 2, the nano concavo-convex structure that this patent relates in full is aperiodicity, quasi periodicity or periodic concaveconvex structure, and the column, parabolic shape, taper that are shaped as one dimension or two dimension of this nano concavo-convex structure or stepped in any one, wherein, the nano concavo-convex structural cycle is below 500nm, groove depth is between 200-900nm, duty ratio is between 0.3-0.7, and more preferably, the cycle is between 200-400nm, groove depth is between 200-600nm, between duty ratio 0.5-0.6; Photoactive layer 140 is the bulk heterojunction layer formed by donor material and acceptor material blend, perhaps for donor material, with acceptor material, become respectively film formed duplex heterojunction layer, the little molecule heterojunction layer perhaps formed for evaporation, wherein, donor material and acceptor material are selected from respectively derivative and the C of poly-(3-hexyl thiophene), polyphenyl or polyphenylene ethylene
60, C
70and any one in functional derivative, organic molecule or inorganic nano-particle, can certainly adopt other well known materials; The material of the first electrode 120 is selected from any one in tin indium oxide, tin oxide or fluorine doped tin oxide; The material layer of the second electrode 160 is selected from any one in aluminium, silver, calcium, copper, gold, platinum.
Shown in Figure 3, nano concavo-convex structure of the present invention is for the action principle of light, when the incident of low-angle light (being less than critical value), overwhelming majority light enters organic solar batteries, and the arrival photoactive layer, due to the duality principle of light, only have few part incident light to be scattered; When high angle scattered light incident (being greater than critical value), light is through repeatedly refraction, the overwhelming majority also enters organic solar batteries, and arrival photoactive layer, only have few part to be scattered, therefore, the nano concavo-convex structure has increased the absorption of organic solar batteries to all angles incident light, effectively increase the light absorption total amount of photoactive layer, final effectively raising photoelectric conversion efficiency of the present invention.
Particularly, shown in Figure 4, in one embodiment, and the manufacture method of organic solar batteries 100 as above, wherein, its operating procedure comprises:
A10), the material layer that is colloidal state or half colloidal state in substrate 110 1 surface-coated; Particularly, the material of substrate is large-area glass substrate or flexible substrate, the material of material layer is selected from any one in zinc oxide, titanium dioxide, ultraviolet cured adhesive, dimethione, polystyrene acrylic acid, PFPE, preferably, in the present embodiment, substrate 110 is common float glass, and material layer is the ultraviolet light polymerization glue-line, continue the ultra-violet curing glue of spin coating 60s on common float glass one surface with the speed of 2000rpm, obtain the ultraviolet light polymerization glue-line;
B10), the ultraviolet light polymerization glue-line carried out to the soft imprint process of nanometer process, obtain antireflection layer 170, there is the first nano concavo-convex structure 171 that its refractive index changes in gradient along the incident light direction on antireflection layer 170, preferably, concrete operation is as follows:
S1), prepare the two-dimensional nano concaveconvex structure by any one technique in laser direct-writing or holography or electron beam deposition or evaporation sputter or chemical synthesis or self-assembling method in substrate, form impression block, wherein, the material of this substrate can be quartzy, silicon, nickel, carbon steel, carborundum, Al-Doped ZnO, Merlon, any one in polyvinyl chloride or polybutyl methacrylate, specifically preferably, in the present embodiment, prepare the first impression block in substrate by the laser interference method, two-dimensional nano concaveconvex structure on this first impression block is moth eye shape,
S2), the two-dimensional nano concaveconvex structure in the first impression block is transferred on soft material, form the first impression die, particularly, soft material is selected from any one in dimethione, polystyrene, olefin(e) acid or PFPE; Specifically preferably, adopt thermo-responsive impression materials--dimethione (PDMS), two-dimensional nano concaveconvex structure in the first impression block is transferred to PDMS upper, heating cure when exerting pressure, formations groove depth is that 100nm, cycle, to be 100nm first impressed die;
S3), adopt the first impression die to be impressed the ultra-violet curing glue-line, solidify, two-dimensional nano concaveconvex structure on the first impression die is transferred on the ultra-violet curing glue-line, specifically preferably, adopt volume to volume or flat to flat stamping technique, and adopt ultraviolet lighting to be cured the ultra-violet curing glue-line, especially, when adopting the stamping technique of volume to volume, above-mentioned the first impression die is fixed on pressure roller, the ultra-violet curing glue-line is carried out to the soft impression of nanometer of volume to volume, solidify, two-dimensional nano concaveconvex structure on the first impression die is transferred on the ultra-violet curing glue-line.Due to the stamping technique of this volume to volume when the impression, contacting between the first impression die and thing to be pressed surface is that line contacts, can avoid flat to demoulding difficulty in the blind impression technology, impress the restrictions such as breadth is little, thereby further improve make efficiency and the product quality of organic solar batteries in the present embodiment.
S4), the demoulding, form antireflection layer 170 on substrate 110, there is the first nano concavo-convex structure 171 that its refractive index changes in gradient along the incident light direction on antireflection layer 170, wherein, the first nano concavo-convex structure 171 is two-dimensional shapes, its groove depth is that 100nm, cycle are 100nm, natch, in other embodiments, the relevant design parameter of the first nano concavo-convex structure 171 can be selected to obtain difform the first nano concavo-convex structure according to the actual requirements, and the present invention does not do concrete restriction.
C10), make successively the first electrode 120, the first charge transport layer 130, photoactive layer 140, the second charge transport layer 150, the second electrode 160 on substrate 110 another surfaces, wherein, the concrete manufacture craft of each layer of structure can be selected from respectively the methods such as solwution method spin coating, vapour deposition, sputter, or other known methods, preferably, in execution mode, concrete operation is as follows:
Generate ito thin film in the upper sputter in another surface of common float glass (as substrate 110), ito thin film is carried out to photoetching treatment, be cut into required size, this ito thin film is as the first electrode 120, then, ito thin film is used to cleaning agent, deionized water, acetone, ethanol, each ultrasonic cleaning of isopropyl alcohol 15min successively, remove the organic pollution of Float Glass Surface, and dry, then UV-ozone treatment 15min is carried out in the ito thin film surface after drying;
Then zinc oxide (ZnO) precursor solution that continues spin coating 40s with the speed of 2000rpm on the ito thin film surface obtains the ZnO precursor thin-film, wherein, zinc oxide (ZnO) precursor solution is by dissolving 100mg bis-water zinc acetates rear acquisition in the monoethanolamine mixed liquor of 1ml methyl cellosolve and 15ul;
With reference to above-mentioned steps S1, step S2) to prepare groove depth be 100nm, the cycle second impression die that is 400nm, and the second impression die is placed on and imposes certain pressure on the ZnO precursor thin-film and impressed 5min, and realize hot curing under the heating condition of 150 ℃ after, the demoulding, obtain the second nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on ZnO film, wherein, the second nano concavo-convex structure is two-dimensional shapes, its groove depth is that 100nm, cycle are 400nm, and wherein this ZnO film is as electron transfer layer 130;
Continue the P3HT:ICBA photoactive layer solution of spin coating 50s with the speed of 600rpm on ZnO film, as photoactive layer 140, wherein, this P3HT:ICBA photoactive layer solution obtains in the 1ml dichloro-benzenes by dissolving 10mgP3HT and 10mg ICBA, at least part of solution of photoactive layer 140 infiltrates to the second nano concavo-convex structure, the surface of this photoactive layer 140 is adopted with reference to above-mentioned steps S1 simultaneously)-step S4) carry out the soft imprint process of nanometer and process, and the 10min that anneals at 110 ℃ of temperature, make the complementary structure of photoactive layer 140 formation and the second nano concavo-convex structure, and then make on the interface between electron transfer layer 130 and photoactive layer 140 and to form the first light trapping structure 181, photoactive layer 140 surfaces obtain the 3rd nano concavo-convex structure (scheming unmarked) that its refractive index changes in gradient along the incident light direction simultaneously,
Evaporation 8nm MoO successively on the photoactive layer 140 with the 3rd nano concavo-convex structure
3with 100nm Al, respectively as hole transmission layer 150 and the second electrode 160, make on hole transmission layer 150 complementary structure formed with the 3rd nano concavo-convex structure, and then make on the interface between hole transmission layer 150 and photoactive layer 140 and to form the second light trapping structure 182, therefore because the thickness of hole transmission layer 150 is little, also make the surface of hole transmission layer 150 form less and the 4th nano concavo-convex structure that its refractive index changes in gradient along the incident light direction of size simultaneously; And then make on the second electrode 160 complementary structure formed with the 4th nano concavo-convex structure, and then make formation the 3rd light trapping structure 183 on the interface between hole transmission layer 150 and the second electrode 160.
D10), complete the making of organic solar batteries 100.
In another embodiment, shown in Figure 5, the manufacture method of organic solar batteries 100 as above, wherein, its operating procedure comprises:
A20), make successively the first electrode 120 on substrate 110 1 surfaces, be the first charge transport layer 130 of colloidal state or half colloidal state, and the material layer that is colloidal state or half colloidal state in substrate 110 another surface-coated, wherein, the concrete manufacture craft of each layer of structure can be referring to the correlation technique content of above-mentioned execution mode;
B20), material layer and the first charge transport layer 130 are carried out to the soft imprint process processing of nanometer simultaneously, obtain respectively the second nano concavo-convex structure that antireflection layer 170 and its refractive index change in gradient along the incident light direction, there is the first nano concavo-convex structure 171 that its refractive index changes in gradient along the incident light direction on antireflection layer 170, preferably, the soft imprint process of nanometer specifically comprises:
S1 '), prepare the nano concavo-convex structure by any one technique in laser direct-writing or holography or electron beam deposition or evaporation sputter or chemical synthesis or self-assembling method in substrate, form respectively the first impression block and the second impression block, the material of this substrate can be any one in quartz, silicon, nickel, carbon steel, carborundum, Al-Doped ZnO, Merlon, polyvinyl chloride or polybutyl methacrylate, specifically can be referring to the correlation technique content of above-mentioned execution mode;
S2 '), by the nano concavo-convex structure in the first impression block and the second impression block, transfer to respectively on soft material, corresponding the first impression die 191 and the second impression die 192 of forming, particularly, soft material is selected from any one in dimethione, polystyrene acrylic acid or PFPE, specifically can be referring to the correlation technique content of above-mentioned execution mode;
S3 '), adopt respectively the first impression die 191 and the second impression die 192 material layer and the first charge transport layer 130 to be impressed simultaneously, solidify, nano concavo-convex structure in the first impression die 191 and the second impression die 192 is transferred to respectively on material layer and the first charge transport layer 130, particularly, adopt volume to volume or flat to flat stamping technique, further preferably, with above reason is described, in the present embodiment, adopt the stamping technique of volume to volume, please specifically shown in Figure 6, the first impression die 191 and the second impression die 192 are separately fixed on pressure roller (Fig. 6 does not carry out mark), by band impression thing obtained above, (Fig. 6 does not carry out mark, and its position signal during only for stamp work, as the other guide implication, do not limit) with from left to right or direction from right to left carry out the displacement transmission, make the first impression die 191 and the second impression die 192 that are positioned at this band impression thing below and top carry out respectively the rotation of rightabout (arrow as shown in Figure 6) on corresponding pressure roller, and then make the first impression die 191 and the second impression die 192 realize respectively the soft impression of nanometer to ultra-violet curing glue-line and the first charge transport layer 130, and in the soft moulding process of this nanometer, adopt ultraviolet lighting to be cured the ultra-violet curing glue-line, adopt heat treated to be cured the first charge transport layer 130,
S4 '), shown in Figure 7, the demoulding, form respectively the second nano concavo-convex structure that antireflection layer 170 and its refractive index change in gradient along the incident light direction on substrate 110 and the first charge transport layer 130, there is the first nano concavo-convex structure 171 that its refractive index changes in gradient along the incident light direction on antireflection layer 170;
C20), make photoactive layer 140 on the first charge transport layer 130, in at least part of infiltration to the second nano concavo-convex structure of photoactive layer 140, form the complementary structure with the second nano concavo-convex structure, make on the interface between the first charge transport layer 130 and photoactive layer 140 and form the first light trapping structure 181, concrete manufacture craft can be referring to the correlation technique content of above-mentioned execution mode;
D20), make successively the second charge transport layer 150, the second electrode 160 on photoactive layer 140, concrete manufacture craft can be referring to the correlation technique content of above-mentioned execution mode,, concrete manufacture craft can be referring to the correlation technique content of above-mentioned execution mode;
E20), complete the making of organic solar batteries 100.
Refer to shown in Fig. 8 and Fig. 9, Fig. 8 is the voltage-to-current density curve comparison diagram of the specific embodiment of the invention and prior art; Fig. 9 is the external quantum efficiency curve comparison diagram of the specific embodiment of the invention and prior art, from Fig. 8 and Fig. 9, can obviously find out, the present invention can effectively improve the light conversion efficiency of organic solar batteries with respect to prior art.
Shown in Figure 10, Figure 10 is the contact angle resolution chart of the specific embodiment of the invention.From Figure 10, can obviously find out, organic solar batteries provided by the invention has very large contact angle, has represented good hydrophobic property, makes the present invention have self_cleaning effect.
To those skilled in the art, obviously the invention is not restricted to the details of above-mentioned example embodiment, and in the situation that do not deviate from spirit of the present invention or essential characteristic, can realize the present invention with other concrete form.Therefore, no matter from which point, all should regard embodiment as exemplary, and be nonrestrictive, scope of the present invention is limited by claims rather than above-mentioned explanation, therefore is intended to include in the present invention dropping on the implication that is equal to important document of claim and all changes in scope.Any Reference numeral in claim should be considered as limit related claim.
In addition, be to be understood that, although this specification is described according to execution mode, but not each execution mode only comprises an independently technical scheme, this narrating mode of specification is only for clarity sake, those skilled in the art should make specification as a whole, and the technical scheme in each embodiment also can, through appropriate combination, form other execution modes that it will be appreciated by those skilled in the art that.
Claims (10)
1. an organic solar batteries, the first electrode, the first charge transport layer, photoactive layer, the second charge transport layer and the second electrode that comprise substrate and be positioned at successively described substrate one surface, it is characterized in that, another surface of described substrate is provided with antireflection layer, has the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on described antireflection layer.
2. organic solar batteries as claimed in claim 1, it is characterized in that, interface between described the first charge transport layer and described photoactive layer is provided with the first light trapping structure, this first light trapping structure comprises the second nano concavo-convex structure be arranged on described the first charge transport layer, with be arranged on described photoactive layer and with the complementary structure of described the second nano concavo-convex structure, wherein, the refractive index of described the second nano concavo-convex structure changes in gradient along the incident light direction.
3. organic solar batteries as claimed in claim 2, it is characterized in that, interface between described the second charge transport layer and described photoactive layer is provided with the second light trapping structure, this second light trapping structure comprises the 3rd nano concavo-convex structure be arranged on described photoactive layer, with be arranged on described the second charge transport layer and with the complementary structure of described the 3rd nano concavo-convex structure, wherein, the refractive index of described the 3rd nano concavo-convex structure changes in gradient along the incident light direction.
4. organic solar batteries as claimed in claim 3, it is characterized in that, interface between described the second charge transport layer and described the second electrode is provided with the 3rd light trapping structure, the 3rd light trapping structure comprises the 4th nano concavo-convex structure be arranged on described the second charge transport layer, with be arranged on described the second electrode and with the complementary structure of described the 4th nano concavo-convex structure, wherein, the refractive index of described the 4th nano concavo-convex structure changes in gradient along the incident light direction.
5. organic solar batteries as claimed in claim 1, is characterized in that, described the first charge transport layer is electron transfer layer or hole transmission layer, and, when described the first charge transport layer is electron transfer layer, described the second charge transport layer is hole transmission layer; When described the first charge transport layer is hole transmission layer, described the second charge transport layer is electron transfer layer.
6. organic solar batteries as claimed in claim 1, is characterized in that, the material of described the first charge transport layer or the second transport layer is selected from any one in transition metal oxide, cesium fluoride, high molecular polymer;
Described nano concavo-convex structure is aperiodicity, quasi periodicity or periodic concaveconvex structure, and the column that is shaped as one dimension or two dimension of this nano concavo-convex structure, parabolic shape, taper or stepped in any one;
Described photoactive layer is the bulk heterojunction layer formed by donor material and acceptor material blend, or becomes respectively film formed duplex heterojunction layer for donor material with acceptor material, or the little molecule heterojunction layer formed for evaporation;
The material of described the first electrode is selected from any one in tin indium oxide, tin oxide or fluorine doped tin oxide; The material layer of described the second electrode is selected from any one in aluminium, silver, calcium, copper, gold, platinum.
7. the manufacture method as the described organic solar batteries of claim 1-6 any one, is characterized in that, its operating procedure comprises:
A10), the material layer that is colloidal state or half colloidal state in substrate one surface-coated;
B10), described material layer carried out to the soft imprint process of nanometer process, obtain antireflection layer, there is the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on described antireflection layer;
C10), make successively the first electrode, the first charge transport layer, photoactive layer, the second charge transport layer, the second electrode on another surface of described substrate;
D10), complete the making of organic solar batteries.
8. the manufacture method of organic solar batteries as claimed in claim 7, is characterized in that, the material of described material layer is selected from any one in zinc oxide, titanium dioxide, ultraviolet cured adhesive, dimethione, polystyrene acrylic acid, PFPE.
9. the manufacture method of an organic solar batteries as claimed in claim 2, is characterized in that, its operating procedure comprises:
A20), make successively the first electrode on substrate one surface, be the first charge transport layer of colloidal state or half colloidal state, and be the material layer of colloidal state or half colloidal state in another surface-coated of described substrate;
B20), described material layer and described the first charge transport layer are carried out to the soft imprint process processing of nanometer simultaneously, obtain respectively the second nano concavo-convex structure that antireflection layer and its refractive index change in gradient along the incident light direction, there is the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on described antireflection layer;
C20), make photoactive layer on described the first charge transport layer, at least part of infiltration of described photoactive layer is to described the second nano concavo-convex structure, the complementary structure of formation and the second nano concavo-convex structure, make on the interface between the first charge transport layer and photoactive layer and form the first light trapping structure;
D20), make successively the second charge transport layer, the second electrode on described photoactive layer;
E20), complete the making of organic solar batteries.
10. the manufacture method of organic solar batteries as claimed in claim 9, is characterized in that, the soft imprint process of described nanometer specifically comprises:
S1 '), by any one technique in laser direct-writing or holography or electron beam deposition or evaporation sputter or chemical synthesis or self-assembling method, prepare the nano concavo-convex structure in substrate, form respectively the first impression block and the second impression block;
S2 '), the nano concavo-convex structure in the first impression block and the second impression block is transferred to respectively on soft material to corresponding first making ide Renhe the second impression die that forms;
Adopt first making ide Renhe the second impression die described material layer and described the first charge transport layer to be impressed, solidify simultaneously, the nano concavo-convex structure in first making ide Renhe the second impression die is transferred to respectively on material layer and the first charge transport layer S3 '), respectively;
S4 '), the demoulding, form respectively the second nano concavo-convex structure that antireflection layer and its refractive index change in gradient along the incident light direction on substrate and the first charge transport layer, there is the first nano concavo-convex structure that its refractive index changes in gradient along the incident light direction on described antireflection layer.
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Application publication date: 20131225 |