CN102751386A - Short wave response crystalline silicon solar battery preparation method based on multiple layers of silicon quantum dot - Google Patents
Short wave response crystalline silicon solar battery preparation method based on multiple layers of silicon quantum dot Download PDFInfo
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Abstract
The invention discloses a short wave response crystalline silicon solar battery preparation method based on multiple layers of silicon quantum dot. The method comprises the following technical steps of: preparing a textured surface on a P type crystalline silicon substrate; depositing an amorphous silicon thin film; forming the silicon quantum dot through a rapid thermal annealing process; forming a layer of silicon quantum dot thin film; repeatedly executing the processes from the step two to the step 3 for many times to finish the preparation of multiple layers of silicon quantum dot thin films; forming a PN junction and boosting a constant surface concentration diffusion source; depositing a Si3N4 anti-reflection film on the front surface of the P type crystalline silicon substrate; respectively executing positive and negative electricity screen printing on the back and the front of the Si3N4 anti-reflection film; and annealing a silk-screen electrode, and finishing the preparation of a short wave response crystalline silicon solar battery based on multiple layers of silicon quantum dot. The preparation method provided by the invention has the advantage of effectively improving the quantum efficiency of the 350-600nm short wave band, increasing the light current and finally realizing the aim of high-efficiency conversion.
Description
[technical field]
The present invention relates to a kind of solar cell fabrication process, be specially short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot.
[background technology]
Along with rapid increase and various countries' rapid economy development of world population, more and more to demands for energy; Energy problem has become the permanent fast-developing strategic problem of a country.Extensive at present traditional energy that uses such as oil and coal are because reserves are limited; By present consumption will be exhausted after to more than 100 years after decades; Frequent use fossil energy causes serious air pollution and greenhouse effect at present simultaneously, and is therefore also more and more urgent to the demand of clean reproducible energy; Solar cell has obtained fast development thus as clean energy resource a kind of.Since AT&T Labs in 1954 reported first commercial silicon (Si) solar cell, various solar cells were come out one after another.Through the continuous development of recent decades, solar cell is from the thin-film solar cells of the monocrystaline silicon solar cell of the first generation, the second generation high performance solar batteries of the third generation till now, and its cost of manufacture progressively reduces, and conversion efficiency improves constantly.
In the various solar cells of crystal silicon battery (monocrystalline and polycrystalline) battery, its market proportion has accounted for more than 90% at present, but conversion efficiency is generally not high.How preparing the high battery of conversion efficiency is that various countries are engaged in the key issue that the photovoltaic industry faces, and this also is the key means that reduces the solar energy cost.Because Si is a kind of indirect bandgap material, its concerning the ability of light absorption with respect to wanting weak many direct gap semiconductor.Conventional crystal silicon cell is in the light of 350-600nm wave band owing to the single attribute that can be with, and the energy of this short-wave band photon is high, and after being absorbed by conventional crystal silicon cell, major part becomes heat and consumes.How improving short wave response, is the topic of industry common concern.
For solving the problems of the technologies described above, the necessary preparation method that a kind of advanced person's short wave response crystal silicon solar batteries is provided is to overcome said defective of the prior art.
[summary of the invention]
For addressing the above problem; The object of the present invention is to provide short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot; The quantum efficiency that it promotes the 350-600nm short-wave band effectively makes photoelectric current increase, and finally reaches aim of efficient conversion.
For realizing above-mentioned purpose, the technical scheme that the present invention takes is: based on the short wave response crystal silicon solar batteries preparation method of multilayer silicon quantum dot, it comprises following processing step:
(1), preparation making herbs into wool face on P type crystalline silicon substrate;
(2), utilize dull and stereotyped plasma-reinforced chemical vapor deposition, carry out the deposition of amorphous silicon membrane at the P type crystalline silicon substrate surface that matte is arranged;
(3), to depositing the P type crystalline silicon substrate of amorphous silicon membrane, utilize rapid thermal annealing process to form silicon quantum dot;
(4),, utilize dull and stereotyped plasma-reinforced chemical vapor deposition, carry out the silicon nitride film deposition of Silicon-rich again, form the preparation of one deck silicon quantum dot film forming the P type crystalline silicon substrate of silicon quantum dot;
(5), repeating step (2) to step (4) is repeatedly accomplished the preparation of multilayer silicon quantum dot film;
(6), utilize tubular type stopped pipe diffusion furnace, the P type crystalline silicon substrate with multilayer silicon quantum dot film is carried out phosphorous diffusion, form PN junction, and under 500-1500 ℃ of temperature, carry out the propelling of constant surface concentration diffuse source;
(7), utilize tubular type or flat plasma-reinforced chemical vapor deposition method at P type crystalline silicon substrate face deposit Si
3N
4Antireflective film;
(8), frontal is deposited with Si
3N
4The P type crystalline silicon substrate of antireflective film carries out the silk screen printing of positive and negative electricity respectively in its back side and front;
(9), the P type crystalline silicon substrate to after the silk screen printing carries out the annealing of silk-screen electrode, accomplishes the preparation based on the short wave response crystal silicon solar batteries of multilayer silicon quantum dot.
Short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot of the present invention further is: the P type crystalline silicon substrate in the step (1) is selected from a kind of in p type 125mm * 125mm monocrystalline silicon piece, p type 156mm * 156mm monocrystalline silicon piece and the p type 156 * 156mm polysilicon chip.
Short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot of the present invention further is: the thickness of the amorphous silicon membrane that forms in the step (2) is between the 1-15nm.
Short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot of the present invention further is: the rapid thermal annealing process of step (3), utilize the chain type annealing furnace, and under the nitrogen atmosphere protection, anneal with the mode of rapid thermal annealing; Or utilize band to carry out in-situ annealing with the panel PECVD of rapid thermal annealing equipment; The highest annealing temperature of rapid thermal annealing process is between 700-900 ℃, and annealing time is 20-400s.
Short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot of the present invention further is: the molecular formula of the silicon nitride film of the Silicon-rich in the step (4) is Si
xN, wherein, x＞0.75, the thickness of the silicon nitride film of Silicon-rich is between 1nm-30nm.
Short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot of the present invention further is: the number of times of the repeating step (2) in the step (5) to step (4) is in 100 times, and the gross thickness of the multilayer silicon quantum dot film that forms is in 1000nm.
Short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot of the present invention further is: in the step (6); Utilize tubular type stopped pipe diffusion furnace, liquid POCl3 is a diffuse source, and the P type crystalline silicon substrate with multilayer silicon quantum dot film is carried out phosphorous diffusion; Form PN junction; After diffusion finishes, close POCl3 diffuse source, and original position is carried out the propelling and the distribution again of the phosphorus of the constant surface concentration of high temperature; The temperature that high temperature advances is between 500-1500 ℃, and advancing distribution time is 1s-10h again, and the logical nitrogen of this process is protected.
Short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot of the present invention further is: the Si in the step (7)
3N
4The thickness of antireflective film is between 70nm-120nm.
Short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot of the present invention further is: in the step (8); Utilize screen process press; Silk screen printing aluminum paste material is carried out at the back side,, form the positive pole and the negative pole of battery respectively at positive printed silver slurry.
Compared with prior art; The present invention utilizes the quantum limitation effect of Si quantum dot; When changing the exciton Bohr radius cause through the quantum dot size and intending with size compared, the Si quantum dot can be with the generation broadening, can absorb high-energy photon (350-600nm); The relaxation heating process of high-energy photon is suppressed, and then photo-generated carrier is effectively separated by PN junction; Can promote the quantum efficiency of 350-600nm wave band effectively, make photoelectric current increase, finally reach aim of efficient conversion; Processing step with increase is few, can with the process compatible on the big production line, be easy to realize characteristics such as large-scale production, finally reach the purpose that reduces cost; After the surface had multilayer silicon quantum dot structure, the change that silicon amount point can be with can absorb high-energy photon, and formed superlattice structure between silicon quantum dot layer and the layer, except that can fully absorbing the short wavelength light, also helped the separation of photo-generated carrier and transported.
[description of drawings]
Fig. 1 is the preparation method's of the short wave response crystal silicon solar batteries based on a multilayer Si quantum dot of the present invention flow chart.
Fig. 2 is a P type crystalline silicon substrate sketch map of the present invention.
Fig. 3 is the present invention's sketch map after the substrate positive and negative is prepared matte.
Fig. 4 is dull and stereotyped plasma-reinforced chemical vapor deposition (flat-plate type PECVD) amorphous silicon membrane sketch map for the present invention utilizes.
Fig. 5 forms Si quantum dot sketch map for the present invention through rapid thermal annealing process.
Fig. 6 utilizes the Si of the rich Si of flat-plate type PECVD deposit for the present invention
xThe N film.
Fig. 7 repeats the Si that deposit forms Si quantum dot and rich Si for the present invention
xThe N film forms multilayer Si quantum dot membrane structure.
Fig. 8 forms PN junction for the present invention carries out phosphorous diffusion, and at high temperature advances, and makes phosphorus doping distribute again, then utilizes flat or tubular type PECVD growth Si
3N
4The antireflective film sketch map.
Fig. 9 prints negative electrode and positive electrode sketch map for the present invention utilizes screen printing technique respectively at front and back.
[embodiment]
Below in conjunction with accompanying drawing 1 to Fig. 9 embodiments of the invention are described in further detail.
As shown in Figure 1, it is the preparation method flow chart of preparation provided by the invention based on the short wave response crystal silicon solar batteries of multilayer Si quantum dot, and this method may further comprise the steps:
Step 101: preparation making herbs into wool face on P type crystalline silicon substrate;
Step 102: utilize the flat-plate type PECVD deposited amorphous silicon thin film;
Step 103: the rapid thermal annealing under the nitrogen atmosphere protection forms silicon quantum dot;
Step 104: the silicon nitride film that utilizes flat-plate type plasma reinforced chemical vapor deposition Silicon-rich;
Step 105: repeat 102-104 step multipass, form multilayer silicon quantum film;
Step 106: diffuse to form PN junction, and the propelling of at high temperature carrying out diffuse source distributes again;
Step 107: at P type crystalline silicon substrate face deposit Si
3N
4Antireflective film;
Step 108: deposit silicon nitride antireflective film, the back side, positive silk screen printing positive and negative electrode electrode;
Step 109: the annealing of silk-screen electrode metal, accomplish the preparation of the efficient crystal silicon solar batteries of short wave response.
Fig. 2 to Fig. 9 is the sketch map that is used for explaining a specific embodiment of the present invention.
See also Fig. 2, be to realize step 101 selection among Fig. 1, the crystal silicon substrate of choosing 201 for commercial 125 monocrystalline or 156 polycrystalline can, substrate type is a P type substrate, monocrystalline resistivity is 0.5-3 Ω cm, polycrystalline resistivity is 0.5-6 Ω cm.The P type crystalline silicon substrate that is to say step 102 is selected from a kind of in p type 125mm * 125mm monocrystalline silicon piece, p type 156mm * 156mm monocrystalline silicon piece and the p type 156 * 156mm polysilicon chip.
See also Fig. 3, it realizes the step 101 among Fig. 1, for utilizing the method for preparing matte on the large-scale production line, is that crystal silicon substrate (that is to say crystal silicon substrate 201) between 180 microns to 250 microns is positioned over prepared NaOH, Na by a certain percentage with thickness
2SiO
3In the Woolen-making liquid that mixes with absolute ethyl alcohol, because chemical reaction takes place, can carry out anisotropic etch to crystal silicon and form matte 301, the shape of matte 301 presents inverted pyramid shape; Wherein the polysilicon mode for preparing matte is slightly different.Because substrate positive and negative in the preparation process are because all place corrosive liquid, so the matte 301 characteristic basically identicals prepared of tow sides.
See also Fig. 4, it realizes the step 102 among Fig. 1, for utilizing flat-plate type PECVD; With silane and hydrogen is deposited gas; Having the P type crystalline silicon substrate of matte 301 (that is to say the matte 301 of crystal silicon substrate 201) surface to carry out the deposition of ultra-thin amorphous silicon membrane, power selection is at 80KW, and gas flow ratio is between 1: 4 to 1: 10; Underlayer temperature is chosen in 400 degree, and then a layer thickness is at the amorphous silicon membrane 302 of 2nm.The thickness of the ultra-thin amorphous silicon membrane 302 that forms in the step (2) is between the 1-15nm.
See also Fig. 5; It realizes the step 103 among Fig. 1, and for after the ultra-thin amorphous silicon membrane 302 of deposit finishes, the mode of utilizing original position formula radiation rapid thermal anneler or chain type rapid thermal annealing is between 700-900 ℃; Annealing time is 20-400s, and rapid thermal annealing forms silicon nanocrystal 401.The size of silicon nanocrystal 401, density can be come Comprehensive Control by thickness, annealing temperature and the annealing time of Si film; Best annealing time and condition need provide the size of quantum dot according to Theoretical Calculation, and pairing ability is with variation and deposition and treatment conditions are set under this size.
See also Fig. 6, it realizes the step 104 among Fig. 1, for utilizing the Si of the rich Si of flat-plate type PECVD deposit
xN film 501.The Si of rich Si
xN film 501 is the non-stoicheiometries that wait, and this point is most important in the deposition preparation.Radio frequency source can be selected 40kHz-13.56MHz, uses silane, ammonia, argon gas, and radio-frequency power is according to the flat 1800W that reaches, and vacuum is set pressure can select 480 degree for the 0.5Pa underlayer temperature, and deposition pressure is adjusted between the 180Pa-220Pa.The entire process process can realize the multi-disc batch process.In gas flow is regulated; The gas flow ratio of silane and ammonia makes that through calculating the atomicity of Si and the ratio of the atomicity of N must be greater than 0.75, promptly; X＞0.75; The thickness of the silicon nitride film 501 of ultra-thin Silicon-rich preferably, makes the thickness of silicon nitride film 501 of ultra-thin Silicon-rich about 10-15nm between 1nm-30nm.
See also Fig. 7; It realizes the step 105 among Fig. 1; For repeating step 102,103, more than 104 time form multilayer silicon quantum dot film 602, an optimum thickness ratio is arranged here, like the silicon quantum dot diameter under the situation of 3nm; The gross thickness of multilayer silicon quantum dot film 602 can be no more than 45nm, repeats 10 cycles.Therefore, number of repetition is preferably in 100 times, and the gross thickness of the multilayer silicon quantum dot film 602 that forms is controlled in the 1000nm.
See also Fig. 8, it realizes the step 106 among Fig. 1, utilizes tubular type stopped pipe diffusion furnace; Liquid POCl3 is a diffuse source; P type crystalline silicon substrate to having multilayer silicon quantum dot film 602 carries out phosphorous diffusion, forms PN junction, after diffusion finishes; Close POCl3 diffuse source, and original position is carried out the propelling and the distribution again of the phosphorus of the constant surface concentration of high temperature; The temperature that high temperature advances is between 500-1500 ℃, and advancing distribution time is 1s-10h again, and the logical nitrogen of this process is protected.Particularly, be the diffusion of POCl3 701, the diffusion furnace temperature can be 300 ℃ to 1300 ℃ variations.Choose diffusion temperature between 850-950 ℃, diffuse source is liquid POCl
3Can realize the diffusion of single face PN junction, also can realize the double-sided PN junction diffusion.In this example, be diffused as example with the single face PN junction, its junction depth of the PN junction that diffuses out has expanded the multilayer silicon quantum dot and has passed through between 200-500nm; In the diffusion process, look for one to accompany (reference sample), so that make formed square resistance change after having spread about 20-120 Ω/.Because in the diffusion process, can form phosphorosilicate glass at battery surface, it can influence the efficient of battery, therefore with HF acid, HNO
3The acid and the hybrid corrosion liquid of water are eliminated phosphorosilicate glass, clean up and dry with deionized water after having removed phosphorosilicate glass.
Please consult Fig. 8 once more, it also realizes the step 107 among Fig. 1, is Si
3N
4The deposition of antireflective coating 601.Substrate is put in tubular type or the flat-plate type PECVD again growth Si
3N
4Film 601, film thickness monitoring is between 70-120nm.For the individual layer antireflective film situation of crystal silicon battery, it is best that its anti-reflection effect to light can reach.
See also Fig. 9, it realizes step 108 and step 109 among Fig. 1, for positive and negative electrode prepares process.Utilize silk screen printing that aluminum slurry is printed in cell backside, form aluminium back of the body field plate, finish printing the back and also solidify, form the positive electrode 801 at the back side 200 ℃ of heat treatments.Then with screen process press at front surface coated negative electrode silver paste, form grid line and busbar, finish printing the back 200 ℃ of heat treatments and solidify, form the negative electrode 802 in front.Last annealed alloy mode according to large-scale production line; The negative electrode 802 of frontal, the positive electrode at the back side 801 carry out the staged thermal anneal process from 300 ℃ to 900 ℃, the final preparation of accomplishing based on the efficient crystal silicon solar batteries of good short wave response of multilayer Si quantum dot.
The present invention utilizes the quantum limitation effect of Si quantum dot; When changing the exciton Bohr radius cause through the quantum dot size with the size compared plan; Broadening takes place in being with of Si quantum dot; Can absorb high-energy photon (350-600nm), the relaxation heating process of high-energy photon is suppressed, and then photo-generated carrier is effectively separated by PN junction; Can promote the quantum efficiency of 350-600nm wave band effectively, make photoelectric current increase, finally reach aim of efficient conversion; Processing step with increase is few, can with the process compatible on the big production line, be easy to realize characteristics such as large-scale production, finally reach the purpose that reduces cost; After the surface had multilayer silicon quantum dot structure, the change that silicon amount point can be with can absorb high-energy photon, and formed superlattice structure between silicon quantum dot layer and the layer, except that can fully absorbing the short wavelength light, also helped the separation of photo-generated carrier and transported.
The above preparation technology only is preferred embodiment of the present invention, is not the present invention is done any pro forma restriction; Though the present invention discloses as above with preferred embodiment; Yet be not in order to limiting the present invention, anyly be familiar with the professional and technical personnel, in not breaking away from technical scheme scope of the present invention; When the technology contents of above-mentioned announcement capable of using is made a little change or is modified to the equivalent embodiment of equivalent variations; In every case be the content that does not break away from technical scheme of the present invention, to any simple modification, equivalent variations and modification that above embodiment did, all still belong in the scope of technical scheme of the present invention according to technical spirit of the present invention.
Claims (10)
1. based on the short wave response crystal silicon solar batteries preparation method of multilayer silicon quantum dot, it is characterized in that: it comprises following processing step:
(1), preparation making herbs into wool face on P type crystalline silicon substrate;
(2), utilize dull and stereotyped plasma-reinforced chemical vapor deposition, carry out the deposition of amorphous silicon membrane at the P type crystalline silicon substrate surface that matte is arranged;
(3), to depositing the P type crystalline silicon substrate of amorphous silicon membrane, utilize rapid thermal annealing process to form silicon quantum dot;
(4),, utilize dull and stereotyped plasma-reinforced chemical vapor deposition, carry out the silicon nitride film deposition of Silicon-rich again, form the preparation of one deck silicon quantum dot film forming the P type crystalline silicon substrate of silicon quantum dot;
(5), repeating step (2) to step (4) is repeatedly accomplished the preparation of multilayer silicon quantum dot film;
(6), utilize tubular type stopped pipe diffusion furnace, the P type crystalline silicon substrate with multilayer silicon quantum dot film is carried out phosphorous diffusion, form PN junction, and under 500-1500 ℃ of temperature, carry out the propelling of constant surface concentration diffuse source;
(7), utilize tubular type or flat plasma-reinforced chemical vapor deposition method at P type crystalline silicon substrate face deposit Si
3N
4Antireflective film;
(8), frontal is deposited with Si
3N
4The P type crystalline silicon substrate of antireflective film carries out the silk screen printing of positive and negative electricity respectively in its back side and front;
(9), the P type crystalline silicon substrate to after the silk screen printing carries out the annealing of silk-screen electrode, accomplishes the preparation based on the short wave response crystal silicon solar batteries of multilayer silicon quantum dot.
2. the short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot as claimed in claim 1 is characterized in that: the P type crystalline silicon substrate in the step (1) is selected from a kind of in p type 125mm * 125mm monocrystalline silicon piece, p type 156mm * 156mm monocrystalline silicon piece and the p type 156 * 156mm polysilicon chip.
3. the short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot as claimed in claim 1 is characterized in that: the thickness of the amorphous silicon membrane that forms in the step (2) is between the 1-15nm.
4. the short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot as claimed in claim 1; It is characterized in that: the rapid thermal annealing process of step (3); Utilize the chain type annealing furnace, under the nitrogen atmosphere protection, anneal with the mode of rapid thermal annealing; Or utilize band to carry out in-situ annealing with the panel PECVD of rapid thermal annealing equipment; The highest annealing temperature of rapid thermal annealing process is between 700-900 ℃, and annealing time is 20-400s.
5. the short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot as claimed in claim 1, it is characterized in that: the molecular formula of the silicon nitride film of the Silicon-rich in the step (4) is Si
xN, wherein, x＞0.75, the thickness of the silicon nitride film of Silicon-rich is between 1nm-30nm.
6. the short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot as claimed in claim 1; It is characterized in that: the number of times of the repeating step (2) in the step (5) to step (4) is in 100 times, and the gross thickness of the multilayer silicon quantum dot film that forms is in 1000nm.
7. the short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot as claimed in claim 1 is characterized in that: in the step (6), utilize tubular type stopped pipe diffusion furnace; Liquid POCl3 is a diffuse source; P type crystalline silicon substrate to having multilayer silicon quantum dot film carries out phosphorous diffusion, forms PN junction, after diffusion finishes; Close POCl3 diffuse source, and original position is carried out the propelling and the distribution again of the phosphorus of the constant surface concentration of high temperature; The temperature that high temperature advances is between 500-1500 ℃, and advancing distribution time is 1s-10h again, and the logical nitrogen of this process is protected.
8. the short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot as claimed in claim 1 is characterized in that: the Si in the step (7)
3N
4The thickness of antireflective film is between 70nm-120nm.
9. the short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot as claimed in claim 1; It is characterized in that: in the step (8), utilize screen process press, silk screen printing aluminum paste material is carried out at the back side; At positive printed silver slurry, form the positive pole and the negative pole of battery respectively.
10. the short wave response crystal silicon solar batteries preparation method based on the multilayer silicon quantum dot as claimed in claim 1; It is characterized in that: annealed alloy in the step (9); Positive negative electrode, the positive electrode at the back side be annealed alloy simultaneously, accomplishes the preparation based on the short wave response crystal silicon solar batteries of multilayer silicon quantum dot.
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| CN103972079A (en) * | 2014-04-01 | 2014-08-06 | 三峡大学 | Preparation method for ordered silicon quantum dots in three-dimensional space |
| CN107785447A (en) * | 2016-08-25 | 2018-03-09 | 比亚迪股份有限公司 | A kind of crystal silicon solar energy battery and preparation method thereof |
| CN110246908A (en) * | 2019-07-18 | 2019-09-17 | 深圳黑晶光电科技有限公司 | Antireflective film, production method and lamination solar cell are converted under a kind of spectrum |
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| CN110246908A (en) * | 2019-07-18 | 2019-09-17 | 深圳黑晶光电科技有限公司 | Antireflective film, production method and lamination solar cell are converted under a kind of spectrum |
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Application publication date: 20121024 |