WO2013058291A1 - 半導体素子の接合方法および接合構造 - Google Patents
半導体素子の接合方法および接合構造 Download PDFInfo
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- WO2013058291A1 WO2013058291A1 PCT/JP2012/076867 JP2012076867W WO2013058291A1 WO 2013058291 A1 WO2013058291 A1 WO 2013058291A1 JP 2012076867 W JP2012076867 W JP 2012076867W WO 2013058291 A1 WO2013058291 A1 WO 2013058291A1
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- semiconductor element
- bonding
- solar cell
- semiconductor
- conductive nanoparticles
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Definitions
- the present invention relates to a semiconductor element bonding method and a bonding structure.
- High performance of the semiconductor device can be achieved by bonding individual semiconductor elements.
- a solar cell that is a photoelectric conversion semiconductor element a solar cell having different band gaps is stacked to be multi-junction, thereby absorbing a wide sunlight spectrum and improving photoelectric conversion efficiency.
- Such a multi-junction solar cell generally has a monolithic stack structure in which III-V group semiconductor cells (GaAs-based) are formed by batch growth on a GaAs substrate or Ge substrate.
- GaAs-based III-V group semiconductor cells
- the bottom cell is sensitive to a long wavelength band.
- the performance exceeding 40% is obtained by applying Ge or InGaAs system.
- these material combinations are lattice-mismatched systems, so that the growth technique is complicated and increases costs.
- the smart stack structure that has recently attracted attention is a structure that allows multiple cells to be mechanically joined together, and can easily combine various cells. It is a key technology for next-generation solar cells from the viewpoint of high performance and low cost. is there.
- the smart stack structure it is important to realize a junction structure that ensures transparency as well as conductivity at the junction interface of each solar cell. It is also important to realize optical characteristics that are advantageous for solar cell characteristics, equivalent to or more than ensuring transparency.
- conductive nanoparticles covered with organic molecules having a diameter size of 100 nanometers or less are used, and between conductive nanoparticles using melting point reduction based on nano-sizing.
- a method for joining semiconductor elements based on low-temperature sintering has been reported.
- Patent Documents 1 and 2 non-contact of a particulate metal compound or metal nanowire is caused by thermal expansion of an organic polymer resin induced by heat generated from the element itself or a change in ambient temperature during operation of the device after bonding. May occur, leading to a decrease in conductivity or deactivation. Moreover, in order to maintain the light transmittance, it is necessary to reduce the concentration of the particulate metal compound or the metal nanowire, which adversely affects the conductivity.
- the conductive nanoparticles having a diameter of 100 nanometers or less that are used are usually covered with a protective film made of organic molecules for the purpose of improving handleability.
- a protective film made of organic molecules for the purpose of improving handleability.
- the concentration of the conductive nanoparticles is lowered, and the conductive nanoparticles are uniformly present at the interface, thereby generating a large conductive nanoparticle sintered body.
- the bonding itself can be difficult.
- Non-Patent Document 1 Non-Patent Document 1
- Non-Patent Document 2 Non-Patent Document 2
- semiconductor elements can be conductively bonded to each other without using an adhesive such as an organic molecule or an adhesive material via metal (conductive) nanoparticles arranged on the surface. Has not been studied at all.
- the present invention is a technique developed to compensate for the weaknesses of the existing techniques for bonding semiconductors as described above, and its purpose is to bond semiconductor elements while ensuring excellent conductivity and transparency at the interface. It is to provide a method and a joining structure by the joining method. Another object of the present invention is to provide a semiconductor element bonding method capable of ensuring excellent electrical conductivity at the interface and designing optical characteristics that favor the element characteristics, and a bonding structure by the bonding method. There is.
- the present inventor has generally used organic molecules, etc., even when conductive nanoparticles not covered with organic molecules are arranged at the interface of the semiconductor element to be joined. It has been found that both semiconductor elements can be joined without using any adhesive or bonding material, and the semiconductor elements can be conductively connected.
- the bonding method of the present invention is based on the above-mentioned knowledge based on the above-mentioned object.
- a monolayer (single layer) of conductive nanoparticles not covered with organic molecules is arranged on the surface of a semiconductor element, The other semiconductor element is bonded to the substrate.
- the present invention has the following characteristics.
- a method for bonding semiconductor elements comprising arranging conductive nanoparticles not covered with organic molecules on the surface of one semiconductor element and pressing the other semiconductor element on the conductive nanoparticle.
- the conductive nanoparticles are composed of Pd, Au, Ag, Pt, Ni, Al, In, In 2 O 3 , Zn, ZnO, or a composite thereof.
- the semiconductor element is a single-junction solar cell using a crystalline Si, amorphous Si, microcrystalline Si, organic, or chalcopyrite material, or a GaAs, InP, GaSb, or Ge substrate.
- (14) The semiconductor element laminate according to (13), wherein the semiconductor element having a photoelectric conversion function is a solar cell.
- a semiconductor element bonding structure excellent in conductivity and transparency can be obtained.
- a wide sunlight spectrum can be absorbed and the photoelectric conversion efficiency can be improved.
- photoelectric conversion efficiency can be improved also by the optical confinement effect using the optical characteristic derived from a nanostructure.
- the schematic diagram which shows the cross section of the junction structure of the semiconductor element in the embodiment using the joining method of this invention Illustration of hexagonal array shown by atomic force microscope image of block copolymer thin film used in Examples of the present invention Example of hexagonal array of metal nanostructures created by the shape pattern stamp used in the embodiment of the present invention Schematic diagram showing a cross section of a junction structure of a GaAs / CIGSe-based two-junction solar cell fabricated according to an embodiment of the present invention.
- (a) is the IV characteristic of a GaAs / CIGSe two-junction solar cell fabricated according to an embodiment of the present invention
- (b) is the IV characteristic of a GaAs / CIGSe two-junction solar cell not including palladium nanoparticles.
- (a) is an IV characteristic of a GaAs / InP-based two-junction solar cell fabricated according to an embodiment of the present invention
- (b) is an IV characteristic of a GaAs / InP-based two-junction solar cell not including gold nanoparticles.
- Schematic diagram showing a cross section of the junction structure of an amorphous silicon / crystalline silicon-based two-junction solar cell fabricated according to an embodiment of the present invention Schematic diagram showing a cross section of a junction structure of a GaAs / InP-based two-junction solar cell fabricated according to an embodiment of the present invention.
- FIG. 1 is a schematic view showing a cross section of a junction structure of a semiconductor element using the joining method of the present invention.
- the junction structure 101 includes a bottom semiconductor element 102 and a top semiconductor element 103, and the junction structure 101 is joined in a state where conductive nanoparticles 104 exist.
- the bottom semiconductor element 102 and the top semiconductor element 103 preferably have a semiconductor layer or a conductive layer on each bonding surface. In that case, the semiconductor layer on one bonding surface and / or the semiconductor layer on the other bonding surface And / or the conductive layer is conductively connected through the conductive nanoparticles 104.
- the number of semiconductor elements bonded to each other is not limited to one pair, but it is desirable to set the number of the semiconductor elements in a range in which necessary translucency is ensured.
- a light-transmitting element or a photoelectric conversion element is preferably used as the semiconductor element to be bonded.
- the photoelectric conversion element is preferably one that converts light into electric energy like a solar cell, but conversely, one that converts electric energy into light may be used.
- Solar cells include GaAs-based solar cells, CIS-based (chalcopyrite) solar cells, GaAs, InP, GaSb, or compound systems such as solar cells consisting of one or more junctions stacked on a Ge substrate.
- Examples thereof include silicon solar cells such as solar cells, Si crystal solar cells, amorphous Si solar cells, and microcrystalline Si solar cells, organic solar cells, and dye-sensitized solar cells.
- the conductive nanoparticles include metal nanoparticles such as Pd, Au, Ag, Pt, Ni, Al, Zn, and In, and metal oxide nanoparticles such as ZnO and In 2 O 3 .
- the size of the conductive nanoparticles is preferably 10 nanometers or more, more preferably 20 nanometers or more, and even more preferably 30 nanometers or more.
- the nanoparticles in order to suppress absorption and scattering of light by the nanoparticles, it is preferably 100 nanometers or less, more preferably 80 nanometers or less, further preferably 60 nanometers or less, but 200 nanometers or less (more If it is preferably 150 nanometers or less, more preferably 120 nanometers or less, light absorption / scattering can be suppressed more than that of 200 nanometers or more.
- it in order to promote the light confinement effect by introducing nanoparticles, it is preferably 120 nanometers or more and 500 nanometers or less, more preferably 150 nanometers or more and 300 nanometers or less, and further preferably 180 nanometers or more and 250 nanometers or less. It is below nanometer.
- the conductive nanoparticles are not covered with a protective film such as organic molecules, an adhesive or an adhesive material, and form a monolayer in which individual independent particles are uniformly arranged.
- a protective film such as organic molecules, an adhesive or an adhesive material
- it can be arranged in a (pseudo-positive) hexagonal array in which six particles form a hexagon around any one particle.
- the arrangement interval of the conductive nanoparticles preferably has a distance of at least 2 times the size of the nanoparticles (more preferably 3 times or more) in order to transmit light well.
- it is preferably 10 times or less (more preferably 7 times or less).
- the arrangement interval is 80 nanometers or more and 400 nanometers or less.
- the conductive nanoparticles are in ohmic contact with the upper and lower semiconductor elements and are uniformly arranged at the interface, excellent conductivity can be obtained.
- excellent light transmittance can be obtained.
- the arrangement interval is not less than 400 nanometers and not more than 2000 nanometers.
- the conductive nanoparticles are in ohmic contact with the upper and lower semiconductor elements and are uniformly arranged at the interface, excellent conductivity can be obtained.
- the optical properties of the nanoparticles and the nanoparticle arrangement also provide a light confinement effect that favors device properties.
- the arrangement interval L of the conductive nanoparticles in the present invention is defined as follows.
- the joining structure of the present invention can be formed as follows. First, a block copolymer thin film is formed on the surface of the bottom semiconductor element 102 to be bonded.
- a block copolymer thin film is formed on the surface of the bottom semiconductor element 102 to be bonded.
- a block copolymer consisting of polystyrene (hydrophobic moiety) and poly-2-vinylpyridine (hydrophilic moiety) dissolved in an organic solvent such as toluene or ortho-xylene is used to form thin films such as spin coating and dip coating. Apply by technique.
- the surface of the bottom semiconductor element 102 obtained in this way has a poly-2-vinylpyridine block patterned like the white portion shown in FIG. 2 by phase separation of the block copolymer.
- this semiconductor element is immersed in an aqueous solution in which a metal ion salt such as Na 2 PdCl 4 is dissolved.
- a metal ion salt such as Na 2 PdCl 4
- the resulting semiconductor element is subjected to block copolymer removal treatment and metal ion reduction treatment to produce an array of conductive nanoparticles that are not covered with organic molecules while retaining the pattern.
- the top semiconductor element 101 is overlaid on the bottom semiconductor element 102 on which the conductive nanoparticles are arranged, and both are bonded under moderate pressure and heating.
- This bonding does not use an organic or inorganic adhesive or bonding material, and may be based on van der Waals force alone, or a direct bonding method through surface activation or thermal solid phase diffusion. It may be by law.
- a known surface activation treatment method such as plasma treatment, ozone treatment, treatment with an ion beam or the like can be used.
- amphiphilic block copolymer used above is not particularly limited to those composed of polystyrene and poly-2-vinylpyridine, and known ones can be used.
- poly-4-vinylpyridine polyethylene oxide, polypropylene oxide, polymethacrylic acid, polymethyl methacrylate, poly-N-isopropylacrylamide, polysiloxane, polyferrocenyldimethylsilane, polyvinylpyrrolidone, polyethylene, polybutadiene, polyisobutylene, polyvinyl
- the metal ion salt is not particularly limited to Na 2 PdCl 4 , for example, H 2 PdCl 4 , H 2 PdCl 6 , Na 2 PdCl 6 , K 2 PdCl 4 , K 2 PdCl 6 , Na 2 PdBr 4 , K 2 PdBr 4 , K 2 Pd (CN) 4 , K 2 Pd (NO 3 ) 4 , (NH 4 ) 2 PdCl 4 , (NH 4 ) 2 PdCl 6 , Pd (OH) 2 , PdCl 2 , PdBr 2, PdI 2, Pd ( NO 3) 2, Pd (CN) 2, PdSO 4, Pd (OCOCH 3) 2, Pd (OCOCF 3) 2, Pd (C 5 H 7 O 2) 2, palladium etc.
- ion salts HAuCl 4, NaAuCl 4, KAuCl 4, NH 4 AuCl 4, AuCN, KAuCN 2, AuCl, AuCl 3, AuBr, AuI 3, AuCl, AuI 3, Au (OCOCH 3) 3, a gold ion salts and the like, AgNO 3 , AgClO 4 , AgCN, AgSCN, KAg (CN) 2 , Ag 2 CO 3 , Ag 2 SO 4 , AgOCOCH 3 , and other silver ion salts, H 2 PtCl 6 , Na 2 PtCl 4 , Na 2 PtCl 6 , K 2 PtCl 4 , K 2 PtCl 6 , Na 2 PtBr 4 , K 2 PtBr 4 , K 2 Pt (CN) 4 , K 2 Pt (NO 3 ) 4 , (NH 4 ) 2 PtCl 4 , (NH 4 ) 2 PtCl 6, Pt (OH) 2 , P
- the block copolymer removal treatment and metal ion reduction treatment described above are preferably carried out by one-stage treatment, but may be carried out by combining a plurality of stages of treatment.
- Examples of such treatment include ultraviolet ray or electron beam irradiation, plasma treatment, chemical reduction method, or electrochemical reduction method.
- plasma treatment and ultraviolet treatment are preferable.
- the block copolymer thin film as a template is selectively etched by argon plasma and removed from the element surface, while metal ions are not etched by argon plasma, Reduced by the electrons present in
- the gas for plasma treatment is not particularly limited to argon gas, and for example, a mixed gas in which argon and hydrogen are mixed at an arbitrary ratio can be used.
- oxygen gas it is also possible to obtain conductive nanoparticles (ZnO, In 2 O 3, etc.) made of an oxide.
- the junction structure of the present invention can also be formed as follows using a known microcontact printing method as a method for arranging conductive nanoparticles.
- a stamp made of a polymer such as polydimethylsiloxane (PDMS) having minute convex portions formed in a predetermined distribution pattern on the stamp surface is prepared.
- the stamp surface can be formed by a known method such as electron beam lithography after stamp molding, photolithography and etching, or can be formed by an uneven pattern on the mold surface during molding.
- the top surfaces of the minute convex portions are formed in a size corresponding to the planar size of the conductive nanoparticles described above, and are formed in the same arrangement interval and distribution pattern as the conductive particles.
- a conductive thin film such as Ag is deposited on the stamp surface having such a three-dimensional nanoscale structure by thermal evaporation, electron beam evaporation, sputtering, or the like.
- the three-dimensional shape stamp with the conductive thin film thus obtained is pressed so that only the convex portion of the stamp is in contact with the surface of the semiconductor element surface-treated with the compound having a functional group terminal to which the conductive nanoparticles are selectively bonded.
- the conductive thin film having only the contact portion can be transferred onto the semiconductor element by the interaction between the surface of the conductive thin film substance and the functional group terminal.
- the compound having a functional group terminal is removed, and ultraviolet or electron beam irradiation, plasma treatment, or the like is performed so that the conductive thin film is directly bonded to the semiconductor element.
- the top semiconductor element 101 is overlaid on the bottom semiconductor element 102 on which the conductive nanoparticles are arranged, and both are bonded under moderate pressure and heating.
- This bonding does not use an organic or inorganic adhesive or bonding material, and may be based on van der Waals force alone, or a direct bonding method through surface activation or thermal solid phase diffusion. It may be by law.
- a known surface activation treatment method such as plasma treatment, ozone treatment, treatment with an ion beam or the like can be used.
- the conductive thin film is not particularly limited to Ag.
- metals such as Au, Cu, Pt, Pd, and Al, or conductive oxides such as In 2 O 3 and ZnO can be used.
- examples of the functional group to which the conductive nanoparticles of the above compound are bonded include an amino group and a thiol group.
- the compound having a functional group terminal is preferably a compound that can form a self-assembled monolayer (SAM) (SAM-forming compound), but is not limited thereto.
- SAM self-assembled monolayer
- trialkoxysilanes having a terminal thiol group such as 3-mercaptopropyltrimethoxysilane-4-mercaptophenyltrimethoxysilane, and terminal amino groups such as 3-aminopropyltrimethoxysilane-4-aminophenyltrimethoxysilane
- the trialkoxysilane which has is mentioned.
- the microcontact printing method used for arranging the conductive nanoparticles is not limited to the above-described one, and any method that can be used for the semiconductor element bonding method of the present invention, Any thing is good.
- a stamp surface SAM-forming compound formed in a predetermined distribution pattern may be transferred to the surface of a semiconductor element, and conductive nanoparticles may be deposited on the transferred SAM.
- the planar shape and array pattern of the conductive nanoparticles depend on the uneven pattern on the stamp surface. Therefore, within the range of microfabrication performance when forming the stamp surface, the planar shape of the conductive nanoparticles, the arrangement pattern can be set arbitrarily, compared to the case of forming a block copolymer thin film as a template, The degree of freedom in designing the planar shape and arrangement pattern of the conductive nanoparticles is greatly improved. Therefore, it is possible to obtain a conductive nanoparticle planar shape and arrangement pattern that are desirable in terms of optical property design and the resulting light confinement effect.
- Such desirable conductive nanoparticle planar shape is spherical, hemispherical, cylindrical, or ellipsoidal, and the arrangement pattern is hexagonal, regular hexagonal (or pseudo-regular hexagonal), tetragonal, Examples include a square shape (or pseudo-square shape) [In addition, “pseudo ... shape” in each shape means that the standard deviation of the side length in each shape is within 30% of the average side length (preferably within 20%) , More preferably within 10%). ].
- FIG. 4 shows an example of a photoelectric conversion semiconductor element (solar cell) as one of the embodiments.
- a case is shown in which two solar cells composed of a cell 301 having an Al 0.3 Ga 0.7 As light absorption layer as a top solar cell and a cell 302 having a CIGSe semiconductor layer as a bottom solar cell are joined.
- the GaAs solar cell 301 includes a p-type GaAs buffer layer 303, a p-type Al 0.3 Ga 0.7 As light absorbing layer 304, an n-type GaAs emitter layer 305, an n-type GaAs contact layer 306, and an n-type electrode AuGeNi 307.
- the n-type electrode has a comb shape to receive sunlight.
- the CIGSe-based solar cell 302 includes a Mo electrode 309, a CIGSe semiconductor layer 310, a CdS emitter layer 311, and a ZnO transparent conductive layer 312 on a glass substrate 308.
- the nanoparticles 313 are arranged on the surface of the CIGSe solar cell 302. In this example, Pd nanoparticles were used.
- the Pd nanoparticles 313 were arranged on the CIGSe solar cell 302 by forming a thin film of polystyrene-poly-2-vinylpyridine as a block copolymer and using it as a template. That is, a 0.5 wt% ortho-xylene solution of polystyrene-poly-2-vinylpyridine (polystyrene molecular weight: 133000 g / mol, poly-2-vinylpyridine molecular weight: 132000 g / mol) having a total molecular weight of 265000 g / mol was applied to the surface of the CIGSe cell 302. A thin film was formed by spin coating.
- the solar cell 302 was immersed in a 1 mM Na 2 PdCl 4 aqueous solution for 300 seconds. After washing with water, this cell was treated with argon plasma to arrange palladium nanoparticles 313 having an average size of 50 nanometers not covered with organic molecules. The average array spacing between palladium nanoparticles in this arrangement was 100 nanometers. After that, in this example, they were joined by pressure bonding. That is, water was dropped on the CIGSe cell 302, the GaAs cell 301 was set, and both elements were temporarily joined using surface tension. Thereafter, pressurization was performed for 30 minutes or more in a heated state at 150 ° C., and bonding was performed in a state where Pd nanoparticles 313 were present between the elements.
- the solar cell is not particularly limited to GaAs-based and CIGSe-based solar cells.
- a solar cell composed of one junction or two junctions or more laminated on an InP or GaSb substrate, or a Si crystal solar cell.
- Examples include batteries, amorphous Si solar cells, microcrystalline Si solar cells, organic solar cells, sensitized solar cells, solar cells using chalcopyrite materials, and other solar cell combinations.
- the bonding technique is not particularly limited to the pressure bonding, and can be applied to general direct bonding of elements by surface activation using, for example, plasma or ion beam.
- the conductive nanoparticles are not particularly limited to Pd, and have conductivity such as metal nanoparticles such as Au, Ag, Pt, Ni, Al, Zn, In, or ZnO, In 2 O 3 Metal oxide nanoparticles and the like are possible.
- the size of the conductive nanoparticles is not limited to 50 nanometers, and can be applied in the range of 10-200 nanometers.
- the arrangement interval of the conductive nanoparticles is not limited to 100 nanometers, and may be any distance as long as the distance is 2 to 10 times the nanoparticle size.
- FIG. 5 shows the IV characteristics of the solar cell.
- (a) shows the characteristics of the solar cell manufactured according to the embodiment of the present invention
- (b) shows the characteristics of the junction structure without interposing Pd nanoparticles.
- an open-circuit voltage of 1.62 V and a fill factor of 0.53 are obtained, and characteristics that match the predicted characteristics (open-circuit voltage of 1.92 V) in a two-junction cell are obtained.
- the IV characteristics are greatly degraded.
- the open circuit voltage is 1.65V, but the fill factor has dropped to 0.23.
- the junction resistance is estimated from each characteristic, it is 200 ⁇ cm 2 or more in the conventional structure and 10 ⁇ cm 2 in the structure of the present invention. That is, the difference in junction resistance leads to the improvement of IV characteristics.
- FIG. 6 shows an example of a photoelectric conversion semiconductor element (solar cell) as one of the embodiments.
- a case is shown in which two solar cells composed of a cell 501 having a GaAs light absorption layer as a top solar cell and a cell 502 having an InP semiconductor layer as a bottom solar cell are joined.
- a GaAs solar cell 501 includes a p-type GaAs buffer layer 503, a p-type GaAs light absorption layer 504, an n-type GaAs emitter layer 505, an n-type Ga 0.51 In 0.49 P / p-type Ga 0.51 In 0.49 P (506/507) tunnel.
- the n-type electrode has a comb shape to receive sunlight.
- An InP-based solar cell 502 includes a p-type InP buffer layer 513, a p-type In 0.91 Ga 0.09 As 0.2 P 0.8 light absorption layer 514 (band gap energy 1.2 eV), an n-type In 0.91 Ga 0.09 As 0.2 on an InP substrate 512.
- a P 0.8 emitter layer 515 and an n-type InP layer 516 are formed.
- a nanoparticle array 517 is formed on the surface of the InP solar cell 502.
- Au nanoparticles were used.
- the InGaAsP composition is a design factor, and the composition can be freely adjusted according to the target characteristics.
- the Au nanoparticles 517 were arranged on the InP solar cell 502 by making a polystyrene-poly-2-vinylpyridine film as a block copolymer and using it as a template. That is, a 0.3 wt% toluene solution of polystyrene-poly-2-vinylpyridine (polystyrene molecular weight: 125000 g / mol, poly-2-vinylpyridine molecular weight: 58500 g / mol) having a total molecular weight of 183500 g / mol was applied to the surface of InP solar cell 502. A thin film was formed by spin coating.
- the solar cell 502 was immersed in a 1 mM KAuCl 4 aqueous solution for 600 seconds. After washing with water, this cell was treated with argon plasma to align and arrange Au nanoparticles 517 having an average size of 10 nanometers not covered with organic molecules. The average spacing between Au nanoparticles in this arrangement was 30 nanometers. After that, in this example, they were joined by pressure bonding. That is, water was dropped into the InP-based cell 502, the GaAs-based cell 501 was set, and both elements were temporarily joined using surface tension. Thereafter, pressurization was performed for 30 minutes or more in a heated state at 150 ° C., and bonding was performed in a state where Au nanoparticles 517 were present between the elements.
- FIG. 7 shows the IV characteristics of the solar cell.
- (a) shows the characteristics of the solar cell manufactured according to the present example
- (b) shows the characteristics of the junction structure in which no Au nanoparticles are interposed.
- an open circuit voltage of 2.90 V and a fill factor of 0.69 are obtained, and characteristics that match the predicted characteristics (open circuit voltage of 2.97 V) in a three-junction cell are obtained.
- the IV characteristics are greatly degraded. In other words, the open circuit voltage is 2.56V, but the fill factor is reduced to 0.45.
- the present invention structure When estimating the junction resistance than each characteristic, in the conventional structure is a 200Omucm 2 or more, in the present invention structure is 20 .OMEGA.cm 2 or less. That is, the difference in junction resistance leads to the improvement of IV characteristics.
- the structure having the InGaAsP light absorption layer 514 on the InP substrate 512 is used as the bottom cell.
- the present invention can also be applied to a structure in which an InGaAsP light absorption layer or an InGaAs strained light absorption layer is similarly formed on the Ge substrate. .
- FIG. 8 shows an example of a photoelectric conversion semiconductor element (solar cell) as one of the embodiments.
- a photoelectric conversion semiconductor element solar cell
- FIG. 8 shows an example of a photoelectric conversion semiconductor element (solar cell) as one of the embodiments.
- Amorphous Si solar cell 701 includes ZnO transparent conductive layer 703, n-type amorphous Si layer 704, i-type amorphous Si light absorption layer 705, p-type amorphous Si layer 706, fluorine-doped SnO 2 transparent conductive layer 707, and glass substrate 708.
- a photoelectric conversion semiconductor element solar cell
- the crystalline silicon solar cell 702 includes an n-type crystalline Si layer 710, a p-type crystalline Si layer 711, and an ITO transparent conductive layer 712 on an Al electrode 709.
- a nanoparticle array 713 is formed on the surface of the crystalline Si solar cell 702. In this example, Pt nanoparticles were used.
- Pt nanoparticles 713 were arranged on a crystalline silicon cell by forming a thin film of polystyrene-poly-4-vinylpyridine as a block copolymer and using it as a template. That is, a 0.6 wt% toluene solution of polystyrene-poly-4-vinylpyridine (polystyrene molecular weight: 20000 g / mol, poly-4-vinylpyridine molecular weight: 19000 g / mol) having a total molecular weight of 39000 g / mol was applied to the surface of the crystalline Si solar cell 702. A thin film was formed by spin coating.
- the solar cell 702 was immersed in a 1 mM Na 2 PtCl 4 aqueous solution for 1800 seconds. After washing with water, this cell was treated with argon plasma to align and arrange Pt nanoparticles 712 having an average size of 20 nanometers that were not covered with organic molecules. The average spacing between Pt nanoparticles in this arrangement was 40 nanometers. After that, in this example, they were joined by pressure bonding. That is, water was dropped onto the crystalline silicon cell 702, the amorphous silicon cell 701 was set, and both elements were temporarily bonded using surface tension. Thereafter, pressure was applied for 30 minutes or more in a heated state at 150 ° C., and bonding was performed in a state where Pt nanoparticles 712 were present between the elements.
- the solar cell operation according to this example will be described.
- the former obtained an open-circuit voltage of 1.45 V and a fill factor of 0.63.
- a characteristic that matches the predicted characteristic (open circuit voltage 1.5V) was obtained.
- the open circuit voltage was 1.40V, but the fill factor decreased to 0.25.
- the junction resistance is estimated from each characteristic, it is 100 ⁇ cm 2 or more in the conventional structure, and 10 ⁇ cm 2 or less in the example structure of the present invention. That is, the difference in junction resistance leads to the improvement of IV characteristics.
- Example 1-3 in the structure of the present invention, by arranging the monolayers of conductive nanoparticles at various solar cell bonding interfaces and bonding them in that state, the light transmittance at the interfaces can be improved. By significantly improving the junction resistance without loss, good solar cell characteristics can be obtained.
- the application of the present invention is not limited to solar cells, and can be widely applied to bonding of semiconductor elements that require electrical conductivity and light transmittance.
- FIG. 9 shows an example of a photoelectric conversion semiconductor element (solar cell) as one of the embodiments.
- a case is shown in which two solar cells composed of a cell 901 having a GaAs-based light absorption layer as a top solar cell and a cell 902 having an InP-based semiconductor layer as a bottom solar cell are joined.
- a GaAs solar cell 901 includes a p-type GaAs buffer layer 903, a p-type GaAs light absorption layer 904, an n-type GaAs emitter layer 905, an n-type InGaP emitter layer 906, an n-type GaAs contact layer 907, and an n-type electrode AuGeNi 908. Become.
- the n-type electrode has a comb shape to receive sunlight.
- An InP-based solar cell 902 includes a p-type InP buffer layer 910, a p-type In 0.83 Ga 0.17 As 0.37 P 0.63 light absorbing layer 911 (band gap energy 1.15 eV), an n-type In 0.83 Ga 0.17 As 0.37 on an InP substrate 909. It consists of a P 0.63 emitter layer 912 and an n-type InP layer 913.
- a nanoparticle array 914 is formed on the surface of the InP solar cell 902. In this example, Ag nanoparticles were used.
- the InGaAsP composition is a design factor, and the composition can be freely adjusted according to the target characteristics.
- the Ag nanoparticles 914 were arranged on the InP cell by a transfer method using a stamp made of polydimethylsiloxane (PDMS) on which minute protrusions were formed. That is, an Ag thin film having a thickness of 50 nanometers was formed by electron beam evaporation on a PDMS stamp in which a cylindrical structure having a diameter of 230 nanometers and a height of 200 nanometers was arranged in a hexagonal shape with a center distance of 460 nanometers.
- PDMS polydimethylsiloxane
- this Ag thin film stamp was transferred to an InP solar cell 902 having a 3-mercaptopropyltrimethoxysilane SAM film on the surface for 5 minutes at room temperature to transfer the Ag nanoparticle structure by contacting only the convex part, and then the cell As shown in FIG. 3, Ag nanoparticles (cylindrical shape) 914 having a diameter of 230 nanometers and a height of 50 nanometers, which are not covered with organic molecules, were aligned. The center-to-center distance of Ag nanoparticles in this arrangement was 460 nanometers. Thereafter, in this example, the GaAs cell 901 and the InP cell 902 were joined by pressure bonding.
- the conductive nanoparticle monolayers are arranged at the solar cell bonding interface and bonded in that state, thereby realizing conductive connection between different solar cells.
- the application of the present invention is not limited to solar cells, and can be widely applied to the joining of semiconductor elements that require electrical conductivity and optical property design at the interface.
- the present invention relates to a bonding method and a bonding structure of semiconductor elements, and these can be used for multi-junction of semiconductor elements that require conductivity and transparency, or optical characteristic design at a bonding interface.
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Abstract
Description
まず、特許文献1、2においては、接合後の装置動作時に素子自体から発生する熱や外気温変化などで誘起される有機高分子樹脂の熱膨張により、粒子状金属化合物や金属ナノワイヤの非接触が起こり導電性の低下または失活を招く可能性がある。また、光の透過性を維持するためには、粒子状金属化合物や金属ナノワイヤの濃度を低くする必要があり、これは導電性に対しては不利に働く。
また、上述のように、界面において透明性乃至光の透過性を維持するためには、導電性ナノ粒子濃度を低くし、界面に均一に存在させ、大きな導電性ナノ粒子焼結体の生成を防ぐ必要もある。しかしながら、粒子濃度の低下は、焼結頻度の低下につながるため、接合自体が困難となりうる。
また、本発明の別の目的は、界面において優れた導電性を確保し、かつ素子特性に有利に働く光学特性の設計が可能な半導体素子の接合方法、およびその接合方法による接合構造を提供することにある。
(1)有機分子で覆われていない導電性ナノ粒子を一方の半導体素子表面に配列し、その上に他方の半導体素子を圧着させることを特徴とする半導体素子の接合方法。
(2)前記半導体素子表面への導電性ナノ粒子の配列が、ブロック共重合体薄膜をテンプレートとして形成されることを特徴とする上記(1)に記載の半導体素子の接合方法。
(3)前記半導体素子表面への導電性ナノ粒子の配列が、形状パターンが施されたスタンプを用いる転写手法で形成されることを特徴とする上記(1)に記載の半導体素子の接合方法。
(4)前記導電性ナノ粒子のサイズが、100ナノメートル以上500ナノメートル以下であることを特徴とする上記(1)~(3)のいずれか1項に記載の半導体素子の接合方法。
(5)前記導電性ナノ粒子のサイズが、10ナノメートル以上200ナノメートル以下であることを特徴とする上記(1)又は(2)に記載の半導体素子の接合方法。
(6)前記導電性ナノ粒子の配列間隔が、導電性ナノ粒子サイズの2倍以上10倍以下の距離であることを特徴とする上記(1)~(5)のいずれか1項に記載の半導体素子の接合方法。
(7)前記導電性ナノ粒子が、Pd、Au、Ag、Pt、Ni、Al、In、In2O3、Zn、ZnO、もしくはこれらの複合体からなることを特徴とする上記(1)~(6)のいずれか1項に記載の半導体素子の接合方法。
(8)前記半導体素子が、結晶Si系、アモルファスSi系、微結晶Si系、有機系、もしくは、カルコパイライト系材料を用いた単接合太陽電池、またはGaAs、InP、GaSb、もしくは、Ge基板上等に積層された2接合以上からなる太陽電池であることを特徴とする上記(1)~(7)のいずれか1項に記載の半導体素子の接合方法。
(9)一対の半導体素子の接合構造であって、両方の半導体素子の接合面に有機分子で覆われていない導電性ナノ粒子が介在している半導体素子の接合構造。
(10)両方の半導体素子の接合面に介在する導電性ナノ粒子は、モノレイヤー(単一層)であることを特徴とする上記(9)に記載の半導体素子の接合構造。
(11)一対の半導体素子は、接合面に半導体層又は導電層を有するものである上記(9)又は(10)に記載の半導体素子の接合構造。
(12)上記(9)~(11)のいずれか1項に記載の接合構造を隣接する半導体素子間に備える半導体素子積層体であって、半導体素子積層体の積層方向の一方の端面から、接合面のうち少なくとも最も遠くに位置する接合面までは透光性を具備する半導体素子積層体。
(13)半導体素子が光電変換機能を有するものである上記(12)に記載の半導体素子積層体。
(14)光電変換機能を有する半導体素子が太陽電池である上記(13)に記載の半導体素子積層体。
図1は、本発明の接合方法を利用した半導体素子の接合構造の断面を示す模式図である。図1において、接合構造101はボトム半導体素子102とトップ半導体素子103からなり、これらの間は導電性ナノ粒子104が存在した状態で接合している。
ボトム半導体素子102とトップ半導体素子103は、それぞれの接合面に半導体層又は導電層を有するものが好ましく、その場合、一方の接合面の半導体層及び/又は導電層と他方の接合面の半導体層及び/又は導電層が導電性ナノ粒子104を介して導電接続される。
D=(ΣDi)/n
[ここで、Dは導電性ナノ粒子のサイズ、Diは所定の観察領域に存在する任意の粒子の粒子径〔=(長径+短径)/2〕、nは該観察領域に存在する粒子の個数(nは統計処理上十分に大きな数、通常20以上)]
まず、スタンプ面に微小凸部が所定の分布パターンに形成されたポリジメチルシロキサン(PDMS)等のポリマーからなるスタンプを準備する。該スタンプ面は、スタンプ成形後の電子ビームリソグラフィー、フォトリソグラフィーとエッチング等、公知の手法によって形成できるし、また、成形時に型面の凹凸パターンによっても形成することができる。微小凸部は、その上面が上述の導電性ナノ粒子の平面サイズに対応する大きさに形成され、導電性粒子と同様の配列間隔、分布パターンに形成される。このような3次元のナノスケール構造を有するスタンプ面に、熱蒸着、電子ビーム蒸着、またはスパッタリング等によりAg等の導電性薄膜を堆積させる。
こうして得られた導電性薄膜付き3次元形状スタンプを、導電性ナノ粒子が選択的に結合する官能基末端を有する化合物で表面処理した半導体素子表面にスタンプの凸部分のみが接触するように押し付ける。このとき、導電性薄膜物質表面と官能基末端の相互作用により、接触部のみの導電性薄膜を半導体素子上において転写することができる。転写後、官能基末端を有する化合物を除去し、導電性薄膜が半導体素子に直接的に接合するように、紫外線又は電子線照射、プラズマ処理等を行う。この後、トップ半導体素子101を導電性ナノ粒子が配置されたボトム半導体素子102上に重ね、適度な加圧・加温下で両者の接合を行う。この接合は、有機系や無機系の接着剤乃至接着用材料を用いないものであり、ファンデルワールス力のみによるものであっても良いし、表面活性化を経た直接接合法や熱固相拡散法によるものであっても良い。表面活性化には、プラズマ処理、オゾン処理、イオンビーム等による処理など、公知の表面活性化処理法を用いることができる。
なお、本発明において、導電性ナノ粒子を配列するのに利用するマイクロコンタクトプリント法は、上述のものに限定されず、本発明の半導体素子の接合方法に利用することができるものであれば、どのようなものでも良い。例えば、所定の分布パターンに形成されたスタンプ面のSAM形成性化合物を半導体素子表面に転写し、転写されたSAM上に導電性ナノ粒子を析出するものでも良い。
図4に、本実施形態の一つとして光電変換半導体素子(太陽電池)の例を示す。本実施例においては、トップ太陽電池としてAl0.3Ga0.7As光吸収層を有するセル301、ボトム太陽電池としてCIGSe半導体層を有するセル302からなる2つの太陽電池を接合した場合を示す。GaAs系太陽電池301は、p型GaAsバッファ層303、p型Al0.3Ga0.7As光吸収層304、n型GaAsエミッタ層305、n型GaAsコンタクト層306、およびn型電極AuGeNi 307からなる。n型電極は、太陽光を受光するために、櫛型状の形態を有している。CIGSe系太陽電池302は、ガラス基板308上に、Mo電極309、CIGSe半導体層310、CdSエミッタ層311、ZnO透明伝導層312からなっている。ここで、CIGSe系太陽電池302表面には、ナノ粒子313の配列がなされている。本実施例では、Pdのナノ粒子を用いた。
また、前記接着手法に関しては、圧着に特に制限されることなく、例えばプラズマやイオンビームを用いた表面活性化による素子の直接接合全般に適用できる。
また、導電性ナノ粒子に関しては、Pdに特に制限されることなく、Au、Ag、Pt、Ni、Al、Zn、In等の金属ナノ粒子、またはZnO、In2O3等の導電性を有する金属酸化物ナノ粒子などが可能である。
また、導電性ナノ粒子のサイズに関しては、50ナノメートルに制限されることなく、10-200ナノメートルの範囲において適用できる。
また、導電性ナノ粒子の配置間隔に関しては、100ナノメートルに制限されることなく、ナノ粒子サイズの2倍以上10倍以下の距離が離れていれば差し支えない。
図6に、本実施形態の一つとして光電変換半導体素子(太陽電池)の例を示す。本実施例においては、トップ太陽電池としてGaAs系光吸収層を有するセル501、ボトム太陽電池としてInP系半導体層を有するセル502からなる2つの太陽電池を接合した場合を示す。GaAs系太陽電池501は、p型GaAsバッファ層503、p型GaAs光吸収層504、n型GaAsエミッタ層505、n型Ga0.51In0.49P/p型Ga0.51In0.49P (506/507)トンネル層、p型Ga0.51In0.49P光吸収層508、n型Ga0.51In0.49Pエミッタ層509、n型GaAsコンタクト層510、およびn型電極AuGeNi 511からなる。n型電極は、太陽光を受光するために、櫛型状の形態を有している。InP系太陽電池502は、InP基板512上に、p型InPバッファ層513、p型In0.91Ga0.09As0.2P0.8光吸収層514(バンドギャップエネルギー1.2eV)、n型In0.91Ga0.09As0.2P0.8エミッタ層515、n型InP層516からなっている。ここで、InP系太陽電池502表面には、ナノ粒子配列517がなされている。本実施例では、Auのナノ粒子を用いた。なお、InGaAsP組成は設計的要素であり、目標特性に応じて自在に組成を調整できるものである。
なお、本実施例ではInP基板512上にInGaAsP光吸収層514を有する構造をボトムセルとして用いたが、Ge基板上に同様にInGaAsP光吸収層あるいはInGaAs歪み光吸収層を形成した構造においても適用できる。
図8に、本実施形態の一つとして光電変換半導体素子(太陽電池)の例を示す。本実施例においては、トップ太陽電池としてアモルファスSi光吸収層を有する太陽電池701、ボトム太陽電池として結晶Si系半導体層を有する太陽電池702からなる2つの太陽電池を接合した場合を示す。アモルファスSi太陽電池701は、ZnO透明導電層703、n型アモルファスSi層704、i型アモルファスSi光吸収層705、p型アモルファスSi層706、フッ素ドープSnO2透明導電層707、およびガラス基板708からなる。結晶シリコン太陽電池702は、Al電極709上に、n型結晶Si層710、p型結晶Si層711、ITO透明導電層712からなる。ここで、結晶Si太陽電池702表面には、ナノ粒子配列713がなされている。本実施例では、Ptのナノ粒子を用いた。
図9に、本実施形態の一つとして光電変換半導体素子(太陽電池)の例を示す。本実施例においては、トップ太陽電池としてGaAs系光吸収層を有するセル901、ボトム太陽電池としてInP系半導体層を有するセル902からなる2つの太陽電池を接合した場合を示す。GaAs系太陽電池901は、p型GaAsバッファ層903、p型GaAs光吸収層904、n型GaAsエミッタ層905、n型InGaPエミッタ層906、n型GaAsコンタクト層907、およびn型電極AuGeNi 908からなる。n型電極は、太陽光を受光するために、櫛型状の形態を有している。InP系太陽電池902は、InP基板909上に、p型InPバッファ層910、p型In0.83Ga0.17As0.37P0.63光吸収層911(バンドギャップエネルギー1.15eV)、n型In0.83Ga0.17As0.37P0.63エミッタ層912、n型InP層913からなっている。ここで、InP系太陽電池902表面には、ナノ粒子配列914がなされている。本実施例では、Agのナノ粒子を用いた。なお、InGaAsP組成は設計的要素であり、目標特性に応じて自在に組成を調整できるものである。
102:ボトム半導体素子
103:トップ半導体素子
104:導電性ナノ粒子
301:GaAs系太陽電池(GaAs系セル)
302:CIGSe系太陽電池(CIGSe系セル)
303:p-GaAsバッファ層
304:p-Al0.3Ga0.7As光吸収層
305:-N-GaAsエミッタ層
306:-N-GaAsコンタクト層
307:-N-AuGeNi櫛型電極
308:ガラス基板
309:Mo電極
310:CIGSe半導体層
311:CdSエミッタ層
312:ZnO透明電極
313:Pdナノ粒子
501:GaAs系太陽電池(GaAs系セル)
502:InP系太陽電池(InP系セル)
503:p-GaAsバッファ層
504:p-GaAs光吸収層
505:-N-GaAsエミッタ層
506:-N-Ga0.51In0.49Pトンネル層
507:p-Ga0.51In0.49Pトンネル層
508:p-Ga0.51In0.49P光吸収層
509:-N-Ga0.51In0.49Pエミッタ層
510:-N-GaAsコンタクト層
511:-N-AuGeNi櫛型電極
512:InP基板
513:p-InPバッファ層
514:p-In0.91Ga0.09As0.2P0.8光吸収層
515:-N-In0.91Ga0.09As0.2P0.8エミッタ層
516:-N-InP層
517:Auナノ粒子
701:アモルファスSi太陽電池(アモルファスシリコン系セル)
702:結晶Si太陽電池(結晶シリコン系セル)
703:ZnO透明導電層
704:-N-アモルファスSi層
705:i-アモルファスSi光吸収層
706:p-アモルファスSi層
707:フッ素ドープSnO2透明導電層
708:ガラス基板
709:Al電極
710:-N-結晶Si層
711:p-結晶Si層
712:ITO透明導電層
713:Ptナノ粒子
901:GaAs系太陽電池(GaAs系セル)
902:InP系太陽電池(InP系セル)
903:p-GaAsバッファ層
904:p-GaAs光吸収層
905:-N-GaAsエミッタ層
906:-N-InGaPエミッタ層
907:-N-GaAsコンタクト層
908:-N-AuGeNi櫛型電極
909:InP基板
910:p-InPバッファ層
911:p-In0.83Ga0.17As0.37P0.63光吸収層
912:-N-In0.83Ga0.17As0.37P0.63エミッタ層
913:-N-InP層
914:Agナノ粒子
Claims (14)
- 有機分子で覆われていない導電性ナノ粒子を一方の半導体素子表面に配列し、その上に他方の半導体素子を圧着させることを特徴とする半導体素子の接合方法。
- 前記半導体素子表面への導電性ナノ粒子の配列が、ブロック共重合体薄膜をテンプレートとして形成されることを特徴とする請求項1に記載の半導体素子の接合方法。
- 前記半導体素子表面への導電性ナノ粒子の配列が、形状パターンが施されたスタンプを用いる転写手法で形成されることを特徴とする請求項1に記載の半導体素子の接合方法。
- 前記導電性ナノ粒子のサイズが、100ナノメートル以上500ナノメートル以下であることを特徴とする請求項1~3のいずれか1項に記載の半導体素子の接合方法。
- 前記導電性ナノ粒子のサイズが、10ナノメートル以上200ナノメートル以下であることを特徴とする請求項1又は2に記載の半導体素子の接合方法。
- 前記導電性ナノ粒子の配列間隔が、導電性ナノ粒子サイズの2倍以上10倍以下の距離であることを特徴とする請求項1~5のいずれか1項に記載の半導体素子の接合方法。
- 前記導電性ナノ粒子が、Pd、Au、Ag、Pt、Ni、Al、In、In2O3、Zn、ZnO、もしくはこれらの複合体からなることを特徴とする請求項1~6のいずれか1項に記載の半導体素子の接合方法。
- 前記半導体素子が、結晶Si系、アモルファスSi系、微結晶Si系、有機系、もしくは、カルコパイライト系材料を用いた単接合太陽電池、またはGaAs、InP、GaSb、もしくは、Ge基板上等に積層された2接合以上からなる太陽電池であることを特徴とする請求項1~7のいずれか1項に記載の半導体素子の接合方法。
- 一対の半導体素子の接合構造であって、両方の半導体素子の接合面に有機分子で覆われていない導電性ナノ粒子が介在している半導体素子の接合構造。
- 両方の半導体素子の接合面に介在する導電性ナノ粒子は、モノレイヤー(単一層)であることを特徴とする請求項9に記載の半導体素子の接合構造。
- 一対の半導体素子は、接合面に半導体層又は導電層を有するものである請求項9又は10に記載の半導体素子の接合構造。
- 請求項9~11のいずれか1項に記載の接合構造を隣接する半導体素子間に備える半導体素子積層体であって、半導体素子積層体の積層方向の一方の端面から、接合面のうち少なくとも最も遠くに位置する接合面までは透光性を具備する半導体素子積層体。
- 半導体素子が光電変換機能を有するものである請求項12に記載の半導体素子積層体。
- 光電変換機能を有する半導体素子が太陽電池である請求項13に記載の半導体素子積層体。
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- 2012-10-17 WO PCT/JP2012/076867 patent/WO2013058291A1/ja active Application Filing
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JP2019153747A (ja) * | 2018-03-06 | 2019-09-12 | 株式会社東芝 | 太陽電池、多接合型太陽電池、太陽電池モジュール及び太陽光発電システム |
WO2020004475A1 (ja) * | 2018-06-29 | 2020-01-02 | 国立研究開発法人産業技術総合研究所 | 多接合光電変換素子及び多接合太陽電池 |
JP2020161546A (ja) * | 2019-03-25 | 2020-10-01 | 国立研究開発法人産業技術総合研究所 | 太陽電池およびその製造方法 |
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JP7416403B2 (ja) | 2019-11-29 | 2024-01-17 | 国立研究開発法人産業技術総合研究所 | 半導体装置およびその製造方法 |
Also Published As
Publication number | Publication date |
---|---|
EP2770540A4 (en) | 2015-05-20 |
CN103890976A (zh) | 2014-06-25 |
JPWO2013058291A1 (ja) | 2015-04-02 |
JP5875124B2 (ja) | 2016-03-02 |
US10608136B2 (en) | 2020-03-31 |
US20140238485A1 (en) | 2014-08-28 |
EP2770540A1 (en) | 2014-08-27 |
CN103890976B (zh) | 2016-11-02 |
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