WO2017057095A1 - 光電変換装置 - Google Patents
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- WO2017057095A1 WO2017057095A1 PCT/JP2016/077696 JP2016077696W WO2017057095A1 WO 2017057095 A1 WO2017057095 A1 WO 2017057095A1 JP 2016077696 W JP2016077696 W JP 2016077696W WO 2017057095 A1 WO2017057095 A1 WO 2017057095A1
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- H01L31/035209—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions comprising a quantum structures
- H01L31/035218—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions comprising a quantum structures the quantum structure being quantum dots
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- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0352—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions
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Definitions
- the present invention relates to a photoelectric conversion device using quantum dots.
- FIG. 3 is a schematic cross-sectional view partially showing a conventional photoelectric conversion device taking a quantum dot solar cell as an example.
- the quantum dot layer 103 is provided on the semiconductor substrate 101.
- the quantum dot layer 103 is composed of quantum dots 103a, which are semiconductor particles, and an inorganic matrix 103b disposed around the quantum dots 103a.
- the photoelectric conversion device of the present disclosure includes a quantum dot layer in which a plurality of quantum dots are integrated on a main surface of a semiconductor substrate.
- the quantum dot layer has two or more organic molecules having different carbon numbers between the plurality of quantum dots.
- (A) is sectional drawing which shows typically one Embodiment of the photoelectric conversion apparatus of this indication, (b) expanded and showed the quantum dot aggregate shown in the broken-line frame in (a). It is a schematic diagram. It is a schematic diagram which shows the state where the aggregate of quantum dots was connected and integrated
- the quantum dots 103a and the matrix 103b often differ greatly in thermal expansion coefficient due to their materials.
- the quantum dot layer on the semiconductor substrate 101 side is caused by a difference in thermal expansion coefficient between the quantum dot layer 103 and the semiconductor substrate 101. Large distortion may occur in the 103.
- the quantum dot layer 103 is formed on the main surface of the semiconductor substrate 101 with a large area, the strain increases depending on the area of the quantum dot layer 103, and thus obtained as a result of the quantum confinement effect. Variation in energy levels and continuity of the band structure are hindered. As a result, it becomes difficult to take out the carriers generated in the quantum dot layer 103 to the outside, and it becomes difficult to increase the power generation efficiency.
- the present disclosure has been made in view of such problems. And the power generation efficiency can be improved by the configuration shown below.
- FIG. 1A is a cross-sectional view schematically showing an embodiment of the photoelectric conversion device of the present disclosure
- FIG. 1B is an enlarged view of the quantum dot aggregate shown in the broken line frame in FIG. It is the shown schematic diagram.
- the photoelectric conversion device of the present disclosure includes the semiconductor substrate 1 and the quantum dot layer 3 provided on the upper surface side as the photoelectric conversion layer 5.
- a glass substrate 9 is attached to the upper surface side of the photoelectric conversion layer 5 via a transparent conductive film 7.
- an electrode layer 11 is provided on the lower surface side of the photoelectric conversion layer 5.
- the glass substrate 9 side is the sunlight incident side
- the electrode layer 11 side is the sunlight emission side.
- FIG. 1A the number of quantum dot layers 3 formed on the semiconductor substrate 1 is simplified and only one layer is shown, but the quantum dot layer 3 has a structure in which at least several tens of layers are stacked.
- the quantum dot layer 3 has two or more types of organic molecules 4 having different carbon numbers between the plurality of quantum dots 3a.
- the quantum dots 3a integrated in the quantum dot layer 3 are connected by organic molecules 4 having a lower elastic modulus than the inorganic matrix. ing. Thereby, the quantum dot layer 3 becomes low overall in rigidity. In addition, distortion due to the difference in thermal expansion coefficient generated between the quantum dot layer 3 and the semiconductor substrate 1 is reduced. Thereby, the continuity of the band structure in the quantum dot layer 3 is easily maintained. Thus, carriers generated in the quantum dot layer 3 can be easily taken out and the power generation efficiency can be increased.
- the difference in the thermal expansion coefficient between the quantum dot layer 3 and the semiconductor substrate 1 is 1 ⁇ 10 ⁇ 6 / ° C. or more, particularly 2 ⁇ 10 ⁇ 6 / ° C.
- the above photoelectric conversion layer 5 is effective.
- the semiconductor substrate 1 for example, Si (CTE: 3.6 ⁇ 4.1 ⁇ 10 -6 /K),GaAs(CTE:5.5 ⁇ 6.5 ⁇ 10 -6 / K), InP (4.
- One type selected from the group of 1 to 4.8 ⁇ 10 ⁇ 6 / K) and GaN (CTE: 3.1 to 5.8 ⁇ 10 ⁇ 6 / K) can be selected as a preferable one.
- the semiconductor substrate 1 is selected based on a semiconductor substrate having a lattice constant and a thermal expansion coefficient that are close to the lattice constant and the thermal expansion coefficient of the semiconductor particles that form the quantum dots 3a and that has a small band gap.
- organic molecules 4 having different carbon numbers are bonded to the quantum dots 3a.
- the organic molecules 4 having a small number of carbon atoms are present so that the plurality of quantum dots 3a are brought into close proximity to each other. In this way, an aggregate 3A formed by collecting a plurality of quantum dots 3a is formed.
- the organic molecule 4 having a small number of carbon atoms present around the quantum dots 3a exhibits a function as a passivation film. Thereby, the confinement effect of the carriers generated in the quantum dots 3a is enhanced, and the short circuit current density (Jsc) can be improved.
- the quantum dot layer 3 is in a state in which the aggregate 3A of the quantum dots 3a formed by bonding the organic molecules 4 to the plurality of quantum dots 3a as one unit is connected by the organic molecules 4. .
- FIG. 1 (a) only the organic molecules 4 (4a) extending toward the outside of the aggregate 3A are shown for convenience of the size of the drawing, but this aggregate 3A is shown in FIG. 1 (b).
- organic molecules 4b that connect adjacent quantum dots 3a are provided.
- Aggregates 3A are connected by organic molecules 4a extending outward.
- the organic molecules 4a and the organic molecules 4b differ in the number of carbons that are elements constituting the main chain.
- the organic molecule 4a is an organic molecule 4 having more carbon atoms than the organic molecule 4b, it is referred to as a high carbon number organic molecule 4a.
- the organic molecule 4b is an organic molecule 4 having a smaller number of carbon atoms than the high carbon number organic molecule 4a, the organic molecule 4b is a low carbon number organic molecule 4b.
- the high carbon number organic molecule 4a and the low carbon number organic molecule 4b may have different carbon numbers in each.
- the low carbon number organic molecules 4b forming the aggregate 3A organic molecules 4 having 20 or less carbon atoms are preferable because the degree of integration between the quantum dots 3a can be increased.
- the low carbon number organic molecules 4b for bonding the quantum dots 3a and the high carbon number organic molecules 4a for connecting the aggregates 3A are significantly different in carbon number.
- the high carbon number organic molecule 4a is preferably one having 1.5 or more times the carbon number of the low carbon number organic molecule 4b.
- the ratio of the carbon number of the high carbon number organic molecule 4a to the carbon number of the low carbon number organic molecule 4b is 1.5 times or more, the quantum dots 3a are preferentially connected to each other by the low carbon number organic molecule 4b. .
- the aggregates 3A are preferentially connected by the high carbon number organic molecules 4a.
- the quantum effect of the quantum dots 3a is easily developed.
- the plurality of aggregates 3A are connected mainly by the high carbon number organic molecules 4a, the rigidity of the quantum dot layer 3 can be reduced.
- various methane series hydrocarbons having a carbon skeleton having a chain structure and a carbon number of 20 or less are preferably used.
- Specific examples include pentene (5 carbon atoms), hexane (6 carbon atoms), heptane (7 carbon atoms), dodecene (12 carbon atoms), and octadecene (17 carbon atoms).
- pentene 5 carbon atoms
- hexane (6 carbon atoms)
- dodecene (12 carbon atoms) dodecene (12 carbon atoms)
- octadecene 17 carbon atoms
- a combination in which octadecene or dodecene is applied as the high carbon number organic molecule 4a and pentene or hexane is applied as the low carbon number organic molecule 4b is preferable.
- These are combinations in which the carbon number ratio between the high carbon number organic molecule 4a and
- the shape of the quantum dot 3a may be any shape such as a spherical shape such as an ellipsoid or a sphere, a hexahedron shape including a cube or a rectangular parallelepiped, a thin film shape, and a wire shape, but 3 between the adjacent quantum dots 3a.
- a spherical shape or a polyhedron with an aspect ratio close to 1 (1 to 1.5) is preferable because it is easy to form a dimensionally continuous band structure.
- the carrier conductivity in the quantum wire is increased.
- the aspect ratio is close to 1 (1 to 1.5) and is equivalent to the polyhedron.
- Short circuit current density can be obtained.
- the number of quantum wires having a diameter decreasing in the length direction within the unit area is 10% or more of the total number of quantum dots 3a. good.
- the maximum diameter in a spherical shape or a thin film shape is preferably 3 nm to 50 nm.
- the diameter of the wire (quantum wire) is preferably 3 to 50 nm and the length is preferably 100 to 10000 nm.
- the interval between the quantum dots 3a in the aggregate 3A, that is, the length of the low carbon number organic molecules 4b existing between the quantum dots 3a is preferably 2 to 10 nm.
- the size of the quantum dots 3a constituting the aggregate 3A and the interval between the quantum dots 3a are within the above ranges, a regular long-period structure of electrons is formed between the plurality of quantum dots 3a in the aggregate 3A. It becomes easier to form. This makes it possible to form a continuous band structure.
- the size of the quantum dots 3a and the interval between the quantum dots 3a can be adapted to various conditions according to the specific application and the conditions of the manufactured device.
- the quantum dots 3a are mainly composed of semiconductor particles and preferably have an energy gap (Eg) of 0.15 to 1.20 ev.
- FIG. 2 shows a part of the quantum dot layer, and is a schematic diagram showing a state in which the aggregates of the quantum dots are linked by high carbon number organic molecules.
- the state in which the high carbon number organic molecules 4a exist around the aggregate 3A is surrounded by a circle and represented as a complex 3B of quantum dots, but when the quantum dot layer 3 is viewed in a longitudinal section, or When viewed in plan, high carbon number organic molecules 4a exist between the actual aggregates 3A so as to fill the gaps (S).
- a region where a plurality of (in this case, three) composites 3B are adjacent is surrounded by a broken line. In this case, the three adjacent composite bodies 3B are arranged so as to form a triple point at the center.
- the composite 3B may include a mixture having a variation range of 0.5 to 2 when the average size is 1.
- the composites 3B having a small size are filled in the gaps between the composites 3B having a large size, so that the filling rate of the composites 3B can be increased.
- the degree of integration of the composite 3B is increased, and the amount of carriers generated can be increased.
- the short circuit current density (Jsc) can be increased.
- Aggregate 3A is a composite structure formed by densely gathering a plurality of quantum dots 3a.
- the aggregate 3A and the high carbon number organic molecule 4a which are portions where the quantum dots 3a are densely gathered, have different color tones when the cross section of the quantum dot layer 3 is observed using a reflection electron image of an electron microscope. Can be distinguished from what appears.
- the actual contour Lo of the complex 3B is a region that follows the midpoint between two adjacent aggregates 3A and connects the midpoints around the aggregate 3A.
- the high carbon number organic molecule 4a and the low carbon number organic molecule 4b can be distinguished by observation with a scanning tunneling microscope.
- the cross-sectional view shown in FIG. 2 shows the vicinity of the outermost surface of the quantum dot layer 3, that is, when the composite bodies 3B are stacked, the outermost surface of the composite body 3B
- the quantum dots 3a constituting the body 3B have irregularities due to the difference in density.
- the surface of the composite 3B is curved due to the unevenness formed by the plurality of quantum dots 3a.
- the surface of the composite 3B has such a concave-convex curved surface, sunlight can be received vertically somewhere on the curved surface even if the direction of the sun changes. Thereby, the fall of the intensity
- an organic molecule solution containing one or more organic molecules 4 having different carbon numbers was prepared in a predetermined container.
- the organic molecule 4 pentene (carbon number 5), hexane (carbon number 6), heptane (carbon number 7), dodecene (carbon number 12) and octadecene (carbon number 17) were used.
- the composition was adjusted so as to be equimolar.
- Acetone was used as the solvent.
- the solvent may have to be changed depending on the type of the organic molecule 4, but any one of organic solvents selected from toluene, isopropyl alcohol, ethanol, methanol, and the like can be used in the same manner in addition to acetone.
- PbS lead sulfide
- the addition amount of the organic molecules 4 was adjusted so as to be 5 when the semiconductor particles were 1 by mass ratio.
- the low carbon number organic molecules 4b were bonded to the surface of the quantum dots 3a by the stirring operation for a long time, and the quantum dots 3a were aggregated by a certain number (several tens to thousands).
- high carbon number organic molecules 4a having a large number of carbon atoms were mainly bonded around the aggregate 3A in which the quantum dots 3a were aggregated.
- a precursor of the aggregate 3A was formed.
- the viscosity characteristics of the organic molecule solution containing the precursor of the aggregate 3A showed thixotropic properties.
- the silicon substrate had a thickness of 100 ⁇ m and an area of 10 mm ⁇ 10 mm.
- the integrated film (quantum dot layer 3) of aggregates 3A of quantum dots 3a was formed on the silicon substrate by drying the solvent.
- the quantum dot layer 3 thus formed had a thickness of about 0.1 ⁇ m.
- a transparent conductive film 7 made of indium tin is formed on the surface of the quantum dot layer 3 formed on the silicon substrate by vapor deposition, and finally, a glass substrate 9 is used on the surface of the transparent conductive film 7 with an adhesive.
- the sample of the produced photoelectric conversion device was processed and cross-sectional observation was performed using a transmission electron microscope.
- the aggregate 3A was stacked in the quantum dot layer 3 as shown in FIG.
- the surface of the quantum dot layer 3 observed before forming the transparent conductive film 7 was a shape having an uneven curved surface.
- the low molecular number organic molecules 4b are mainly present inside the aggregate 3A analyzed by the flight secondary ion mass spectrometer (TOF-SIMS) together with the transmission electron microscope, and the high carbon is mainly disposed around the aggregate 3A. It was confirmed that several organic molecules 4a exist.
- quantum wires made of ZnTe (average diameter: 3 nm, average length: 1500 nm) prepared by a pulse electrolysis method were prepared. In this case, a quantum wire having a diameter reduction of 10% in the length direction was used.
- the short-circuit current density (Jsc) is 8.5 mA / cm for samples (Nos. 4 to 8) prepared using organic molecules having high and low carbon numbers as organic molecules.
- the short circuit current density (Jsc) was higher than that of the samples (No. 1 to 3) in which only one kind of organic molecule was used.
- sample No. in Table 1 The electromotive force was detected in any of the samples prepared by replacing the quantum dots 3a of 1 to 8 with PbS to ZnTe quantum wires, and a short-circuit current density comparable to that of Samples 1 to 8 was obtained.
Abstract
Description
3、103・・・・・量子ドット層
3a、103a・・・量子ドット
3A・・・・・・・・凝集体
3B・・・・・・・・複合体
4・・・・・・・・・有機分子
4a・・・・・・・・高炭素数有機分子
4b・・・・・・・・低炭素数有機分子
5・・・・・・・・・光電変換層
7・・・・・・・・・透明導電膜
9・・・・・・・・・ガラス基板
11・・・・・・・・電極層
Claims (5)
- 半導体基板の主面上に複数の量子ドットが集積されてなる量子ドット層を備え、該量子ドット層は、前記複数の量子ドット間に炭素数の異なる2種以上の有機分子を有していることを特徴とする光電変換装置。
- 前記有機分子として、低炭素数有機分子と、該低炭素数有機分子よりも炭素数が多い高炭素数有機分子とを有するとともに、前記複数の量子ドットが前記低炭素数有機分子によって結合されて量子ドットの凝集体を成しており、該凝集体の外側に前記高炭素数有機分子が結合していることを特徴とする請求項1に記載の光電変換装置。
- 複数の前記凝集体が前記高炭素数有機分子により連結されていることを特徴とする請求項2に記載の光電変換装置。
- 前記有機分子は炭素数が20以下であり、前記高炭素数有機分子の炭素数は前記低炭素数有機分子の炭素数の1.5倍以上であることを特徴とする請求項1乃至3のうちいずれかに記載の光電変換装置。
- 前記高炭素数有機分子がオクタデセンまたはドデセンであり、前記低炭素数有機分子がペンテンまたはヘキサンであることを特徴とする請求項1乃至4のうちいずれかに記載の光電変換装置。
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JP2009532851A (ja) * | 2006-02-16 | 2009-09-10 | ソレクサント・コーポレイション | ナノ粒子増感ナノ構造太陽電池 |
JP2009537994A (ja) * | 2006-05-15 | 2009-10-29 | スティオン コーポレイション | 半導体材料を用いた薄膜光電材料のための方法及び構造 |
WO2011037041A1 (ja) * | 2009-09-28 | 2011-03-31 | 株式会社 村田製作所 | ナノ粒子材料及び光電変換デバイス |
JP2013105952A (ja) * | 2011-11-15 | 2013-05-30 | Kyocera Corp | 太陽電池 |
JP2015103609A (ja) * | 2013-11-22 | 2015-06-04 | 国立大学法人 奈良先端科学技術大学院大学 | 基板上へのナノ粒子の配列方法 |
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JP2009532851A (ja) * | 2006-02-16 | 2009-09-10 | ソレクサント・コーポレイション | ナノ粒子増感ナノ構造太陽電池 |
JP2009537994A (ja) * | 2006-05-15 | 2009-10-29 | スティオン コーポレイション | 半導体材料を用いた薄膜光電材料のための方法及び構造 |
WO2011037041A1 (ja) * | 2009-09-28 | 2011-03-31 | 株式会社 村田製作所 | ナノ粒子材料及び光電変換デバイス |
JP2013105952A (ja) * | 2011-11-15 | 2013-05-30 | Kyocera Corp | 太陽電池 |
JP2015103609A (ja) * | 2013-11-22 | 2015-06-04 | 国立大学法人 奈良先端科学技術大学院大学 | 基板上へのナノ粒子の配列方法 |
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