WO2009122458A1 - 量子ドットの製造方法 - Google Patents
量子ドットの製造方法 Download PDFInfo
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- WO2009122458A1 WO2009122458A1 PCT/JP2008/000819 JP2008000819W WO2009122458A1 WO 2009122458 A1 WO2009122458 A1 WO 2009122458A1 JP 2008000819 W JP2008000819 W JP 2008000819W WO 2009122458 A1 WO2009122458 A1 WO 2009122458A1
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- Prior art keywords
- quantum dots
- film
- gas
- substrate
- type silicon
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- 239000002096 quantum dot Substances 0.000 title claims description 102
- 238000000034 method Methods 0.000 title abstract description 21
- 230000008569 process Effects 0.000 title abstract description 10
- 239000000758 substrate Substances 0.000 claims abstract description 45
- 238000010438 heat treatment Methods 0.000 claims abstract description 38
- 238000001816 cooling Methods 0.000 claims abstract description 9
- 239000010408 film Substances 0.000 claims description 190
- 229910052710 silicon Inorganic materials 0.000 claims description 60
- 239000010703 silicon Substances 0.000 claims description 57
- 238000004519 manufacturing process Methods 0.000 claims description 35
- 239000000463 material Substances 0.000 claims description 27
- 239000010409 thin film Substances 0.000 claims description 19
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 9
- 229910052732 germanium Inorganic materials 0.000 claims description 6
- 230000000630 rising effect Effects 0.000 claims description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 4
- 229910052799 carbon Inorganic materials 0.000 claims description 4
- 229910052757 nitrogen Inorganic materials 0.000 claims description 4
- 239000001301 oxygen Substances 0.000 claims description 4
- 229910052760 oxygen Inorganic materials 0.000 claims description 4
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 claims description 3
- 229910052718 tin Inorganic materials 0.000 claims description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 2
- 238000000151 deposition Methods 0.000 claims description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 abstract description 56
- 229910052814 silicon oxide Inorganic materials 0.000 abstract description 49
- 238000005268 plasma chemical vapour deposition Methods 0.000 abstract description 13
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical compound [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 abstract description 2
- 239000007789 gas Substances 0.000 description 62
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 56
- 229910052581 Si3N4 Inorganic materials 0.000 description 43
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 43
- 238000004151 rapid thermal annealing Methods 0.000 description 35
- 229910021420 polycrystalline silicon Inorganic materials 0.000 description 22
- 238000010586 diagram Methods 0.000 description 12
- 229910004298 SiO 2 Inorganic materials 0.000 description 10
- 230000004888 barrier function Effects 0.000 description 6
- 239000000498 cooling water Substances 0.000 description 6
- 239000004065 semiconductor Substances 0.000 description 6
- 235000012239 silicon dioxide Nutrition 0.000 description 6
- 229910021417 amorphous silicon Inorganic materials 0.000 description 5
- 239000013078 crystal Substances 0.000 description 5
- 239000010453 quartz Substances 0.000 description 5
- 238000005468 ion implantation Methods 0.000 description 4
- 238000004518 low pressure chemical vapour deposition Methods 0.000 description 3
- 150000004767 nitrides Chemical class 0.000 description 3
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 3
- 230000005476 size effect Effects 0.000 description 3
- 230000001133 acceleration Effects 0.000 description 2
- 229910052796 boron Inorganic materials 0.000 description 2
- 238000005229 chemical vapour deposition Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 238000001451 molecular beam epitaxy Methods 0.000 description 2
- 229910052698 phosphorus Inorganic materials 0.000 description 2
- 239000011574 phosphorus Substances 0.000 description 2
- -1 phosphorus ions Chemical class 0.000 description 2
- 230000004044 response Effects 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 238000004544 sputter deposition Methods 0.000 description 2
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 1
- 229910005793 GeO 2 Inorganic materials 0.000 description 1
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000005234 chemical deposition Methods 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 230000005684 electric field Effects 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 125000004435 hydrogen atom Chemical class [H]* 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000000206 photolithography Methods 0.000 description 1
- 229920005591 polysilicon Polymers 0.000 description 1
- 229910000077 silane Inorganic materials 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
Images
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/005—Processes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y10/00—Nanotechnology for information processing, storage or transmission, e.g. quantum computing or single electron logic
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
- H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
- H01L21/02104—Forming layers
- H01L21/02365—Forming inorganic semiconducting materials on a substrate
- H01L21/02518—Deposited layers
- H01L21/02521—Materials
- H01L21/02524—Group 14 semiconducting materials
- H01L21/02532—Silicon, silicon germanium, germanium
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
- H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
- H01L21/02104—Forming layers
- H01L21/02365—Forming inorganic semiconducting materials on a substrate
- H01L21/02518—Deposited layers
- H01L21/02521—Materials
- H01L21/02524—Group 14 semiconducting materials
- H01L21/02535—Group 14 semiconducting materials including tin
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
- H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
- H01L21/02104—Forming layers
- H01L21/02365—Forming inorganic semiconducting materials on a substrate
- H01L21/02612—Formation types
- H01L21/02617—Deposition types
- H01L21/0262—Reduction or decomposition of gaseous compounds, e.g. CVD
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/02—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies
- H01L33/04—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies with a quantum effect structure or superlattice, e.g. tunnel junction
- H01L33/06—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies with a quantum effect structure or superlattice, e.g. tunnel junction within the light emitting region, e.g. quantum confinement structure or tunnel barrier
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/02—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies
- H01L33/26—Materials of the light emitting region
Definitions
- the present invention relates to a method for manufacturing quantum dots, and more particularly to a method for manufacturing quantum dots capable of controlling the size and density of quantum dots.
- quantum dots made of silicon have been formed using LPCVD (Low Pressure Chemical Vapor Deposition) method (Japanese Patent Laid-Open No. 2006-3254).
- the quantum dots are formed by performing a reaction for 50 to 70 seconds at a reaction pressure of 0.5 Torr and a substrate temperature of 560 to 600 ° C. using silane (SiH 4 ) gas as a material gas. .
- quantum dots are produced using conventional quantum dot manufacturing methods, the size and density of the quantum dots can be controlled.
- the production time proportional to the number of layers is required. There is a problem that it is necessary.
- an object of the present invention is to provide a method for producing multilayer quantum dots capable of controlling size and density.
- the quantum dot manufacturing method sets the amount ratio of the second material containing the second element to the first material containing the first element to be equal to or higher than the reference value, and the thin film is formed on the substrate.
- the reference value is the amount ratio of the second material to the first material when forming the insulating film containing the first and second elements.
- a thin film made of an amorphous phase is deposited on the substrate.
- the quantum dot manufacturing method further includes a fourth step of cooling the thin film at a temperature lowering rate equal to or higher than a reference temperature lowering rate after the third step.
- the quantum dot manufacturing method further includes a fourth step of cooling the thin film at a temperature lowering rate lower than the reference temperature lowering rate after the third step.
- the first element is made of any of oxygen, nitrogen, and carbon
- the second element is made of any of Si, Ge, C, and Sn.
- the second element is made of either silicon or germanium.
- the first reference value is an amount ratio of the second material to the first material when forming the insulating film including the first and second elements
- the second reference value is the third reference value.
- the amount ratio of the second material to the third material containing the third element when the insulating film containing the element and the second element is formed.
- the amount ratio of the second material to the first material is set to be equal to or higher than the first reference value
- the amount ratio of the second material to the third material is set to the second reference value.
- a thin film is deposited on the substrate with the value set above.
- the first element is made of oxygen
- the second element is made of either silicon or germanium
- the third element is made of nitrogen.
- the rate of temperature rise is in the range of 0.2 ° C./s to 500 ° C./s.
- the rate of temperature decrease is in the range of 5 ° C./s to 50 ° C./s.
- a thin film containing a second element more than a reference value when forming an insulating film containing the first and second elements is formed, and the formed thin film is converted into a reference film.
- a quantum dot is manufactured by heating at a temperature rising rate equal to or higher than the temperature rate. In this case, the size and density of the quantum dots change depending on the temperature rising rate and the heat treatment time length.
- the size and density of the quantum dots can be controlled.
- FIG. 5 is a conceptual diagram in steps (b) to (d) shown in FIG.
- FIG. 6 is a conceptual diagram in steps (b) to (d) shown in FIG. It is sectional drawing of the light emitting element produced using the manufacturing method by embodiment of this invention.
- FIG. 9 is an enlarged cross-sectional view of the n-type silicon oxide film, i-type silicon nitride film, and p-type silicon oxynitride film shown in FIG. 8. It is an energy band figure at the time of the zero bias of the light emitting element shown in FIG. It is an energy band figure at the time of the current supply of the light emitting element shown in FIG.
- FIG. 10 is a first process diagram for explaining a method of manufacturing the light emitting element shown in FIG. 8.
- FIG. 10 is a second process diagram for explaining the manufacturing method of the light emitting element shown in FIG. 8.
- FIG. 1 is a schematic view of a plasma CVD (Chemical Vapor Deposition) apparatus.
- a plasma CVD apparatus 100 includes a reaction chamber 101, an electrode plate 102, a sample holder 103, a heater 104, an RF (Radio Frequency) power source 105, pipes 106 to 108, and a gas cylinder 109 to 111.
- RF Radio Frequency
- the reaction chamber 101 is a hollow container and has an exhaust port 101A.
- the electrode plate 102 and the sample holder 103 have a flat plate shape, and are disposed in the reaction chamber 101 substantially in parallel at an interval of 50 mm.
- Each of the electrode plate 102 and the sample holder 103 has a diameter of 200 mm ⁇ .
- the heater 104 is disposed in the sample holder 103.
- the RF power source 105 is connected to the electrode plate 102 and the sample holder 103.
- the pipe 106 has one end connected to the reaction chamber 101 and the other end connected to a gas cylinder 109.
- the pipe 107 has one end connected to the reaction chamber 101 and the other end connected to the gas cylinder 110.
- the pipe 108 has one end connected to the reaction chamber 101 and the other end connected to the gas cylinder 111.
- the sample holder 103 holds the substrate 1.
- the heater 104 heats the substrate 1 to a predetermined temperature.
- the RF power source 105 applies 13.56 MHz RF power between the electrode plate 102 and the sample holder 103.
- the gas cylinder 109 holds N 2 O (100%) gas, the gas cylinder 110 holds 10% SiH 4 gas diluted with hydrogen (H 2 ) gas, and the gas cylinder 111 contains NH 3 (100%). Hold the gas.
- the pipe 106 supplies N 2 O gas into the reaction chamber 101.
- the pipe 107 supplies SiH 4 gas into the reaction chamber 101.
- the pipe 108 supplies NH 3 gas into the reaction chamber 101.
- N 2 O gas, SiH 4 gas, and NH 3 gas supplied into the reaction chamber 101 are exhausted from the exhaust port 101A by an exhaust device (not shown) such as a rotary pump. As a result, the inside of the reaction chamber 101 is set to a predetermined pressure.
- the plasma CVD apparatus 100 applies a silicon oxide film by applying RF power between the electrode plate 102 and the sample holder 103 by the RF power source 105 in a state where N 2 O gas and SiH 4 gas are supplied into the reaction chamber 101. Deposit on the substrate 1.
- the plasma CVD apparatus 100 applies RF power between the electrode plate 102 and the sample holder 103 by the RF power source 105 in a state where NH 3 gas and SiH 4 gas are supplied into the reaction chamber 101, and a silicon nitride film Is deposited on the substrate 1.
- the plasma CVD apparatus 100 applies RF power between the electrode plate 102 and the sample holder 103 by the RF power source 105 in a state where N 2 O gas, NH 3 gas, and SiH 4 gas are supplied into the reaction chamber 101. Then, a silicon oxynitride film is deposited on the substrate 1.
- FIG. 2 is a schematic diagram of an RTA (Rapid Thermal Annealing) apparatus.
- an RTA apparatus 200 includes a container 210, a holder 220, a quartz window 230, a lamp house 240, a lamp 250, a pipe 260, a cooler 270, a thermocouple 280, and a control device. 290.
- the container 210 has a gas inlet 211 and a gas outlet 212.
- the holder 220 is installed on the bottom surface 210 ⁇ / b> A of the container 210.
- the quartz window 230 is installed on the upper surface 210 ⁇ / b> B of the container 210 so as to face the holder 220.
- the lamp house 240 is installed on the upper side of the quartz window 230.
- the lamp 250 is housed in the lamp house 230.
- the pipe 260 partially penetrates the holder 220 and both ends are connected to the cooler 270.
- the thermocouple 280 has one end embedded in the holder 220 and the other end connected to the control device 290.
- the gas inlet 211 allows, for example, nitrogen (N 2 ) gas to flow into the container 210 from the outside.
- the gas discharge port 212 discharges the N 2 gas in the container 210 to the outside.
- the holder 220 supports the sample 300.
- the quartz window 230 transmits the light from the lamp 250.
- the lamp 250 heats the sample 300 through the quartz window 230.
- the pipe 260 circulates cooling water between the holder 220 and the cooler 270.
- the cooler 270 causes cooling water to flow through the pipe 260 in accordance with control from the control device 290.
- the thermocouple 280 detects the temperature Ts of the sample 300 and outputs the detected temperature Ts to the control device 290.
- Control device 290 receives temperature Ts from thermocouple 280. When the sample 300 is heated, the control device 290 supplies the lamp 250 with power PW1 for increasing the temperature Ts from room temperature to 1000 ° C. in 2 seconds.
- control device 290 supplies power PW2 for maintaining the temperature Ts at 1000 ° C. to the lamp 250.
- control device 290 controls the cooler 270 to flow cooling water when the temperature Ts is rapidly cooled.
- the sample 300 When heat treatment by RTA is performed on the sample 300 using the RTA apparatus 200, the sample 300 is set on the holder 220. Thereafter, flow from the gas inlet port 211 and N 2 gas into the container 210 to replace the inside of the container 210 by N 2 gas.
- control device 290 supplies the power PW1 to the lamp 250.
- the lamp 250 receives the power PW1 from the control device 290, heats the sample 300, and raises the temperature Ts of the sample 300 from room temperature to 1000 ° C. in 2 seconds.
- thermocouple 280 detects the temperature Ts of the sample 300 and outputs the detected temperature Ts to the control device 290.
- the control device 290 receives the temperature Ts from the thermocouple 280, and supplies power PW2 for maintaining the temperature Ts to 1000 ° C. to the lamp 250 based on the received temperature Ts.
- the lamp 250 receives the power PW2 from the control device 290 and holds the temperature Ts of the sample 300 at 1000 ° C.
- the control device 290 outputs a signal OFF for turning off the lamp 250 to the lamp 250, and the lamp 250 stops heating the sample 300 in response to the signal OFF. Thereby, the sample 300 is naturally cooled.
- control device 290 when a predetermined time has elapsed and the sample 300 is rapidly cooled, the control device 290 generates a signal WON for flowing cooling water and outputs the signal WON to the cooler 270. Cooler 270 causes cooling water to flow through pipe 260 in response to signal WON from control device 290. Thereby, the sample 300 is rapidly cooled.
- FIG. 3 is a timing chart of heat treatment by RTA using the RTA apparatus 200 shown in FIG.
- the vertical axis represents temperature
- the horizontal axis represents time
- Straight lines k1, k2, and k3 indicate the first heat treatment method using RTA
- straight lines k1, k2, and k4 indicate the second heat treatment method using RTA.
- the sample 300 is heated from room temperature RT to 1000 ° C. in 5 seconds from timing t0 to timing t1 (see straight line k1). And the sample 300 is hold
- the lamp 250 is turned off at timing t2, and the cooling water is caused to flow through the pipe 260. Then, the sample 300 is cooled from 1000 ° C. to room temperature RT in 30 seconds from timing t2 to timing t3 (see the straight line k3).
- the sample 300 is heated from room temperature RT to 1000 ° C. and held at 1000 ° C. by the same method as the first heat treatment method. Then, the lamp 250 is turned off at timing t2, and the sample 300 is cooled from 1000 ° C. to room temperature RT in 30 minutes from timing t2 to timing t4 (see the straight line k4).
- the sample 300 is heat-treated by rapid heating and rapid cooling, and the sample 300 is heat-treated by rapid heating and natural cooling.
- FIG. 4 is a process diagram for manufacturing quantum dots.
- a substrate 1 made of silicon (Si) is prepared (see step (a) in FIG. 4), and after the substrate 1 is RCA cleaned, the plasma CVD apparatus 100 shown in FIG. The substrate 1 is placed on the sample holder 103.
- N 2 O gas is supplied from the gas cylinder 109 to the reaction chamber 101
- SiH 4 gas is supplied from the gas cylinder 110 to the reaction chamber 101
- the silicon oxide film 2 is deposited on the substrate 1 using the reaction conditions shown in Table 1. (See step (b) in FIG. 4).
- the silicon oxide film 2 is made of an amorphous phase that does not contain a crystal flow.
- FIG. 5 is another process diagram for manufacturing quantum dots.
- the silicon oxide film 2 is deposited on the substrate 1 according to the same steps (a) and (b) in FIG. 4 (steps (a) and (b in FIG. 5). )reference).
- the quantum dots 22 have a larger diameter than the quantum dots 21.
- FIG. 6 is a conceptual diagram in steps (b) to (d) shown in FIG.
- silicon oxide film 2 deposited in step (b) shown in FIG. 4 is made of an amorphous phase (see FIG. 6 (a)).
- FIG. 7 is a conceptual diagram in steps (b) to (d) shown in FIG.
- the silicon oxide film 2 is made of an amorphous phase as in the case shown in FIG. 6 (see FIG. 7A).
- crystal grains 20 are generated as in the case shown in FIG. 6 (see FIG. 7B).
- the quantum dots 22 are larger in size than the quantum dots 21 and higher in density than the quantum dots 21.
- the size and density of the quantum dots can be controlled by controlling the cooling rate in the heat treatment by RTA.
- the flow rate ratio of SiH 4 gas to the N 2 O gas in the condition (Table 1) forming a silicon nitride film 2, the flow rate of SiH 4 gas to the N 2 O gas when forming an SiO 2 film as the insulating film Is greater than the ratio ( reference flow rate ratio). That is, in the present invention, the silicon oxide film 2 is formed with a flow rate of SiH 4 gas larger than the reference, and is called a so-called silicon-rich oxide film.
- the silicon-rich oxide film 2 is deposited on the substrate 1 using the plasma CVD apparatus 100, and the deposited silicon-rich oxide film 2 is subjected to heat treatment by RTA, so that the desired size and It is characterized by manufacturing quantum dots having a desired density.
- the quantum dots are manufactured by performing heat treatment by RTA on the silicon oxide film.
- the present invention is not limited to this, and heat treatment by RTA is performed on the silicon nitride film.
- the quantum dots may be manufactured, or the silicon oxynitride film may be heat-treated by RTA to manufacture the quantum dots.
- a silicon nitride film is deposited on the substrate 1 using the reaction conditions shown in Table 2, and an RTA apparatus is applied to the deposited silicon nitride film. 200 is used for heat treatment by RTA.
- a silicon-rich nitride film is deposited on the substrate 1 using the plasma CVD apparatus 100, and the deposited silicon-rich nitride film is subjected to heat treatment by RTA, so that a desired size and a desired size are obtained. Quantum dots having a density are manufactured.
- a quantum dot is manufactured by subjecting a silicon oxynitride film to heat treatment by RTA
- a silicon oxynitride film is deposited on the substrate 1 using the reaction conditions shown in Table 3, and the deposited silicon oxynitride film
- heat treatment by RTA is performed using the RTA apparatus 200.
- a silicon-rich oxynitride film is deposited on the substrate 1 using the plasma CVD apparatus 100, and the deposited silicon-rich oxynitride film is subjected to a heat treatment by RTA to obtain a desired size and It is characterized by manufacturing quantum dots having a desired density.
- the film after heat-treating the silicon oxide film is composed of Si dots (semiconductor quantum dots) and SiO 2 (insulating film), and the film after heat-treating the silicon nitride film is Si dots (semiconductor quantum dots). And Si 3 N 4 (insulating film), and after the silicon oxynitride film is heat-treated, the film is composed of Si dots (semiconductor quantum dots) and SiO x N 4 / 3-2x / 3 (0 ⁇ x ⁇ 2) (insulating film).
- the semiconductor quantum dots are not limited to those composed of Si dots, but the semiconductor quantum dots are composed of any one of Ge, C, and Sn, and the surroundings are SiO 2 , SiO x N 4 / 3-2x / 3 (0 ⁇ x ⁇ 2), Si 3 N 4 , GeO 2 , GeO x N 4 / 3-2x / 3 (0 ⁇ x ⁇ 2), or Ge 3 N 4 That's fine.
- the thin film before the heat treatment by RTA is not limited to the above-described plasma CVD apparatus 100, but various types such as a MOCVD (Metal Organic Chemical Deposition) apparatus, an MBE (Molecular Beam Epitaxy) apparatus, an LPCVD apparatus, and a sputtering apparatus. It is produced using an apparatus.
- MOCVD Metal Organic Chemical Deposition
- MBE Molecular Beam Epitaxy
- LPCVD Molecular Beam Epitaxy
- sputtering apparatus It is produced using an apparatus.
- the temperature rising rate in the heat treatment by RTA is described as 200 ° C./s.
- FIG. 8 is a cross-sectional view of a light emitting device manufactured using the manufacturing method according to the embodiment of the present invention.
- a light emitting device 400 includes a substrate 401, an n-type silicon oxide film 402, an i-type silicon nitride film 403, a p-type silicon oxynitride film 404, and p + -type polysilicon (poly-Si). )
- a film 405 and electrodes 406 and 407 are provided.
- the substrate 401 is made of n + type silicon (n + -Si) having a specific resistance of about 0.1 ⁇ ⁇ cm.
- the n-type silicon oxide film 402 includes a plurality of quantum dots made of n-type Si and is formed on one main surface of the substrate 1.
- the n-type silicon oxide film 402 has a thickness of about 150 nm.
- the i-type silicon nitride film 403 includes a plurality of i-type Si quantum dots, and is formed on the n-type silicon oxide film 402 in contact with the n-type silicon oxide film 402.
- the i-type silicon nitride film 403 has a thickness of about 10 nm.
- the p-type silicon oxynitride film 404 is formed on the i-type silicon nitride film 403 in contact with the i-type silicon nitride film 403.
- the p-type silicon oxynitride film 404 includes a plurality of quantum dots made of p-type Si and has a composition of SiO 1 N 0.33 .
- the p-type silicon oxynitride film 404 has a thickness of about 100 nm.
- the p + -type poly-Si film 405 includes p + -type poly-Si films 4051 to 4054 and is formed on the p-type silicon oxynitride film 404 in contact with the p-type silicon oxynitride film 404.
- the p + -type poly-Si film 405 includes a boron concentration of about 10 20 cm ⁇ 3 and a film thickness of about 50 nm.
- the electrode 406 includes electrodes 4061 to 4064.
- the electrodes 4061 to 4064 are formed on the p + type poly-Si films 4051 to 4054 in contact with the p + type poly-Si films 4051 to 4054, respectively.
- Each of the electrodes 4061 to 4064 is made of aluminum (Al).
- the electrode 407 is made of Al, and is formed on the back surface of the substrate 401 (the surface opposite to the surface on which the n-type silicon oxide film 402 and the like are formed).
- FIG. 9 is an enlarged cross-sectional view of n-type silicon oxide film 402, i-type silicon nitride film 403, and p-type silicon oxynitride film 404 shown in FIG.
- n-type silicon oxide film 402 includes a plurality of quantum dots 4021.
- Each of the plurality of quantum dots 4021 is made of n-type Si dots and includes a phosphorus (P) concentration of about 10 19 cm ⁇ 3 .
- the plurality of quantum dots 4021 are irregularly arranged in the n-type silicon oxide film 402.
- the i-type silicon nitride film 403 includes a plurality of quantum dots 4031.
- Each of the plurality of quantum dots 4031 is made of i-type Si dots.
- the plurality of quantum dots 4031 are irregularly arranged in the i-type silicon nitride film 403.
- the p-type silicon oxynitride film 404 includes a plurality of quantum dots 4041.
- Each of the plurality of quantum dots 4041 is made of p-type Si dots and includes a B concentration of about 10 19 cm ⁇ 3 .
- the plurality of quantum dots 4041 are irregularly arranged in the p-type silicon oxynitride film 404.
- n-type silicon oxide film 402 includes quantum dots 4021 made of n-type Si dots, and i-type silicon nitride film 403 and p-type silicon oxynitride film 404 are quantum dots made of i-type Si dots, respectively. 4031 and quantum dots 4041 made of p-type Si dots. Therefore, n-type silicon oxide film 402, i-type silicon nitride film 403, and p-type silicon oxynitride film 404 form a pin junction.
- FIG. 10 is an energy band diagram of the light-emitting element 400 illustrated in FIG. 8 at the time of zero bias.
- conduction band Ec1 and valence band Ev1 exist in n + Si constituting substrate 401, and n + Si has an energy band gap Eg1 of 1.12 eV.
- p + poly-Si film 405 there is conduction band Ec2 and the valence band Ev2, p + poly-Si film 405 has an energy band gap Eg1 of 1.12 eV.
- n + Si constituting the substrate 401 is doped with P at a high concentration
- the p + poly-Si film 405 is doped with B at a high concentration
- the end of the conduction band Ec1 of n + Si is p
- the energy is close to the end of the valence band Ev2 of the + poly-Si film 404.
- the n-type silicon oxide film 402 includes the plurality of quantum dots 4021 as described above, the n-type silicon oxide film 402 has a stacked structure of the quantum dots 4021 and the silicon dioxide (SiO 2 ) layer 4022 that does not include the quantum dots 4021. As a result, the quantum dots 4021 are sandwiched between the SiO 2 layers 4022.
- the SiO 2 layer 4022 has an energy band gap of about 9 eV. Further, the quantum dot 4021, because it is sandwiched by two SiO 2 layer 4022, by the quantum size effect, has a sub-level L sub 1 in the conduction band Ec1 side of n + Si, the n + Si valence The sub-level L sub 2 is provided on the band Ev1 side.
- the sub-level L sub 1 is higher in energy than the conduction band Ec1 of n + Si, and the sub-level L sub 2 is higher in energy than the end of the valence band Ev1 of n + Si.
- the energy difference between the sub-level L sub 1 and the sub-level L sub 2 is larger than the energy gap Eg1 of n + Si.
- the i-type silicon nitride film 403 includes a plurality of quantum dots 4031 as described above, the i-type silicon nitride film 403 has a stacked structure of the quantum dots 4031 and the silicon nitride film (Si 3 N 4 ) layer 4032 not including the quantum dots 4031. . As a result, the quantum dots 4031 are sandwiched between the Si 3 N 4 layers 4032.
- the Si 3 N 4 layer 4032 has an energy band gap of about 5.2 eV. Further, since the quantum dot 4031 is sandwiched between the two Si 3 N 4 layers 4032, the quantum dot effect has a sub-level L sub 3 on the conduction band Ec 2 side of the p + poly-Si film 405 due to the quantum size effect. The p + poly-Si film 405 has a sub-level L sub 4 on the valence band Ev4 side.
- the sub-level L sub 3 is energetically higher than the end of the conduction band Ec2 of the p + poly-Si film 405, and the sub-level L sub 4 is the end of the valence band Ev2 of the p + poly-Si film 405. Higher in energy. As a result, the energy difference between the sub-level L sub 3 and the sub-level L sub 4 is larger than the energy gap Eg1 of the p + poly-Si film 405.
- the p-type silicon oxynitride film 404 includes the plurality of quantum dots 4041 as described above, the p-type silicon oxynitride film 404 has a stacked structure of the quantum dots 4041 and the silicon oxynitride film layer 4042 that does not include the quantum dots 4041. As a result, the quantum dots 4041 are sandwiched between the silicon oxynitride film layers 4042.
- the silicon oxynitride film layer 4042 has an energy band gap of 7.1 eV. Further, the quantum dot 4041, because it is sandwiched by two silicon oxynitride film layer 4042, by the quantum size effect, it has a sub-level L sub 5 in the conduction band Ec2 side of p + Si, the p + Si It has a sub-level L sub 6 on the valence band Ev2 side.
- the sub-level L sub 5 is energetically higher than the conduction band Ec2 of p + Si, and the sub-level L sub 6 is energetically higher than the end of the valence band Ev2 of p + Si.
- the energy difference between the sub-level L sub 5 and the sub-level L sub 6 is larger than the energy gap Eg1 of p + Si.
- the energy difference ⁇ E5 the end of the conduction band edge and a silicon oxynitride film layer 4042 of the conduction band Ec2 of p + Si is 4.2 eV
- the energy difference ⁇ E6 from the end of the valence band of the film layer 4042 is about 1.78 eV.
- FIG. 11 is an energy band diagram of the light emitting element 400 illustrated in FIG.
- a voltage is applied between the electrodes 406 and 407 with the electrode 406 side being positive and the electrode 407 side being negative, as shown in FIG. 11, the energy band of n + Si constituting the substrate 401 is raised, and electrons in the n + Si are raised.
- 11 conducts through the n-type silicon oxide film 402 through the plurality of quantum dots 4021 in the n-type silicon oxide film 402 and is injected into the i-type silicon nitride film 403.
- the p-type silicon oxynitride film 404 has a larger barrier to electrons than the i-type silicon nitride film 403, the electrons injected into the i-type silicon nitride film 403 are converted into the p-type silicon oxynitride film 404. And accumulated in the quantum dots 4031 of the i-type silicon nitride film 403.
- the holes 12 in the p + poly-Si film 405 are conducted in the p-type silicon oxynitride film 404 through the quantum dots 4041 in the p-type silicon oxynitride film 404, and in the i-type silicon nitride film 403. Injected into. Since the n-type silicon oxide film 402 has a larger barrier against holes than the i-type silicon nitride film 403, the holes injected into the i-type silicon nitride film 403 are converted into the n-type silicon oxide film 402. And accumulated in the quantum dots 4031 of the i-type silicon nitride film 403.
- the electrons 13 accumulated in the quantum dots 4031 recombine with the holes 14 accumulated in the quantum dots 4031 to emit light.
- the light emitting element 400 confines electrons injected from the n + Si 401 into the i-type silicon nitride film 403 in the i-type silicon nitride film 403 by the p-type silicon oxynitride film 404, and the p + poly-Si film 405.
- the holes injected into the i-type silicon nitride film 403 are confined in the i-type silicon nitride film 403 by the n-type silicon oxide film 402. That is, the light emitting element 400 is characterized in that both holes and electrons are confined in the i-type silicon nitride film 403. As a result, the light emission efficiency of the light emitting element 400 can be increased.
- the n-type silicon oxide film 402 includes a plurality of quantum dots 4021 irregularly
- the i-type silicon nitride film 403 includes a plurality of quantum dots 4031 irregularly
- the p-type silicon oxynitride film 404 includes a plurality of p-type silicon oxynitride films 404. Since the quantum dots 4041 are irregularly included, the efficiency of injecting electrons and holes is improved by the electric field enhancement effect of the randomly arranged quantum dots 4021, 4031, and 4041.
- the luminous efficiency can be increased.
- FIG. 12 and 13 are first and second process diagrams for explaining a method of manufacturing the light-emitting element 400 shown in FIG. 8, respectively.
- substrate 401 made of n + Si is prepared (see step (a)), and after cleaning substrate 401, sample holder of plasma CVD apparatus 100 is prepared.
- a substrate 1 is set on 103.
- a silicon oxide film 4011 is deposited on one main surface of the substrate 1 under the reaction conditions shown in Table 1.
- a silicon nitride film 4012 is deposited on the silicon oxide film 4011 under the reaction conditions shown in Table 2.
- a silicon oxynitride film 4013 is deposited on the silicon nitride film 4012 under the reaction conditions shown in Table 3.
- an amorphous silicon (a-Si) film 4014 is deposited on the silicon oxynitride film 4013 under the reaction conditions in which N 2 O gas and NH 3 gas are stopped under the reaction conditions shown in Table 3 (step of FIG. 12). (See (b)).
- phosphorus ions (P + ) are implanted into the silicon oxide film 4011 by ion implantation (see step (c) in FIG. 12).
- the acceleration voltage for ion implantation is set so that P + ions are implanted only into the silicon oxide film 4011.
- boron ions (B + ) are implanted into the silicon nitride film 4012, the silicon oxynitride film 4013, and the a-Si film 4014 by ion implantation (see step (d) in FIG. 12).
- the acceleration voltage for ion implantation is set so that B + ions are implanted into the silicon nitride film 4012, the silicon oxynitride film 4013, and the a-Si film 4014.
- the substrate 1 / n-type silicon oxide film 4011 / p-type silicon nitride film 4012 / p-type silicon oxynitride film 4013 / p-type a-Si film 4014 is subjected to RTA by the method described above. (See step (e) in FIG. 13).
- an n-type silicon oxide film 402 an i-type silicon nitride film 403, a p-type silicon oxynitride film 404, and a p + poly-Si film 405 are formed (see step (f) in FIG. 13).
- the p + poly-Si film 405 is patterned into p + poly-Si films 4051 to 4054 using a photolithography technique (see step (g) in FIG. 13).
- electrodes 406 (4061 to 4064) are formed on the p + poly-Si films 4051 to 4054 by sputtering of Al, respectively, and an electrode 407 is formed on the back surface of the substrate 401 (see step (h) in FIG. 13). ). Thereby, the light emitting element 400 is completed.
- the present invention is applied to a method for producing multilayer quantum dots capable of controlling size and density.
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Abstract
Description
Claims (10)
- 第1の元素を含む第1の材料に対する、第2の元素を含む第2の材料の量比を基準値以上に設定して薄膜を基板上に堆積する第1の工程と、
前記第1の工程において堆積された前記薄膜を基準昇温レート以上の昇温レートで設定温度に昇温する第2の工程と、
前記薄膜を前記設定温度で熱処理する第3の工程とを備え、
前記基準値は、前記第1および第2の元素を含む絶縁膜を形成するときの前記第1の材料に対する前記第2の材料の量比である、量子ドットの製造方法。 - 前記第1の工程において、非晶質相からなる前記薄膜が前記基板上に堆積される、請求の範囲第1項に記載の量子ドットの製造方法。
- 前記第3の工程の後、前記薄膜を基準降温レート以上の降温レートで冷却する第4の工程をさらに備える、請求の範囲第1項に記載の量子ドットの製造方法。
- 前記第3の工程の後、前記薄膜を基準降温レートよりも低い降温レートで冷却する第4の工程をさらに備える、請求の範囲第1項に記載の量子ドットの製造方法。
- 前記第1の元素は、酸素、窒素およびカーボンのいずれかからなり、
前記第2の元素は、Si,Ge,CおよびSnのいずれかからなる、請求の範囲第1項に記載の量子ドットの製造方法。 - 前記第2の元素は、SiおよびGeのいずれかからなる、請求の範囲第5項に記載の量子ドットの製造方法。
- 第1の基準値は、前記第1および第2の元素を含む絶縁膜を形成するときの前記第1の材料に対する前記第2の材料の量比であり、
第2の基準値は、第3の元素および前記第2の元素を含む絶縁膜を形成するときの前記第3の元素を含む第3の材料に対する前記第2の材料の量比であり、
前記第1の工程において、前記第1の材料に対する前記第2の材料の量比を前記第1の基準値以上に設定し、かつ、前記第3の材料に対する前記第2の材料の量比を前記第2の基準値以上に設定して前記薄膜を前記基板上に堆積する、請求の範囲第1項に記載の量子ドットの製造方法。 - 前記第1の元素は、酸素からなり、
前記第2の元素は、シリコンおよびゲルマニウムのいずれかからなり、
前記第3の元素は、窒素からなる、請求の範囲第7項に記載の量子ドットの製造方法。 - 前記昇温レートは、0.2℃/s~500℃/sの範囲である、請求の範囲第1項に記載の量子ドットの製造方法。
- 前記降温レートは、5℃/s~50℃/sの範囲である、請求の範囲第1項に記載の量子ドットの製造方法。
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JP2015220249A (ja) * | 2014-05-14 | 2015-12-07 | 富士通株式会社 | 量子ドットアレイの製造装置及び製造方法 |
JP2020500416A (ja) * | 2016-10-08 | 2020-01-09 | 中国科学院蘇州納米技術与納米倣生研究所Suzhou Institute Of Nano−Tech And Nano−Bionics(Sinano),Chinese Academy Of Sciences | 量子ドット構造の製造方法 |
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CN113359347B (zh) * | 2021-05-28 | 2022-12-23 | 深圳市华星光电半导体显示技术有限公司 | 一种量子点沉积装置 |
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