# US 12,014,907 B2 · Method and device for forming graphene structure > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 12,014,907 B2 - Document ID: US12014907B2 - Status: Granted - Kind: B2 - Application number: 17/593,220 - Filed: 2020-02-26 - Published: 2022-07-14 - Granted: 2024-06-18 - Earliest claimed: 2019-03-15 - Assignees: Tokyo Electron Limited - Applicants: Tokyo Electron Limited - Inventors: Ryota Ifuku; Takashi Matsumoto; Masahito Sugiura - Web page: https://patentgrep.com/patent/US12014907B2 ## CPC - H01J 37/32724: {Temperature} - C01B 32/186: by chemical vapour deposition [CVD] - C23C 16/0218: {in a reactive atmosphere (C23C16/0227 takes precedence)} - C23C 16/26: Deposition of carbon only - C23C 16/511: using microwave discharges - H01J 37/3222: {Antennas} - H01J 37/32357: {Generation remote from the workpiece, e.g. down-stream} - H05H 1/46: using applied electromagnetic fields, e.g. high frequency or microwave energy (H05H1/26 takes precedence) - H10P 14/24: using chemical vapour deposition [CVD] - H10P 14/3406: {Carbon, e.g. diamond-like carbon} - H10P 14/43: Chemical deposition, e.g. chemical vapour deposition [CVD] - H10P 14/6336: {in the presence of a plasma [PECVD]} - H10P 14/6504: {In-situ cleaning} - H10P 14/6902: {composed of carbon, e.g. alpha-C, diamond or hydrogen doped carbon} - H10W 20/038: {covering conductive structures (H10W20/037 takes precedence)} - H01J 2237/3321: CVD [Chemical Vapor Deposition] - H10P 14/3206: {Carbon, e.g. diamond-like carbon} - H10P 14/36: {characterised by treatments done before the formation of the materials} - H01J: ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS (spark-gaps H01T; electric arc lamps H05B31/00; particle accelerators H05H) - C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C} - C23C: COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL (making metal-coated products by extrusion B21C23/22; covering with metal by connecting pre-existing layers to articles, see the relevant places, e.g. B21D39/00, B23K; metallising of glass C03C; metallising mortars, concrete, artificial stone, ceramics or natural stone C04B41/00; enamelling of, or applying a vitreous layer to, metals C23D; treating metal surfaces or coating of metals by electrolysis or electrophoresis C25D; single-crystal film growth C30B; by metallising textiles D06M11/83; decorating textiles by locally metallising D06Q1/04) - H05H: PLASMA TECHNIQUE (apparatus or processes specially adapted for producing X-rays H05G2/00); PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS - H10P: GENERIC PROCESSES OR APPARATUS FOR THE MANUFACTURE OR TREATMENT OF DEVICES COVERED BY CLASS H10 - H10W: GENERIC PACKAGES, INTERCONNECTIONS, CONNECTORS OR OTHER CONSTRUCTIONAL DETAILS OF DEVICES COVERED BY CLASS H10 ## Abstract A method of forming a graphene structure, includes: providing a substrate; performing a preprocessing by supplying a first processing gas including a carbon-containing gas to the substrate while heating the substrate, without using plasma; and after the preprocessing, forming the graphene structure on a surface of the substrate through a plasma CVD using plasma of a second processing gas including a carbon-containing gas. ## Claims ### Claim 1 A method of forming a graphene structure, the method comprising: providing a substrate; performing a preprocessing by supplying a first processing gas including a carbon-containing gas to the substrate while heating the substrate, without using plasma; and after the preprocessing, forming the graphene structure on a surface of the substrate through a plasma chemical vapor deposition (CVD) using plasma of a second processing gas including a carbon-containing gas, wherein the carbon-containing gas included in the first processing gas is a hydrocarbon gas. ### Claim 2 (depends on 1) The method of claim 1, wherein the preprocessing has a processing time of 30 seconds or more. ### Claim 3 (depends on 2) The method of claim 2, wherein the preprocessing has the processing time in a range of 1 to 10 minutes. ### Claim 4 (depends on 1) The method of claim 1, wherein the preprocessing is performed while heating the substrate at a temperature in a range of 300 to 1,000 degrees C. ### Claim 5 (depends on 1) The method of claim 1, wherein the hydrocarbon gas has an unsaturated bond. ### Claim 6 (depends on 1) The method of claim 1, wherein the first processing gas further includes a hydrogen gas. ### Claim 7 (depends on 1) The method of claim 1, wherein the carbon-containing gas included in the first processing gas and the carbon-containing gas contained in the second processing gas are a same gas. ### Claim 8 (depends on 1) The method of claim 1, wherein, in the forming the graphene structure, the graphene structure is formed in a state in which the surface of the substrate does not have a catalytic function. ### Claim 9 (depends on 8) The method of claim 8, wherein the surface of the substrate is an insulator, a semiconductor, or a non-activated metal. ### Claim 10 (depends on 1) The method of claim 1, wherein the plasma CVD is a remote microwave plasma CVD. ### Claim 11 (depends on 10) The method of claim 10, wherein the forming the graphene structure is performed under a condition in which a temperature of the substrate is in a range of 350 to 1,000 degrees C., a microwave power is in a range of 100 to 5,000 W, and a time is in a range of 1 to 200 minutes. ### Claim 12 (depends on 1) The method of claim 1, wherein the second processing gas further includes a hydrogen gas. ### Claim 13 An apparatus for forming a graphene structure, comprising: a processing container in which a substrate is accommodated; a heating mechanism configured to heat the substrate; a planar slot antenna having a slot and provided on the processing container via a microwave transmission plate made of a dielectric material that constitutes a ceiling wall of the processing container; a microwave introduction mechanism configured to introduce microwaves into the processing container through the slot and the microwave transmission plate; a gas introduction mechanism configured to supply a processing gas including a carbon-containing gas and an oxidizing gas into the processing container; an exhaust mechanism configured to exhaust an interior of the processing container; and a controller configured to control the heating mechanism, the microwave introduction mechanism, the gas introduction mechanism, and the exhaust mechanism to execute: after the substrate is loaded into the processing container, performing a preprocessing by supplying a first processing gas including the carbon-containing gas to the substrate while heating the substrate, without using plasma; and after the preprocessing, forming the graphene structure on a surface of the substrate through a plasma CVD using plasma of a second processing gas including the carbon-containing gas, wherein the carbon-containing gas included in the first processing gas is a hydrocarbon gas.