TWI785510B - Substrate processing apparatus, semiconductor device manufacturing method, and recording medium - Google Patents

Abstract

The present invention provides a technique comprising: a processing chamber for processing a substrate; a substrate supporter for holding a plurality of substrates vertically in multiple stages; The buffer structure and the external electrode are arranged outside the above-mentioned processing chamber corresponding to the position where the buffer structure is installed, and generate plasma.

Description

Substrate processing apparatus, manufacturing method of semiconductor device, and recording medium

The present invention relates to a substrate processing device, a method for manufacturing a semiconductor device, and a recording medium.

As one of the manufacturing steps of a semiconductor device, the substrate carried into the processing chamber of the substrate processing device is activated and supplied with a raw material gas or a reactive gas by plasma, and an insulating film, a semiconductor film, a conductive film, etc. are formed on the substrate. Various films, or substrate processing to remove various films. For example, in Patent Document 1, a buffer chamber for generating plasma is provided in the reaction tube. [Prior Art Literature] [Patent Document]

Patent Document 1: Japanese Patent Laid-Open No. 2016-106415

(Problem to be solved by the invention)

An object of the present invention is to provide a technology capable of supplying a plasma active species gas formed with high efficiency to a substrate. (technical means to solve the problem)

According to one aspect of the present invention, a technology is provided, which has: A processing chamber for processing substrates; A substrate support for holding a plurality of the above-mentioned substrates vertically in multiple stages; and The plasma generation part is provided in the above-mentioned processing chamber, and has a buffer structure for plasmaizing the gas, and an external electrode. Plasma. (compared to the effect of previous technology)

According to the present invention, it is possible to provide a technology capable of supplying a plasma active species gas formed with high efficiency to a substrate.

<Embodiment of the present invention> An embodiment of the present invention will be described below with reference to FIGS. 1 to 5 .

(1) Composition of substrate processing equipment (heating equipment) As shown in FIG. 1 , the processing furnace 202 used in the substrate processing apparatus is a so-called vertical furnace capable of storing substrates in multiple stages in the vertical direction, and has a heater 207 as a heating device (heating mechanism). The heater 207 has a cylindrical shape and is vertically supported by a heater base (not shown) as a holding plate. The heater 207 also has a function as an activation mechanism (activation unit) for activating (exciting) gas with heat as described later.

(Processing Chamber) Inside the heater 207 , the reaction tube 203 is arranged concentrically with the heater 207 . The reaction tube 203 is made of a heat-resistant material such as quartz (SiO ₂ ) or silicon carbide (SiC), and is formed in a cylindrical shape with a closed upper end and an open lower end. Below the reaction tube 203 , a manifold (inlet flange) 209 is arranged concentrically with the reaction tube 203 . The manifold 209 is made of metal such as stainless steel (SUS), and is formed in a cylindrical shape with open upper and lower ends. The upper end of the manifold 209 is engaged with the lower end of the reaction tube 203 to support the reaction tube 203 . Between the manifold 209 and the reaction tube 203, an O-ring 220a as a sealing member is provided. The manifold 209 is supported by the heater base so that the reaction tubes 203 are vertically erected. The processing container (reaction container) is mainly composed of the reaction tube 203 and the manifold 209 . A processing chamber 201 is formed in the hollow portion of the cylinder inside the processing container. The processing chamber 201 is configured to accommodate a plurality of wafers 200 serving as substrates. In addition, the processing container is not limited to the above configuration, and only the reaction tube 203 may be referred to as a processing container.

In the processing chamber 201 , the nozzle 249 a and the piping 249 b are installed so as to penetrate the side wall of the manifold 209 . The gas supply pipes 232a and 232b are respectively connected to the nozzle 249a and the pipe 249b. In this way, one nozzle 249a, one pipe 249b, and two gas supply pipes 232a, 232b are provided in the processing chamber 201, and plural kinds of gases can be supplied into the processing chamber 201.

Mass flow controllers (MFC) 241a, 241b belonging to flow controllers (flow control parts) and valves 243a, 243b belonging to on-off valves are provided in the gas supply pipes 232a, 232b in order from the upstream side of the gas flow. Gas supply pipes 232c, 232d for supplying an inert gas are connected to the downstream side of the gas supply pipes 232a, 232b from the valves 243a, 243b, respectively. In the gas supply pipes 232c and 232d, MFCs 241c and 241d and valves 243c and 243d are provided in this order from the upstream side of the gas flow.

As shown in FIG. 2 , the nozzle 249a is located in the space between the inner wall of the reaction tube 203 and the wafer 200, and is arranged to stand vertically from the lower part of the inner wall of the reaction tube 203 along the upper part toward the upper part of the stacking direction of the wafer 200. rise. That is, the nozzles 249a are arranged along the wafer arrangement region in the side of the wafer arrangement region (loading region) where the wafer 200 is arranged (loaded), horizontally surrounding the region of the wafer arrangement region . That is, the nozzles 249a are provided on the side of the end (peripheral edge) of each wafer 200 carried into the processing chamber 201 in a direction perpendicular to the surface (flat surface) of the wafer 200 . On the side surface of the nozzle 249a, a gas supply hole 250a for supplying gas is provided. The gas supply hole 250 a opens toward the center of the reaction tube 203 and can supply gas toward the wafer 200 . The gas supply holes 250a are provided in plural from the lower part to the upper part of the reaction tube 203, each having the same opening area and arranged at the same opening pitch.

The pipe 249b is connected to the front end of the gas supply pipe 232b. The pipe 249b is connected to the inside of the buffer structure 237 . In the present embodiment, the two buffer structures 237 are disposed sandwiching a straight line passing through the center of the reaction tube 203 (processing chamber 201) and the nozzle 249a in a plan view, or sandwiching a line passing through the center of the reaction tube 203 (processing chamber 201) and the nozzle 249a. The exhaust pipe (exhaust portion) 231 is arranged in a straight line, and the two buffer structures 237 are arranged symmetrically with respect to the line connecting the nozzle 249a and the exhaust pipe 231 . A partition plate 237a is provided in the buffer structure 237, and the partition plate 237a partitions into a gas introduction region 237b into which gas is introduced through the pipe 249b and a plasma region 237c in which the gas is plasmatized. The plasma region 237c is also referred to as a buffer chamber 237c belonging to the gas dispersion space. The buffer chamber 237c is arranged on the nozzle 249a side, and the gas introduction area 237b is arranged on the exhaust pipe 231 side.

As shown in FIG. 2 , the buffer chamber 237c is in the annular space between the inner wall of the reaction tube 203 and the wafer 200 when viewed from above, and is a part that covers from the lower part to the upper part of the inner wall of the reaction tube 203 , arranged along the loading direction of the wafer 200 . That is, the buffer chamber 237c is formed by the buffer structure 237 in such a manner that it surrounds the wafer arrangement region horizontally on the side of the wafer arrangement region and along the wafer arrangement region. The buffer structure 237 is made of an insulating material such as quartz or SiC, which is a heat-resistant material, and gas supply ports 302 and 304 for supplying gas are formed on the arc-shaped wall surface of the buffer structure 237 . The gas supply ports 302 and 304 are provided in multiples in the horizontal direction of the stacked wafers 200 , and open toward the center of the reaction tube 203 to supply gas to the wafers 200 . The gas supply ports 302 and 304 are arranged in plural along the loading direction of the wafer 200 from the lower part to the upper part of the reaction tube 203 , have the same opening area and are arranged at the same opening pitch.

The gas introduction area 237 b is set so as to rise from the lower part of the inner wall of the reaction tube 203 along the upper part toward the upper side of the loading direction of the wafer 200 . The partition plate 237a is provided with a gas supply hole 237d for supplying gas to the plasma region 237c from the gas introduction region 237b. Thereby, the reaction gas supplied to the gas introduction area 237b is dispersed in the buffer chamber 237c. Like the gas supply holes 250a, the gas supply holes 237d are provided in plural from the lower part to the upper part of the reaction tube 203 . In addition, instead of the piping 249b and the gas introduction area 237b, a nozzle, for example, a multi-hole nozzle similar to the nozzle 249a may be provided in the buffer chamber 237c to supply the processing gas.

In this way, in the present embodiment, it passes through the circular ring-shaped vertical space defined by the inner wall of the side wall of the reaction tube 203 and the ends of the plurality of wafers 200 arranged in the reaction tube 203 ( That is, the nozzle 249a and the buffer chamber 237c arranged in the cylindrical space) convey the gas. Then, the gas is first blown into the reaction tube 203 near the wafer 200 through the gas supply hole 250a and the gas supply ports 302 and 304 respectively opened in the nozzle 249a and the buffer chamber 237c. Then, the main flow of the gas in the reaction tube 203 is made to be a direction parallel to the surface of the wafer 200, that is, a horizontal direction. With such a configuration, the gas can be uniformly supplied to each wafer 200, and the film thickness uniformity of the film formed on each wafer 200 can be improved. The gas flowing on the surface of the wafer 200 , that is, the residual gas after the reaction flows toward the exhaust port, that is, the direction of the exhaust pipe 231 described later. However, the flow direction of the remaining gas is appropriately specified by the position of the exhaust port, and is not limited to the vertical direction.

From the gas supply pipe 232a, a raw material containing a predetermined element, for example, a silane raw material gas containing silicon (Si) as a predetermined element is supplied into the processing chamber 201 through the MFC 241a, the valve 243a, and the nozzle 249a.

The so-called raw material gas refers to a raw material in a gaseous state, such as a gas obtained by vaporizing a raw material that is in a liquid state at normal temperature and pressure, or a raw material that is in a gaseous state at normal temperature and pressure. In this specification, when the term "raw material" is used, it means the case of "liquid raw material in liquid state", the case of "raw material gas in gaseous state", or both of these cases.

As the silane source gas, for example, a source gas containing Si and a halogen element, that is, a halosilane source gas can be used. Halosilane raw material gas system refers to silane raw materials with halogen groups. The halogen element system contains at least one kind selected from the group consisting of chlorine (Cl), fluorine (F), bromine (Br), and iodine (I). That is, the halosilane raw material contains at least one halogen group selected from the group consisting of chlorine, fluorine, bromine, and iodine. Halosilane raw materials can also be described as a kind of halides.

As the halosilane source gas, for example, a source gas containing Si and Cl, that is, a chlorosilane source gas can be used. As the chlorosilane raw material gas, for example, dichlorosilane (SiH ₂ Cl ₂ , abbreviated: DCS) gas can be used.

The gas supply pipe 232b is configured to pass a reactant (reactant) containing an element different from the aforementioned predetermined element, for example, nitrogen (N)-containing gas as a reaction gas, through the MFC 241b, the valve 243b, the piping 249b, and the gas introduction area. 237b is supplied into the buffer chamber 237c. As the N-containing gas, for example, a hydrogen nitride-based gas can be used. The hydrogen nitride-based gas is also called a substance composed of only two elements of N and H, and can function as a nitriding gas, that is, a N source. As the hydrogen nitride-based gas, for example, ammonia (NH ₃ ) gas can be used.

From the gas supply pipes 232c and 232d, nitrogen (N ₂ ) gas as an inert gas is supplied into the processing chamber 201 through the MFCs 241c and 241d, the valves 243c and 243d, the gas supply pipes 232a and 232b, the nozzle 249a and the pipe 249b, respectively.

The raw material gas supply system which is a 1st gas supply system is comprised mainly by the gas supply pipe 232a, MFC241a, and the valve 243a. A reactant supply system (a reactant supply system) as a second gas supply system is mainly composed of the gas supply pipe 232b, the MFC 241b, and the valve 243b. The inert gas supply system is mainly composed of gas supply pipes 232c, 232d, MFCs 241c, 241d, and valves 243c, 243d. The raw material supply system, the reactant supply system, and the inert gas supply system are also collectively referred to as a gas supply system (gas supply unit) for short.

(Plasma Generation Department) Next, the plasma generation unit will be described using FIGS. 1 to 3 .

As shown in Figure 2, the plasma system uses capacitively coupled plasma (CCP for short), and when the reaction gas is supplied, it is inside the reaction tube 203 (processing chamber 201) which is made of quartz and belongs to the vacuum partition. The buffer structure 237 is generated.

As shown in FIG. 2 and FIG. 3( a ), the external electrodes 300 are composed of rectangular thin plates having long sides in the arrangement direction of the wafers 200 . As shown in Figure 1 and Figure 3(b), the external electrode 300 is the first external electrode (Hot electrode) 300-1 connected to the high-frequency power supply 273 through the integrator 272, and the second external electrode (Hot electrode) 300-1 connected to the reference potential 0V and grounded through the earth. The external electrodes (ground electrodes) 300-2 are arranged at equal intervals. In the present invention, it will be described as the external electrode 300 unless it is necessary to distinguish and explain.

The external electrode 300 is located between the reaction tube 203 and the heater 207 and is located outside the processing chamber 201 corresponding to the position where the buffer structure 237 is provided. Specifically, the buffer structure is provided with a plasma region (buffer chamber) 237c as a region for plasmating the gas, and the external electrode 300 is along the outer wall of the reaction tube 203 corresponding to the position where the buffer chamber 237c is provided ( The outside of the processing chamber 201) is arranged in a slightly arc shape. The external electrode 300 is arranged, for example, fixed to the inner wall surface of an arcuate quartz cover with a central angle of not less than 30 degrees and not more than 240 degrees. That is, the external electrode 300 is disposed on the outer periphery of the reaction tube 203 (outside the processing chamber 201 ) corresponding to the position where the buffer chamber (plasma region) 237c is provided. Furthermore, the buffer structure 237 is provided with a gas supply portion (gas introduction region) 237b as a region for supplying gas to the buffer chamber 237c. The external electrode 300 is not disposed on the outer periphery of the reaction tube 203 (outside of the processing chamber 201 ) corresponding to the position where the gas introduction area (gas supply portion) 237 b is provided. The external electrode 300 is input with a high frequency such as 13.56 MHz from the high frequency power supply 273 through the integrator 272, thereby generating plasma active species 306 in the buffer chamber 237c. With the plasma thus generated, plasma active species 306 for substrate processing can be supplied from the periphery of the wafer 200 to the surface of the wafer 200 . The plasma generating unit is mainly composed of the buffer structure 237 , the external electrode 300 and the high-frequency power supply 273 .

The external electrode 300 can also be made of metals such as aluminum, copper, and stainless steel, but it is made of an oxidation-resistant material such as nickel, which can suppress deterioration of electrical conductivity and allow substrate processing. In particular, by being made of an aluminum-added nickel alloy material, an AlO film belonging to an oxide film having high heat resistance and corrosion resistance can be formed on the electrode surface. Due to the effect of this film formation, the progress of deterioration toward the inside of the electrode can be suppressed, so the reduction in plasma generation efficiency due to the reduction in electrical conductivity can be suppressed.

(Electrode Fixture) Next, a quartz cover 301 as an electrode fixing jig for fixing the external electrode 300 will be described using FIG. 3 . As shown in Fig. 3(a) and (b), the plurality of external electrodes 300 are provided by hooking their notches (not shown) on the inner wall surface of the curved quartz cover 301 belonging to the electrode fixing jig. The protruding part 310 is provided so as to slide and fix, and is unitized (hook-type electrode unit) so as to be integrated with the quartz cover 301 and provided on the outer periphery of the reaction tube 203 . Herein, the electrode fixing unit including the external electrode 300 and the quartz cover 301 belonging to the electrode fixing jig is called. Also, as materials for the quartz cover 301 and the external electrodes 300, quartz and nickel alloys are used, respectively.

In order to obtain high processing capacity according to the substrate temperature below 500°C, it is preferable to set the occupancy rate of the quartz cover 301 as an arc shape with a central angle of 30 degrees or more and 240 degrees or less, and avoid the exhaust port in order to avoid particles. The arrangement of the exhaust pipe 231 or the nozzle 249a, etc. If the central angle is less than 30 degrees, the number of external electrodes 300 to be arranged will decrease, and the amount of plasma production will decrease. If the central angle is larger than 240 degrees, the area covered by the quartz cover 301 on the side of the reaction tube 203 becomes too large, and thermal energy from the heater 207 is blocked. In this embodiment, two quartz covers with a central angle of 110 degrees are arranged symmetrically.

The reaction tube 203 is provided with an exhaust pipe 231 as an exhaust unit for exhausting the atmosphere in the processing chamber 201 . In the exhaust pipe 231, it passes through the pressure sensor 245 as a pressure detector (pressure detection part) for detecting the pressure in the processing chamber 201, and through the APC (Auto Pressure Controller) as an exhaust valve (pressure adjustment part). Pressure controller) valve 244, is connected as the vacuum pump 246 of vacuum exhaust device. The APC valve 244 is configured to: switch the valve according to the state of the vacuum pump 246, and perform vacuum exhaust in the processing chamber 201 and stop the vacuum exhaust; The detected pressure data is used to adjust the valve opening, thereby adjusting the pressure in the processing chamber 201 . The exhaust system is mainly composed of exhaust pipe 231 , APC valve 244 and pressure sensor 245 . In addition, the vacuum pump 246 can also be regarded as being included in the exhaust system. The exhaust pipe 231 is not limited to being provided in the reaction tube 203 , and may be provided in the manifold 209 similarly to the nozzle 249 a.

Below the manifold 209, there is provided a sealing cover 219 as a furnace mouth cover which can airtightly close the lower opening of the manifold 209. The sealing cap 219 is configured to contact the lower end of the manifold 209 from the lower side in the vertical direction. The sealing cap 219 is made of a metal material such as SUS, and is formed in a disc shape. On the upper surface of the sealing cover 219, an O-ring 220b as a sealing member abutting against the lower end of the manifold 209 is provided. On the side opposite to the processing chamber 201 of the sealing cover 219, a rotation mechanism 267 for rotating the wafer boat 217 described later is provided. The rotating shaft 255 of the rotating mechanism 267 passes through the sealing cover 219 and is connected to the wafer boat 217 . The rotation mechanism 267 is configured to rotate the wafer 200 by rotating the wafer boat 217 . The sealing cover 219 is configured to be lifted in the vertical direction by the boat lifter 115 as a lifting mechanism vertically arranged outside the reaction tube 203 . The wafer boat lifter 115 is configured to carry the wafer boat 217 in and out of the processing chamber 201 by lifting and lowering the sealing cover 219 . The boat lifter 115 is configured as a transfer device (transfer mechanism) for transferring the wafer boat 217 , that is, the wafer 200 inside and outside the processing chamber 201 . Also, below the manifold 209, a shutter 219s as a furnace door cover is provided which can airtightly close the opening of the lower end of the manifold 209 when the sealing cover 219 is lowered by the boat lifter 115. The shutter 219s is made of metal such as SUS, and is formed in a disc shape. On the upper surface of the shutter 219s, an O-ring 220c as a sealing member abutting against the lower end of the manifold 209 is provided. The switching action (lifting or rotating action, etc.) of the door stopper 219s is controlled by the door stopper switch mechanism 115s.

(substrate support) As shown in FIG. 1 , the wafer boat 217 as a substrate support is configured so that a plurality of wafers 200 , for example, 25 to 200 wafers 200 are aligned in a horizontal posture and centered with each other, and are arranged neatly in the vertical direction in multiple stages. ground support, that is, arranged at predetermined intervals. The wafer boat 217 is made of heat-resistant materials such as quartz or SiC. The lower part of the wafer boat 217 is supported in multiple sections by a heat shield 218 made of heat-resistant materials such as quartz or SiC.

As shown in FIG. 1 , inside the reaction tube 203 , a temperature sensor 263 as a temperature detector is provided. According to the temperature information detected by the temperature sensor 263, the power supply to the heater 207 is adjusted, so that the temperature in the processing chamber 201 becomes a desired temperature distribution. The temperature sensor 263 is provided along the inner wall of the reaction tube 203 similarly to the nozzle 249a.

(control device) Next, the control device will be described using FIG. 4 . As shown in FIG. 4, the controller 121 belonging to the control unit (control device) is constituted as a computer including a CPU (Central Processing Unit) 121a, a RAM (Random Access Memory) 121b, a memory device 121c, and an I/O port 121d. The RAM 121b, the memory device 121c, and the I/O port 121d are configured to exchange data with the CPU 121a via the internal bus 121e. An input/output device 122 configured as a touch panel or the like is connected to the controller 121 .

The memory device 121c is composed of, for example, a flash memory, HDD (Hard Disk Drive), and the like. In the memory device 121c, a control program for controlling the operation of the substrate processing apparatus, a recipe, etc. in which the procedures and conditions of the film formation process described later are stored in a readable manner. The process recipe functions as a program by combining various procedures in the various processes (film formation process) described later by the controller 121 so that a predetermined result can be obtained. Hereinafter, the general term of process recipe or control program is also referred to as program for short. Also, the process recipe is sometimes referred to simply as the recipe. When the term "program" is used in this specification, it refers to the case where only the formula monomer is included, the case where only the control program monomer is included, or the case where both of these are included. The RAM 121b is configured as a memory area (work area) for temporarily storing programs and data read by the CPU 121a.

The I/O port 121d is connected to the above MFC241a~241d, valves 243a~243d, pressure sensor 245, APC valve 244, vacuum pump 246, heater 207, temperature sensor 263, integrator 272, high frequency power supply 273, rotation mechanism 267, crystal boat lifter 115, gate switch mechanism 115s etc.

The CPU 121a is configured to read the control program from the memory device 121c and execute it, and to read the recipe from the memory device 121c in accordance with the input of operation commands from the input/output device 122 . The CPU 121a is configured to control according to the content of the read recipe: the control of the rotating mechanism 267, the flow adjustment actions of various gases by the MFC 241a~241d, the switching actions of the valves 243a~243d, and the high frequency power supply 273 based on impedance monitoring The adjustment action of the APC valve 244, the switch action of the APC valve 244 and the pressure adjustment action based on the pressure sensor 245 using the APC valve 244, the start and stop of the vacuum pump 246, the temperature adjustment action of the heater 207 based on the temperature sensor 263, and the rotation The forward and reverse rotation, rotation angle and rotation speed adjustment of the wafer boat 217 by the mechanism 267, the lifting operation of the wafer boat 217 by the wafer boat elevator 115, the plasma generation by the high frequency power supply 273 and the external electrode 300, etc.

The controller 121 can be configured by installing the above-mentioned programs stored in an external memory device (such as a magnetic disk such as a hard disk, an optical disk such as a CD, a magneto-optical disk such as MO, and a semiconductor memory such as a USB memory) 123 into a computer. The memory device 121c or the external memory device 123 is constituted as a computer-readable recording medium. Hereinafter, these collective terms and abbreviations are also referred to as recording media. When the word recording medium is used in this specification, it refers to the case where only the memory device 121c is included alone, the case where only the external memory device 123 is included alone, or the case where both are included. Furthermore, the computer programs can be provided without using the external memory device 123, but by using communication means such as a network or a dedicated line.

(2) Substrate processing steps Next, a step of forming a thin film on the wafer 200 as one of the steps of manufacturing a semiconductor device using a substrate processing apparatus will be described with reference to FIG. 5 . In the following description, the operation of each part constituting the substrate processing apparatus is controlled by the controller 121 .

Here, by performing the step of supplying DCS gas as the source gas and the step of supplying plasma-excited NH ₃ gas as the reaction gas a predetermined number of times (more than 1 time) at the same time, the wafer 200 A silicon nitride film (SiN film) formed thereon will be described as an example of a film containing Si and N. Also, for example, a predetermined film may be formed on the wafer 200 in advance. Also, a predetermined pattern may be formed in advance on the wafer 200 or a predetermined film.

In this specification, the process flow of the film formation process shown in FIG. 5 is also shown as follows for convenience. (DCS→NH ₃ ^* )×n => SiN

When the word "wafer" is used in this specification, it means the case of the wafer itself, or the case of the laminated body of the wafer and a predetermined layer or film formed on the surface thereof. When the term "wafer surface" is used in this specification, it means the surface of the wafer itself or the surface of a predetermined layer formed on the wafer. When "a predetermined layer is formed on the wafer" is described in this specification, it means that the predetermined layer is directly formed on the surface of the wafer itself, or it means that the layer formed on the wafer, etc. The situation where a predetermined layer is formed above. When the word "substrate" is used in this specification, it has the same meaning as when the word "wafer" is used.

(Move-in step: S1) A plurality of wafers 200 are loaded (wafer filling) into the wafer boat 217, and the shutter 219s is moved by the shutter opening and closing mechanism 115s, so that the opening at the lower end of the manifold 209 is opened (the shutter is opened). Thereafter, as shown in FIG. 1 , the wafer boat 217 supporting a plurality of wafers 200 is lifted by the wafer boat elevator 115 and carried into the processing chamber 201 (wafer loading). In this state, the sealing cap 219 seals the lower end of the manifold 209 via the O-ring 220b.

(Pressure and temperature adjustment step: S2) Vacuum evacuation (decompression evacuation) is performed by the vacuum pump 246 so that the inside of the processing chamber 201 , that is, the space in which the wafer 200 exists, becomes a required pressure (vacuum degree). At this time, the pressure in the processing chamber 201 is measured by the pressure sensor 245, and the APC valve 244 is controlled in feedback according to the measured pressure information. The vacuum pump 246 is kept in a constant operating state at least until the film forming step described later is completed.

Furthermore, the wafer 200 in the processing chamber 201 is heated by the heater 207 so that the temperature becomes desired. At this time, the degree of energization to the heater 207 is feedback-controlled based on the temperature information detected by the temperature sensor 263 so as to achieve a desired temperature distribution in the processing chamber 201 . The heating in the processing chamber 201 by the heater 207 is continued at least until the film forming step described later is completed. Wherein, when the film forming step is performed at a temperature below room temperature, the heating in the processing chamber 201 may not be performed by the heater 207 . Also, when processing only at such a temperature, the heater 207 is unnecessary, and the heater 207 does not need to be provided in the substrate processing apparatus. In this case, the configuration of the substrate processing apparatus can be simplified. Next, the rotation of the wafer boat 217 and the wafer 200 by the rotation mechanism 267 is started. The rotation of the boat 217 and the wafer 200 by the rotation mechanism 267 is continued at least until the film forming step is completed.

(Source gas supply steps: S3, S4) In step S3, DCS gas is supplied to the wafer 200 in the processing chamber 201. The valve 243a is opened, and the DCS gas flows through the gas supply pipe 232a. The flow rate of the DCS gas system is adjusted by the MFC 241 a , supplied into the processing chamber 201 through the gas supply hole 250 a through the nozzle 249 a , and exhausted through the exhaust pipe 231 . At the same time, the valve 243c is opened, and N ₂ gas is passed through the gas supply pipe 232c. The flow rate of the N ₂ gas system is adjusted by the MFC 241c, supplied into the processing chamber 201 together with the DCS gas, and exhausted through the exhaust pipe 231 .

Moreover, in order to suppress the intrusion of DCS gas into the pipe 249b, the valve 243d is opened, and _N2 gas flows through the gas supply pipe 232d. N ₂ gas is supplied into the processing chamber 201 through the gas supply pipe 232 b and the pipe 249 b, and is exhausted through the exhaust pipe 231 .

The supply flow rate of the DCS gas controlled by the MFC 241a is, for example, set to a flow rate in the range of 1 sccm to 6000 sccm, preferably 3000 sccm to 5000 sccm. The supply flow rates of the N ₂ gas controlled by the MFCs 241c and 241d are, for example, set to flow rates within the range of 100 sccm or more and 10000 sccm or less, respectively. The pressure in the processing chamber 201 is, for example, set to a pressure in the range of not less than 1 Pa and not more than 2666 Pa, preferably not less than 665 Pa and not more than 1333 Pa. The time during which the wafer 200 is exposed to the DCS gas is, for example, about 20 seconds per cycle. Also, the time for which the wafer 200 is exposed to the DCS gas varies depending on the film thickness.

The temperature of the heater 207 is set so that the temperature of the wafer 200 falls within a range of, for example, 0°C to 700°C, preferably room temperature (25°C) to 550°C, more preferably 40°C to 500°C. temperature inside. As in this embodiment, by setting the temperature of the wafer 200 to be 700°C or lower, further 550°C or lower, and further 500°C or lower, the amount of heat applied to the wafer 200 can be reduced, and the wafer 200 can be satisfactorily performed. Control of thermal history.

By supplying DCS gas to the wafer 200 under the above conditions, a Si-containing layer is formed on the wafer 200 (base film on the surface). The Si-containing layer system may contain Cl or H in addition to the Si layer. The Si-containing layer is formed by physical adsorption of DCS on the outermost surface of the wafer 200, chemical adsorption of partially decomposed DCS, or thermal decomposition of DCS to accumulate Si. That is, the Si-containing layer may be an adsorption layer (physical adsorption layer or chemical adsorption layer) of DCS or a partially decomposed substance of DCS, or may be a stacked layer of Si (Si layer).

After forming the Si-containing layer, the valve 243a is closed, and the supply of DCS gas to the processing chamber 201 is stopped. At this time, the APC valve 244 is kept open, and the processing chamber 201 is evacuated by the vacuum pump 246, and the unreacted DCS gas or reaction by-products remaining in the processing chamber 201 or used to form the Si-containing layer are automatically Exhaust in the processing chamber 201 (S4). Also, the valves 243c and 243d are kept open, and the N ₂ gas is kept supplied into the processing chamber 201 . The _N2 gas system acts as a flushing gas. Also, this step S4 can also be omitted.

As the raw material gas, in addition to DCS gas, tetradimethylaminosilane (Si[N(CH ₃ ) ₂ ] ₄ , abbreviation: 4DMAS) gas, paradimethylaminosilane (Si[N(CH 3 ) 2 ] 4 , ₃ ) ₂ ] ₃ H, referred to as: 3DMAS) gas, bisdimethylaminosilane (Si[N(CH ₃ ) ₂ ] ₂ H ₂ , referred to as: BDMAS) gas, bisdiethylaminosilane (Si[N( C ₂ H ₅ ) ₂ ] ₂ H ₂ , referred to as: BDEAS) gas, bis-tertiary butylaminosilane (SiH ₂ [NH(C ₄ H ₉ )] ₂ , referred to as: BTBAS) gas, dimethylaminosilane (DMAS) gas, diethylaminosilane (DEAS) gas, dipropylaminosilane (DPAS) gas, diisopropylaminosilane (DIPAS) gas, butylaminosilane (BAS) gas, hexamethyldisilazane (HMDS) gas and other aminosilane raw material gases, or monochlorosilane (SiH ₃ Cl, referred to as MCS) gas, trichlorosilane (SiHCl ₃ , referred to as: TCS) gas, tetrachlorosilane (SiCl ₄ , referred to as: STC) gas Gas, hexachlorodisilane (Si ₂ Cl ₆ , abbreviated: HCDS) gas, octachlorotrisilane (Si ₃ Cl ₈ , abbreviated: OCTS) gas and other inorganic halosilane raw material gases, or monosilane (SiH ₄ , abbreviated : MS) gas, disilane (Si ₂ H ₆ , abbreviation: DS) gas, trisilane (Si ₃ H ₈ , abbreviation: TS) gas, etc., are halogen-free inorganic silane raw material gases.

As the inert gas, in addition to N ₂ gas, rare gases such as Ar gas, He gas, Ne gas, and Xe gas can be used.

(Reactive gas supply steps: S5, S6) After the film formation process is completed, plasma-excited NH ₃ gas is supplied as a reactive gas to the wafer 200 in the processing chamber 201 (S5).

In this step, the switching control of the valves 243b to 243d is performed according to the same procedure as the switching control of the valves 243a, 243c, and 243d in step S3. The flow rate of the NH ₃ gas system is adjusted by the MFC 241b, and supplied into the buffer chamber 237c through the pipe 249b. At this time, high-frequency power is supplied to the external electrodes 300 . The NH ₃ gas supplied into the buffer chamber 237c is excited into a plasma state (plasmaized and activated), supplied into the processing chamber 201 as an active species (NH ₃ *), and exhausted through the exhaust pipe 231 .

The supply flow rate of NH ₃ gas controlled by the MFC 241b is, for example, set to a flow rate in the range of 100 sccm to 10000 sccm, preferably 1000 sccm to 2000 sccm. The high-frequency power applied to the external electrode 300 is, for example, a power within a range of 50W or more and 600W or less. The pressure in the processing chamber 201 is, for example, set to a pressure within a range of not less than 1 Pa and not more than 500 Pa. By using the plasma, the NH ₃ gas can be activated even if the pressure in the processing chamber 201 is in such a lower pressure range. The time for supplying the active species obtained by plasma excitation of _NH3 gas to the wafer 200, that is, the gas supply time (irradiation time) is set to be, for example, not less than 1 second and not more than 180 seconds, preferably 1 second. The time in the range of more than one second and less than 60 seconds. Other processing conditions were set to the same processing conditions as S3 above.

By supplying NH ₃ gas to the wafer 200 under the above conditions, the Si-containing layer formed on the wafer 200 was plasma-nitrided. At this time, the Si-Cl bond and Si-H bond of the Si-containing layer are cut by the energy of the NH ₃ gas excited by the plasma. The Cl and H bonded to Si will be detached from the Si-containing layer after cutting. Then, the Si system in the Si-containing layer having unbonded groups (dangling bonds) is bonded to the N contained in the NH ₃ gas due to detachment of Cl or the like to form a Si-N bond. As this reaction progresses, the Si-containing layer is changed (modified) into a layer containing Si and N, that is, a silicon nitride layer (SiN layer).

Furthermore, when modifying the Si-containing layer to a SiN layer, it is necessary to excite and supply NH ₃ gas plasma. This is because even if _NH3 gas is supplied in a non-plasma environment, in the above temperature range, the necessary energy for nitriding the Si-containing layer is insufficient, and it is difficult to sufficiently detach Cl or H from the Si-containing layer, or it is difficult to make the Si-containing layer The Si-containing layer is sufficiently nitrided to increase Si-N bonding.

After changing the Si-containing layer to a SiN layer, the valve 243b is closed to stop the supply of NH ₃ gas. Also, the supply of high-frequency power to the external electrodes 300 is stopped. Then, the NH ₃ gas or reaction by-products remaining in the processing chamber 201 are removed from the processing chamber 201 by the same processing procedures and processing conditions as step S4 (S6). Also, this step S6 can also be omitted.

As the nitriding agent, that is, the N-containing gas excited by the plasma, in addition to NH ₃ gas, diimine (N ₂ H ₂ ) gas, hydrazine (N ₂ H ₄ ) gas, N ₃ H ₈ gas etc.

As the inert gas, for example, various rare gases exemplified in step S4 can be used in addition to N ₂ gas.

(Implement the predetermined number of times: S7) By setting the above-mentioned S3, S4, S5, and S6 in this order non-simultaneously, that is, asynchronously, as one cycle, and carrying out this cycle for a predetermined number of times (n times), that is, more than one time (S7), you can A SiN film with a predetermined composition and a predetermined film thickness is formed on the wafer 200 . The above cycle is preferably repeated a plurality of times. That is, it is preferable to make the thickness of the SiN layer formed per cycle smaller than the required film thickness, and repeat the above-mentioned cycle multiple times until the film thickness of the SiN film formed by the SiN stacked layer becomes the required film thickness.

(Atmospheric Pressure Restoration Step: S8) After the above-mentioned film forming process is completed, N ₂ gas as an inert gas is supplied into the processing chamber 201 through the gas supply pipes 232c and 232d respectively, and exhausted through the exhaust pipe 231 . Thereby, the inside of the processing chamber 201 is flushed with an inert gas, and the gas and the like remaining in the processing chamber 201 are removed from the processing chamber 201 (inert gas flushing). Thereafter, the atmosphere in the processing chamber 201 is replaced with an inert gas (inert gas replacement), and the pressure in the processing chamber 201 is returned to normal pressure (S8).

(moving step: S9) Thereafter, the sealing cover 219 is lowered by the crystal boat lifter 115, the lower end of the manifold 209 is opened, and the processed wafer 200 is carried out from the lower end of the manifold 209 to the reaction tube in the state supported by the wafer boat 217. 203 outside (wafer unloading) (S9). After the wafer boat is unloaded, the shutter 219s is moved, and the lower opening of the manifold 209 is sealed by the shutter 219s via the O-ring 220c (the shutter is closed). After the processed wafer 200 is carried out to the outside of the reaction tube 203, it is taken out from the wafer boat 217 (wafer unloading). Moreover, after the wafers are unloaded, an empty wafer boat 217 can also be carried into the processing chamber 201 .

(3) Effects of this embodiment According to the present embodiment, one or more effects shown below can be obtained.

(a) By disposing the external electrode on the outer periphery of the reaction tube corresponding to the position where the plasma generation part for plasmaizing the processing gas is formed, the processing gas supplied into the reaction tube can be utilized by the external electrode The plasma is activated, and the activated process gas is supplied to the substrate.

(b) The external electrode is provided at the position where the plasma generation part is formed, except for the gas supply part that supplies gas to the plasma generation part, thereby preventing plasma formation in the gas supply part.

(c) A buffer chamber is arranged along the inner wall of the reaction tube, and an external electrode for forming plasma is arranged on the outer periphery of the reaction tube corresponding to the position where the buffer chamber is installed, and the processing gas supplied to the buffer chamber is supplied to the buffer chamber by the external electrode Activation is performed with plasma, and the activated processing gas is supplied to the substrate, whereby high-efficiency plasma can be formed in the buffer chamber, and the plasma active species gas formed with high efficiency can be supplied to the substrate.

(d) By making the processing gas supply port for supplying the activated processing gas to the substrate facing the center of the substrate and a plurality of them in the horizontal direction of the substrate, the supply amount of the plasmaized gas to the center of the substrate can be increased.

(e) In the buffer structure forming the buffer chamber, a partition plate is provided, by which the partition plate is divided into the processing gas introduction area and the plasma area as the buffer chamber, and the processing gas introduction area and the plasma area can be separated separate.

(f) By providing the gas supply hole for supplying gas from the process gas introduction area to the plasma area in the area partition plate, the process gas can be supplied to the plasma area according to the separation state of the process gas introduction area and the plasma area.

(g) A plurality of holes for supplying processing gas to the plasma area are provided in the partition plate, the processing gas is supplied from the lower part of the processing gas introduction area, and the processing gas is supplied to the plasma area through the plurality of holes, so that the buffer chamber can The gas concentration is homogenized.

(h) By not providing external electrodes on the outer periphery of the reaction tube corresponding to the position where the process gas introduction area is provided, plasma formation in the process gas introduction area can be prevented.

(i) Plasma can be formed in the plasma region by providing external electrodes on the outer periphery of the reaction tube corresponding to the position where the plasma region is provided.

(j) The buffer structure is located on the part covering from the upper part to the lower part of the inner wall of the processing chamber side, and is arranged along the loading direction of the substrate, and is provided with a gas supply port for supplying the plasmaized gas to the processing chamber. This homogenizes the gas concentration within the processing chamber.

(k) By arranging buffer chambers sandwiching the material gas supply nozzles in a plan view, and disposing external electrodes for forming plasma on the outer circumference of the reaction tubes corresponding to the locations where the respective buffer chambers are installed, the plasma region can be enlarged.

The embodiments of the present invention have been specifically described above. However, this invention is not limited to the said embodiment, Various changes are possible in the range which does not deviate from the summary.

For example, in the above-mentioned embodiment, the example in which a reaction gas is supplied after supplying a raw material was demonstrated. The present invention is not limited to this aspect, and the supply order of raw materials and reaction gases may be reversed. That is, the raw material may be supplied after supplying the reaction gas. By changing the order of supply, the film quality or composition ratio of the formed film can be changed.

In the above-mentioned embodiments and the like, an example in which a SiN film is formed on the wafer 200 has been described. The present invention is not limited to this aspect, and can also be suitably applied to forming a silicon oxide film (SiO film), a silicon oxycarbide film (SiOC film), a silicon oxycarbonitride film (SiOCN film), etc. on the wafer 200. Si-based oxide films such as silicon oxynitride films (SiON films), or silicon carbonitride films (SiCN films), silicon boron nitride films (SiBN films), silicon boron carbonitride films, etc. Si-based nitride films such as SiBCN films. In these cases, as the reaction gas, in addition to O-containing gas, C-containing gas such as C ₃ H ₆ , N-containing gas such as NH ₃ , or B-containing gas such as BCl ₃ can be used.

In addition, the present invention can be suitably applied to the formation of metals containing titanium (Ti), zirconium (Zr), hafnium (Hf), tantalum (Ta), niobium (Nb), aluminum (Al), and molybdenum (Mo) on the wafer 200. , tungsten (W) and other metal element oxide films or nitride films, that is, metal-based oxide films or metal-based nitride films. That is, the present invention can be suitably applied to forming a TiO film, a TiN film, a TiOC film, a TiOCN film, a TiON film, a TiBN film, a TiBCN film, a ZrO film, a ZrN film, a ZrOC film, a ZrOCN film, a ZrON film, etc. on the wafer 200. Film, ZrBN film, ZrBCN film, HfO film, HfN film, HfOC film, HfOCN film, HfON film, HfBN film, HfBCN film, TaO film, TaOC film, TaOCN film, TaON film, TaBN film, TaBCN film, NbO film, NbN film, NbOC film, NbOCN film, NbON film, NbBN film, NbBCN film, AlO film, AlN film, AlOC film, AlOCN film, AlON film, AlBN film, AlBCN film, MoO film, MoN film, MoOC film, MoOCN film , MoON film, MoBN film, MoBCN film, WO film, WN film, WOC film, WOCN film, WON film, MWBN film, WBCN film, etc.

In such cases, for example, as a raw material gas, tetrakis(dimethylamino)titanium (Ti[N(CH ₃ ) ₂ ] ₄ , abbreviated as TDMAT) gas, tetrakis(ethylmethylamino)hafnium (Hf[ N((C ₂ H ₅ )(CH ₃ )] ₄ , referred to as TEMAH) gas, tetra(ethylmethylamino) hafnium (Zr[N((C ₂ H ₅ )(CH ₃ )] ₄ , referred to as TEMAZ) gas, trimethylaluminum (Al(CH ₃ ) ₃ , abbreviated as TMA) gas, titanium tetrachloride (TiCl ₄ ) gas, hafnium tetrachloride (HfCl ₄ ) gas, etc. The above-mentioned reaction gases can be used as the reaction gas.

That is, the present invention can be suitably applied to the case of forming a semimetal-based film containing a half-metal element or a metal-based film containing a metal element. The processing procedures and processing conditions of these film-forming treatments can be set to the same processing procedures and processing conditions as those of the film-forming treatments shown in the above-mentioned embodiments or modifications. In such cases, the same effects as those of the above-described embodiment or modifications can be obtained.

The recipe used in the film forming process is preferably prepared individually according to the processing content, and stored in the memory device 121c in advance via the telecommunication channel or the external memory device 123 . Then, preferably, when starting various processes, the CPU 121a appropriately selects a suitable formula according to the processing content from the plurality of formulas stored in the memory device 121c. Thereby, thin films of various film types, composition ratios, film qualities, and film thicknesses can be formed universally and reproducibly with one substrate processing apparatus. In addition, the operator's burden can be reduced, operation errors can be avoided, and various processes can be quickly started.

The above-mentioned recipe is not limited to the case of novel preparation, for example, it can also be prepared by changing the existing recipe installed in the substrate processing apparatus. In the case of changing the recipe, the changed recipe can be installed in the substrate processing apparatus through a telecommunication channel or a recording medium in which the recipe is recorded. In addition, it is also possible to directly change the existing recipe installed in the substrate processing apparatus by operating the input device 122 included in the existing substrate processing apparatus.

115: crystal boat lifter 115s: door switch mechanism 121: Controller 121a: CPU 121b:RAM 121c: memory device 121d: I/O port 121e: Internal busbar 122: I/O device 123: External memory device 200: wafer (substrate) 201: Treatment room 202: processing furnace 203: reaction tube 207: heater 209: Manifold 217: crystal boat (substrate support) 218: heat shield 219: sealing cover 219s: door stop 220a~220c: O-ring 231: exhaust pipe 232a~232d: gas supply pipe 237: Buffer construction 237a: Partition board 237b: gas introduction area 237c: buffer room 237d: gas supply hole 241a~241d: mass flow controller (MFC) 243a~243d: Valve 244:APC valve 245: Pressure sensor 246: Vacuum pump 249a:Nozzle 249b: Piping 250a: gas supply hole 255:Rotary axis 263:Temperature sensor 267:Rotary mechanism 272: Integrator 273: High frequency power supply 300: external electrodes 302, 304: gas supply port 306: Plasma Active Species

FIG. 1 is a schematic configuration diagram of a vertical processing furnace of a substrate processing apparatus suitable for use in an embodiment of the present invention, showing a portion of the processing furnace in a vertical cross-sectional view. FIG. 2 is a schematic configuration diagram of a vertical processing furnace of a substrate processing apparatus suitable for use in an embodiment of the present invention, showing a portion of the processing furnace in a sectional view taken along line A-A of FIG. 1 . Fig. 3(a) is an enlarged cross-sectional view for explaining the buffer structure of the substrate processing apparatus suitable for use in the embodiment of the present invention; (b) is for explaining the buffer structure of the substrate processing apparatus suitable for use in the embodiment of the present invention a sketch of the . Fig. 4 is a schematic configuration diagram of a controller of a substrate processing apparatus suitable for use in an embodiment of the present invention, showing a control system of the controller in a block diagram. Fig. 5 is a flow chart showing the substrate processing steps according to the embodiment of the present invention.

200: wafer (substrate)

201: Treatment room

203: reaction tube

231: exhaust pipe

237: Buffer construction

237a: Partition board

237b: gas introduction area

237c: buffer room

237d: gas supply hole

249a:Nozzle

250a: gas supply hole

300: external electrodes

302, 304: gas supply port

306: Plasma Active Species

Claims (15)

A substrate processing device, comprising: a processing chamber for processing a substrate; a substrate support for holding a plurality of the above-mentioned substrates in multiple stages in a vertical direction; The buffer structure for slurrying, and the external electrodes, which are located outside the above-mentioned processing chamber corresponding to the position where the buffer structure is installed, and generate plasma; the above-mentioned external electrodes are connected to a high-frequency power supply by at least one The first external electrode and at least one second external electrode whose reference potential is grounded; the first external electrode and the second external electrode are arranged at equal intervals outside the processing chamber. The substrate processing apparatus according to claim 1, wherein the first external electrode and the second external electrode are formed of thin plates. The substrate processing apparatus according to claim 2, wherein the first external electrode and the second external electrode are formed of the thin plate having a rectangular shape and are arranged in the vertical direction. The substrate processing apparatus according to claim 1, further comprising a heating device for heating the substrate; the first external electrode and the second external electrode are provided between the processing chamber and the heating device. The substrate processing apparatus according to claim 1, wherein the buffer structure includes a gas supply unit for supplying the gas; The first external electrode and the second external electrode are provided at a position where the buffer structure is provided and at a position excluding the gas supply unit. The substrate processing apparatus according to claim 5, wherein, in the buffer structure, a buffer chamber is provided as a region for plasmating the gas. The substrate processing apparatus according to claim 5, wherein a partition plate is provided in the buffer structure, and the gas supply unit and the buffer chamber are partitioned by the partition plate. The substrate processing apparatus according to claim 7, wherein a gas supply hole for supplying the gas from the gas supply unit to the buffer chamber is provided in the partition plate. The substrate processing apparatus according to claim 7, wherein a plurality of the gas supply holes are provided in the vertical direction on the partition plate. The substrate processing apparatus according to claim 1, wherein the above-mentioned buffer structure is arranged along the above-mentioned vertical direction on the part from the upper part to the lower part of the inner wall of the above-mentioned processing chamber, and is provided with a power supply to the above-mentioned processing chamber. The gas supply port for the above-mentioned gas to be slurried. The substrate processing apparatus according to claim 10, wherein the gas supply ports are provided in plural in the horizontal direction of the substrate toward the center of the substrate. The substrate processing apparatus according to claim 1, wherein it is provided with a source gas supply unit for supplying source gas, and a plurality of the above-mentioned plasma generation units; in a plan view, the plurality of the above-mentioned plasma generation units sandwich a part passing through the above-mentioned processing chamber The center is arranged in a straight line with the above-mentioned raw material gas supply part. The substrate processing apparatus according to claim 1, wherein an exhaust unit for exhausting gas and a plurality of the plasma generation units are provided; and the plurality of the plasma generation units pass through the processing chamber in a plan view. It is arranged in a straight line between the center of the center and the above-mentioned exhaust part. A method of manufacturing a semiconductor device, comprising the following steps performed in a substrate processing device; the substrate processing device includes: a processing chamber for processing a substrate; a substrate supporter for holding a plurality of the above-mentioned substrates in multiple stages in a vertical direction; and a plasma generation part, which is provided in the above-mentioned processing chamber, has a buffer structure for plasmaizing gas, and an external electrode, and the external electrode is provided outside the above-mentioned processing chamber corresponding to the position where the buffer structure is provided and Generate plasma; the above-mentioned external electrodes are composed of at least one first external electrode connected to a high-frequency power supply, and at least one second external electrode whose grounding is the reference potential; the above-mentioned first external electrode and the above-mentioned second The external electrodes are arranged at equal intervals outside the above-mentioned processing chamber; the steps are: a step of carrying the above-mentioned substrate into the above-mentioned processing chamber; a step of plasmating the above-mentioned gas; Step above gas. A recording medium, which is computer-readable, which records a program for causing a substrate processing device to perform the following procedures by a computer; the substrate processing device is equipped with: a processing chamber for processing substrates; A substrate support held in multiple stages in the direction; and a plasma generating unit, which is provided in the above-mentioned processing chamber, has a buffer structure for plasmaizing gas, and an external electrode, which is provided in the buffer structure. Corresponding to the outside of the above-mentioned processing chamber and generating plasma; the above-mentioned external electrode is composed of at least one first external electrode connected to a high-frequency power supply, and at least one second external electrode whose grounding is used as a reference potential; The above-mentioned first external electrode and the above-mentioned second external electrode are arranged at equal intervals outside the above-mentioned processing chamber; the procedure is: The procedure of carrying the substrate into the processing chamber; the procedure of plasmaizing the gas; and the procedure of supplying the plasmaized gas to the substrate.

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