TW202145838A - Substrate treatment device, production method for semiconductor device, and program - Google Patents

Abstract

Provided is a technology comprising: a treatment chamber in which a substrate is treated; a substrate support tool that supports a plurality of substrates at multiple levels in the vertical direction; and a plasma generation unit having a buffer structure that is provided inside the treatment chamber and that turns a gas into a plasma, and an external electrode that generates plasma and that is provided on the outside of the treatment chamber at a position corresponding to the position to which the buffer structure is provided.

Description

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

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

As one of the manufacturing steps of a semiconductor device, a substrate loaded into a processing chamber of a substrate processing apparatus is activated and supplied by plasma, such as a raw material gas or a reaction gas, and an insulating film, a semiconductor film, a conductor 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 Literature]

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

(The problem that the invention intends to solve)

An object of the present invention is to provide a technique for supplying a plasma active species gas formed with high efficiency to a substrate. (Technical means to solve problems)

According to one aspect of the present invention, there is provided a technique having: A processing chamber for processing substrates; A substrate supporter for holding a plurality of the above-mentioned substrates in multiple stages in a vertical direction; and A plasma generating unit is provided in the processing chamber, and has a buffer structure for plasmaizing gas, and an external electrode, which is provided outside the processing chamber corresponding to the position where the buffer structure is provided, and generates a plasma plasma. (Compared to the efficacy of the prior art)

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> Hereinafter, an embodiment of the present invention will be described with reference to FIGS. 1 to 5 .

(1) Configuration of a substrate processing apparatus (heating apparatus) As shown in FIG. 1 , the processing furnace 202 used in the substrate processing apparatus is a so-called vertical furnace capable of accommodating 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 erected by being supported by a heater base (not shown) serving as a holding plate. The heater 207 also functions as an activation mechanism (excitation unit) for activating (exciting) the gas by 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, for example _{, a heat-resistant material such as quartz (SiO 2} ) or silicon carbide (SiC), and has 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), for example, and is formed in a cylindrical shape with an upper end and a lower end opened. The upper end portion of the manifold 209 is engaged with the lower end portion of the reaction tube 203 to support the reaction tube 203 . Between the manifold 209 and the reaction tube 203, an O-ring 220a serving as a sealing member is provided. The manifold 209 is supported by the heater base, whereby 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-mentioned configuration, and only the reaction tube 203 may be referred to as a processing container.

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

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

As shown in FIG. 2 , the nozzle 249 a is located in the space between the inner wall of the reaction tube 203 and the wafers 200 , and is arranged to stand upward from the lower part of the inner wall of the reaction tube 203 along the upper part and upward in the direction of loading the wafers 200 . rise. That is, the nozzles 249a are arranged along the wafer arranging area in the side of the wafer arranging area (the placing area) in which the wafers 200 are arranged (placed) and horizontally surrounding the area of the wafer arranging area. . That is, the nozzles 249a are provided in a direction perpendicular to the surface (flat surface) of the wafer 200 on the side of the end (peripheral edge) of each wafer 200 carried into the processing chamber 201 . A gas supply hole 250a for supplying gas is provided on the side surface of the nozzle 249a. The gas supply hole 250 a is opened toward the center of the reaction tube 203 , and can supply gas to the wafer 200 . The gas supply holes 250a are arranged in plural from the lower part to the upper part of the reaction tube 203, and have the same opening area and the same opening spacing.

A pipe 249b is connected to the front end of the gas supply pipe 232b. The piping 249b is connected to the inside of the buffer structure 237 . In the present embodiment, the two buffer structures 237 in plan view are arranged so as to sandwich a straight line passing through the center of the reaction tube 203 (processing chamber 201 ) and the nozzle 249 a, or between the center of the reaction tube 203 (processing chamber 201 ) and the nozzle 249 a. 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 . The buffer structure 237 is provided with a partition plate 237a, and the partition plate 237a partitions into a gas introduction region 237b for introducing gas from a pipe 249b and a plasma region 237c for plasmaizing the gas. 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 region 237b is arranged on the exhaust pipe 231 side.

As shown in FIG. 2 , the buffer chamber 237c is a space between the inner wall of the reaction tube 203 and the wafer 200 in a circular shape when viewed from above, and the part from the lower part to the upper part of the inner wall of the reaction tube 203 is included , arranged along the loading direction of the wafer 200 . That is, the buffer chamber 237c is formed by the buffer structure 237 along the side of the wafer arrangement region and the region horizontally surrounding 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 plural 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 from the lower part to the upper part of the reaction tube 203 along the stacking direction of the wafers 200 , and have the same opening area and the same opening spacing.

The gas introduction area 237b is provided so as to stand up from the lower part of the inner wall of the reaction tube 203 along the upper part and upward in the stacking direction of the wafers 200 . The partition plate 237a is provided with a gas supply hole 237d for supplying gas from the gas introduction region 237b to the plasma region 237c. Thereby, the reaction gas supplied to the gas introduction region 237b is dispersed in the buffer chamber 237c. The gas supply holes 237d are provided in plural from the lower part to the upper part of the reaction tube 203, similarly to the gas supply holes 250a. Moreover, instead of the piping 249b and the gas introduction area 237b, a nozzle, for example, a porous 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, through the longitudinal space ( That is, the nozzle 249a and the buffer chamber 237c arranged in the cylindrical space) convey the gas. Then, the gas is first ejected into the reaction tube 203 near the wafer 200 through the gas supply hole 250a and the gas supply ports 302 and 304 opened in the nozzle 249a and the buffer chamber 237c, respectively. 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 uniformity of the film thickness 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 system 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 residual 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 in a liquid state at normal temperature and pressure, or a raw material in a gaseous state at normal temperature and normal pressure. In this specification, when the term "raw material" is used, it is intended to mean "a liquid raw material in a liquid state", "a raw material gas in a gaseous state", or both.

As the silane raw material gas, for example, a raw material gas containing Si and a halogen element, that is, a halosilane raw material gas can be used. The halosilane raw material gas system refers to a silane raw material with a halogen group. The halogen element contains at least one 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 a chlorine group, a fluorine group, a bromine group, and an iodine group. Halosilane raw materials can also be described as a kind of halide.

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 through the MFC 241b, the valve 243b, the piping 249b, and the gas introduction area as a reactant (reactant) containing an element different from the above-mentioned predetermined element, for example, a nitrogen (N)-containing gas as a reactant gas. 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 referred to as a substance composed of only two elements of N and H, and functions as a nitriding gas, that is, an 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, for example, nitrogen (N ₂ ) gas as an inert gas is supplied into the processing chamber 201 through the MFCs 241c and 241d, valves 243c and 243d, gas supply pipes 232a and 232b, nozzles 249a and piping 249b, respectively.

A raw material gas supply system serving as a first gas supply system is mainly composed of the gas supply pipe 232a, the MFC 241a, and the valve 243a. The reactant supply system (reactant supply system) as the 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 and 232d, MFCs 241c and 241d, and valves 243c and 243d. The raw material supply system, the reactant supply system, and the inert gas supply system are collectively referred to as a gas supply system (gas supply unit) for short.

(Plasma generation section) Next, the plasma generating portion will be described with reference to FIGS. 1 to 3 .

As shown in FIG. 2 , the plasma is a capacitively coupled plasma (CCP), and when the reaction gas is supplied, the reaction tube 203 (processing chamber 201 ) made of quartz and the like is a vacuum partition. The buffer structure 237 is generated.

As shown in FIGS. 2 and 3( a ), the external electrodes 300 are formed of rectangular thin plates having long sides in the arrangement direction of the wafers 200 . As shown in FIG. 1 and FIG. 3( b ), the external electrode 300 is a first external electrode (Hot electrode) 300 - 1 connected to the high frequency power supply 273 via the integrator 272 , and a second external electrode (Hot electrode) 300 - 1 connected to the reference potential 0V and grounded via the ground The external electrodes (ground electrodes) 300-2 are arranged at equal intervals. In the present invention, when there is no need for special distinction and description, the description will be described as the external electrode 300 .

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

The external electrode 300 may be made of metal such as aluminum, copper, and stainless steel, but it is made of an oxidation-resistant material such as nickel, so that deterioration of electrical conductivity can be suppressed and substrate processing can be performed. In particular, the AlO film, which is an oxide film with high heat resistance and corrosion resistance, can be formed on the electrode surface by forming it with an aluminum-added nickel alloy material. By the effect of this film formation, the progress of the deterioration to the inside of the electrode can be suppressed, so that the decrease in the plasma generation efficiency due to the decrease in the electrical conductivity can be suppressed.

(Electrode Fixture) Next, the quartz cover 301 as the electrode fixing jig for fixing the external electrode 300 will be described with reference to FIG. 3 . As shown in FIGS. 3( a ) and ( b ), a plurality of external electrodes 300 are provided, and their notch parts (not shown) are hooked to the inner wall surface of the curved quartz cover 301 belonging to the electrode fixing jig. The provided protruding portion 310 is slid and fixed, and is provided on the outer periphery of the reaction tube 203 in a unitized manner (hook electrode unit) so as to be integrated with the quartz cover 301 . Here, the outer electrode 300 and the quartz cover 301 belonging to the electrode fixing jig are referred to as an electrode fixing unit. In addition, as the material of the quartz cover 301 and the external electrode 300, quartz and nickel alloy are used, respectively.

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

The reaction tube 203 is provided with an exhaust pipe 231 serving as an exhaust part for exhausting the environment in the processing chamber 201 . In the exhaust pipe 231, 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 the exhaust valve (pressure adjustment part), it is automatically pressure controller) valve 244, connected to a vacuum pump 246 serving as a vacuum exhaust. The APC valve 244 is configured to: open and close the valve according to the state in which the vacuum pump 246 is activated, so as to perform vacuum evacuation and stop of the vacuum evacuation in the processing chamber 201; The detected pressure data is used to adjust the valve opening, whereby the pressure in the processing chamber 201 can be adjusted. The exhaust system is mainly composed of the exhaust pipe 231 , the APC valve 244 , and the pressure sensor 245 . Also, the vacuum pump 246 can also be considered to be 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 249a.

Below the manifold 209, there is provided a sealing cover 219 that can airtightly close the opening at the lower end of the manifold 209 as a furnace mouth cover. The sealing cover 219 is configured to abut the lower end of the manifold 209 from the lower side in the vertical direction. The sealing cover 219 is made of, for example, a metal material such as SUS, and is formed in a disk shape. On the upper surface of the sealing cover 219, there is provided an O-ring 220b as a sealing member which is in contact with the lower end of the manifold 209. On the side of the sealing cover 219 opposite to the processing chamber 201, a rotation mechanism 267 for rotating the wafer boat 217 described later is provided. The rotating shaft 255 of the rotating mechanism 267 penetrates 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 raised and lowered in the vertical direction by the boat lifter 115 which is vertically disposed outside the reaction tube 203 as a lifting mechanism. The boat lifter 115 is configured to move the wafer boat 217 in and out of the processing chamber 201 by raising and lowering the sealing cover 219 . The boat lifter 115 is configured as a transfer device (transfer mechanism) that transfers the wafer boat 217 , that is, the wafers 200 inside and outside the processing chamber 201 . In addition, below the manifold 209, a shutter 219s serving as a furnace mouth cover is provided to airtightly close the opening at the lower end of the manifold 209 while 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 disk shape. On the upper surface of the shutter 219s, there is provided an O-ring 220c as a sealing member which is in contact with the lower end of the manifold 209. The opening and closing actions (elevating action or rotating action, etc.) of the door 219s are controlled by the door opening and closing mechanism 115s.

(substrate support) As shown in FIG. 1 , the wafer boat 217 serving as a substrate supporter is configured such that a plurality of wafers 200 , for example, 25 to 200 wafers 200 are arranged in a vertical direction in a state where their centers are aligned with each other in a horizontal posture. ground support, that is, arranged at predetermined intervals. The wafer boat 217 is made of a heat-resistant material such as quartz or SiC. In the lower part of the wafer boat 217, a heat insulating plate 218 made of a heat-resistant material such as quartz or SiC is supported in multiple stages.

As shown in FIG. 1 , inside the reaction tube 203, a temperature sensor 263 serving as a temperature detector is provided. According to the temperature information detected by the temperature sensor 263, the energization state of 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 with reference to FIG. 4 . As shown in FIG. 4, the controller 121 belonging to the control unit (control device) is configured 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 so that data can be exchanged 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 constituted by, for example, a flash memory, an HDD (Hard Disk Drive), or the like. In the memory device 121c, a control program for controlling the operation of the substrate processing apparatus, or a recipe for describing the procedures and conditions of the film-forming process to be described later are stored in a readable manner. The process recipe functions as a program by combining each procedure of the various processes (film forming process) described later by the controller 121 so that a predetermined result can be obtained. Hereinafter, process recipes, control programs, etc., are also collectively referred to as programs for short. Also, the process recipe is sometimes simply referred to as a recipe. In this specification, when the term "program" is used, it refers to the case of containing only the formulation monomer, the case of containing only the control program monomer, or the case of containing both of these. The RAM 121b is configured as a memory area (work area) in which programs, data, and the like read out by the CPU 121a are temporarily stored.

The I/O port 121d is connected to the MFCs 241a to 241d, the valves 243a to 243d, the pressure sensor 245, the APC valve 244, the vacuum pump 246, the heater 207, the temperature sensor 263, the integrator 272, the high-frequency power supply 273, and the rotating mechanism 267. Crystal boat lifter 115, door-stop switch mechanism 115s, etc.

The CPU 121a is configured to read the control program from the memory device 121c and execute it, and read the recipe from the memory device 121c in accordance with the input of the operation command from the I/O device 122 and the like. The CPU 121a is configured to control according to the contents of the read recipe: the control of the rotation mechanism 267, the flow rate adjustment operation of various gases by the MFCs 241a to 241d, the switching operation of the valves 243a to 243d, and the high frequency power supply 273 based on impedance monitoring. adjustment operation, opening and closing operation of the APC valve 244, and pressure adjustment operation using the APC valve 244 by the pressure sensor 245, start and stop of the vacuum pump 246, temperature adjustment operation of the heater 207 by the temperature sensor 263, and rotation The mechanism 267 performs forward and reverse rotation of the boat 217, adjustment of the rotation angle and rotation speed, the lifting and lowering of the boat 217 by the boat lift 115, and the plasma generation by the high frequency power supply 273 and the external electrode 300.

The controller 121 can be configured by installing the above-mentioned program stored in an external memory device (eg, 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 recording medium that can be read by a computer. Hereinafter, these are also collectively referred to or simply referred to as recording media. In this specification, when the term recording medium is used, it refers to the case of containing only the memory device 121c alone, the case of containing only the external memory device 123 alone, or the case of containing both of these. Furthermore, the program provision to the computer may be performed without using the external memory device 123, but using a communication means such as a network or a dedicated line.

(2) Substrate processing step 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, the step of supplying the DCS gas as the raw material gas and the step of supplying the plasma-excited NH ₃ gas as the reaction gas are performed asynchronously, that is, asynchronously for a predetermined number of times (more than once) on the wafer 200 . A silicon nitride film (SiN film) formed thereon will be described as an example of a film containing Si and N. In addition, for example, a predetermined film may be formed on the wafer 200 in advance. In addition, a predetermined pattern may be formed in advance on the wafer 200 or a predetermined film.

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

When the term "wafer" is used in this specification, it is intended to refer to the wafer itself, or to a laminate of a predetermined layer or film formed on the wafer and its surface. When the term "wafer surface" is used in this specification, it is intended to refer to the surface of the wafer itself, or to the surface of a predetermined layer or the like formed on the wafer. In this specification, "a predetermined layer is formed on a wafer" is described, which means that a predetermined layer is directly formed on the surface of the wafer itself, or that a predetermined layer is formed on the wafer itself. The situation in which a predetermined layer is formed on it. When the term "substrate" is used in this specification, it has the same meaning as when the term "wafer" is used.

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

(Pressure and temperature adjustment step: S2) The inside of the processing chamber 201 , that is, the space where the wafer 200 exists, is evacuated (decompressed exhaust) by the vacuum pump 246 so that the required pressure (vacuum degree) is achieved. At this time, the pressure in the processing chamber 201 is measured by the pressure sensor 245, and the APC valve 244 is fed back and controlled according to the measured pressure information. The vacuum pump 246 is kept in a state of constant operation 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 desired temperature is obtained. At this time, according to the desired temperature distribution in the processing chamber 201 , according to the temperature information detected by the temperature sensor 263 , the degree of energization to the heater 207 is feedback-controlled. The heating in the processing chamber 201 by the heater 207 is continued at least until the film forming step described later is completed. Here, 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 . In addition, when performing processing only at such a temperature, the heater 207 is not required, and the heater 207 may not 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 boat 217 and the wafer 200 is started by the rotation mechanism 267 . The rotation of the wafer boat 217 and the wafer 200 by the rotation mechanism 267 is continued at least until the film formation step is completed.

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

Moreover, in order to suppress the intrusion of DCS gas into the piping 249b, the valve 243d was opened, and N ₂ gas was circulated in the gas supply pipe 232d. The N ₂ gas system is supplied into the processing chamber 201 via the gas supply pipe 232 b and the piping 249 b , and is exhausted by the exhaust pipe 231 .

The supply flow rate of the DCS gas controlled by the MFC241a is, for example, 1 sccm or more and 6000 sccm or less, preferably a flow rate in the range of 3000 sccm or more and 5000 sccm or less. _{The supply flow rate of the N 2} gas controlled by the MFCs 241c and 241d is, for example, a flow rate within a range of 100 sccm or more and 10000 sccm or less, respectively. The pressure in the processing chamber 201 is, for example, 1 Pa or more and 2666 Pa or less, preferably 665 Pa or more and 1333 Pa or less. The time during which the wafer 200 is exposed to the DCS gas is, for example, about 20 seconds per cycle. In addition, the time during 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 is, for example, 0° C. or higher and 700° C. or lower, preferably room temperature (25° C.) or higher and 550° C., more preferably 40° C. or higher and 500° C. or lower. temperature inside. As in the present 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 received. 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 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 a partially decomposed substance of DCS, or thermal decomposition of DCS to deposit Si. That is, the Si-containing layer may be an adsorption layer (physical adsorption layer or chemical adsorption layer) of DCS or a substance in which DCS is partially decomposed, or may be an accumulation layer (Si layer) of Si.

After the Si-containing layer is formed, the valve 243 a is closed, and the supply of the DCS gas to the processing chamber 201 is stopped. At this time, the APC valve 244 is kept open, 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 for forming the Si-containing layer are removed from the processing chamber 201. The inside of the processing chamber 201 is removed (S4). In addition, the valves 243c and 243d are kept open, and the N ₂ gas is kept supplied into the processing chamber 201 . N ₂ gas system acts as a flushing gas. In addition, this step S4 may be omitted.

As the raw material gas, in addition to DCS gas, tetra-dimethylaminosilane (Si[N(CH ₃ ) ₂ ] ₄ , abbreviated as 4DMAS) gas, tetra-dimethylaminosilane (Si[N(CH 3 ) 2 ] 4 gas, ₃ ) ₂ ] ₃ H, abbreviation: 3DMAS) gas, bis-dimethylaminosilane (Si[N(CH ₃ ) ₂ ] ₂ H ₂ , abbreviation: BDMAS) gas, bis-diethylamino silane (Si[N( C ₂ H ₅ ) ₂ ] ₂ H ₂ , abbreviation: BDEAS) gas, bis-tert-butylaminosilane (SiH ₂ [NH(C ₄ H ₉ )] ₂ , abbreviation: BTBAS) gas, dimethylamino silane (DMAS) gas, diethylaminosilane (DEAS) gas, dipropylaminosilane (DPAS) gas, diisopropylaminosilane (DIPAS) gas, butylaminosilane (BAS) gas, hexamethyldisilazane (HMDS) gas and other various amino silane raw materials, 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, hexachlorodisilane (Si ₂ Cl ₆ , abbreviated: HCDS) gas, octachlorotrisilane (Si ₃ Cl ₈ , abbreviated: OCTS) gas and other inorganic halosilane raw materials, or monosilane (SiH ₄ , abbreviated as: OCTS) gas : MS) gas, disilane (Si ₂ H ₆ , abbreviated: DS) gas, trisilane (Si ₃ H ₈ , abbreviated: TS) gas and other inorganic silane raw material gases that do not contain halogen groups.

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 Step: 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 on-off control of the valves 243b to 243d is performed according to the same procedure as the on-off 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 is supplied into the buffer chamber 237c through the piping 249b. At this time, high-frequency power is supplied to the external electrode 300 . _{The NH 3} gas supplied into the buffer chamber 237 c is excited into a plasma state (is activated by _{plasmaization), is supplied into the processing chamber 201 as an active species (NH 3} *), and is exhausted from the exhaust pipe 231 .

_{The supply flow rate of the NH 3} gas controlled by the MFC241b is, for example, 100 sccm or more and 10,000 sccm or less, preferably 1,000 sccm or more and 2,000 sccm or less. The high-frequency electric power applied to the external electrode 300 is, for example, electric power in the range of 50 W or more and 600 W or less. The pressure in the processing chamber 201 is, for example, a pressure within a range of 1 Pa or more and 500 Pa or less. _{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 band. The time for supplying the active species obtained by plasma excitation of the NH ₃ gas to the wafer 200 , that is, the gas supply time (irradiation time) is, for example, 1 second or more and 180 seconds or less, preferably 1 Time within the range of seconds or more and less than 60 seconds. The other processing conditions are the same as those of the above-mentioned S3.

_{By supplying NH 3} gas to the wafer 200 under the above conditions, the Si-containing layer formed on the wafer 200 is plasma nitrided. At this time, the Si-Cl bond and the 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 that have broken the bond with Si will be released from the Si-containing layer. Then, by desorption of Cl or the like, the Si system in the Si-containing layer having an unbonded group (dangling bond) is _{bonded to N included in the NH 3} gas, thereby forming a Si-N bond. By this reaction, the Si-containing layer is changed (modified) into a layer containing Si and N, that is, a silicon nitride layer (SiN layer).

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

After the Si-containing layer is changed to a SiN layer, the valve 243b is closed, and the supply of the _{NH 3 gas is stopped.} In addition, the supply of high-frequency power to the external electrodes 300 is stopped. _{Then, NH 3} gas or reaction by-products remaining in the processing chamber 201 are removed from the processing chamber 201 by the same processing procedure and processing conditions as in step S4 ( S6 ). In addition, this step S6 may be omitted.

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

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

(Predetermined number of implementations: S7) By setting the above-mentioned S3, S4, S5, and S6 to be performed non-simultaneously, that is, asynchronously in this order, as one cycle, and performing this cycle a predetermined number of times (n times), that is, one or more times (S7), it can be A SiN film with a predetermined composition and a predetermined thickness is formed on the wafer 200 . The above cycle is preferably repeated a plurality of times. That is, it is preferable that the thickness of the SiN layer formed in each cycle is smaller than the desired film thickness, and the cycle is repeated several times until the thickness of the SiN film formed by the SiN lamination layer becomes the desired film thickness.

(Atmospheric pressure recovery 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 from the gas supply pipes 232 c and 232 d respectively, and the exhaust pipe 231 exhausts the gas. Thereby, the inside of the processing chamber 201 is flushed with the inert gas, and the gas etc. remaining in the processing chamber 201 are removed from the processing chamber 201 (inert gas flushing). After that, the environment 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 out step: S9) Then, the sealing cover 219 is lowered by the boat lifter 115 to open the lower end of the manifold 209, 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 boat 217. 203 outside (wafer unloading) (S9). After the boat is unloaded, the shutter 219s is moved, and the lower end opening of the manifold 209 is sealed by the shutter 219s through 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). Furthermore, after the wafers are unloaded, the empty wafer boat 217 can also be carried into the processing chamber 201 .

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

(a) By disposing the external electrode on the outer periphery of the reaction tube corresponding to the position where the plasma generating portion for plasmaizing the process gas is formed, the process 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 generating portion is formed and at a position excluding the gas supplying portion that supplies gas to the plasma generating portion, thereby preventing the formation of plasma in the gas supplying portion.

(c) A buffer chamber is arranged along the inner wall of the reaction tube, and an outer electrode for forming plasma is arranged on the outer periphery of the reaction tube corresponding to the position where the buffer chamber is arranged, and the process gas supplied into the buffer chamber is supplied by the outer electrode through the outer electrode. By activating with plasma and supplying the activated process gas to the substrate, high-efficiency plasma can be formed in the buffer chamber, and the high-efficiency plasma-active species gas can be supplied to the substrate.

(d) The supply amount of plasmatized gas to the center of the substrate can be increased by arranging a plurality of process gas supply ports for supplying the activated process gas to the substrate toward the center of the substrate and in the horizontal direction of the substrate.

(e) In the buffer structure forming the buffer chamber, a partition plate is provided, and by this partition plate, the processing gas introduction area and the plasma area serving as the buffer chamber are partitioned, so that the processing gas introduction area and the plasma area can be separated. separation.

(f) Since the partition plate is provided with gas supply holes for supplying gas from the processing gas introduction area to the plasma area, the processing gas can be supplied to the plasma area according to the separation state of the processing gas introduction area and the plasma area.

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

(h) Since no external electrode is provided on the outer periphery of the reaction tube corresponding to the position where the processing gas introduction area is provided, the formation of plasma in the processing gas introduction area can be prevented.

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

(j) The buffer structure is provided in the part from the upper part to the lower part of the inner wall on the side of the processing chamber, and is provided along the stacking direction of the substrates. This can homogenize the gas concentration in the processing chamber.

(k) Plasma region can be enlarged by arranging buffer chambers sandwiching the feed gas supply nozzle in plan view, and arranging plasma-forming external electrodes on the outer periphery of the reaction tube corresponding to the positions where each buffer chamber is installed.

The embodiments of the present invention have been specifically described above. However, the present invention is not limited to the above-described embodiment, and various modifications can be made without departing from the gist of the present invention.

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

In the above-described embodiments and the like, the example in which the 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 the formation of a silicon oxide film (SiO film), a silicon oxycarbide film (SiOC film), a silicon oxycarbonitride film (SiOCN film), In the case of a Si-based oxide film such as a silicon oxynitride film (SiON film), or a silicon carbonitride film (SiCN film), a silicon boron nitride film (SiBN film), or a silicon boron nitride film (SiBN film) is formed on the wafer 200 Si-based nitride film such as film (SiBCN film). In these cases, 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 as the reaction gas.}

In addition, the present invention can be suitably applied to the formation on the wafer 200 containing titanium (Ti), zirconium (Zr), hafnium (Hf), tantalum (Ta), niobium (Nb), aluminum (Al), molybdenum (Mo) , in the case of an oxide film or a nitride film of a metal element such as tungsten (W), that is, a metal-based oxide film or a metal-based nitride film. That is, the present invention can be suitably applied to the formation of 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, and a ZrON film 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 these cases, for example, as the raw material gas, tetra(dimethylamino)titanium (Ti[N(CH ₃ ) ₂ ] ₄ , abbreviated as TDMAT) gas, tetra(ethylmethylamino) hafnium (Hf[N(CH 3 ) 2 ] 4 , 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, trimethyl aluminum (Al(CH ₃ ) ₃ , abbreviated as TMA) gas, titanium tetrachloride (TiCl ₄ ) gas, hafnium tetrachloride (HfCl ₄ ) gas, etc. The above-mentioned reactive gas can be used as the reactive gas.

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

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

The above-mentioned recipe is not limited to the case of novel creation, and can be prepared by, for example, changing an existing recipe already installed in a substrate processing apparatus. In the case of changing the recipe, the changed recipe can be installed in the substrate processing apparatus via a telecommunication channel or a recording medium on which the recipe is recorded. In addition, the input device 122 included in the existing substrate processing apparatus may be operated to directly change the existing recipe already installed in the substrate processing apparatus.

115: Crystal boat lifter 115s: door stop switch mechanism 121: Controller 121a:CPU 121b:RAM 121c: Memory Devices 121d: I/O port 121e: Internal busbar 122: Input and output device 123: External memory device 200: Wafer (substrate) 201: Processing Room 202: Processing furnace 203: reaction tube 207: Heater 209: Manifold 217: Crystal boat (substrate support) 218: Insulation Board 219: sealing cover 219s: blocking the door 220a~220c: O-ring 231: exhaust pipe 232a~232d: Gas supply pipe 237: Buffer Construction 237a: Zone Separator 237b: Gas introduction area 237c: Buffer Chamber 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 electrode 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, and is a diagram showing a part of the processing furnace in a vertical cross-sectional view. 2 is a schematic configuration diagram of a vertical processing furnace of a substrate processing apparatus suitable for use in the embodiment of the present invention, and is a diagram showing a part of the processing furnace in a cross-sectional view taken along the line A-A of FIG. 1 . 3(a) is an enlarged cross-sectional view for illustrating a buffer structure of a substrate processing apparatus suitable for use in an embodiment of the present invention; (b) is an enlarged view for illustrating a buffer structure for a substrate processing apparatus suitable for use in an embodiment of the present invention sketch map. 4 is a schematic configuration diagram of a controller of a substrate processing apparatus suitable for use in the embodiment of the present invention, and is a block diagram showing a control system of the controller. FIG. 5 is a flow chart showing a substrate processing procedure according to the embodiment of the present invention.

200: Wafer (substrate)

201: Processing Room

203: reaction tube

231: exhaust pipe

237: Buffer Construction

237a: Zone Separator

237b: Gas introduction area

237c: Buffer Chamber

237d: Gas supply hole

249a: Nozzle

250a: Gas supply hole

300: External electrode

302,304: Gas supply port

306: Plasma Active Species

Claims (18)

A substrate processing device is provided with: A processing chamber for processing substrates; A substrate supporter for holding a plurality of the above-mentioned substrates in multiple stages in a vertical direction; and A plasma generating unit is provided in the processing chamber, and has a buffer structure for plasmaizing gas, and an external electrode, which is provided outside the processing chamber corresponding to the position where the buffer structure is provided, and generates a plasma plasma. The substrate processing apparatus of claim 1, wherein the 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 grounded as a reference potential. The substrate processing apparatus according to claim 2, wherein the first external electrode and the second external electrode are provided outside the processing chamber. The substrate processing apparatus according to claim 2, wherein 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 2, wherein the first external electrode and the second external electrode are formed of thin plates. The substrate processing apparatus according to claim 5, 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 2, 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 2, wherein the buffer structure is provided with a gas supply part for supplying the gas; The said 1st external electrode and the said 2nd external electrode are provided in the position where the said buffer structure is provided, and the position except the said gas supply part. The substrate processing apparatus according to claim 8, wherein in the buffer structure, a buffer chamber is provided as a region for plasmaizing the gas. The substrate processing apparatus of claim 8, wherein a partition plate is provided in the buffer structure, and the gas supply portion and the buffer chamber are partitioned by the partition plate. The substrate processing apparatus according to claim 10, wherein the partition plate is provided with a gas supply hole for supplying the gas to the buffer chamber from the gas supply portion. The substrate processing apparatus according to claim 10, wherein in the partition plate, the gas supply holes are provided in plural in the vertical direction. The substrate processing apparatus according to claim 1, wherein the buffer structure is provided along the vertical direction in the portion from the upper part to the lower part of the inner wall of the processing chamber, and is provided with a power supply to the processing chamber. A gas supply port for the above-mentioned gas to be slurried. The substrate processing apparatus according to claim 13, wherein the gas supply ports are provided in plural numbers in the horizontal direction of the substrate toward the center of the substrate. The substrate processing apparatus according to claim 1, further comprising 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 plasma generating units are arranged so as to sandwich a straight line passing through the center of the processing chamber and the source gas supply unit. The substrate processing apparatus according to claim 1, further comprising an exhaust unit for exhausting gas, and a plurality of the plasma generation units; and the plurality of plasma generation units pass through the processing chamber in a plan view. The center and the straight line of the above-mentioned exhaust part are arranged. A method for manufacturing a semiconductor device, comprising the following steps performed in a substrate processing apparatus; the substrate processing apparatus is provided with: 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 generating unit, which is provided in the processing chamber, and has a buffer structure for plasmaizing gas, and an external electrode, which is provided on the outside of the processing chamber corresponding to the position where the buffer structure is provided. generate plasma; This step is: the step of carrying the above-mentioned substrate into the above-mentioned processing chamber; the step of subjecting the above gas to plasma; and The step of supplying the plasma-formed gas to the substrate. A recording medium that is readable by a computer and records a program for causing a substrate processing apparatus to perform the following procedures by a computer; The substrate processing apparatus includes: a processing chamber for processing a substrate; a substrate supporter for holding a plurality of the substrates in multiple stages in the vertical direction; a buffer structure formed by chemical conversion, and an external electrode, the external electrode is arranged on the outside of the processing chamber corresponding to the position where the buffer structure is provided, and generates plasma; The procedure is: Procedures for carrying the above-mentioned substrate into the above-mentioned processing chamber; procedures for plasmaizing the above gas; and A procedure of supplying the above-mentioned gas that has been plasmatized to the above-mentioned substrate.

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