Substrate processing method, semiconductor device manufacturing method, program, and substrate processing apparatus.

Abstract

This technology provides a method for improving the film deposition rate. [Solution] The process includes: a) supplying a first gas containing the main elements and halogen elements that constitute the film to a substrate; b) supplying a first reducing gas containing hydrogen to the substrate; c) supplying a second reducing gas containing hydrogen and made of a different material from the first reducing gas to the substrate; d) performing a) and b) in parallel, and during this parallel process, reducing the amount of the first reducing gas supplied compared to the amount at the start of the supply of the first reducing gas; and e) performing d) and c) a predetermined number of times to form the film on the substrate.

Description

Technical Field

[0001] The present disclosure relates to a substrate processing method, a method for manufacturing a semiconductor device, a program, and a substrate processing apparatus.

Background Art

[0002] As one of the manufacturing steps of a semiconductor device, there is a step of forming a film on the surface of a substrate. (See, for example, Patent Document 1).

Prior Art Documents

Patent Documents

[0003]

Patent Document 1

Summary of the Invention

Problems to be Solved by the Invention

[0004] In the film formation step, the film formation rate may decrease.

[0005] The present disclosure provides a technology capable of improving the film formation rate.

Means for Solving the Problems

[0006] According to one aspect of the present disclosure, a) a step of supplying a first gas containing a main element and a halogen element constituting a film to a substrate; b) a step of supplying a first reducing gas containing hydrogen to the substrate; c) a step of supplying a second reducing gas containing hydrogen and made of a material different from the first reducing gas to the substrate; d) performing a) and b) in parallel, and while they are being performed in parallel, reducing the supply amount of the first reducing gas compared to the start of the supply of the first reducing gas; and e) performing d) and c) a predetermined number of times to form the film on the substrate. A technology is provided.

Effects of the Invention

[0007] According to the present disclosure, it becomes possible to improve the film formation rate. [Brief explanation of the drawing]

[0008] [Figure 1] Figure 1 is a longitudinal cross-sectional view showing a schematic of the substrate processing apparatus. [Figure 2] Figure 2 is a schematic cross-sectional view of line AA in Figure 1. [Figure 3] Figure 3 is a schematic diagram of the controller of the substrate processing device, showing the controller's control system in block diagram form. [Figure 4] Figure 4 is a flowchart showing a series of steps including the substrate processing process. [Figure 5] Figure 5 shows the timing of gas supply during the substrate processing process. [Figure 6] Figure 6 shows the supply timing of the first and second gases. [Figure 7] Figure 7 shows the supply timing of the first and second gases. [Figure 8] Figure 8 shows the supply timing of the first and second gases. [Figure 9] Figure 9 shows the supply timing of the first and second gases. [Figure 10] Figure 10 shows an example of table data illustrating the relationship between processing temperature and the rate of decrease of the second gas. [Modes for carrying out the invention]

[0009] <Embodiment> Hereinafter, one aspect of this disclosure will be described with reference to Figures 1 to 10. The drawings used in the following description are all schematic, and the dimensional relationships and proportions of each element shown in the drawings do not necessarily correspond to reality. Furthermore, the dimensional relationships and proportions of each element do not necessarily correspond between multiple drawings.

[0010] (1) Configuration of substrate processing apparatus The substrate processing apparatus 10 includes a processing furnace 202 equipped with a heater 207 as a heating means (heating mechanism, heating system). The heater 207 is cylindrical in shape and is mounted vertically by being supported by a heater base (not shown) which serves as a holding plate.

[0011] Inside the heater 207, an outer tube 203 is arranged concentrically with the heater 207 to form a processing container. The outer tube 203 is made of a heat-resistant material such as quartz or silicon carbide (SiC) and is formed in a cylindrical shape with a closed upper end and an open lower end. Below the outer tube 203, an MF209 (hereinafter referred to as MF209) is arranged concentrically with the outer tube 203. The MF209 is made of a metal such as stainless steel and is formed in a cylindrical shape with open upper and lower ends. An O-ring 220a is provided between the upper end of the MF209 and the outer tube 203 as a sealing member. The outer tube 203 is installed vertically when the MF209 is supported by the heater base.

[0012] An inner tube 204, which constitutes the processing container, is arranged inside the outer tube 203. The inner tube 204 is made of a heat-resistant material such as quartz or SiC, and is formed in a cylindrical shape with a closed upper end and an open lower end. The processing container is mainly composed of the outer tube 203, the inner tube 204, and MF209. A processing chamber 201 is formed in the hollow cylindrical part of the processing container (inside the inner tube 204).

[0013] The processing chamber 201 is configured to accommodate wafers 200 as substrates, arranged in a horizontal position in multiple vertical layers by boats 217, which will be described later.

[0014] Within the processing chamber 201, nozzles 410, 420, and 430 are installed so as to penetrate the side wall and inner pipe 204 of the MF209. Gas supply pipes 310, 320, and 330 are connected to nozzles 410, 420, and 430, respectively.

[0015] In the gas supply pipes 310, 320, and 330, mass flow controllers (MFCs) 312, 322, and 332, which are flow rate controllers (flow rate control units), are provided in order from the upstream side. Also, valves 314, 324, and 334, which are on-off valves, are provided in the gas supply pipes 310, 320, and 330, respectively. Gas supply pipes 510, 520, and 530 for supplying inert gas are connected to the downstream sides of the valves 314, 324, and 334 in the gas supply pipes 310, 320, and 330, respectively. In the gas supply pipes 510, 520, and 530, MFCs 512, 522, and 532, which are flow rate controllers (flow rate control units), and valves 514, 524, and 534, which are on-off valves, are provided in order from the upstream side, respectively.

[0016] Nozzles 410, 420, and 430 are respectively connected to the tip ends of the gas supply pipes 310, 320, and 330. The nozzles 410, 420, and 430 are configured as L-shaped nozzles, and their horizontal portions are provided so as to penetrate the side wall and the inner pipe 204 of the MF209. The vertical portions of the nozzles 410, 420, and 430 are provided inside a prechamber 201a having a channel shape (groove shape) that protrudes radially outward from the inner pipe 204 and extends in the vertical direction, and are provided along the inner wall of the inner pipe 204 upward (upward in the arrangement direction of the wafers 200) inside the prechamber 201a.

[0017] The nozzles 410, 420, and 430 are provided so as to extend from the lower region to the upper region of the processing chamber 201, and a plurality of gas supply holes 410a, 420a, and 430a are provided at positions facing the wafers 200, respectively. Thereby, the processing gas is supplied to the wafers 200 from the gas supply holes 410a, 420a, and 430a of the nozzles 410, 420, and 430, respectively. A plurality of these gas supply holes 410a, 420a, and 430a are provided from the lower part to the upper part of the inner pipe 204, each having the same opening area, and are further provided with the same opening pitch.

[0018] Multiple gas supply holes 410a, 420a, and 430a of nozzles 410, 420, and 430 are provided at a height from the bottom to the top of the boat 217, which will be described later. Therefore, the processing gas supplied into the processing chamber 201 from the gas supply holes 410a, 420a, and 430a of nozzles 410, 420, and 430 is supplied to the entire area of ​​the wafer 200 housed in the boat 217 from the bottom to the top. Nozzles 410, 420, and 430 only need to be provided to extend from the lower region to the upper region of the processing chamber 201, but it is preferable that they extend to near the ceiling of the boat 217.

[0019] From the gas supply pipe 310, a first element-containing gas (first gas), which includes the first element, is supplied into the processing chamber 201 via the MFC 312, valve 314, and nozzle 410 as the first material (raw material, processing gas).

[0020] From the gas supply pipe 320, a second gas is supplied into the processing chamber 201 as a first reactant (processing gas, reactant) via the MFC 322, valve 324, and nozzle 420. The term "agent" as used in this disclosure includes at least one of gaseous substances and liquid substances. Liquid substances include mist-like substances. That is, film-forming agents, modifiers, and etching agents may contain gaseous substances, liquid substances such as mist-like substances, or both.

[0021] From the gas supply pipe 330, a third gas is supplied into the processing chamber 201 as a second reactant (processing gas, reactant) via the MFC 332, valve 334, and nozzle 430.

[0022] From the gas supply pipes 510, 520, and 530, nitrogen (N2) gas, for example, is supplied as an inert gas into the processing chamber 201 via MFCs 512, 522, and 532, valves 514, 524, and 534, and nozzles 410, 420, and 430, respectively. The following describes an example in which N2 gas is used as the inert gas, but other noble gases such as Ar gas, He gas, Ne gas, and Xe gas may also be used as the inert gas.

[0023] The gas supply system (gas supply section) mainly consists of gas supply pipes 310, 320, 330, MFCs 312, 322, 332, valves 314, 324, 334, and nozzles 410, 420, 430, although nozzles 410, 420, 430 may be considered as the gas supply system alone. The processing gas supply system may simply be called the gas supply system. In addition, the inert gas supply system mainly consists of gas supply pipes 510, 520, 530, MFCs 512, 522, 532, and valves 514, 524, 534.

[0024] When supplying the first gas from the gas supply pipe 310, the first gas supply system (first gas supply section) mainly consists of the gas supply pipe 310, MFC 312, and valve 314. Here, the nozzle 410 may also be considered as part of the first gas supply system. When supplying the second gas from the gas supply pipe 320, the second gas supply system (second gas supply section) mainly consists of the gas supply pipe 320, MFC 322, and valve 324. Here, the nozzle 420 may also be considered as part of the second gas supply system. When supplying the third gas from the gas supply pipe 330, the third gas supply system (third gas supply section) mainly consists of the gas supply pipe 330, MFC 332, and valve 334. Here, the nozzle 430 may also be considered as part of the third gas supply system. Furthermore, the processing gas supply system is configured by including gas supply pipes 310, 320, 330, MFCs 312, 322, 332, valves 314, 324, 334, nozzles 410, 420, 430, gas supply pipe 340, MFC 342, and valve 344.

[0025] In this embodiment, the gas supply method involves transporting gas through nozzles 410, 420, and 430 located in a preliminary chamber 201a within a vertically elongated, annular space defined by the inner wall of the inner tube 204 and the edges of multiple wafers 200. Gas is then ejected into the inner tube 204 from multiple gas supply holes 410a, 420a, and 430a located on the nozzles 410, 420, and 430 facing the wafers. More specifically, the first gas and the like are ejected in a direction parallel to the surface of the wafers 200 through the gas supply hole 410a of nozzle 410, the gas supply hole 420a of nozzle 420, and the gas supply hole 430a of nozzle 430.

[0026] The exhaust port (exhaust vent) 204a is a through-hole formed in the side wall of the inner tube 204, opposite the nozzles 410, 420, and 430, and is, for example, a slit-shaped through-hole that is elongated vertically. The gas supplied into the processing chamber 201 from the gas supply holes 410a, 420a, and 430a of the nozzles 410, 420, and 430, and flowing over the surface of the wafer 200, flows through the exhaust port 204a into the exhaust passage 206, which is formed by the gap between the inner tube 204 and the outer tube 203. The gas that has flowed into the exhaust passage 206 then flows into the exhaust pipe 231 and is discharged outside the processing furnace 202.

[0027] The exhaust port 204a is located opposite the multiple wafers 200, and the gas supplied from the gas supply ports 410a, 420a, and 430a to the vicinity of the wafers 200 in the processing chamber 201 flows horizontally before flowing into the exhaust passage 206 through the exhaust port 204a. The exhaust port 204a is not limited to being a slit-shaped through-hole, but may also be composed of multiple holes.

[0028] The MF209 is equipped with an exhaust pipe 231 for exhausting the atmosphere inside the processing chamber 201. Connected to the exhaust pipe 231, in order from upstream, are a pressure sensor 245 (which acts as a pressure detector (pressure detection unit) for detecting the pressure inside the processing chamber 201), an APC (Auto Pressure Controller) valve 243, and a pump 246 (which acts as an exhaust device). The APC valve 243 can be opened and closed while the pump 246 is operating to exhaust and stop the exhaust from the processing chamber 201, and the pressure inside the processing chamber 201 can be adjusted by adjusting the valve opening while the pump 246 is operating. The exhaust system mainly consists of the exhaust port 204a, the exhaust passage 206, the exhaust pipe 231, the APC valve 243, and the pressure sensor 245. The pump 246 may also be considered as part of the exhaust system.

[0029] Below the MF209, a seal cap 219 (hereinafter SC219) is provided as a furnace opening cover capable of airtightly closing the lower end opening of the MF209. The SC219 is configured to abut the lower end of the MF209 from the vertically downward side. The SC219 is made of a metal such as SUS and is formed in a disc shape. An O-ring 220b is provided on the upper surface of the SC219 as a sealing member that abuts the lower end of the MF209. On the opposite side of the processing chamber 201 in the SC219, a rotating mechanism 267 is installed to rotate a boat 217 that houses the wafers 200. The rotation shaft 255 of the rotating mechanism 267 passes through the SC219 and is connected to the boat 217. The rotating mechanism 267 is configured to rotate the wafers 200 by rotating the boat 217. The SC219 is configured to be raised and lowered vertically by a boat elevator 115 (hereinafter BE115), which is installed vertically outside the outer tube 203 as a lifting mechanism. BE115 is configured to allow the boat 217 to be moved in and out of the processing chamber 201 by raising and lowering SC219. BE115 is configured as a transport device (transport system) for transporting the boat 217 and the wafers 200 contained in the boat 217 to the processing chamber 201.

[0030] The boat 217, as a substrate support, is configured to arrange multiple wafers 200, for example, 10 to 200 wafers, in a horizontal position with vertical spacing between them. Here, numerical range notations such as "10 to 200 wafers" in this specification mean that the lower and upper limits are included within that range. Therefore, for example, "10 to 200 wafers" means "10 wafers or more and 200 wafers or less." The same applies to other numerical ranges.

[0031] Boat 217 is made of a heat-resistant material such as quartz or SiC. At the bottom of boat 217, multiple (not shown) insulating plates 218, also made of a heat-resistant material such as quartz or SiC, are supported in a horizontal position.

[0032] As shown in Figure 2, a temperature sensor 263 is installed inside the inner tube 204 as a temperature detector. The amount of current supplied to the heater 207 is adjusted based on the temperature information detected by the temperature sensor 263 so that the temperature inside the processing chamber 201 reaches a desired temperature distribution. The temperature sensor 263 is configured in an L-shape, similar to the nozzles 410, 420, and 430, and is installed along the inner wall of the inner tube 204.

[0033] As shown in Figure 3, the controller 121, which is the control unit (control means), is configured as a computer equipped with a CPU (Central Processing Unit) 121a, RAM (Random Access Memory) 121b, storage device 121c, and I / O port 121d. The RAM 121b, storage device 121c, and I / O port 121d are configured to exchange data with the CPU 121a via an internal bus. An input / output device 122, configured as, for example, a touch panel, is connected to the controller 121. The controller 121 is also configured to be able to connect to an external storage device (for example, a magnetic disk such as a hard disk, an optical disk such as a CD or DVD, or a semiconductor memory such as a USB memory or memory card) 123.

[0034] Here, the substrate processing apparatus may be configured to have one control unit, or it may be configured to have multiple control units. That is, the control for performing the substrate processing steps described later may be performed using one control unit, or it may be performed using multiple control units. Furthermore, the multiple control units may be configured as a control system connected to each other by a wired or wireless communication network, and the control for performing the substrate processing steps described later may be performed by the entire control system. In this specification, the term "control unit" may include one control unit, multiple control units, or a control system composed of multiple control units.

[0035] The storage device 121c is composed of, for example, flash memory, an HDD (Hard Disk Drive), etc. The storage device 121c contains, in a readable format, a control program configured to control the operation of the substrate processing device, a process recipe describing the procedures and conditions for the semiconductor device manufacturing method (described later), table data showing the relationship between processing temperature and the decrease in the second gas (first reducing gas), and so on. The process recipe is configured to allow the controller 121 to execute each step in the semiconductor device manufacturing method (described later), and is combined to obtain a predetermined result; it functions as a program. Hereinafter, this process recipe, control program, etc., will be collectively referred to simply as a program. In this specification, the term "program" may include only the process recipe, only the control program, or a combination of the process recipe and the control program. The RAM 121b is configured as a memory area where programs and data read by the CPU 121a are temporarily held.

[0036] I / O port 121d is connected to the aforementioned MFCs 312, 322, 332, 512, 522, 532, valves 314, 324, 334, 514, 524, 534, pressure sensor 245, APC valve 243, vacuum pump 246, heater 207, temperature sensor 263, rotary mechanism 267, BE115, etc.

[0037] The CPU 121a is configured to read and execute a control program from the storage device 121c, and to read recipes and other information from the storage device 121c in response to input of operation commands from the input / output device 122. The CPU 121a is configured to control the flow rate adjustment operations of various gases by MFCs 312, 322, 332, 512, 522, and 532, the opening and closing operations of valves 314, 324, 334, 514, 524, and 534, the opening and closing operations of the APC valve 243 and the pressure adjustment operations based on the pressure sensor 245 by the APC valve 243, the temperature adjustment operations of the heater 207 based on the temperature sensor 263, the starting and stopping of the vacuum pump 246, the rotation and rotation speed adjustment operations of the boat 217 by the rotating mechanism 267, the raising and lowering operations of the boat 217 by the BE 115, and the loading operations of wafers 200 into the boat 217, in accordance with the contents of the read recipe.

[0038] The controller 121 can be configured by installing the above-mentioned program stored in the external storage device 123 onto a computer. The storage device 121c and the external storage device 123 are configured as computer-readable recording media. Hereinafter, these will be collectively referred to simply as recording media. In this specification, the recording media may include only the storage device 121c, only the external storage device 123, or both. The program (program product) may be provided to the computer using communication means such as the Internet or a dedicated line, without using the external storage device 123.

[0039] (2) Substrate processing process (film formation process) An example of a process for forming a film on a wafer 200 as one step in the manufacturing process of a semiconductor device will be explained using Figures 4 to 10. The film formation process is performed using the substrate processing apparatus 10 described above. In the following explanation, the operation of each part constituting the substrate processing apparatus 10 is controlled by the controller 121.

[0040] In the substrate processing process (semiconductor manufacturing process) according to this embodiment, a) A step of supplying a first gas containing the main elements and halogen elements that constitute the film to the wafer 200, b) A step of supplying a first reducing gas (second gas) containing hydrogen to the wafer 200, c) A step of supplying a second reducing gas (third gas) containing hydrogen and made of a different material from the first reducing gas to the wafer 200, d) a) and b) are performed in parallel, and during this parallel process, the amount of first reducing gas supplied is reduced compared to the amount supplied at the start of the first reducing gas supply. Steps e)d) and c) are performed a predetermined number of times to form a film on the wafer 200.

[0041] In this specification, the term "wafer" may mean either "the wafer itself" or "a laminate of a wafer and a predetermined layer or film formed on its surface." In this specification, the term "surface of a wafer" may mean either "the surface of the wafer itself" or "the surface of a predetermined layer or film formed on the wafer." In this specification, the term "substrate" has the same meaning as the term "wafer."

[0042] (Wafer (substrate) delivery: S101) Once multiple wafers 200 are placed on the boat 217, as shown in Figure 1, the boat 217 supporting the multiple wafers 200 is lifted by the BE 115 and carried into the processing chamber 201 of the processing container, where it is housed.

[0043] (Pressure adjustment and temperature adjustment: S102) The processing chamber 201, i.e., the space where the wafer 200 is located, is evacuated by the pump 246 to a desired pressure. At this time, the pressure in the processing chamber 201 is measured by the pressure sensor 245, and the APC valve 243 is feedback-controlled based on this measured pressure information (pressure adjustment). The pump 246 is kept running continuously at least until the processing of the wafer 200 is completed. The processing chamber 201 is also heated by the heater 207 to a desired temperature. At this time, the amount of power supplied to the heater 207 is feedback-controlled based on the temperature information detected by the temperature sensor 263 so that the processing chamber 201 has a desired temperature distribution (temperature adjustment). Heating of the processing chamber 201 by the heater 207 is continued at least until the processing of the wafer 200 is completed. In the film formation process of this disclosure, the temperature of the heater 207 is set to a temperature such that the temperature of the wafer 200 is, for example, in the range of 200 to 650°C.

[0044] (Substrate processing: S103)

[0045] (First gas supply process: S1031) The valve 314 is opened, and the first gas flows into the gas supply pipe 310. The first gas, whose flow rate has been adjusted by the MFC 312, is supplied into the processing chamber 201 from the gas supply hole 410a of the nozzle 410 and exhausted from the exhaust pipe 231.

[0046] At this time, the APC valve 243 is adjusted to set the pressure in the processing chamber 201 to a pressure within the range of, for example, 1 to 3990 Pa. The supply flow rate of the first gas controlled by the MFC 312 is set to a flow rate within the range of, for example, 0.01 to 3 slm. In this disclosure, numerical range notations such as "1 to 3990 Pa" mean that the lower limit and upper limit are included in that range. Therefore, for example, "1 to 3990 Pa" means "1 Pa or more and 3990 Pa or less". The same applies to other numerical ranges.

[0047] At this time, a first gas is supplied to the wafer 200. By supplying the first gas to the wafer 200, a material containing the first element is adsorbed onto the wafer 200 (the underlying film on the surface). The first element is, for example, at least one of the following elements: titanium (Ti), zirconium (Zr), hafnium (Hf), molybdenum (Mo), ruthenium (Ru), aluminum (Al), gallium (Ga), silicon (Si), germanium (Ge), niobium (Nb), manganese (Mn), nickel (Ni), cobalt (Co), yttrium (Y), etc. As raw materials, a gas containing the first element and a halogen element can be used. The halogen element is, for example, at least one of chlorine (Cl), fluorine (F), bromine (Br), etc. Examples of such gases include WCl6, WF6, TiF4, MoCl5, MoF5, MoO2Cl2, RuCl3, RuF3, HfCl4, HfF4, ZrCl4, ZrF4, AlCl3, AlF), SiH3Cl, SiH2Cl2, Si2Cl6, SiCl4, TaCl5, TaF5, WCl6, CoCl2, CoF2, YCl3, YF3, NbF3, NbCl3, MnF2, MnCl2, NiF2, NiCl2, SiCl4, and one or more of these can be used. Preferably, the raw material contains a chlorine element among the halogen elements. In this disclosure, the case in which TiCl4 is used as the raw material will be described. When TiCl4 is used as the raw material for the first gas, TiClx (where X is an integer less than or equal to 4) is adsorbed onto the wafer 200 (surface underlayer) by supplying the TiCl4 gas, and a Ti-containing layer is formed.

[0048] (Second gas supply process: S1032) Next, we will explain the supply process for the second gas. The supply process for the second gas has a period in which it is carried out in parallel with the supply process for the first gas.

[0049] The valve 324 is opened, and the second gas flows into the gas supply pipe 320. The raw material, whose flow rate has been adjusted by the MFC 322, is supplied into the processing chamber 201 from the gas supply hole 420a of the nozzle 420 and exhausted from the exhaust pipe 231.

[0050] At this time, the APC valve 243 is adjusted to set the pressure in the processing chamber 201 to a pressure within the range of, for example, 1 to 3990 Pa. The supply flow rate of the second gas controlled by the MFC 322 is set to a flow rate within the range of, for example, 0.1 to 10 slm. The time for supplying the first gas and the second gas to the wafer 200 in parallel is set to a time within the range of, for example, 0.01 to 70 seconds.

[0051] At this time, the first gas and the second gas are supplied to the wafer 200. That is, at least the first gas and the second gas are supplied at the same time. A reducing gas can be used as the second gas. A different reducing gas than the third gas described later is used. The second gas is also called the first reducing gas. For example, the second gas can be a gas containing a predetermined element and hydrogen. The predetermined element is, for example, at least one element from group 13 and group 14 of the periodic table. Specific examples of such gases include silane gases such as SiH4, Si2H6, and Si3H8, and borane gases such as BH3 and B2H6. Such gases are also called hydrides of the predetermined element. In the following explanation, we will describe the case in which SiH4 is used as the second gas.

[0052] By supplying the second gas in this manner, by-products, such as hydrogen chloride (HCl), which are adsorption inhibitors that hinder film formation, are removed. Furthermore, by-products such as HCl that were adsorbed in areas where no by-products were adsorbed can be removed. As a result, adsorption sites on the wafer 200 where raw materials can be adsorbed become available, and adsorption sites where raw materials such as TiClx can be adsorbed can be formed on the surface of the wafer 200. Here, adsorption sites where raw materials can be adsorbed refer to areas on the wafer 200 where no by-products are adsorbed.

[0053] (Suspension of supply of gas 1 and continuation of supply of gas 2) After a predetermined time has elapsed since the start of supplying the first gas, the valve 314 may be closed to stop the supply of the first gas. In other words, after a predetermined time has elapsed since the start of supplying the second gas, and while the second gas is being supplied, the supply of the first gas may be stopped midway through the supply of the second gas. The supply process may be configured so that the stopping of the supply of the first gas and the stopping of the supply of the second gas occur at the same time. Furthermore, the supply of the first gas may be stopped after the supply of the second gas has been stopped.

[0054] At this time, the APC valve 243 is adjusted to set the pressure in the processing chamber 201 to a pressure within the range of, for example, 1 to 3990 Pa. The time for simultaneously supplying the first gas and the fourth gas to the wafer 200 is set to a time within the range of, for example, 0.1 to 30 seconds.

[0055] At this time, the second gas is supplied to the wafer 200.

[0056] In this way, by stopping the supply of the first gas while the second gas is being supplied, and stopping the supply of the second gas after a predetermined time has elapsed since the first gas was stopped, the amount of by-products remaining in the processing chamber 201 can be reduced, and the film quality of the first element-containing film, such as the titanium nitride (TiN) film, can be improved.

[0057] By supplying a second gas, the number of adsorption sites on the wafer 200 where raw materials can be adsorbed can be increased. On the other hand, molecules of the second gas present on the wafer 200 and in the processing chamber 201 may prevent molecules of the first gas from adsorbing onto the wafer 200. In particular, after the amount of by-products on the wafer 200 and in the processing chamber 201 has decreased to a certain extent, the suppression of adsorption of first gas molecules by molecules of the second gas becomes significant.

[0058] One method to suppress the adsorption of first gas molecules by second gas molecules is the gas supply patterns A to K shown in Figures 6 to 8.

[0059] (Pattern A) Pattern A is a pattern in which the supply amount of the second gas is reduced compared to the start of the second gas supply. By supplying the second gas in this manner, as described above, by-products are removed by the second gas, and after the by-products have been reduced to a certain extent, the molecules of the second gas can also be reduced. As a result, at the start of the second gas supply, the inhibition of adsorption of the first gas by by-products can be suppressed. Furthermore, by reducing the supply flow rate (partial pressure) of the second gas, the inhibition of adsorption of the first gas by the molecules of the second gas can be suppressed. Note that in Pattern A, the timing of the end of the supply of the second gas is synchronized with the timing of the end of the supply of the first gas. With this configuration, especially just before the end of the supply of the second gas, the partial pressure of the first gas in the processing chamber 201 becomes high, and the probability of the molecules of the first gas adsorbing onto the wafer 200 can be improved.

[0060] Here, the supply quantity in this disclosure is adjusted by at least one of the gas supply flow rate and gas supply time set in each MFC. The supply quantity may also be considered in terms of concentration and partial pressure. Reducing the gas supply quantity means, for example, reducing the gas supply flow rate over time.

[0061] (Pattern B) Pattern B is a pattern in which the supply of the second gas is terminated after the supply of the first gas is terminated. By configuring it in this way, it is possible to facilitate the discharge of by-products generated just before the termination of the supply of the first gas from the processing chamber 201.

[0062] (Pattern C) Pattern C is a pattern that delays the timing of the termination of the supply of the second gas compared to Pattern B.

[0063] Patterns A to C can also be described as changing the rate (speed) of decrease in the supply amount of the second gas. The rate of decrease in the supply amount of the second gas may be changed based on the processing temperature. Due to the reaction of the second gas, components of the material of the second gas may be incorporated into the film. Here, the components are, for example, predetermined elements contained in the material of the second gas. If components of the second gas are incorporated into the film, the properties of the film may not be the desired properties. If the film is a conductive film, the electrical properties may deteriorate. The reaction amount of the second gas may depend on the processing temperature. For example, if the processing temperature is raised above a predetermined temperature, the reaction amount increases. On the other hand, if the processing temperature is lowered below a predetermined temperature, the reaction amount decreases. An increase in the reaction amount may result in a larger amount of components of the second gas being incorporated into the film. If it is desired to suppress the incorporation of components of the second gas into the film, the supply amount of the second gas can be reduced. However, simply reducing the supply amount reduces the amount of adsorption inhibitors removed, which leads to the problem that the amount of first gas molecules adsorbed on the wafer 200 decreases. To address these challenges, as described in this disclosure, the amount of second gas can be reduced during the supply period of the second gas, from immediately after the start of supply until the end of the supply period. By reducing the amount of second gas in this way, it is possible to reduce the total supply amount of second gas during the supply period while suppressing a decrease in the amount of adsorption inhibitors removed. Although it is also possible to increase the supply flow rate of second gas from the start to the end of supply during the supply period of second gas, from the viewpoint of efficiently removing adsorption inhibitors, it is preferable to supply it as shown in the pattern in the diagram of this disclosure. This is because more adsorption inhibitors are generated at the start of supply during the supply period of the first gas. Note that changing the rate of reduction of the supply amount of second gas also changes the supply time of second gas. This changes the time that the second gas stays in the processing chamber 201. By changing the time that the second gas stays in the processing chamber 201, the reaction amount of second gas can be changed. By shortening the residence time of second gas, the reaction amount of second gas can be reduced.

[0064] The rate of decrease in the supply amount of the second gas can be set based on the processing temperature of the wafer 200. For example, a table data as shown in Figure 10 is prepared, and the rate of decrease corresponding to the set processing temperature is read from the table data to set the rate of decrease of the second gas. Figure 10 shows that processing temperatures a1, a2, a3...an increase in this order. As the processing temperature increases, the rate of decrease increases. As shown in Figure 10, the rate of decrease can be set, for example, between 10% and 90%. If the processing temperature is higher than a predetermined temperature, the data with a large rate of decrease is read from the table data and the rate of decrease of the second gas is set. For example, as in pattern A, the rate of decrease (the slope that reduces the supply amount of the second gas) from the start of supplying the second gas to the end of supplying the second gas is increased. By configuring the supply of the second gas in this way, it is possible to suppress the incorporation of products generated by the decomposition of the second gas into the film. Furthermore, the effect of pattern A described above can also be obtained. Conversely, if the processing temperature is lower than a predetermined temperature, the rate of decrease is set to be small. For example, a second gas can be supplied as shown in pattern C. While this example shows setting a reduction rate, it is not limited to this; a supply time can also be set. The program recipe can also be configured so that the supply flow rate (partial pressure) becomes zero within the set supply time period from the initial supply flow rate (partial pressure).

[0065] (Pattern D) Pattern D is an example of a pattern in which the supply amounts of the first gas and the second gas are changed relatively. By increasing the supply amount of the first gas, the supply amount (partial pressure) of the second gas can be relatively decreased. In this case, the supply amount of the second gas may be kept constant. As described above, the molecules of the second gas prevent the molecules of the first gas from reaching the wafer 200, so by increasing the number of first gas molecules present on the wafer 200 or in the processing chamber 201, the number of first gas molecules that reach the wafer 200 can be increased. It is also thought that the molecules of the first gas themselves have the effect of pushing away (pushing out) the second gas molecules. However, since increasing the supply amount of the first gas may increase the amount of by-products generated, it is preferable to gradually increase the supply amount of the first gas, as shown in Pattern D.

[0066] (Pattern E) Pattern E is a pattern in which the supply of the first gas is increased while the supply of the second gas is decreased, as in patterns A to C.

[0067] (Pattern F) In patterns D and E, the supply rate of the first gas is gradually increased immediately after the start of supplying the first gas. This method raises concerns about the generation of large amounts of by-products. Pattern F addresses this concern. In pattern F, the supply of the first gas begins immediately after the supply of the second gas starts. This configuration reduces the amount of by-products generated by the supply of the first gas compared to patterns D and E.

[0068] Furthermore, as shown in Pattern F, it is preferable to start increasing the supply rate of the first gas after the supply of the second gas has begun. This is because if the supply rate of the first gas is increased immediately after the supply of the first gas has begun, the amount of adsorption inhibitors generated by the supply of the first gas will increase. Therefore, it is preferable to increase the supply rate of the first gas after the supply of the second gas has begun.

[0069] (Pattern G) Pattern G is a sequence that further reduces the amount of by-products generated by the supply of the first gas. Pattern G starts the supply of the first gas at approximately zero and gradually increases it. By configuring it in this way, the amount of by-products generated by the supply of the first gas can be reduced. Note that the initial supply amount of the first gas does not have to be zero; a small amount may be supplied. Here, a small amount is, for example, a flow rate of about 0.1 to 1 slm.

[0070] So far, we have shown examples where the supply of the first gas and the supply of the second gas are changed continuously. The methods of increasing and decreasing are not limited to these, and as shown in patterns H, I, and J of Figure 8, they may also be changed in steps. The same effects as the patterns described above can be obtained by changing them in steps in this way. Preferably, the changes are made continuously. By changing them continuously, it is possible to suppress abrupt changes in the reaction occurring on the wafer 200. As a result, the in-plane uniformity of the Ti-containing layer on the wafer 200 can be improved.

[0071] In addition, in pattern J, as with pattern F, it is preferable to start increasing the supply of the first gas after the supply of the second gas has begun.

[0072] (Pattern K) Pattern K is a pattern in which the supply amount of the second gas is gradually reduced, and after the supply of the first gas is terminated, the supply amount of the second gas is kept constant. This maintains the effect of removing by-products present on the wafer 200 and in the processing chamber 201 after the supply of the first gas.

[0073] (Pattern L) Pattern L is a pattern in which the rate of decrease of the supply of the second gas is changed midway through the process. The change in the rate of decrease means that the rate of decrease of the supply of the second gas is increased midway through the process. For example, the timing for increasing the rate of decrease is after the supply of the first gas is terminated. After the supply of the first gas is terminated, the amount of adsorption inhibitors generated decreases, so the amount of the second gas used to remove the adsorption inhibitors may be reduced. By increasing the rate of decrease, the amount of the supply of the second gas can be reduced.

[0074] (Pattern M) Pattern M is a pattern in which the supply rate of the second gas is reduced in fewer stages compared to patterns such as Pattern H. In Pattern M in Figure 9, an example is shown in which the second gas is supplied at two different supply rates. Similar effects can be obtained by configuring the supply of the second gas in this way.

[0075] (Pattern N) Pattern N is a pattern that can be taken when the supply process of the first gas S1031 and the supply process of the second gas S1032 are performed consecutively multiple times. The first supply process of the first gas is shown as S1031a, and the first supply process of the second gas as S1032a. The second supply process of the first gas is shown as S1031b, and the first supply process of the second gas as S1032b. As shown in Figure 9, in the second supply process of the second gas S1032b, the amount of second gas supplied is less than the amount supplied in the first supply process of the second gas S1032a. The amount of by-products (adsorption inhibitors) generated in the second and subsequent supply processes of the first gas is less than the amount of by-products generated in the first supply process of the first gas. Therefore, the amount of second gas required decreases from the second time onward. By supplying a smaller amount from the second time onward than in the previous supply, the adsorption inhibition of the first gas due to the presence of the second gas can be reduced, and the amount of adsorption of the first gas can be increased. Furthermore, it is possible to reduce the amount of components of the second gas that are mixed into the layer formed in the second and subsequent stages. It is desirable that the flow rate (partial pressure) during the second gas supply process from the second stage onward inherits the flow rate (partial pressure) at the end of the first second gas supply. By configuring it in this way, insufficient removal of adsorption inhibitors can be suppressed.

[0076] (Inert gas supply (purge): S1033) After a predetermined time has elapsed since the start of supplying the second gas, valve 324 is closed to stop the supply of the second gas. At this time, valves 514, 524, 534, and 544 are opened to allow inert gas to flow through the gas supply pipes 510, 520, 530, and 540 (purging). In other words, inert gas is supplied into the processing chamber 201.

[0077] At this time, the APC valve 243 is adjusted to set the pressure in the processing chamber 201 to a pressure within the range of, for example, 1 to 3990 Pa. The supply flow rates of the inert gas controlled by MFCs 512, 522, 532, and 542 are set to flow rates within the range of, for example, 0.1 to 30 slm.

[0078] (Exhaust process: S1033) After a predetermined time has elapsed since the start of the inert gas supply, valves 514, 524, 534, and 544 are closed to stop the supply of inert gas. At this time, the APC valve 243 of the exhaust pipe 231 is opened, and the processing chamber 201 is evacuated using the pump 246. As a result, residual gas is removed from the wafer 200, and any remaining gases and reaction by-products in the processing chamber 201 are removed from the processing chamber 201. The time for evacuating the processing chamber 201 is, for example, within the range of 0.1 to 30 seconds.

[0079] (Third gas supply process: S1034) Next, valve 334 is opened, and the third gas is introduced into the gas supply pipe 330. The flow rate of the third gas is adjusted by MFC 332 and supplied into the processing chamber 201 through the gas supply hole 430a of nozzle 430, and exhausted through exhaust pipe 231.

[0080] At this time, the APC valve 243 is adjusted to set the pressure in the processing chamber 201 to a pressure within the range of, for example, 1 to 3990 Pa. The supply flow rate of the first reactant controlled by the MFC 332 is set to a flow rate within the range of, for example, 0.1 to 30 slm. The time for supplying the third gas to the wafer 200 is set to a time within the range of, for example, 0.01 to 30 seconds.

[0081] At this time, a third gas is supplied to the wafer 200. Here, a reactant can be used as the third gas. For example, a nitride can be used. A nitride is a gas containing nitrogen. Specifically, gases containing nitrogen and hydrogen such as NH3, N2H2, and N2H4 can be used. Such reducing gases can be used as the third gas. The third gas is a different gas from the second gas and is also called the second reducing gas. Below, an example in which NH3 gas is used as the first reactant will be described. When NH3 is supplied, it undergoes a substitution reaction with at least a portion of the Ti-containing layer formed on the wafer 200. During the substitution reaction, the Ti contained in the Ti-containing layer and the N contained in the NH3 gas combine to form a TiN layer on the wafer 200. Specifically, a TiN film is formed on the wafer 200 by the reaction of TiClx adsorbed on the wafer 200 with NH3. In addition, reaction byproducts such as HCl, ammonium chloride (NH4Cl), and H2 are produced during the substitution reaction.

[0082] (Inert gas supply: S1035) After a predetermined time has elapsed since the start of supplying the third gas, valve 334 is closed to stop the supply of the third gas. At this time, valves 514, 524, 534, and 544 are opened to allow inert gas to flow through the gas supply pipes 510, 520, 530, and 540. In other words, inert gas is supplied into the processing chamber 201.

[0083] At this time, the APC valve 243 is adjusted to set the pressure in the processing chamber 201 to a pressure within the range of, for example, 1 to 3990 Pa. The supply flow rate of the inert gas controlled by MFCs 512, 522, 532, and 542 is set to a flow rate within the range of, for example, 0.1 to 30 slm. At this time, the time for supplying the inert gas to the wafer 200 is set to a time within the range of, for example, 0.1 to 30 seconds.

[0084] At this time, an inert gas is supplied into the processing chamber 201. This reduces the amount of unreacted material, third gases that have contributed to film formation, and reaction by-products remaining in the processing chamber 201.

[0085] (Exhaust process: S1035) After a predetermined time has elapsed since the start of the inert gas supply, valves 514, 524, 534, and 544 are closed to stop the supply of inert gas. At this time, the APC valve 243 of the exhaust pipe 231 is opened, and the processing chamber 201 is evacuated by the pump 246. This removes residual gas from the wafer 200, and eliminates unreacted or third gases that have contributed to film formation, as well as reaction by-products, that remain in the processing chamber 201. The time for evacuating the processing chamber 201 is, for example, within the range of 0.1 to 30 seconds.

[0086] (Performed the prescribed number of times: S1036) In the film formation process, the above-described first gas supply process, second gas supply process, and third gas supply process are performed sequentially a predetermined number of times (X times, where X is an integer of 1 or more than 2) to form a film of a predetermined thickness on the wafer 200. In this case, for example, a titanium nitride (TiN) film is formed.

[0087] As described above, after forming a predetermined film on the wafer 200, a purging and atmospheric pressure return process, and a wafer 200 removal process are performed.

[0088] (Purge and return to atmospheric pressure: S104) Inert gas is supplied into the processing chamber 201 from gas supply pipes 510 to 530 and exhausted through exhaust pipe 231. The inert gas acts as a purge gas, purging the processing chamber 201 and removing any remaining gases and reaction by-products. Subsequently, the atmosphere inside the processing chamber 201 is replaced with the inert gas, and the pressure inside the processing chamber 201 is returned to atmospheric pressure.

[0089] (Wafer (substrate) unloading: S105) Subsequently, SC219 is lowered by BE115, opening the lower end of the outer tube 203. Then, the processed wafer 200, supported by the boat 217, is transported out of the outer tube 203 from the lower end. After that, the processed wafer 200 is removed from the boat 217.

[0090] (3) Effects of this embodiment According to this embodiment, one or more of the following effects (A) to (G) can be obtained. (A) By supplying each gas as in pattern A described above, the adsorption of the first gas molecule onto the surface of the wafer 200 can be promoted. (B) By supplying each gas as in patterns B and C described above, the discharge of by-products by the second gas can be promoted. (C) By changing the rate of decrease in the supply amount of the second gas based on the processing temperature of the wafer 200, it is possible to suppress the incorporation of decomposition products of the second gas into the film. (D) As shown in patterns D to G, the adsorption of the first gas molecules onto the surface of the wafer 200 can be promoted by increasing the supply amount of the first gas. (E) As shown in pattern F, by maintaining a constant supply rate of the first gas and increasing the supply rate of the first gas after the start of supplying the second gas, it is possible to suppress the increase in reaction byproducts generated by the supply of the first gas while promoting the adsorption of the first gas molecules onto the surface of the wafer 200. (F) As in pattern G, by supplying a small amount of the first gas at the start of supply and increasing the amount over time, the amount of reaction byproducts generated immediately after the start of supply of the first gas can be reduced. (G) As shown in pattern K, after the supply of the first gas is terminated, the amount of by-products present on the wafer 200 and in the processing chamber 201 can be reduced by maintaining a constant supply amount of the second gas.

[0091] (4) Other embodiments The embodiments of this disclosure have been described in detail above. However, this disclosure is not limited to the embodiments described above, and can be modified in various ways without departing from its essence.

[0092] In the above embodiment, the case in which a nitride agent is used as the third gas (first reactant) was described, but this disclosure is not limited thereto. When forming a film of a single metal instead of a nitride film on a substrate, a hydrogen-containing gas that does not contain nitrogen may be used. Examples of hydrogen-containing gases that do not contain nitrogen include H2 gas and deuterium (D2) gas. Furthermore, when forming an oxide film, an oxidizing agent may be used. As an oxidizing agent, an oxygen-containing gas can be used. Specifically, at least one of O2, O3, H2O, H2+O2, H2O2, and N2O can be used. Note that each of the nitride agent, reducing agent, and oxidizing agent can be a gas obtained by activating at least one of the gases of this disclosure.

[0093] In the above embodiment, an example using a silane-based gas as the second gas was described, but the invention is not limited to this, and a halosilane-based gas containing a halogen may also be used. Because it contains a halogen, the removal effect of adsorption inhibitors is weaker than when a silane-based gas without a halogen is used, but because it contains hydrogen, a similar effect may be obtained in some cases.

[0094] In the above embodiment, an example was shown in which the supply flow rate (partial pressure) of the second gas is decreased over time. However, if the components of the second gas are intentionally included in the membrane, the flow rate may be increased over time instead.

[0095] It is preferable to prepare (or have multiple) process recipes (programs describing processing procedures and conditions, etc.) used for forming these various thin films, according to the content of the substrate processing (type of film to be formed, composition ratio, film quality, film thickness, processing procedure, processing conditions, etc.). When starting the substrate processing, it is preferable to appropriately select an appropriate process recipe from among the multiple process recipes according to the content of the substrate processing. Specifically, it is preferable to pre-store (install) multiple process recipes (program products) prepared individually according to the content of the substrate processing into the storage device 121c of the substrate processing apparatus via a telecommunications line or a recording medium (external storage device 123) on which the process recipes are recorded. When starting the substrate processing, it is preferable for the CPU 121a of the substrate processing apparatus to appropriately select an appropriate process recipe from among the multiple process recipes stored in the storage device 121c according to the content of the substrate processing. With this configuration, a single substrate processing apparatus can form thin films of various types, composition ratios, film quality, and film thickness in a general-purpose and reproducible manner. Furthermore, it reduces the operator's workload (such as the burden of inputting processing procedures and conditions), allowing for quicker initiation of board processing while avoiding operational errors.

[0096] Furthermore, this disclosure can also be implemented, for example, by changing the process recipe of an existing substrate processing apparatus. When changing the process recipe, it is possible to install the process recipe relating to this disclosure into the existing substrate processing apparatus via a telecommunications line or a recording medium on which the process recipe is stored, or to change the process recipe itself to the process recipe relating to this disclosure by operating the input / output device of the existing substrate processing apparatus.

[0097] Furthermore, this disclosure can be used, for example, in the wordline portion of NAND flash memory or DRAM having a three-dimensional structure.

[0098] Furthermore, the above embodiments and modifications describe examples of forming a film using a batch-type substrate processing apparatus that processes multiple wafers 200 at once. This disclosure is not limited to the above embodiments and can be suitably applied, for example, when forming a film using a single-wafer substrate processing apparatus that processes one or several wafers 200 at once. Furthermore, the above embodiments describe examples of forming a film using a substrate processing apparatus having a hot-wall type processing furnace. This disclosure is not limited to the above embodiments and can be suitably applied when forming a film using a substrate processing apparatus having a cold-wall type processing furnace.

[0099] In the above-described embodiments, an example was given in which the above-described processing sequence is performed in the same processing chamber of the same processing apparatus (in situ). This disclosure is not limited to the above-described embodiments, and for example, one step of the above-described processing sequence and another step may be performed in different processing chambers of different processing apparatuses (ex situ), or they may be performed in different processing chambers of the same processing apparatus.

[0100] Even when using these substrate processing devices, each process can be carried out using the same processing procedures and conditions as described above, and the same effects as described above can be obtained.

[0101] The above-described embodiments and modifications can be used in combination as appropriate. The processing procedure and processing conditions in this case can be the same as, for example, the processing procedure and processing conditions of the above-described embodiments and modifications.

Claims

1. a) A step of supplying a first gas containing the main elements and halogen elements that constitute the film to the substrate, b) A step of supplying a first reducing gas containing hydrogen to the substrate, c) A step of supplying a second reducing gas to the substrate, which contains hydrogen and is made of a different material from the first reducing gas; d) a) and b) are performed in parallel, and during this parallel process, the amount of the first reducing gas supplied is reduced compared to the amount supplied at the start of the supply of the first reducing gas. The steps of performing e) d) and c) a predetermined number of times to form the film on the substrate, A substrate processing method having the following characteristics.

2. d) The supply amount of the first reducing gas is gradually reduced. The substrate processing method according to claim 1.

3. d) The supply amount of the first reducing gas is continuously reduced. The substrate processing method according to claim 1.

4. Based on the temperature at which e) is performed, adjust the rate of decrease in the supply amount of the first reducing gas in d). The substrate processing method according to claim 1.

5. If the temperature is higher than a predetermined temperature, the rate of decrease is set to be greater than a predetermined value. The substrate processing method according to claim 4.

6. If the temperature is lower than a predetermined temperature, the rate of decrease is made smaller than a predetermined value. The substrate processing method according to claim 4.

7. The process further comprises the step of continuing to supply the first reducing gas after f) and d). The substrate processing method according to claim 1.

8. f) The supply amount of the first reducing gas is kept constant. The substrate processing method according to claim 7.

9. f) The supply amount of the first reducing gas is reduced as in d). The substrate processing method according to claim 7.

10. f) The supply amount of the first reducing gas is reduced by a second reduction rate that is greater than the reduction rate in d). The substrate processing method according to claim 9.

11. d) The supply amount of the first reducing gas is reduced relative to the supply amount of the first gas. The substrate processing method according to claim 1.

12. d) The substrate processing method according to claim 11, wherein the supply amount of the first reducing gas is relatively reduced by increasing the supply amount of the first gas.

13. d) In this case, the supply amount of the first reducing gas is increased after the start of supply of the first reducing gas. The substrate processing method according to claim 12.

14. d) The supply amount of the first gas is increased. The substrate processing method according to claim 1.

15. d) The supply amount of the first gas is increased in stages. The substrate processing method according to claim 12.

16. d) The supply amount of the first gas is continuously increased. The substrate processing method according to claim 12.

17. g) After d), a) and b) are performed in parallel separately from d), and during this parallel process, the amount of the first reducing gas supplied is reduced compared to the amount of the first reducing gas supplied in d), A substrate processing method according to claim 1, comprising:

18. a) A step of supplying a first gas containing the main elements and halogen elements that constitute the film to the substrate, b) A step of supplying a first reducing gas containing hydrogen to the substrate, c) A step of supplying a second reducing gas to the substrate, which contains hydrogen and is made of a different material from the first reducing gas; d) a) and b) are performed in parallel, and during this parallel process, the amount of the first reducing gas supplied is reduced compared to the amount supplied at the start of the supply of the first reducing gas. The steps of performing e) d) and c) a predetermined number of times to form the film on the substrate, A method for manufacturing a semiconductor device having [a certain feature].

19. a) A procedure for supplying a first gas containing the main elements and halogen elements that constitute the film to the substrate, b) A procedure for supplying a first reducing gas containing hydrogen to the substrate, c) A procedure for supplying a second reducing gas, which contains hydrogen and is made of a different material from the first reducing gas, to the substrate, d) a) and b) are performed in parallel, and during this parallel process, the supply amount of the first reducing gas is reduced compared to the amount at the start of the supply of the first reducing gas. A procedure to perform steps e) and c) a predetermined number of times to form the film on the substrate, A program that causes a circuit board processing unit to execute commands via a computer.

20. A first supply system that supplies a first gas containing the main elements and halogen elements that make up the film to the substrate, A second supply system that supplies a first reducing gas containing hydrogen to the substrate, A third supply system that supplies a second reducing gas, which contains hydrogen and is made of a different material from the first reducing gas, to the substrate, a) A process of supplying the first gas to the substrate, b) A process of supplying the first reducing gas to the substrate, c) A process of supplying the second reducing gas to the substrate, d) Perform a) and b) in parallel, and while they are in parallel, reduce the supply amount of the first reducing gas compared to the amount at the start of supply of the first reducing gas. A control unit configured to control the first supply system, the second supply system, and the third supply system so as to perform the process of forming the film on the substrate by performing steps e), d), and c) a predetermined number of times, A substrate processing apparatus having

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