Substrate treatment method, method for manufacturing semiconductor device, program, and substrate treatment device

Abstract

Provided is a technology which enables the formation of a film that has a low resistance.　The present invention comprises: (a) a step of supplying a first element-containing gas to a substrate; (b) a step of supplying a first reducing gas to the substrate; (c) a step of supplying a second reducing gas to the substrate; (d) a step of supplying an inert gas to the substrate; (e) a step of, during step (d), performing steps (a) and (b) at least partially in parallel and increasing the supply flow rate of the inert gas during step (b); and (f) a step of performing (e) and (c) a predetermined number of times to form, on the substrate, a film comprising the first element.

Description

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

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

[0002] For example, a low-resistance metal film is used as a word line in a three-dimensional structured 3D NAND flash memory or DRAM, and a barrier film may be formed between the metal film and an insulating film (see, for example, Patent Documents 1 and 2).

[0003] JP 2011-252221 A JP 2017-069407 A

[0004] The present disclosure provides a technique that allows for the formation of a low-resistance film.

[0005] According to one aspect of the present disclosure, there is provided a technique comprising: (a) a step of supplying a first element-containing gas to a substrate; (b) a step of supplying a first reducing gas to the substrate; (c) a step of supplying a second reducing gas to the substrate; (d) a step of supplying an inert gas to the substrate; (e) a step of performing (a) and (b) at least partially in parallel while performing (d), and increasing the supply flow rate of the inert gas when performing (b); and (f) a step of performing (e) and (c) a predetermined number of times to form a film containing the first element on the substrate.

[0006] According to the present disclosure, it is possible to form a low-resistance film.

[0007] Fig. 1 is a longitudinal sectional view showing an outline of a substrate processing apparatus. Fig. 2 is a schematic transverse sectional view taken along line A-A in Fig. 1. Fig. 3 is a schematic configuration diagram of a controller of the substrate processing apparatus, showing a control system of the controller in a block diagram. Fig. 4 is a diagram showing a substrate processing flow. Fig. 5 is a diagram showing a substrate processing sequence. Fig. 6 is a diagram showing a substrate processing sequence.

[0008] Hereinafter, one embodiment of the present disclosure will be described mainly with reference to Figures 1 to 6. Note that all drawings used in the following description are schematic, and the dimensional relationships, ratios, etc. of elements shown in the drawings do not necessarily match those of reality. Furthermore, the dimensional relationships, ratios, etc. of elements between multiple drawings do not necessarily match.

[0009] (1) Configuration of the Substrate Processing Apparatus The substrate processing apparatus 10 includes a processing furnace 202 provided with a heater 207 as a heating means (heating mechanism, heating system). The heater 207 has a cylindrical shape and is installed vertically by being supported by a heater base (not shown) as a holding plate.

[0010] An outer tube 203 (hereinafter referred to as outer tube 203) that constitutes a reaction vessel (processing vessel) is disposed inside the heater 207 concentrically with the heater 207. The outer tube 203 is made of, for example, quartz (SiO ２ The outer tube 203 is made of a heat-resistant material such as silicon carbide (SiC). The outer tube 203 is cylindrical with a closed upper end and an open lower end. A manifold 209 (hereinafter referred to as MF 209) is disposed concentrically with the outer tube 203 below the outer tube 203. The MF 209 is made of a metal material such as stainless steel (SUS). The MF 209 is cylindrical with open upper and lower ends. An O-ring 220a is provided as a sealing member between the upper end of the MF 209 and the outer tube 203. The MF 209 is supported on a heater base, allowing the outer tube 203 to be installed vertically.

[0011] An inner tube 204 (hereinafter referred to as the inner tube 204) that constitutes a reaction vessel is disposed inside the outer tube 203. The inner tube 204 is made of the heat-resistant material described above. The inner tube 204 is formed in a cylindrical shape with a closed upper end and an open lower end. The processing vessel (reaction vessel) is mainly constituted by the outer tube 203, the inner tube 204, and the MF 209. A processing chamber 201 is formed in the cylindrical hollow portion of the processing vessel (inside the inner tube 204). The processing chamber 201 is also referred to as the space in which the wafers 200 exist.

[0012] The processing chamber 201 is configured to accommodate wafers 200 as substrates arranged in multiple stages in the vertical direction in a horizontal position on a boat 217 (described later).

[0013] Nozzles 410, 420, and 430 are provided in the processing chamber 201 so as to penetrate the sidewall of the MF 209 and the inner pipe 204. Gas supply pipes 310, 320, and 330 are connected to the nozzles 410, 420, and 430, respectively. However, the processing furnace 202 of the present disclosure is not limited to the above-described configuration.

[0014] Mass flow controllers (MFCs) 312, 322, and 332, which are flow rate controllers (flow rate control parts), are respectively provided on the gas supply pipes 310, 320, and 330 in this order from the upstream side. Also, valves 314, 324, and 334, which are on-off valves, are respectively provided on the gas supply pipes 310, 320, and 330. Gas supply pipes 510, 520, and 530, which supply inert gas, are connected to the downstream sides of the valves 314, 324, and 334 of the gas supply pipes 310, 320, and 330, respectively. The gas supply pipes 510, 520, and 530, which are on-off valves, are respectively provided on the gas supply pipes 510, 520, and 530 in this order from the upstream side. MFCs 512, 522, and 532, which are flow rate controllers (flow rate control parts), and valves 514, 524, and 534, which are on-off valves, are respectively provided.

[0015] Nozzles 410, 420, 430 are respectively connected to the tip ends of the gas supply pipes 310, 320, 330. The nozzles 410, 420, 430 are configured as L-shaped nozzles, and their horizontal portions are provided so as to penetrate the side wall of the MF 209 and the inner pipe 204. The vertical portions of the nozzles 410, 420, 430 are arranged to protrude radially outward from the inner pipe 204 and are provided inside the channel-shaped (groove-shaped) pre-chamber 201a formed to extend vertically, and are provided upward (upward in the arrangement direction of the wafers 200) along the inner wall of the inner pipe 204 within the pre-chamber 201a.

[0016] The nozzles 410, 420, and 430 are provided extending from the lower region of the processing chamber 201 to the upper region thereof, with multiple gas supply holes 410a, 420a, and 430a respectively provided at positions facing the wafer 200. This allows processing gas to be supplied to the wafer 200 from the gas supply holes 410a, 420a, and 430a of the nozzles 410, 420, and 430. The gas supply holes 410a, 420a, and 430a are provided in multiple locations from the lower to the upper portion of the inner tube 204, each having the same opening area and arranged at the same opening pitch. However, the gas supply holes 410a, 420a, and 430a are not limited to the above configuration. For example, the opening area may gradually increase from the lower portion to the upper portion of the inner tube 204. This allows the flow rate of gas supplied from the gas supply holes 410a, 420a, and 430a to be more uniform.

[0017] The gas supply holes 410a, 420a, 430a of the nozzles 410, 420, 430 are provided at a plurality of positions at a height from the bottom to the top of the boat 217, which will be described later. Therefore, the process gas supplied into the process chamber 201 from the gas supply holes 410a, 420a, 430a of the nozzles 410, 420, 430 is supplied to the entire area of ​​the wafers 200 accommodated in the boat 217 from the bottom to the top. The nozzles 410, 420, 430 may be provided so as to extend from the lower region to the upper region of the process chamber 201, but are preferably provided so as to extend to near the ceiling of the boat 217.

[0018] A first element-containing gas containing a first element is supplied as a processing gas from the gas supply pipe 310 into the processing chamber 201 via the MFC 312 , the valve 314 , and the nozzle 410 .

[0019] A first reducing gas is supplied as a processing gas from the gas supply pipe 320 into the processing chamber 201 via the MFC 322 , the valve 324 , and the nozzle 420 .

[0020] A second reducing gas is supplied as a processing gas from the gas supply pipe 330 into the processing chamber 201 via the MFC 332 , the valve 334 , and the nozzle 430 .

[0021] Inert gas is supplied from gas supply pipes 510, 520, and 530 into the processing chamber 201 via MFCs 512, 522, and 532, valves 514, 524, and 534, and nozzles 410, 420, and 430, respectively.

[0022] The process gas supply unit is mainly composed of the gas supply pipes 310, 320, and 330, the MFCs 312, 322, and 332, the valves 314, 324, and 334, and the nozzles 410, 420, and 430, but the nozzles 410, 420, and 430 alone may be considered to be the process gas supply unit. The process gas supply unit may also be simply referred to as a gas supply unit. When a first-element-containing gas is flowed from the gas supply pipe 310, the first gas supply unit is mainly composed of the gas supply pipe 310, the MFC 312, and the valve 314, but the nozzle 410 may also be considered to be included in the first gas supply unit. Furthermore, when a first reducing gas is flowed from the gas supply pipe 320, the second gas supply unit is mainly composed of the gas supply pipe 320, the MFC 322, and the valve 324, but the nozzle 420 may also be considered to be included in the second gas supply unit. Furthermore, when the second reducing gas is flowed from the gas supply pipe 330, a third gas supply unit is mainly composed of the gas supply pipe 330, the MFC 332, and the valve 334, but the nozzle 430 may also be included in the third gas supply unit. Furthermore, a fourth gas supply unit is mainly composed of the gas supply pipes 510, 520, and 530, the MFCs 512, 522, and 532, and the valves 514, 524, and 534.

[0023] In the gas supply method of this embodiment, gas is transported via nozzles 410, 420, and 430 arranged in a vertically elongated annular space, a preliminary chamber 201a, defined by the inner wall of the inner pipe 204 and the ends of the multiple wafers 200. Gas is then ejected into the inner pipe 204 from multiple gas supply holes 410a, 420a, and 430a provided in the nozzles 410, 420, and 430 at positions facing the wafers. More specifically, gas is ejected in a direction parallel to the surface of the wafer 200 from the gas supply hole 410a of the nozzle 410, the gas supply hole 420a of the nozzle 420, and the gas supply hole 430a of the nozzle 430.

[0024] The exhaust hole (exhaust port) 204a is a through-hole formed in the sidewall of the inner tube 204 at a position facing the nozzles 410, 420, and 430, and is, for example, a slit-shaped through-hole that is elongated in the vertical direction. Gas is supplied into the process chamber 201 from the gas supply holes 410a, 420a, and 430a of the nozzles 410, 420, and 430 and flows over the surface of the wafer 200. The gas flows through the exhaust hole 204a into the exhaust path 206, which is formed by a gap between the inner tube 204 and the outer tube 203. The gas that has flowed into the exhaust path 206 then flows into the exhaust pipe 231 and is discharged to the outside of the process furnace 202.

[0025] The exhaust hole 204a is provided at a position facing the side surface of the plurality of wafers 200, and the gas supplied from the gas supply holes 410a, 420a, and 430a to the vicinity of the wafers 200 in the processing chamber 201 flows horizontally and then flows into the exhaust path 206 via the exhaust hole 204a. The exhaust hole 204a is not limited to being configured as a slit-shaped through-hole, and may be configured as a plurality of holes.

[0026] The MF 209 is provided with an exhaust pipe 231 for exhausting the atmosphere inside the processing chamber 201. The exhaust pipe 231 is connected, in order from upstream, to a pressure sensor 245 serving as a pressure detector (pressure detection unit) for detecting the pressure inside the processing chamber 201, an APC (Auto Pressure Controller) 243 serving as an exhaust valve, and a pump 246 serving as a vacuum exhaust device. The APC 243 can evacuate and stop the vacuum exhaust inside the processing chamber 201 by opening and closing a valve while the pump 246 is operating. Furthermore, the pressure inside the processing chamber 201 can be adjusted by adjusting the valve opening while the pump 246 is operating, thereby adjusting the exhaust conductance. The exhaust hole 204 a, the exhaust path 206, the exhaust pipe 231, the APC 243, and the pressure sensor 245 mainly constitute an exhaust unit. At least the exhaust port 204 a may be considered to be the exhaust unit. The pump 246 may also be considered to be included in the exhaust unit.

[0027] A seal cap 219 (hereinafter referred to as the cap 219) is provided below the MF 209 as a furnace port cover capable of airtightly closing the lower end opening of the MF 209. The cap 219 is configured to abut against the lower end of the MF 209 from below in the vertical direction. The cap 219 is made of a metal material such as SUS. The cap 219 is disk-shaped. An O-ring 220b is provided on the upper surface of the cap 219 as a sealing member that abuts against the lower end of the MF 209. A rotation mechanism 267 is installed on the opposite side of the cap 219 from the process chamber 201 to rotate a boat 217 that accommodates wafers 200. A rotation shaft 255 of the rotation mechanism 267 passes through the cap 219 and is connected to the boat 217. The rotation mechanism 267 is configured to rotate the boat 217 to rotate the wafers 200. The cap 219 is configured to be raised and lowered in the vertical direction by a boat elevator 115 (hereinafter referred to as the elevator 115) as an elevating mechanism installed vertically outside the outer tube 203. The elevator 115 is configured to be able to load and unload the boat 217 into and out of the processing chamber 201 by raising and lowering the cap 219. The elevator 115 is configured as a transfer device (transfer mechanism) that transfers the boat 217 and the wafers 200 accommodated in the boat 217 into and out of the processing chamber 201.

[0028] The boat 217, serving as a substrate support, is configured to accommodate multiple wafers 200, e.g., 1 to 200, arranged horizontally and with their centers aligned and spaced apart in the vertical direction. The boat 217 is made of a heat-resistant material such as quartz or SiC. A heat insulating plate 218, also made of a heat-resistant material such as quartz or SiC, is supported horizontally in multiple stages (not shown) at the bottom of the boat 217. This configuration makes it difficult for heat from the heater 207 to be transmitted to the cap 219. However, this embodiment is not limited to the above configuration. For example, instead of providing the heat insulating plate 218 at the bottom of the boat 217, a heat insulating cylinder configured as a cylindrical member made of a heat-resistant material such as quartz or SiC may be provided.

[0029] 2, a temperature sensor 263 serving as a temperature detector is installed inside the inner pipe 204, and the amount of power supplied to the heater 207 is adjusted based on temperature information detected by the temperature sensor 263, thereby achieving a desired temperature distribution inside the processing chamber 201. The temperature sensor 263 is configured in an L-shape similar to the nozzles 410, 420, and 430, and is provided along the inner wall of the inner pipe 204.

[0030] As shown in FIG. 3 , the controller 121, which is a control unit (control means), is configured as a computer including a CPU (Central Processing Unit) 121a, a RAM (Random Access Memory) 121b, a storage device 121c, and an I / O port 121d. The RAM 121b, the storage device 121c, and the I / O port 121d are configured to exchange data with the CPU 121a via an internal bus. An input / output device 122, such as a touch panel, is connected to the controller 121. The substrate processing apparatus may be configured with one or more control units. That is, control for performing the processing sequence described below may be performed using one control unit or multiple control units. Furthermore, the multiple control units may be configured as a control system connected to each other via a wired or wireless communication network, and control for performing the processing sequence described below may be performed by the entire control system. In this specification, when the term "control unit" is used, it may include one control unit, multiple control units, or a control system configured by multiple control units.

[0031] The storage device 121c is composed of, for example, a flash memory, an HDD (Hard Disk Drive), etc. The storage device 121c readably stores a control program for controlling the operation of the substrate processing apparatus, a process recipe (hereinafter referred to as a recipe) describing the procedures and conditions of a semiconductor device manufacturing method (described later), and the like. The recipe is a combination of steps in a semiconductor device manufacturing method (described later) that are executed by the controller 121 to obtain a predetermined result, and functions as a program. Hereinafter, the recipe, control program, etc. are collectively referred to simply as a program. In this disclosure, the term "program" may refer to a recipe alone, a control program alone, or a combination of a recipe and a control program. The RAM 121b is configured as a memory area for temporarily storing programs, data, etc. read by the CPU 121a.

[0032] The I / O port 121d is controllably connected to the above-mentioned MFCs 312, 322, 332, 512, 522, 532, valves 314, 324, 334, 514, 524, 534, pressure sensor 245, APC 243, pump 246, heater 207, temperature sensor 263, rotation mechanism 267, elevator 115, etc. Here, connection includes being electrically directly connected or indirectly connected, and being configured to be able to send and receive electrical signals directly or indirectly.

[0033] The CPU 121a is configured to read and execute a control program from the storage device 121c, and also to read a recipe or the like from the storage device 121c in response to an input of an operation command from the input / output device 122. The CPU 121a is configured to control, in accordance with the contents of the read recipe, the flow rate adjustment operation of various gases by the MFCs 312, 322, 332, 512, 522, and 532, the opening and closing operations of the valves 314, 324, 334, 514, 524, and 534, the opening and closing operation of the APC 243 and the pressure adjustment operation based on the pressure sensor 245 by the APC 243, the temperature adjustment operation of the heater 207 based on the temperature sensor 263, the start and stop of the pump 246, the rotation and rotation speed adjustment operation of the boat 217 by the rotation mechanism 267, the lifting and lowering operation of the boat 217 by the elevator 115, the accommodation operation of the wafers 200 in the boat 217, and the like.

[0034] The controller 121 can install the above-mentioned program stored in an external storage device 123 (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 a memory card) into 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 the present disclosure, the recording medium may include only the storage device 121c, only the external storage device 123, or both. The program may be provided to the computer using a communication means such as the Internet or a dedicated line, without using the external storage device 123.

[0035] (2) Substrate Processing Step As one step in the manufacturing process of a semiconductor device, an example of a step of forming a thin film on a wafer 200 will be described with reference to Figures 4 to 6. In the following description, the operation of each part constituting the substrate processing apparatus 100 is controlled by a controller 121.

[0036] The substrate processing process (semiconductor device manufacturing process) according to this embodiment includes: (a) a step of supplying a first element-containing gas to the wafer 200; (b) a step of supplying a first reducing gas to the wafer 200; (c) a step of supplying a second reducing gas to the wafer 200; (d) a step of supplying an inert gas to the wafer 200; (e) a step of performing (a) and (b) at least partially in parallel while performing (d), and increasing the supply flow rate of the inert gas when performing (b); and (f) a step of performing (e) and (c) a predetermined number of times to form a film containing the first element on the wafer 200.

[0037] In this specification, the term "wafer" may mean "the wafer itself" or "a laminate of a wafer and a predetermined layer, film, etc. formed on its surface." In this specification, the term "surface of a wafer" may mean "the surface of the wafer itself" or "the surface of a predetermined layer, film, etc. formed on the wafer." In this specification, the term "substrate" is synonymous with the term "wafer."

[0038] The flow and gas supply sequence of the device manufacturing method of the present disclosure will be described below with reference to Figures 4 to 6. Note that the horizontal axis of Figures 5 and 6 represents time, and the vertical axis represents the gas supply amount, valve opening, and pressure, respectively. The supply amount, valve opening, and pressure are expressed in arbitrary units.

[0039] 1, the boat 217 supporting the wafers 200 is lifted by the elevator 115 and loaded into the processing chamber 201. In this state, the cap 219 closes the lower end opening of the reaction tube 203 via the O-ring 220.

[0040] (Atmosphere Adjustment Step S302) The pump 246 evacuates the processing chamber 201 to a desired pressure (vacuum level). At this time, the pressure inside the processing chamber 201 is measured by the pressure sensor 245, and the APC 243 is feedback-controlled (pressure adjustment) based on the measured pressure information. The pump 246 is kept in a constantly operating state at least until the processing of the wafer 200 is completed. The processing chamber 201 is heated by the heater 207 to a desired temperature. At this time, the amount of power supplied to the heater 207 is feedback-controlled (temperature adjustment) based on temperature information detected by the temperature sensor 263 so that the processing chamber 201 has a desired temperature distribution. The heater 207 continues to heat the processing chamber 201 at least until the processing of the wafer 200 is completed. The temperature of the heater 207 is set to a temperature such that the temperature of the wafer 200 is within a range of, for example, 300 to 700°C.

[0041] (Film Forming Step S300) Next, the film forming step S300 is performed, which is composed of a first step S303, a second step S304, a third step S305, and a fourth step S306, as shown in FIGS.

[0042] [First Step S303] (Supply of First-Element-Containing Gas) The valve 314 is opened, and a first-element-containing gas, which is a source gas, is flowed into the gas supply pipe 310. The flow rate of the first-element-containing gas is adjusted by the MFC 312, and the first-element-containing gas is supplied into the processing chamber 201 through the gas supply holes 410a of the nozzle 410 and exhausted through the exhaust pipe 231. At this time, the first-element-containing gas is supplied to the wafer 200. Concurrently, the valve 514 is opened, and an inert gas is flowed into the gas supply pipe 510. The inert gas flowing through the gas supply pipe 510 has its flow rate adjusted by the MFC 512, and is supplied into the processing chamber 201 together with the first-element-containing gas and exhausted through the exhaust pipe 231. At this time, in order to prevent the first-element-containing gas from entering the nozzles 420 and 430, the valves 524 and 534 are opened, and the inert gas is flowed into the gas supply pipes 520 and 530. The inert gas is supplied into the processing chamber 201 through gas supply pipes 320 and 330 and nozzles 420 and 430 , and is exhausted from an exhaust pipe 231 .

[0043] Here, the first element is, for example, a metal element of Groups 3 to 13 of the periodic table, or a Group 14 element. Examples of this element include: Group 3 elements such as yttrium (Y) and lanthanum (La), Group 4 elements such as cerium (Ce), titanium (Ti), zirconium (Zr), and hafnium (Hf), Group 5 elements such as vanadium (V), niobium (Nb), and tantalum (Ta), Group 6 elements such as chromium (Cr), molybdenum (Mo), and tungsten (W), Group 8 elements such as ruthenium (Ru), Group 10 elements such as nickel (Ni), Group 12 elements such as zinc (Zn), Group 13 elements such as aluminum (Al), gallium (Ga), and indium (In), and Group 14 elements such as silicon (Si) and germanium (Ge).

[0044] The first element-containing gas is a gas containing the above-mentioned first element and a halogen element. Therefore, the first element-containing gas is preferably a gas containing the above-mentioned element and a halogen element. Examples of such gases include the following gases: titanium chloride (TiCl ４ ) gas, hafnium chloride (HfCl ４ ) gas, zirconium chloride (ZrCl ４ ) gas, tungsten hexafluoride (WF ６ ) gas, tungsten hexachloride (WCl ６ ) gas, tungsten pentachloride (WCl ５ ) gas, molybdenum pentachloride (MoCl ５ ) gas, molybdenum dichloride dioxide (MoO ２ Cl ２ ) gas, molybdenum oxide tetrachloride (MoOCl ４ ) gas, molybdenum hexafluoride (MoF ６ ) gas, molybdenum dioxide difluoride (MoO ２ F ２ ) gas, molybdenum tetrafluoride oxide (MoOF ４ ) gas, aluminum chloride (AlCl ３ ) gas, silicon tetrachloride (SiCl ４ ) gas, dichlorosilane (SiH ２ Cl ２ ) gas, hexachlorodisilane (Si ２ Cl６ ) gas, trichlorosilane (SiHCl ３ Preferably, a gas that reacts with a part of the first reducing gas and the second reducing gas described below to produce hydrogen halide is used.

[0045] The inert gas may be, for example, nitrogen (N ２ In addition to the inert gas, rare gases such as argon (Ar) gas, helium (He) gas, neon (Ne) gas, and xenon (Xe) gas can be used. One or more of these can be used as the inert gas.

[0046] At this time, the APC 243 is adjusted to set the pressure inside the processing chamber 201 to, for example, a pressure in the range of 1 to 3990 Pa. The supply flow rate of the first element-containing gas controlled by the MFC 312 is set to, for example, a flow rate in the range of 0.1 to 2.0 slm. The supply flow rates of the inert gases controlled by the MFCs 512, 522, and 532 are each set to, for example, a flow rate in the range of 0.1 to 20 slm.

[0047] At this time, the gases flowing into the processing chamber 201 are a first-element-containing gas and an inert gas. By supplying the first-element-containing gas, a first-element-containing layer is formed on the wafer 200 (the surface underlayer). The first-element-containing layer may be a first-element layer containing halogen, or may be an adsorption layer of molecules or a portion of the molecules of the first-element-containing gas, or may contain all of these. The time during which only the first-element-containing gas and the inert gas are supplied is a predetermined time T1. The supply of the inert gas, which is performed in parallel during the time T1, is called the (d1) process.

[0048] (Supply of First Reducing Gas) After a predetermined time (T1) has elapsed since the start of supply of the first-element-containing gas, for example, 0.01 to 5 seconds, the valve 324 is opened to allow a first reducing gas, which is a reducing gas, to flow into the gas supply pipe 320. The flow rate of the first reducing gas is adjusted by the MFC 322, and the first reducing gas is supplied into the processing chamber 201 through the gas supply hole 420a of the nozzle 420, and is exhausted from the exhaust pipe 231. At this time, the valve 524 is opened to allow an inert gas to flow into the gas supply pipe 520. The inert gas flowing through the gas supply pipe 520 has its flow rate adjusted by the MFC 522, and is supplied into the processing chamber 201 together with the first reducing gas, and is exhausted from the exhaust pipe 231. At this time, in order to prevent the first-element-containing gas and the first reducing gas from entering the nozzle 430, the valve 534 is opened to allow an inert gas to flow into the gas supply pipe 530. The inert gas is supplied into the processing chamber 201 via the gas supply pipe 330 and the nozzle 430 and exhausted through the exhaust pipe 231. At this time, the first element-containing gas, the first reducing gas, and the inert gas are simultaneously supplied to the wafers 200. That is, there is a period (timing) during which at least the first element-containing gas and the first reducing gas are supplied in parallel. This period is also referred to as the first process. The period during which the first process is performed is also referred to as the first timing. The time during which the first element-containing gas and the first reducing gas are simultaneously supplied is designated S1. Preferably, the S1 time is greater than the T1 time. This configuration can suppress the adsorption of hydrogen halide onto the surface of the wafers 200 and enhance the removal effect of hydrogen halide in the processing chamber 201. Furthermore, by setting the temperature of the wafers 200 (in the processing chamber 201) at a temperature at which the first reducing gas can be decomposed (a decomposable atmosphere), the removal effect of hydrogen halide can be enhanced. Here, the temperature at which the first reducing gas can be decomposed is, for example, 400 to 700°C.

[0049] Here, the hydrogen halide refers to at least one of hydrogen chloride (HCl), hydrogen fluoride (HF), hydrogen iodide (HI), hydrogen bromide (HBr), etc. The hydrogen halide is a by-product generated by a reaction between a halogen contained in the first element-containing gas and a hydrogen-element-containing group present on the wafer 200. When the first element-containing gas is a gas containing chlorine (Cl) and at least one of the first reducing gas and the second reducing gas is a gas containing hydrogen, HCl is generated as the hydrogen halide.

[0050] At this time, the APC 243 is adjusted to set the pressure in the process chamber 201 to, for example, 130 to 3990 Pa, preferably 500 to 2660 Pa, and more preferably 600 to 1500 Pa. If the pressure in the process chamber 201 is lower than 130 Pa, the second element contained in the first reducing gas may penetrate into the first-element-containing layer, resulting in a film with a high content of the second element, and thus resulting in a film containing the second element in addition to the first element. Similarly, if the pressure in the process chamber 201 is higher than 3990 Pa, the second element contained in the first reducing gas may penetrate into the first-element-containing layer, resulting in a film with a high content of the second element. Thus, if the pressure in the process chamber 201 is too low or too high, the elemental composition of the film formed will change. The supply flow rate of the first reducing gas controlled by the MFC 322 is set to be equal to or higher than the flow rate of the first-element-containing gas. The flow rate of the inert gas controlled by the MFCs 512, 522, and 532 is, for example, 0.01 to 20 slm, preferably 0.1 to 10 slm, and more preferably 0.1 to 1 slm.

[0051] Here, if the temperature inside the process chamber 201 or the temperature of the wafer 200 is high, the first reducing gas decomposes, causing a problem in that the second element contained in the first reducing gas is incorporated into the film formed on the wafer 200. Here, a high temperature refers to, for example, 400 to 700°C. This decomposition reaction of the first reducing gas can be suppressed by increasing the supply rate of the inert gas supplied when the first reducing gas is supplied. As shown in FIGS. 5 and 6, it is preferable to increase the supply rate of the inert gas when the first reducing gas is supplied. The supply rate of the inert gas is adjusted, for example, in the range of 0.1 to 20 slm, preferably 1 to 10 slm, using the MFCs 512, 522, 532, etc.

[0052] After a predetermined time has elapsed since the start of the supply of the first-element-containing gas, for example, 0.01 to 10 seconds, the valve 314 of the gas supply pipe 310 is closed to stop the supply of the first-element-containing gas. In other words, the time (T1+S1) during which the first-element-containing gas is supplied to the wafer 200 is, for example, within a range of 0.01 to 10 seconds. The time (step) during which the first-element-containing gas is supplied to the wafer is shown as step (a) in FIGS. 5 and 6 . After the supply of the first-element-containing gas is stopped, the first reducing gas and the inert gas are supplied to the wafer 200 for a predetermined time S2. This process during which the first reducing gas is supplied to the wafer 200 without the first-element-containing gas being supplied to the wafer 200 is referred to as the second process. The period during which the second process is being performed is also referred to as the second timing. The time (S1+S2) during which the first reducing gas is supplied to the wafer 200 is shown as step (b) in FIGS. 5 and 6 . Furthermore, the inert gas continues to be supplied from the gas supply pipes 510 and 530 to the processing chamber 201 via the gas supply pipes 310 and 330 and the nozzles 410 and 430. This prevents the first reducing gas from entering the nozzles 410 and 430 from the processing chamber 201. In parallel with the process (b) shown in FIGS. 5 and 6 , the process (d2) increases the supply amount of the inert gas from the amount supplied in the process (d1) to a value greater than the amount supplied in the process (d1). If the supply flow rate of the inert gas in the process (d1) is defined as the first supply flow rate and the supply flow rate of the inert gas in the process (d2) is defined as the second supply flow rate, the first supply flow rate < the second supply flow rate. This relationship prevents the molecules of the first element-containing gas from being impeded from being supplied to the wafers 200 in the process (d1). Furthermore, the decomposition reaction of the first reducing gas can be suppressed in the process (d2).

[0053] As the first reducing gas, for example, a hydrogen-containing gas containing hydrogen (H) can be used. ２ Gas, deuterium (D ２ ) gas, which is composed of hydrogen element alone. ４ ) gas, disilane (Si ２ H ６ ) gas, trisilane (Si ３ H ８Gases containing H and silicon elements (silicon hydride gases), such as monoborane (BH ３ ) gas, diborane (B ２ H ６ ) gas, Triborane (B ３ H ８ A gas containing H and boron (boron hydride gas), such as phosphine (PH ３ ) gas, activated hydrogen-containing gas, trisdimethylaminosilane (SiH[N(CH ３ ) ２ ] ３ ) gas, etc. can be used. Preferably, a gas that can be decomposed in the process chamber 201 is used. For example, silicon hydride gas is used. Also preferably, a gas of a substance different from the second reducing gas described below is selected.

[0054] [Second Step S304] (Residual Gas Removal) After a predetermined time has elapsed since the start of the supply of the first reducing gas, e.g., 0.01 to 60 seconds, preferably 0.1 to 30 seconds, and more preferably 1 to 20 seconds, the valve 324 is closed to stop the supply of the first reducing gas. That is, the time for supplying the first reducing gas to the wafer 200 is, for example, 0.01 to 60 seconds, preferably 0.1 to 30 seconds, and more preferably 1 to 20 seconds. If the time for supplying the first reducing gas to the wafer 200 is shorter than 0.01 seconds, the hydrogen halide, which is a growth inhibitor, may not be sufficiently reduced by the first reducing gas and may remain in the Ti-containing layer. If the time for supplying the first reducing gas to the wafer 200 is longer than 60 seconds, the second element contained in the first reducing gas may penetrate into the first-element-containing layer, resulting in a film with a high second-element content. Preferably, the supply time of the first reducing gas is configured to be longer than the supply time of the first-element-containing gas. Furthermore, the supply time (S2) of the first reducing gas after the supply of the first-element-containing gas is stopped is configured to be equal to or longer than S1. That is, there is a relationship of S2≧S1. This configuration can enhance the reduction of halogen components in the first-element-containing layer and the removal effect of hydrogen halide in the processing chamber 201.

[0055] Next, simultaneously with stopping the supply of the first reducing gas, the supply rate of the inert gas into the process chamber 201 is increased from the nozzles 410, 420, and 430. Furthermore, the APC 243 of the exhaust pipe 231 is left open, and the atmosphere in the process chamber 201 is exhausted by the pump 246 to remove the first-element-containing gas and the first reducing gas remaining in the process chamber 201, either unreacted or having contributed to the formation of the first-element-containing layer. At this time, the valves 514, 524, and 534 are left open, and the supply of the inert gas into the process chamber 201 is maintained. The inert gas acts as a purge gas, and can enhance the effect of removing the first-element-containing gas and the first reducing gas remaining in the process chamber 201, either unreacted or having contributed to the formation of the first-element-containing layer. Here, hydrogen halide, which is a growth inhibitor, reacts with the first reducing gas to be generated and is discharged from the process chamber 201 as a reaction by-product. The first reducing gas remaining in the processing chamber 201 is diluted with the inert gas and exhausted to the exhaust pipe 231. As shown in Figures 5 and 6, the inert gas supplying step performed after the supply of the first reducing gas is stopped is step (g).

[0056] At this time, the MFCs 512, 522, and 532 are controlled so that the total flow rate of the inert gas from the nozzles 410, 420, and 430 is 10 to 60 slm. Preferably, it is set to 60 slm. The APC opening is set to 0% to 70%. At this time, the valve opening of the APC 243 and / or the flow rates of the MFCs 512, 522, and 532 are controlled so that the pressure Pa2 inside the processing chamber 201 is equal to the pressure Pa1 during the supply of the first reducing gas. The pressure Pa2 is, for example, 1 Torr to 20 Torr, and specifically, is set to 10 Torr. In this way, the pressure Pa2 inside the processing chamber 201 is controlled by adjusting the pressure Pa2 of SiH ４ The process of maintaining the pressure substantially equal to the pressure Pa1 during gas supply is called a third process. The period during which the third process is performed is also called a third timing.

[0057] (Pressures Pa1 and Pa2) Here, the pressure ratio between pressures Pa1 and Pa2 is affected by the dimensions of each part of the substrate processing apparatus 10, the number of wafers 200, the surface area of ​​the wafers 200, etc. Examples of the dimensions of each part of the substrate processing apparatus 10 include the volume of the processing chamber 201, the length of the nozzles 410, 420, and 430, the length of the gas supply pipes 310, 320, and 330, the volume of the exhaust pipe 231, and the position and diameter of the APC 243. The relationship between the pressure ratios Pa1 and Pa2 may be, for example, Pa1 = Pa2 × ±50%. Preferably, the valve openings of the MFCs 512, 522, and 532 and the APC 243 are controlled to satisfy the relationship Pa1 = Pa2 × ±10%. The pressure of Pa2 can be controlled by either or both of the flow rate of each of the MFCs 512, 522, and 532 and the valve opening degree of the APC 243.

[0058] (Inert Gas Flow Rate) Here, the flow rate of the inert gas supplied to each nozzle 410, 420, 430 is controlled by each MFC 512, 522, 532. The flow rates of the inert gas supplied to each nozzle 410, 420, 430 may be controlled to be equal to each other, but preferably, as shown in Fig. 8, the flow rate of the inert gas supplied to the nozzle 420 that has been supplying the first reducing gas is configured to be greater than the flow rates of the inert gas supplied to the other nozzles 410, 430. By configuring in this manner, the efficiency of discharging the first reducing gas present in the nozzle 420 can be improved.

[0059] (Inert Gas Supply Time Pt1) Next, the inert gas supply time Pt1 will be described with reference to FIG. 5 . The time Pt1 during which the inert gas is supplied to maintain the pressure Pa2 is set to be at least equal to the time S2 during which the first reducing gas is supplied after the supply of the first element-containing gas is stopped. By setting the time Pt1 in this manner, the concentration of the first reducing gas and by-products in the processing chamber 201 can be reduced. Note that Pt1 may be set to a time Pt2 equivalent to the subsequent purge process S306. The relationship is Pt1≦Pt2. While it may be set to be longer than this, the overall time of the film formation process S300 would be longer, which would affect the manufacturing throughput of the semiconductor manufacturing equipment, and therefore, the time Pt1 is set to satisfy this relationship.

[0060] (Improvement of Exhaust Efficiency) Next, an improvement in the exhaust efficiency of residual gases and reaction by-products above the wafer 200 (in the process chamber 201) will be described. While FIG. 5 illustrates a process in which the inert gas flow rate is increased simultaneously with the stopping of the supply of the first reducing gas, the present invention is not limited to this. Alternatively, a gas supply sequence such as that shown in FIG. 6 may be configured. In the second step S304, after the step (g1) of increasing the supply rate of the inert gas and performing exhaust for a predetermined time, the aperture of the APC 243 is increased from the first aperture to a second aperture. By increasing the aperture of the APC 243, the pressure in the process chamber 201 is lowered and exhaust is performed (g2). In FIG. 6, as an example, the aperture of the APC 243 is set to a second aperture. The second aperture is, for example, 100% (full open). While an example in which the second aperture is set to 100% is illustrated here, the present invention is not limited thereto and may be any aperture that can reduce the pressure. In step S304, the opening degree may be set so that the pressure inside the process chamber 201 decreases after the supply amount of inert gas is increased. For example, the opening degree is greater than 50% and less than 100%. By increasing the opening degree of the exhaust valve 243 and exhausting the atmosphere above the wafer 200 at a second pressure Pa2 that is lower than the first pressure Pa1, the efficiency of exhausting residual gas and reaction by-products can be improved. Note that "fully open" does not necessarily mean that the valve opening degree is 100%; an error of -10% may be acceptable. The error is preferably -5%. Note that a valve opening degree that includes such an error is also referred to as "approximately fully open" or "substantially fully open."

[0061] [Third Step S305] (Second Reducing Gas Supply) After removing residual gas from the processing chamber 201, the valve 334 is opened to allow a second reducing gas to flow as a reactive gas into the gas supply pipe 330. The flow rate of the second reducing gas is adjusted by the MFC 332, and the second reducing gas is supplied into the processing chamber 201 through the gas supply holes 430a of the nozzle 430 and exhausted through the exhaust pipe 231. At this time, the second reducing gas is supplied to the wafer 200. At this time, the valve 534 is opened to allow an inert gas to flow into the gas supply pipe 530. The flow rate of the inert gas flowing through the gas supply pipe 530 is adjusted by the MFC 532. The inert gas is supplied into the processing chamber 201 together with the second reducing gas and exhausted through the exhaust pipe 231. At this time, in order to prevent the second reducing gas from entering the nozzles 410 and 420, the valves 514 and 524 are opened to allow the inert gas to flow into the gas supply pipes 510 and 520. The inert gas is supplied into the processing chamber 201 through gas supply pipes 310 and 320 and nozzles 410 and 420 , and is exhausted from an exhaust pipe 231 .

[0062] At this time, the APC 243 is adjusted to set the pressure inside the processing chamber 201 to, for example, a pressure in the range of 1 to 3990 Pa. The supply flow rate of the second reducing gas controlled by the MFC 332 is set to, for example, a flow rate in the range of 0.1 to 30 slm. The supply flow rates of the inert gases controlled by the MFCs 512, 522, and 532 are each set to, for example, a flow rate in the range of 0.1 to 30 slm. The time for which the second reducing gas is supplied to the wafers 200 is set to, for example, a time in the range of 0.01 to 30 seconds. The temperature of the heater 207 at this time is set to the same temperature as in the step of supplying the first-element-containing gas.

[0063] At this time, the gases flowing into the process chamber 201 are a second reducing gas and an inert gas. The second reducing gas undergoes a substitution reaction with at least a portion of the first-element-containing layer formed on the wafer 200 in the first step S303. During the substitution reaction, the first element contained in the first-element-containing layer and the third element contained in the second reducing gas combine to form a layer containing the first element and the third element on the wafer 200, the layer containing the first element and the third element and substantially not containing the second element.

[0064] The second reducing gas may be a H-containing gas containing hydrogen. Preferably, ammonia (NH ３ ) gas, hydrazine (N ２ H ４ ) gas, diazene (N ２ H ２ ) gas, deuterium oxide (ND ３ ) gas, or a hydride containing nitrogen (N) as a third element is used.

[0065] [Fourth Step S306] (Removal of Residual Gas) After forming the layer containing the first and second elements, the valve 334 is closed to stop the supply of the second reducing gas. Then, using the same process procedure as in the second step described above, any unreacted second reducing gas or reaction by-products remaining in the process chamber 201 after contributing to the formation of the layer containing the first and third elements are removed from the process chamber 201. Note that the valve opening of the APC 243 here is set to approximately full open (approximately 100%), and the total flow rate of the inert gas is set to 1 slm to 100 slm. Specifically, the MFCs and the APC 243 are controlled so that the pressure is 180 Pa at 60 slm. The pressure Pa4 here is sufficiently lower than the pressure Pa2 described above and the pressure Pa3 in the third step S305, with the relationships Pa4<Pa2 and Pa4<Pa3. By configuring in this way, it is possible to exhaust by-products generated in one cycle, thereby reducing the influence on the next cycle.

[0066] (Determination step) A predetermined film of a predetermined thickness is formed on the wafer 200 by performing a cycle of the first step S303 to the fourth step S306 in order a predetermined number of times (n times, where n is an integer of 1 or 2 or more).

[0067] When forming a TiN film on the wafer 200, the following gases can be used: First element-containing gas: A gas containing a metal element (e.g., Ti) and a halogen element (e.g., Cl) as the first element. First reducing gas: A gas containing Si and H as the second element, such as silicon hydride gas. Second reducing gas: A gas containing N and H as the third element. When these gases are used, the hydrogen halide is HCl.

[0068] Furthermore, in the present disclosure, "TiN film containing no Si atoms" refers to a TiN film containing absolutely no Si atoms, as well as a TiN film containing almost no Si atoms or substantially no Si atoms, and also includes a TiN film having an extremely low Si content, for example, a TiN film having an Si content of about 4%, preferably 4% or less.

[0069] (Atmosphere Adjusting Step S307) An inert gas is supplied into the processing chamber 201 from each of the gas supply pipes 510, 520, and 530, and is exhausted from the exhaust pipe 231. The inert gas acts as a purge gas, thereby purging the processing chamber 201 with the inert gas, and gases and by-products remaining in the processing chamber 201 are removed from the processing chamber 201. Thereafter, the atmosphere in the processing chamber 201 is replaced with the inert gas, and the pressure in the processing chamber 201 is returned to normal pressure (atmospheric pressure).

[0070] (Substrate Unloading Process S308) Thereafter, the cap 219 is lowered by the elevator 115 to open the lower end of the reaction tube 203. Then, the processed wafers 200 supported by the boat 217 are unloaded from the lower end of the reaction tube 203 to the outside of the reaction tube 203. Thereafter, the processed wafers 200 are removed from the boat 217.

[0071] (3) Effects of the Embodiment According to the present embodiment, one or more of the following effects can be obtained. (a) HCl, which is generated during film formation and reduces the film formation rate, can be efficiently discharged, thereby increasing the film formation rate. (b) The concentration of the second element in the film can be reduced. (c) Resistivity can be reduced. (d) Oxidation resistance can be improved. (e) The first reducing gas in the processing chamber can be diluted with an inert gas and discharged from the processing chamber to the exhaust section, preventing gas with a high concentration of the first reducing gas from being momentarily discharged to the exhaust section. This can suppress unexpected reactions of the first reducing gas downstream of the pump. (f) Decomposition of the first reducing gas on the wafer 200 (in the processing chamber 201) can be suppressed. (g) Decomposition of the first reducing gas can be suppressed even when the wafer 200 (in the processing chamber 201) is at a high temperature.

[0072] Furthermore, in the above description, the first reducing gas and the second reducing gas are each described as being one type of gas. However, this is not limiting, and two or more types of reducing gases (hydrogen-containing gases) may be used as each of the first reducing gas and the second reducing gas. For example, a gas composed of simple hydrogen and a silicon hydride gas may be used as the first reducing gas. By supplying a gas composed of simple hydrogen in addition to the silicon hydride gas as the first reducing gas, the reaction of the silicon hydride gas decomposing into silicon and hydrogen can be suppressed. That is, in addition to the above-mentioned effects, the decomposition reaction of the silicon hydride gas can be further suppressed.

[0073] In addition, in the above description, a configuration has been described in which the first element-containing gas and the first reducing gas are supplied into the processing chamber 201 from the nozzles 410 and 420, respectively, but this is not limiting, and the gases may be premixed and supplied from a single nozzle.

[0074] Although the above description has been given of a configuration in which the supply of the first reducing gas is started after the supply of the first element-containing gas is started, the present disclosure is not limited thereto. Alternatively, the supply of the first reducing gas may be started simultaneously with the start of the supply of the first element-containing gas. Alternatively, the supply of the first reducing gas may be stopped simultaneously with the stop of the supply of the first element-containing gas. By doing so, at least one of the effects described in the present disclosure can be obtained.

[0075] In the above description, the substrate processing sequence is described as being performed consecutively (in-situ) in the same processing chamber (processing vessel). However, the present disclosure is not limited to the above embodiment, and each step of the substrate processing sequence may be performed in a separate processing chamber (processing vessel) (ex-situ).

[0076] In the above-described embodiment, an example of forming a film using a batch-type substrate processing apparatus that processes multiple substrates at a time has been described. The present disclosure is not limited to the above-described embodiment and can be suitably applied, for example, to a case where a film is formed using a single-wafer substrate processing apparatus that processes one or several substrates at a time. In the above-described embodiment, an example of forming a film using a substrate processing apparatus having a hot-wall processing furnace has been described. The present disclosure is not limited to the above-described embodiment and can be suitably applied to a case where a film is formed using a substrate processing apparatus having a cold-wall processing furnace.

[0077] Although the above example shows the use of a wafer as a semiconductor substrate, the present invention can also be applied to substrate processing using substrates made of other materials, such as ceramic substrates and glass substrates.

[0078] The above-described embodiments and modifications may be used in combination as appropriate. The processing procedures and processing conditions in such a case may be the same as those of the above-described embodiments and modifications, for example.

[0079] Although the embodiments and modifications of the present disclosure have been specifically described above, the embodiments and modifications of the present disclosure are not limited to the above-described embodiments and modifications, and various modifications are possible without departing from the spirit of the present disclosure.

Claims

1. A substrate processing method comprising the steps of: (a) supplying a first element-containing gas to a substrate; (b) supplying a first reducing gas to the substrate; (c) supplying a second reducing gas to the substrate; (d) supplying an inert gas to the substrate; (e) performing (a) and (b) at least partially in parallel while performing (d), and increasing the supply flow rate of the inert gas when performing (b) compared to before (b) is started; and (f) performing (e) and (c) a predetermined number of times to form a film containing the first element on the substrate.

2. In (e), (b) is started after (a) and (d) are started.

3. The substrate processing method according to claim 1, 3. The substrate processing method of claim 2, wherein in (e), the inert gas is supplied at a first supply flow rate, and then, when performing (b), the supply flow rate of the inert gas is increased to a second supply flow rate that is greater than the first supply flow rate.

4. The substrate processing method according to claim 1, further comprising the step of supplying the inert gas between (e) and (c) of (g) and (f).

5. The substrate processing method according to claim 3, further comprising the step of supplying the inert gas between (e) and (c) of (g) and (f).

6. The substrate processing method according to claim 5, wherein in (g), the supply flow rate of the inert gas is set to a third supply flow rate that is greater than the second supply flow rate.

7. The substrate processing method according to claim 1, wherein in (e), the supply flow rate of the inert gas is set to be greater than the supply flow rate of the first reducing gas.

8. The substrate processing method according to claim 6, wherein the third supply flow rate is greater than the supply flow rate of the first reducing gas.

9. (g) is a substrate processing method as described in claim 4, comprising a period in which an exhaust valve provided in a path for exhausting the atmosphere of the space in which the substrate exists is opened at a first opening degree, and a period in which the exhaust valve is opened at a second opening degree that is larger than the first opening degree.

10. The substrate processing method according to claim 4, wherein (g) includes a period in which the pressure of the space in which the substrate exists is exhausted at a first pressure, and a period in which the pressure is exhausted at a second pressure which is lower than the first pressure.

11. The substrate processing method according to claim 1, further comprising the steps of continuing the supply of the first reducing gas and the supply of the inert gas after (h) and (e), wherein the pressure of the space in which the substrate exists is maintained between (e) and (h).

12. The substrate processing method according to claim 1, wherein (f) is performed in an atmosphere in which the first reducing gas can be decomposed.

13. The substrate processing method according to claim 1, wherein the first element-containing gas is a gas containing the first element and a halogen element.

14. The substrate processing method according to claim 1, wherein the first reducing gas is a gas containing hydrogen and is a gas of a different substance from the second reducing gas.

15. The substrate processing method according to claim 14, wherein the second reducing gas is a gas containing hydrogen.

16. The substrate processing method according to claim 13, wherein the first element is a metal element, the first reducing gas contains a Group 14 element, and the second reducing gas is a gas containing nitrogen.

17. A method for manufacturing a semiconductor device comprising the steps of: (a) supplying a first element-containing gas to a substrate; (b) supplying a first reducing gas to the substrate; (c) supplying a second reducing gas to the substrate; (d) supplying an inert gas to the substrate; (e) performing (a) and (b) at least partially in parallel while performing (d), and increasing the supply flow rate of the inert gas when performing (b); and (f) performing (e) and (c) a predetermined number of times to form a film containing the first element on the substrate.

18. A program for causing a substrate processing apparatus to execute, by a computer, the following steps: (a) supplying a first element-containing gas to the substrate; (b) supplying a first reducing gas to the substrate; (c) supplying a second reducing gas to the substrate; (d) supplying an inert gas to the substrate; (e) performing (a) and (b) at least partially in parallel while performing (d), and increasing the supply flow rate of the inert gas when performing (b); and (f) performing (e) and (c) a predetermined number of times to form a film containing the first element on the substrate.

19. A substrate processing apparatus comprising: a first gas supply unit for supplying a first element-containing gas to a substrate; a second gas supply unit for supplying a first reducing gas to the substrate; a third gas supply unit for supplying a second reducing gas to the substrate; a fourth gas supply unit for supplying an inert gas to the substrate; and a control unit configured to be capable of controlling the first supply unit, the second supply unit, the third supply unit, and the fourth supply unit to perform the following processes: (a) a process of supplying a first element-containing gas to the substrate; (b) a process of supplying a first reducing gas to the substrate; (c) a process of supplying a second reducing gas to the substrate; (d) a process of supplying an inert gas to the substrate; (e) a process of performing (a) and (b) at least partially in parallel while performing (d), and increasing a supply flow rate of the inert gas when performing (b); and (f) a process of performing (e) and (c) a predetermined number of times to form a film containing the first element on the substrate.

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