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

Abstract

The present invention provides a technology capable of suppressing variations in substrate processing.　The present invention includes: a first step including a step (a1) for storing a processing gas in a storage part; and a second step for cyclically performing a step (b1) and a step (b2) in the stated order a predetermined number of times after the first step, the step (b1) being a step for storing the processing gas in the storage part and the step (b2) being a step for supplying at least a part of the processing gas in the storage part to a substrate placed in a processing chamber.

Description

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

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

[0002] A substrate may be processed by repeating a process of storing a process gas in a storage section and a process of supplying the process gas stored in the storage section to the substrate a predetermined number of times (see, for example, Patent Document 1).

[0003] Japanese Patent Application Laid-Open No. 2020-136301

[0004] The present disclosure provides a technique that can suppress variations in substrate processing.

[0005] According to one aspect of the present disclosure, there is provided a technology including: a first step including: (a1) a step of storing a process gas in a storage section; and a second step of performing a cycle of sequentially performing the steps of: (b1) a step of storing the process gas in the storage section; and (b2) a step of supplying at least a portion of the process gas in the storage section to a substrate placed in a processing chamber, a predetermined number of times after the first step.

[0006] According to the present disclosure, it is possible to suppress variations in substrate processing.

[0007] FIG. 1 is a longitudinal cross-sectional view showing an outline of a substrate processing apparatus according to an embodiment of the present disclosure. FIG. 2A is a diagram showing a first process gas supply system according to an embodiment of the present disclosure, FIG. 2B is a diagram showing a second process gas supply system according to an embodiment of the present disclosure, and FIG. 2C is a diagram showing an exhaust system according to an embodiment of the present disclosure. FIG. 3 is a schematic configuration diagram of a controller of a substrate processing apparatus according to an embodiment of the present disclosure, and is a block diagram showing a control system of the controller. FIG. 4 is a diagram showing a schematic change in the amount of a first process gas in a tank according to an embodiment of the present disclosure. FIG. 5 is a diagram showing a schematic change in the amount of a first process gas in a tank according to a comparative example. FIG. 6A is a flowchart of a substrate processing process according to an embodiment of the present disclosure. FIG. 6B is a flowchart of a preparation process according to an embodiment of the present disclosure. FIG. 6C is a flowchart of a film processing process according to an embodiment of the present disclosure. FIG. 6D is a flowchart of a first process gas supply process according to an embodiment of the present disclosure. FIG. 7 is a flowchart of a preparation process according to a first modification of the present disclosure. FIG. 7 is a flowchart of a preparation process in the second modification of the present disclosure.

[0008] Hereinafter, one embodiment of the present disclosure will be described mainly with reference to Figures 1 to 8. 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 configuration of the substrate processing apparatus 10 will be described with reference to FIG.

[0010] The substrate processing apparatus 10 includes a reaction tube storage chamber 206b. The reaction tube storage chamber 206b contains a reaction tube 210, a heater 211 as a heating unit (furnace body) installed around the reaction tube 210, a gas supply structure 212 as a gas supply unit, and a gas exhaust structure 213 as a gas exhaust unit. The gas supply unit may include an upstream flow rectifier 214 and nozzles 223 and 224, which will be described later. The gas exhaust unit may include a downstream flow rectifier 215, which will be described later. A section of the reaction tube 210 where the substrate S is processed is called a processing chamber 201. The processing chamber 201 can also be called a processing space in which the substrate S is placed.

[0011] The gas supplied from the gas supply structure 212 into the reaction tube 210 moves horizontally relative to the substrate S and is exhausted from the gas exhaust structure 213. An upstream rectifier 214 is provided between the reaction tube 210 and the gas supply structure 212. A downstream rectifier 215 is provided between the reaction tube 210 and the gas exhaust structure 213. The lower end of the reaction tube 210 is supported by a manifold 216. Heat from the heater 211 heats the substrate S and the gas in the processing chamber 201.

[0012] The gas supply structure 212 is connected to a gas supply pipe 251 and a gas supply pipe 261 and includes a distribution unit 225 that distributes the gas supplied from each gas supply pipe. A plurality of nozzles 223 and 224 are provided downstream of the distribution unit 225. In this embodiment, the gas supply pipe 251 and the gas supply pipe 261 are collectively referred to as gas supply pipes 221. Each nozzle is also referred to as a gas discharge unit. The distribution unit 225 is configured to supply gas from the gas supply pipe 251 to the nozzle 223 and from the gas supply pipe 261 to the nozzle 224, respectively. The upstream rectification unit 214 includes a housing 227 and a partition plate 226. The nozzles 223 and 224 are provided between the partition plates 226 and between the partition plate 226 and the housing 227. The downstream rectification unit 215 includes a housing 231 and a partition plate 232. The gas exhaust structure 213 is mainly composed of a housing 241 , an exhaust pipe connection part 242 , and an exhaust hole 244 .

[0013] A transfer chamber 217 is formed at the bottom of the reaction tube 210. Inside the transfer chamber 217, a transfer robot (not shown) transfers substrates S between the inside and outside of the transfer chamber 217 through a substrate loading port (not shown), and the substrates S are loaded onto and unloaded from a substrate support 300 (hereinafter sometimes simply referred to as a boat) inside the transfer chamber 217.

[0014] The vertical drive mechanism 400 moves the substrate support 300 and the partition plate support 310 up and down between the reaction tube 210 and the transfer chamber 217. FIG. 1 shows the substrate support 300 and the partition plate support 310 raised by the vertical drive mechanism 400 and stored in the reaction tube 210. The vertical drive mechanism 400 includes a rotation drive mechanism 430 that rotates the substrate support 300 and the partition plate support 310 together, and a boat up and down mechanism 420 that drives the substrate support 300 up and down relative to the partition plate support 310. The rotation drive mechanism 430 and the boat up and down mechanism 420 are fixed to a base flange 401 serving as a lid, which is supported by a side plate 403 on a base plate 402. An O-ring 446 for vacuum sealing is installed on the upper surface of the base flange 401. A support 440 fixed to the partition plate support 310 and a support 441 fixed to the substrate support 300 are connected by a vacuum bellows 443 .

[0015] A plurality of substrates S are placed on the substrate support 300 at predetermined intervals in the vertical direction (perpendicular direction). A plurality of partition plates 314 are arranged on the partition plate support part 310 directly below the substrates S, above and / or below the substrates S. In the substrate processing step described below, it is desirable to align the heights of the partition plates 314 with those of the partition plates 226 and 232. This makes it easier to form a horizontal gas flow across the partition plate 226, over the substrates S, and the partition plate 232, with vertical flow suppressed, allowing each substrate S to be processed uniformly.

[0016] 1 shows an example in which five substrates S are supported on the substrate support 300. However, the present disclosure is not limited to this. The substrate support 300 may be configured to support, for example, approximately 5 to 50 substrates S. In this specification, the notation of a numerical range such as "5 to 50 substrates" means that the lower limit and upper limit are included in the range. Thus, for example, "5 to 50 substrates" means "5 or more and 50 or less substrates." The same applies to other numerical ranges.

[0017] As shown in FIG. 2A , the gas supply pipe 251 is provided with, in this order from the upstream direction, a first processing gas source 252, a mass flow controller (MFC) 253 which is a flow rate controller (flow rate control part), a valve 275 which is an on-off valve, a tank 259 which is a storage part for storing gas therein, a sensor 301 which is a pressure measuring device (pressure measuring part) for measuring the pressure inside the tank 259, and a valve 254.

[0018] The tank 259 is provided with a sensor 448, which is a temperature measuring device (temperature measuring unit) that measures the temperature of the tank 259 and / or the gas stored in the tank 259. The tank 259 is also provided with a heater 447, which is a temperature controller (temperature control unit) that adjusts the temperature of the tank 259 and / or the gas stored in the tank 259. A portion of the gas supply pipe 251 with a larger diameter than the upstream and downstream portions, or a spiral pipe, may be used as the storage unit. By opening and closing the valve 275 on the upstream side of the tank 259 and the valve 254 on the downstream side, the gas supplied from the gas supply pipe 251 can be temporarily stored (filled) in the tank 259, or the gas stored in the tank 259 can be supplied into the processing chamber 201.

[0019] The first process gas source 252 is a gas source for supplying a first process gas (also referred to as a raw material gas) as a process gas. Alternatively, a vaporizer that vaporizes a liquid or solid to generate the first process gas may be used as the first process gas source 252. Hereinafter, an example will be described in which a gas obtained by vaporizing a liquid or solid is used as the first process gas.

[0020] A first process gas supply system 250 (also referred to as a source gas supply system) is mainly composed of the gas supply pipe 251, the MFC 253, the valve 275, the tank 259, the sensor 301, and the valve 254. The first process gas supply system 250 may include a first process gas source 252. The first process gas supply system 250 may also include a sensor 448 and a heater 447. In addition to the heater 447, heaters (not shown) may be provided in various parts of the first process gas supply system 250 to adjust the temperature of the first process gas supply system 250. The first process gas supply system 250 is an example of a process gas supply system that stores a first process gas as a process gas in the tank 259 and supplies the first process gas stored in the tank 259 to the substrate S.

[0021] A gas exhaust pipe 302 is connected to the gas supply pipe 251 between the sensor 301 and the valve 254, for discharging the gas in the tank 259 to the outside of the processing chamber 201 without supplying it to the processing chamber 201. A valve 303 is provided on the gas exhaust pipe 302. A first processing gas exhaust system (also referred to as a source gas exhaust system) is mainly configured by the gas exhaust pipe 302 and the valve 303. The first processing gas exhaust system may be included in the first processing gas supply system 250.

[0022] A gas supply pipe 255 is connected to the gas supply pipe 251 between the valve 275 and the tank 259. An inert gas source 256, an MFC 257, and a valve 258 are provided in the gas supply pipe 255, in this order from the upstream direction. An inert gas is supplied from the inert gas source 256. A first inert gas supply system is mainly configured by the gas supply pipe 255, the MFC 257, and the valve 258. The inert gas source 256 may be included in the first inert gas supply system. The first inert gas supply system may be included in the first process gas supply system 250.

[0023] 2B , the gas supply pipe 261 is provided with, in this order from the upstream side, a second process gas source 262, an MFC 263, and a valve 264. The second process gas source 262 is a gas source for supplying a second process gas (also referred to as a reactive gas) as a process gas. The gas supply pipe 261, the MFC 263, and the valve 264 mainly constitute a second process gas supply system 260 (also referred to as a reactive gas supply system). The second process gas source 262 may be included in the second process gas supply system 260.

[0024] A gas supply pipe 265 is connected to the gas supply pipe 261 on the downstream side of the valve 264. An inert gas source 266, an MFC 267, and a valve 268 are provided in the gas supply pipe 265, in that order from the upstream direction. An inert gas is supplied from the inert gas source 266. A second inert gas supply system is mainly constituted by the gas supply pipe 265, the MFC 267, and the valve 268. The inert gas source 266 may be included in the second inert gas supply system. The second inert gas supply system may be included in the second process gas supply system 260.

[0025] 2C , a vacuum pump 284 serving as a vacuum exhaust device is connected to the exhaust pipe 281 via a valve 282 and an APC (Auto Pressure Controller) valve 283 serving as a pressure regulator (pressure adjustment unit), so that the reaction tube 210 can be evacuated to a predetermined pressure (vacuum level). The exhaust pipe 281 is connected to an exhaust pipe connection unit 242. The exhaust pipe 281, the valve 282, and the APC valve 283 are collectively referred to as an exhaust system 280. The exhaust system 280 is also referred to as a process chamber exhaust system. The exhaust system 280 may include the vacuum pump 284.

[0026] Next, a controller serving as a control section (control means) will be described with reference to Fig. 3. The substrate processing apparatus 10 has a controller 600 that controls the operation of each section of the substrate processing apparatus 10.

[0027] 3 shows an outline of the controller 600. The controller 600 is configured as a computer including a CPU (Central Processing Unit) 601, a RAM (Random Access Memory) 602, a storage device 603 as a storage unit, and an I / O port 604. The RAM 602, the storage device 603, and the I / O port 604 are configured to be able to exchange data with the CPU 601 via an internal bus 605.

[0028] The storage device 603 is configured by, for example, a flash memory, a hard disk drive (HDD), etc. A control program for controlling the operation of the substrate processing apparatus 10, a process recipe describing the procedures and conditions for substrate processing, etc. are readably stored in the storage device 603.

[0029] The process recipe functions as a program, which is a combination of procedures in a substrate processing step (described later) that are executed by the controller 600 to obtain a predetermined result. Hereinafter, the process recipe, control program, etc. are collectively referred to as simply a program. In this specification, the term "program" may refer to a process recipe alone, a control program alone, or both. The RAM 602 is configured as a memory area (work area) in which programs, data, etc. read by the CPU 601 are temporarily stored.

[0030] The I / O port 604 is connected to the above-mentioned vertical drive mechanism 400, heaters 211, 447, APC valve 283, vacuum pump 284, MFCs 253, 257, 263, 267, valves 254, 258, 264, 268, 275, 282, 303, sensors 301, 448, rotation drive mechanism 430, etc.

[0031] The CPU 601 is configured to read and execute a control program from the storage device 603, and also to read a process recipe from the storage device 603 in response to an input of an operation command from the input / output device 681, etc. The CPU 601 is configured to control the vertical drive mechanism 400 to raise and lower the substrate support 300, the heater 211 to heat the substrate, the APC valve 283 to adjust the opening degree, the vacuum pump 284 to start and stop, the MFCs 253, 257, 263, and 267 to adjust the flow rates of various gases, the valves 254, 258, 264, 268, 275, 282, and 303 to open and close, the sensor 301 to measure the pressure inside the tank 259, the sensor 448 to measure the temperature of the tank 259 and / or the gas stored in the tank 259, the heater 447 to control the temperature of the tank 259 and / or the gas stored in the tank 259, and the rotation of the substrate support 300 and the rotation speed adjustment operation by the rotation drive mechanism 430, all in accordance with the contents of the read process recipe. The MFCs 253 , 257 , 263 , and 267 , the valves 254 , 258 , 264 , 268 , 275 , 282 , and 303 , the APC valve 283 , and the vacuum pump 284 can be used as a gas control unit configured to be able to control the supply and exhaust of gas into the processing chamber 201 .

[0032] The controller 600 according to this embodiment can be configured by installing the program into a computer using an external storage device 682 (e.g., a magnetic disk such as a hard disk, an optical disk such as a DVD, a magneto-optical disk such as an MO, or a semiconductor memory such as a USB memory) storing the program. The means for supplying the program to the computer is not limited to supplying the program via the external storage device 682. For example, the program may be supplied via a communication means such as the Internet or a dedicated line, without going through the external storage device 682. The storage device 603 and the external storage device 682 are configured as computer-readable recording media on which the program is recorded. Hereinafter, these are collectively referred to as recording media. In this specification, the term "recording medium" may refer to the storage device 603 alone, the external storage device 682 alone, or both.

[0033] (2) Substrate Processing Process Next, as one step in the manufacturing process of a semiconductor device, a substrate processing process for forming a thin film on a substrate S using the substrate processing apparatus 10 configured as described above will be described with reference to FIGS. 4 and 6A-6D. Here, recesses such as trenches and holes are formed on the surface of the substrate S. As shown in FIG. 6A, this substrate processing process includes a substrate loading step S1, a pressure / temperature adjusting step S2, a preparation step S3, a stabilization step S4, a film processing step S5, a tank exhaust step S6, a pressure / temperature adjusting step S7, and a substrate unloading step S8. In FIG. 4, the height of the hatched portion of the tank 259 from the bottom of the tank 259 represents the amount of first processing gas in the tank 259 during the preparation step S3, the stabilization step S4, the film processing step S5, and the tank exhaust step S6. In the following description, the operation of each component of the substrate processing apparatus 10 is controlled by a controller 600.

[0034] The term "substrate" used in this specification may refer to the substrate itself or to a laminate of the substrate and a predetermined layer or film formed on its surface. The term "surface of the substrate" used in this specification may refer to the surface of the substrate itself or to the surface of a predetermined layer or the like formed on the substrate. When described in this specification, "forming a predetermined layer on a substrate" may mean forming a predetermined layer directly on the surface of the substrate itself or forming a predetermined layer on a layer or the like formed on the substrate. When used in this specification, the term "wafer" is synonymous with the term "substrate".

[0035] (Substrate Loading Step S1) In the transfer chamber 217, a plurality of substrates S are loaded (wafer charge) onto the substrate support 300. Thereafter, the substrate support 300 is raised by the vertical drive mechanism 400, thereby loading the substrates S into the reaction tube 210, i.e., the processing chamber 201 (boat load).

[0036] (Pressure / Temperature Adjustment Step S2) The opening of the APC valve 283 is adjusted and the processing chamber 201 is evacuated by the vacuum pump 284 so that the processing chamber 201 has a desired pressure (pressure adjustment). Furthermore, the output of the heater 211 is controlled so that the processing chamber 201 or the substrate S has a desired temperature (temperature adjustment). That is, the pressure / temperature adjustment step S2 is a step of adjusting at least one of the temperature and pressure in the processing chamber 201. Furthermore, the rotation drive mechanism 430 rotates the substrate support 300 (and the substrate S) and the partition plate support 310. Furthermore, the tank 259 is heated by the heater 447 so that the tank 259 or the gas in the tank 259 has a desired temperature (tank temperature adjustment).

[0037] At this time, the temperature of the first process gas supply system 250 is controlled so that the temperature of the gas supplied from the first process gas source 252 into the tank 259 is lower than the temperature of the tank 259 or the gas inside the tank 259. This makes it possible to suppress the generation of particles caused by liquefaction or solidification of a portion of the first process gas inside the tank 259. These operations are continued at least until the processing of the substrate S is completed.

[0038] 6B, a preparation step S3 including a storage step S31 is performed. The preparation step S3 is an example of a first step in the present disclosure.

[0039] 4A, a case will be described in which the inside of the tank 259 is in a vacuum state at the start of the substrate processing step (or the preparation step S3). This makes it possible to suppress the generation of particles in the tank 259.

[0040] The storage step S31 is a step of storing the first process gas in the tank 259. Storing the first process gas in the tank 259 is initiated by opening the valve 275 while the valves 254, 258, 303, 264, and 268 are closed. Thereafter, storing the first process gas in the tank 259 is terminated by closing the valve 275 after a predetermined time has elapsed. The storage step S31 is performed, for example, as shown in FIG. 4B , so that a predetermined amount X of the first process gas is present in the tank 259 at the end of the storage step S31. In other words, the storage step S31 is performed so that a predetermined amount X of the first process gas is present in the tank 259 at the start of the membrane treatment step S5.

[0041] Hereinafter, "the flow rate of gas stored in tank 259 in a certain process" may be expressed as "the storage flow rate in a certain process." Furthermore, "the time during which gas continues to be stored in tank 259 in a certain process" may be expressed as "the storage time in a certain process." Furthermore, the amount of gas stored in tank 259 in a certain process is controlled, for example, by adjusting the storage flow rate and / or the storage time in that process. Furthermore, the amount of gas present in tank 259 at the end of a certain process is controlled, for example, by adjusting the storage flow rate and / or the storage time in that process.

[0042] (Stabilization Step S4) After the preparation step S3 and before the membrane treatment step S5, a stabilization step S4 is performed in which the first process gas in the tank 259 is heated by the heater 447. This reduces the difference between the temperature of the first process gas in the tank 259 and the temperature of the tank 259, or makes the difference between the two temperatures zero (a thermal equilibrium state is achieved). The stabilization step S4 is performed, for example, for a time period equal to or longer than the time period from the end of the supply step S512 to the start of the next storage step S511 in the membrane treatment step S5 described below.

[0043] At least a part of the preparation step S3 and at least a part of the stabilization step S4 may be performed simultaneously with at least one of the substrate loading step S1 and the pressure and temperature adjustment step S2, thereby shortening the time required for the substrate processing step.

[0044] 6C, a treatment cycle including a first treatment gas supply step S51, a purge gas supply step S52, a second treatment gas supply step S53, and a purge gas supply step S54 is performed a predetermined number of times (n times, where n is an integer of 1 or greater than 2). The treatment step S5 is an example of the second step in the present disclosure.

[0045] 6D , in the first process gas supply step S51, a first process gas is stored in a tank in a storage step S511, and the first process gas stored in the tank 259 is supplied into the process chamber 201 (or the substrate S) in a supply step S52, which is referred to as "flush supply." Note that the storage step S511 and the supply step S512 may be collectively referred to as "flush supply."

[0046] <Storing Step S511> The storing step S511 is a step of storing the first process gas in the tank 259. Storing the first process gas in the tank 259 is started by the same procedure as in the storing step S31. At this time, as shown in FIG. 4B , the first process gas is supplied into the tank 259, which has a predetermined amount X of the first process gas therein. Thereafter, the valve 275 is closed when a predetermined time has elapsed, thereby completing the storing step S511. As shown in FIG. 4C , the storing step S511 is performed so that a predetermined amount Y of the first process gas is present in the tank 259 at the end of the storing step S511.

[0047] Here, at the start of the supply step S512, it is preferable to bring the tank 259 and the temperature of the first process gas in the tank 259 into a non-thermal equilibrium state, for reasons described below. That is, it is preferable to start the supply step S512 before the temperature of the first process gas in the tank 259 becomes stable.

[0048] <Supply Process S512> The supply process S512 is initiated by opening the valve 254 while the valves 258, 275, 303, 264, and 268 are closed. This allows at least a portion of the first process gas stored in the tank 259 in the state shown in FIG. 4C to be supplied to the substrate S placed in the process chamber 201. The supply process S512 is then terminated by closing the valve 254 after a predetermined time has elapsed. This results in a first layer formed on the substrate S, which is composed of at least a portion of the molecular structure of the first process gas. The supply process S512 may be performed under conditions in which the process gas decomposes within the process chamber. Furthermore, during the supply process S512, the valve 282 and the APC valve 283 are preferably open. This increases the flow rate of the first process gas within the process chamber 201, thereby suppressing decomposition of the first process gas.

[0049] Hereinafter, "the flow rate of gas supplied from the tank 259 to the substrate S, the processing chamber 201, etc. in a certain process" may be expressed as "the supply flow rate in a certain process." Furthermore, "the time during which gas is continuously supplied from the tank 259 to the substrate S, the processing chamber 201, etc. in a certain process" may be expressed as "the supply time in a certain process." Furthermore, the amount of gas supplied from the tank 259 to the substrate S, the processing chamber 201, etc. in a certain process is controlled by, for example, adjusting the supply flow rate and / or the supply time in that process. Furthermore, the amount of gas present in the tank 259 at the end of a certain process is controlled by, for example, adjusting the supply flow rate and / or the supply time in that process.

[0050] 4D, the supply step S512 is preferably performed so that a predetermined amount X of the first process gas is present in the tank 259 at the end of the supply step S512. The predetermined amount X may be set to any value between 0.1 and 99% of the amount (predetermined amount Y) of the first process gas stored in the tank 259 at the start of the supply step S512. In this case, the supply step S512 may be terminated when the pressure in the tank 259 measured by the sensor 301 drops to a predetermined pressure. Alternatively, the amount of the first process gas in the tank 259 at the end of the supply step S512 may be controlled by adjusting the predetermined pressure.

[0051] For example, the predetermined amount X to be left in the tank 259 at the end of the supply step S512 is set so that the decomposition rate of the first process gas in the process chamber 201 is equal to or less than the predetermined decomposition rate. This prevents the film thickness from becoming non-uniform in the recess formed on the surface of the substrate S, which would be caused by the decomposition of the first process gas to generate a product with higher reactivity. In other words, the step coverage can be improved.

[0052] Furthermore, for example, the predetermined amount X is set so that the flow rate of the first process gas in the process chamber 201 in the supply step S512 is equal to or greater than the predetermined flow rate. This prevents the decomposition rate of the first process gas supplied to the substrate S from becoming higher than the predetermined decomposition rate. This improves the step coverage. The flow rate of the first process gas may be an average flow rate of the first process gas on the substrate S or in the process chamber 201. Alternatively, the flow rate of the first process gas at a certain point on the substrate S or in the process chamber 201 may be used.

[0053] Furthermore, for example, the predetermined amount X may be set so that the partial pressure of the first process gas in the space where the substrate S exists in this step is equal to or greater than a predetermined partial pressure, which makes it easier for the first process gas to reach the deeper side of the recess, thereby improving the step coverage.

[0054] In the supply step S512, the valve 258 may be opened to supply the inert gas into the gas supply pipe 251 via the gas supply pipe 255. In addition, in order to prevent the first process gas from entering the gas supply pipe 261, the valves 268 and 264 may be opened to supply the inert gas into the gas supply pipe 261.

[0055] [Purge Gas Supply Process S52] In the purge gas supply process S52, the processing chamber 201 is purged. Specifically, while the valves 275, 303, and 264 are closed, the valves 254, 258, and 268 are opened to supply an inert gas as a purge gas into the processing chamber 201, and the processing chamber 201 is evacuated by the vacuum pump 284.

[0056] [Second Process Gas Supply Step S53] In the second process gas supply step S53, the valve 264 is opened while the valves 254, 258, 275, 303, and 268 are closed, and then the valve 264 is closed after a predetermined time has elapsed. As a result, the second process gas, the flow rate of which is adjusted by the MFC 263, is supplied to the substrate S in the process chamber 201 and then exhausted. By supplying the second process gas to the substrate S, the first layer on the substrate S can be modified to a second layer. At this time, the valve 282 and the APC valve 283 are open. Here, the valve 268 may be opened to allow an inert gas to flow into the gas supply pipe 261 via the gas supply pipe 265. Alternatively, the valves 258 and 254 may be opened to allow an inert gas to flow into the gas supply pipe 251.

[0057] [Purge Gas Supply Step S54] In the purge gas supply step S54, the inside of the processing chamber 201 is purged in the same procedure as in the purge gas supply step S52 described above.

[0058] [Performed a Predetermined Number of Times] A process cycle of performing the first process gas supply step S51, the purge gas supply step S52, the second process gas supply step S53, and the purge gas supply step S53 is performed a predetermined number of times (n times, where n is an integer of 1 or greater than 2). As a result, a film of a predetermined thickness containing elements derived from the first process gas and elements derived from the second process gas is formed on the substrate S having a recess.

[0059] In the storing step S511 of the first process gas supply step S51 of the second or subsequent process cycle, the first process gas is supplied into the tank 259 in which a predetermined amount X of the first process gas is present, as shown in Fig. 4(E). Then, the storing step S511 is performed so that a predetermined amount Y of the first process gas is present in the tank 259 at the end of the storing step S31, as shown in Fig. 4(F).

[0060] In the first process gas supply step S51 of the second or subsequent process cycle, at least one of the purge gas supply step S52, the second process gas supply step S53, and the purge gas supply step S53 may be performed partially simultaneously with the storage step S511, thereby improving throughput.

[0061] (Tank Evacuation Process S6) After the film processing process S5, the tank 259 is evacuated as the tank evacuation process S6. After the supply process S512 in the nth processing cycle is completed, the tank evacuation process S6 is initiated by opening the valve 303 while the valves 254, 258, 275, 264, and 268 are closed. As a result, as shown in FIG. 4G, the first process gas in the tank 259 is evacuated by the vacuum pump 284. For example, after the tank 259 reaches a vacuum state as shown in FIG. 4H, the tank evacuation process S6 is terminated by closing the valve 303. Thereafter, the vacuum state in the tank 259 is maintained until the start of the next substrate processing process. This can suppress the generation of particles due to liquefaction, solidification, or decomposition reaction of a portion of the first process gas in the tank 259. Note that the tank 259 may be purged in the tank evacuation process S6. Specifically, the tank 259 may be evacuated by the vacuum pump 284 while an inert gas is supplied to the tank 259 from an inert gas supply source (not shown).

[0062] (Pressure / Temperature Adjustment Step S7) An inert gas serving as a purge gas is supplied into the processing chamber 201 and exhausted through the exhaust pipe 281. This removes gases and reaction by-products remaining in the processing chamber 201 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 (return to atmospheric pressure). In addition, the output of the heater 211 is controlled so that the inside of the processing chamber 201 reaches a desired temperature (temperature adjustment).

[0063] (Substrate Unloading Process S8) The vertical drive mechanism 400 lowers the base flange 401, thereby opening the lower end of the reaction tube 210. Then, the processed substrate S is unloaded (boat unloading) to the transfer chamber 217 while being supported by the substrate support 300. The processed substrate S is removed from the substrate support 300 in the transfer chamber 217 (wafer discharging).

[0064] The tank exhaust step S6 may be performed while either the pressure and temperature adjustment step S7 or the substrate unloading step S8 is being performed, thereby shortening the time required for the substrate processing step.

[0065] According to this aspect, in addition to the above-mentioned effects, one or more of the following effects can be obtained.

[0066] (a) Some of the effects obtained by this embodiment will be described by comparing this embodiment with a comparative example. In the comparative example, the substrate processing process is performed using the substrate processing apparatus 10 described above without performing the preparation process S3 and the stabilization process S4. Other processes are performed in the same manner as in the above embodiment, and elements that are substantially the same as those described in the above embodiment are given the same reference numerals, and their description may be omitted.

[0067] 5 shows the amount of first process gas in the tank 259 during the first to third process cycles of the comparative example. In the comparative example, at the start of the storing step S511 in the first process cycle, the tank 259 is evacuated to a vacuum, as shown in FIG. 5A. In contrast, at the start of the storing step S511 in the second or subsequent process cycles, the tank 259 contains the predetermined amount X, or an amount slightly different from the predetermined amount X, as shown in FIG. 5C. This difference in gas amount results in a difference in the amount of heat received by the first process gas stored in the tank 259 during the first and second storing steps S511. This causes variations in the state inside the tank 259 at the start of the first and second supply steps S512, as shown in FIGS. 5B and 5D, resulting in variations in the processing results for the substrate S. Here, the "condition inside the tank 259" refers to at least one of the amount, temperature, and pressure of the first process gas present in the tank 259, or the temperature of the tank 259 itself.

[0068] Furthermore, if there is a large difference in the state inside the tank 259 between the first and second processing cycles, variations in the state inside the tank 259 and variations in the processing results, as shown in Figures 5(C) to 5(G), may occur continuously in the second and subsequent processing cycles. Note that these variations become smaller with each repetition of the processing cycle, and may occur continuously from the first to twentieth processing cycles, for example. In other words, variations are likely to occur in the content of the processing of the substrate S between the processing cycles performed early on and the processing cycles performed thereafter.

[0069] In this embodiment, by performing the preparation step S3, the difference in the amount of gas in the tank 259 at the start of the first and second storage steps S511 can be reduced or made zero, as shown in Figures 4(B) and 4(D) . Therefore, it is possible to reduce the variation in the processing content of the substrate S between the processing cycle performed at the beginning and the processing cycles performed thereafter.

[0070] (b) In this embodiment, the stabilization step S4 is performed after the preparation step S3, which further reduces the difference in the state of the tank 259 before the start of the storage step S511 between the first and second or subsequent treatment cycles.

[0071] (c) In this embodiment, the stabilization step S4 is performed for the same time as the time from the end of the supply step S512 in the membrane treatment step S5 to the start of the next storage step S511. This further reduces the difference in the state inside the tank 259 before the start of the storage step S511 between the first and second or subsequent treatment cycles.

[0072] (d) In this embodiment, a predetermined amount X of the first process gas is present in the tank 259 at the end of the supply step S512. In such a case, the difference in the state of the tank 259 before the start of the storage step S511 between the first and second times or later is likely to become large. In this embodiment, as shown in FIG. 4B , by performing the preparation step S3 so that the predetermined amount X of the first process gas is present in the tank 259, such an effect can be reduced.

[0073] (e) In this embodiment, the first process gas is a gas obtained by vaporizing a liquid or a solid, and the temperature of the gas supplied from the first process gas source 252 into the tank 259 is set to be lower than the temperature of the tank 259 or the gas inside the tank 259. Even in such a case, by using the technology disclosed herein, it is possible to reduce the difference in the state inside the tank 259 at the start of the storage step S511 between cycles.

[0074] (f) When the supply step S512 is performed under conditions that cause decomposition in the process chamber 201 (or on the surface of the substrate S), the state of the first process gas supplied to the substrate S varies between cycles, resulting in large variations in the process results. Even in such a case, the technique disclosed herein can be used to reduce the variation in the state of the first process gas supplied to the substrate S between cycles.

[0075] (g) In this embodiment, the tank 259 is evacuated at the start of the substrate processing step, in other words, at the start of the storage step S31. In such a case, the state inside the tank 259 before the start of the storage step S511 tends to differ greatly between the first and second or subsequent cycles. Even in such a case, by using the technology disclosed herein, it is possible to reduce the variation in the state of the first processing gas supplied to the substrate S between cycles.

[0076] (3) Modifications Modifications 1 and 2, which are modifications of the above-described embodiment, will be described below. In the description of Modifications 1 and 2, the substrate processing process described below is performed using the substrate processing apparatus 10 described above. The following description of Modifications 1 and 2 will focus on steps that are different from the substrate processing process described above. Note that steps that are common to the substrate processing process described above are performed in the same manner, and essentially identical elements are given the same reference numerals, and their description may be omitted. Modifications 1 and 2 provide one or more of the following effects in addition to the effects described above.

[0077] (Variation 1) In Variation 1, instead of the preparation step S3 in the above-described embodiment, a preparation step S3' as shown in Figure 7 is performed. The preparation step S3' is an example of the first step in the present disclosure. In Variation 1, for example, the steps are performed in the following order: substrate carry-in step S1, pressure / temperature adjustment step S2, preparation step S3', stabilization step S4, film treatment step S5, tank evacuation step S6, pressure / temperature adjustment step S7, and substrate carry-out step S8.

[0078] (Preparation Step S3′) [Storage Step S31′] In the storage step S31′, the first process gas is stored in the tank 259 by the same procedure as in the storage step S31. The storage step S31′ is performed, for example, so that the amount of the first process gas in the tank 259 at the end of the storage step S31′ is approximately the same as that at the end of the storage step S511 in the process cycle.

[0079] [Discharge Step S32'] The discharge step S32' is a step of discharging at least a portion of the first process gas in the tank 259 from the tank 259 so that the first process gas is not supplied to the substrate S. In the discharge step S32', at least a portion of the first process gas stored in the tank 259 is exhausted by the vacuum pump 284 using a procedure similar to that in the tank exhaust step S6. The discharge step S32' is performed, for example, so that the amount of the first process gas in the tank 259 at the end of the discharge step S32' is approximately the same as that at the end of the supply step S512 in the processing cycle.

[0080] The amount of gas discharged from the tank 259 in the discharge step S32' and the amount of gas remaining in the tank 259 at the end of the discharge step S32' are controlled, for example, by the time it takes to exhaust the tank 259. In this case, the supply step S512 may be ended when the pressure in the tank 259 measured by the sensor 301 drops to a predetermined pressure. Alternatively, the amount of the first process gas in the tank 259 at the end of the supply step S512 may be controlled by adjusting the predetermined pressure.

[0081] In this way, by performing the preparation step S3' further including the discharge step S32', the first treatment cycle can be started after the first treatment gas has been stored and discharged in the tank 259, as in the second or subsequent treatment cycles. Therefore, it is possible to further reduce the variation in the state inside the tank 259 at the start of the first and second storage steps S511.

[0082] In the exhaust process S32′, the first process gas discharged from the tank 259 is exhausted via a route that does not pass through the process chamber 201. This allows the preparation process S3′ to be performed in parallel with other processes, such as the substrate loading process S1 and the pressure / temperature adjustment process S2, thereby improving throughput.

[0083] [Performed a Predetermined Number of Times] A preparation cycle including the above-described storage step S31' and discharge step S32' is performed a predetermined number of times (m times, where m is an integer of 1 or 2 or more). The preparation cycle is performed, for example, 1 to 20 times. As described above, variations in the content of the processing of the substrate S are likely to occur between the processing cycles performed early on and the processing cycles performed thereafter. For this reason, by performing the preparation cycle multiple times in the preparation step S3', it is possible to further reduce the difference in the state inside the tank 259 before the start of the storage step S511 between the first processing cycle and the second or subsequent processing cycles.

[0084] (Variation 2) In Variation 2, in the preparation step S3′ described in Variation 1, a discharge step S32″ and a second process gas supply step S9 are performed as shown in FIG. 8 instead of the discharge step S32′. In Variation 2, the preparation step S3′ is started before the substrate carry-in step S1. That is, in Variation 2, the preparation step S3′, substrate carry-in step S1, pressure and temperature adjustment step S2, stabilization step S4, film treatment step S5, tank evacuation step S6, pressure and temperature adjustment step S7, and substrate carry-out step S8 are performed in this order, for example. Note that in Variation 2, the second process gas supply step S9 may be omitted.

[0085] [Discharge Step S32"] The discharge step S32" is a step of discharging at least a portion of the first process gas in the tank 259 from the tank 259 so that the first process gas is not supplied to the substrate S. The discharge step S32" is started and ended in the same manner as the supply step S512. At this time, the valve 282 and the APC valve 283 are opened, and the gas in the process chamber 201 is exhausted by the vacuum pump 284. That is, in the discharge step S32", the first process gas exhausted from the tank 259 is exhausted via the process chamber 201. At this time, a first layer including at least a portion of the molecular structure of the first process gas may be formed on at least a portion of the surface of the process chamber 201. The discharge step S32" is performed, for example, so that the amount of the first process gas in the tank 259 at the end of the discharge step S32" is approximately the same as that at the end of the supply step S512 in the process cycle.

[0086] In the discharge step S32'', the gas conductance in the gas path from the tank 259 to the vacuum pump 284 can be set to the same level as in the supply step 512, and the discharge step S32' can be performed. Therefore, the difference in the state inside the tank 259 before the start of the storage step S511 between the first and second or subsequent processing cycles can be further reduced.

[0087] [Second Process Gas Supply Step S9] In the second process gas supply step S9, a second process gas is supplied into the process chamber 201 without a substrate S present therein. The second process gas supply step S9 can be started and ended by the same procedure as the second process gas supply step S53. At this time, the second process gas supply step S9 may modify the first layer formed on the surface of the process chamber 201 in the exhaust step S32" into a second layer.

[0088] By performing the exhaust step S32" and the second process gas supply step S9, a film similar to the film formed on the substrate S in the film formation step S5 can be formed on the inner wall surface of the process chamber 201, i.e., pre-coating the inside of the process chamber 201 can be performed. By pre-coating the inside of the process chamber 201, for example, a decrease in the amount of process gas supplied to the substrate S due to reaction of the process gas (first process gas and / or second process gas) on the surface of a component in the process chamber 201 in the film formation step S5 can be suppressed. Furthermore, since the preparation step S3' and pre-coating in the process chamber 201 can be performed simultaneously, the consumption of the first process gas can be reduced.

[0089] In addition, in the preparation step S3' of the second modified example, both the discharge step S32" and the discharge step S32' may be performed. For example, in the preparation step S3', the discharge step S32" may be performed one or more times, and then the discharge step S32' may be performed one or more times. Even in this case, the same effects as those described above can be obtained.

[0090] Other Embodiments Although the embodiment of this aspect has been specifically described above, the present invention is not limited to this and various modifications are possible without departing from the spirit of the invention.

[0091] In this embodiment, the first process gas is not stored in the tank 259 in the stabilization step S4. However, the technology of the present disclosure is not limited to this. In the stabilization step S4, the first process gas may be stored in the tank 259 at a flow rate lower than that in the preparation step S3. In addition, in the stabilization step S4, the first process gas may be stored in the tank 259 at a flow rate lower than that in the preparation step S3 and the storage step S511. Even in these cases, some of the effects of the stabilization step S4 can be obtained, and the time required for the substrate processing step can be shortened.

[0092] It is preferable to keep the tank 259 and the first process gas therein in a non-thermal equilibrium state between the end of the storage step S511 and the start of the supply step S512. In this case, it is not necessary to provide time for the tank 259 and the first process gas therein to reach thermal equilibrium (a stable state in which the temperature difference between them is zero) after the end of the storage step S511 of each cycle. On the other hand, if there is a difference in the state inside the tank 259 at the start of the storage step S511 between two cycles, the state of the first process gas supplied from the tank 259 in the supply step S512 is likely to vary. However, by using the technology disclosed herein, such effects can be reduced. Therefore, it is possible to improve throughput while suppressing variations in the processing content of the substrate S between processing cycles.

[0093] In the above-described embodiment and Modifications 1 and 2, an example has been described in which a first process gas (source gas) is flush-supplied to the substrate S, and then a second process gas (reaction gas) is supplied. However, the present disclosure is not limited to this. For example, the first process gas may be supplied to the substrate S, and then a second process gas may be flush-supplied, or the first process gas and the second process gas may be supplied to the substrate S. The above-described effects can also be obtained in these cases.

[0094] The source gas may be, for example, a predetermined element-containing gas containing a predetermined element such as tungsten (W), titanium (Ti), molybdenum (Mo), tantalum (Ta), cobalt (Co), yttrium (Y), ruthenium (Ru), hafnium (Hf), zirconium (Zr), aluminum (Al), or silicon (Si). One or more of these may be used as the source gas. Alternatively, a gas obtained by activating these gases with plasma or the like may be used as the source gas.

[0095] As the predetermined element-containing gas, for example, a halogen-based predetermined element-containing gas containing a predetermined element and a halogen element can be used. As the halogen-based predetermined element-containing gas, for example, hexachlorotungsten (WCl ６ ), hexafluorotungsten (WF ６ ), titanium tetrachloride (TiCl ４ ), titanium tetrafluoride (TiF ４ ), molybdenum pentachloride (MoCl ５ ), molybdenum pentafluoride (MoF ５ ), molybdenum dioxide dichloride (MoO ２ Cl ２ ), molybdenum oxide tetrachloride (MoOCl ４ ), tantalum pentachloride (TaCl ５ ), tantalum pentafluoride (TaF ５ ), cobalt difluoride (CoF ２ ), cobalt dichloride (CoCl ２ ), yttrium trifluoride (YF ３ ), yttrium trichloride (YCl ３ ), ruthenium trichloride (RuCl ３ ), ruthenium trifluoride (RuF ３ ), hafnium tetrachloride (HfCl ４ ), hafnium tetrafluoride (HfF4), zirconium tetrachloride (ZrCl ４ ), zirconium tetrafluoride (ZrF ４ ), aluminum trichloride (AlCl ３ ), aluminum trifluoride (AlF３ ), dichlorosilane (SiH ２ Cl ２ ), 1,2-dichlorodisilane (Si ２ H ４ Cl ２ ), 1,1,1-trichlorodisilane (Si ２ H ３ Cl ３ ), 1,1,2-trichlorodisilane (Si ２ H ３ Cl ３ ), pentachlorodisilane (Si ２ HCl ５ ), hexachlorodisilane (Si ２ Cl ６ ), tetrafluorosilane (SiF ４ ) can be used. Furthermore, the gas containing the predetermined element can be, for example, monosilane (SiH ４ ), disilane (Si ２ H ６ ), trisilane (Si ３ H ８ ), tetrasilane (Si ４ H １０ As the predetermined element-containing gas, one or more of these can be used.

[0096] As the predetermined element-containing gas, for example, an organic predetermined element-containing gas having a predetermined element and an organic ligand can be used. As the organic predetermined element-containing gas, for example, hexadimethylaminoditungsten (W ２ [N(CH ３ ) ２ ] ６ ), bis(tertiarybutylimide)bis(dimethylamido)tungsten ((t-C ４ H ９ NH) ２ W = (Nt-C ４ H ９ ) ２ ), tetrakisethylmethylaminotitanium (Ti[N(C ２ H ５ ) (CH ３ )] ４ ), bisethylcyclopentadienyl ruthenium (Ru(EtCp)２ ), biscyclopentadienyl ruthenium (Ru(Cp) ２ ), tetrakisethylmethylaminohafnium (Hf[N(Me)Et] ４ ), tetrakisdiethylaminohafnium (Hf[N(Et) ２ ]4), tetrakisdimethylaminohafnium (Hf[N(Me) ２ ] ４ ), trisdimethylaminocyclopentadienyl hafnium ((Cp)Hf[N(Me) ２ ] ３ ), tetrakisethylmethylaminozirconium (Zr[N(Me)Cp] ４ ), tetrakisdiethylaminozirconium (Zr[N(Et) ２ ] ４ ), tetrakisdimethylaminozirconium (Zr[N(Me) ２ ] ４ ), tris(dimethylamino)cyclopentadienyl zirconium ((Cp)Zr[N(Me) ２ ] ３ ), trimethylaluminum (Al(CH ３ ) ３ ), trisdimethylaminosilane (Si[N(CH ３ ) ２ ] ３ As the predetermined element-containing gas, one or more of these can be used.

[0097] The reactive gas may be, for example, a gas containing a reducing gas, an oxidizing gas, a nitriding gas, a sulfiding gas, a selenide gas, a telluride gas, or the like. One or more of these may be used as the reactive gas. A gas activated by plasma or the like may also be used as the reactive gas. For example, when the first processing gas is a gas containing a predetermined element and the second processing gas is a reducing gas, a film composed of a single predetermined element can be formed on the substrate S. Furthermore, when the first processing gas is a gas containing a predetermined element and the second processing gas is one of an oxidizing gas, a nitriding gas, a sulfiding gas, a selenide gas, or a telluride gas, a film of an oxide of the predetermined element, a nitride of the predetermined element, a sulfide of the predetermined element, a selenide of the predetermined element, or a telluride of the predetermined element can be formed on the substrate S.

[0098] The reducing gas may be, for example, hydrogen (H ２ ) gas, deuterium (D ２ ) gas, borane (BH ３ ) gas, diborane (B ２ H ６ ) gas, carbon monoxide (CO) gas, ammonia (NH ３ ) gas, monosilane (SiH ４ ) gas, disilane (Si ２ H ６ ) gas, trisilane (Si ３ H ８ ) gas, monogermane (GeH ４ ) gas, digermane (Ge ２ H ６ ) and the like can be used. In addition, as the reactive gas, for example, an oxidizing gas containing oxygen (O) can be used. As the oxidizing gas, for example, oxygen (O ２ ), ozone (O ３ ), water vapor (H ２ O), H ２ and O ２ mixed gas, hydrogen peroxide (H ２ O ２ ), nitrous oxide (N ２ O), etc. As the nitriding gas, for example, ammonia (NH ３ ) gas, diazene (N２ H ２ ) gas, hydrazine (N ２ H ４ ) gas, N ３ H ８ The sulfur gas may be, for example, sulfane (H ２ S), disulfane (H ２ S ２ ), diammonium sulfide ((NH ４ ) ２ S), dimethyl sulfide ((CH ３ ) ２ As the sulfide gas, one or more of these can be used. As the selenide gas, for example, selenium (H ２ Se), diserane (H ２ Se ２ ), dimethylselenium ((CH ３ ) ２ A gas containing, for example, tellurium (H ) can be used. As the selenide gas, one or more of these can be used. As the telluride gas, for example, tellurium (H ) can be used. ２ Te), diterane (H ２ Te ２ ), dimethylselenium ((CH ３ ) ２ One or more of these gases can be used as the telluride gas.

[0099] Examples of inert gases include rare gases such as helium (He), argon (Ar), neon (Ne) gas, and xenon (Xe) gas, and nitrogen (N ２ ) etc. As the inert gas, one or more of these can be used.

[0100] In the above-described embodiment, a case where a film is formed on a substrate S using a first process gas and a second process gas in a film formation process performed by the substrate processing apparatus is exemplified. However, the technology of the present disclosure is not limited to this. For example, the technology of the present disclosure can be applied even when three or more types of process gases are used.

[0101] 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. Furthermore, 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, and the same effects as those of the above-described embodiment and modified examples can be obtained.

[0102] The above-described embodiment, modification 1, and modification 2 can be used in any suitable combination. The processing procedures and processing conditions in this case can be, for example, the same as those of the above-described embodiment, modification 1, and modification 2.

[0103] S: substrate, 201: processing chamber, 259: tank (storage section)

Claims

1. A substrate processing method comprising: a first step including: (a1) a step of storing a processing gas in a storage section; and a second step of performing a cycle of the above steps in sequence a predetermined number of times after the first step; (b1) a step of storing the processing gas in the storage section; and (b2) a step of supplying at least a portion of the processing gas in the storage section to a substrate placed in a processing chamber.

2. The substrate processing method according to claim 1, wherein the processing gas is a gas obtained by vaporizing a liquid or a solid.

3. The substrate processing method according to claim 2, wherein the temperature of the process gas before being stored in the storage portion is made lower than the temperature of the storage portion.

4. The substrate processing method according to claim 1, further comprising the step of: (c) reducing the difference between the temperature of the processing gas in the storage section and the temperature of the storage section after the first step and before the second step.

5. A substrate processing method as described in claim 4, wherein in (c), the processing gas is not stored in the storage section, or in (c), the processing gas is stored in the storage section at a flow rate lower than the storage flow rate in (a1).

6. The substrate processing method according to claim 4, wherein (c) is carried out for a time period equal to or longer than the time period from the end of (b2) to the start of the next (b1).

7. The substrate processing method according to claim 1, wherein (b2) is carried out under conditions in which the processing gas is decomposed in the processing chamber.

8. The method of claim 1, wherein (b2) is performed such that a predetermined amount of said process gas is present in said reservoir at the end of (b2).

9. The substrate processing method according to claim 8, wherein the first step is performed so that the predetermined amount of the processing gas is present in the reservoir at the start of the second step.

10. The substrate processing method according to claim 1, further comprising the step of: (d) evacuating the inside of the reservoir after the second step.

11. The substrate processing method according to claim 1, wherein the inside of the reservoir is in a vacuum state at the start of the first step.

12. The substrate processing method of claim 1, wherein at the start of (b2), the reservoir and the process gas therein are brought into a non-thermal equilibrium state.

13. The substrate processing method of claim 1, further comprising: (e) a step of loading the substrate into the processing chamber; and (f) a step of adjusting at least one of the temperature and pressure within the processing chamber, wherein at least a portion of the first step is performed simultaneously with at least one of (e) and (f).

14. A substrate processing method according to any one of claims 1 to 13, wherein the first step further includes: (a2) a step of discharging at least a portion of the processing gas in the storage section from the storage section so that the processing gas is not supplied to the substrate.

15. The substrate processing method according to claim 14, wherein in the first step, a cycle including (a1) and (a2) is performed a plurality of times.

16. The substrate processing method according to claim 14, wherein in (a2), the gas discharged from the storage section is exhausted via a route that does not pass through the processing chamber.

17. The substrate processing method according to claim 14, wherein in (a2), the processing gas discharged from the storage portion is exhausted via a path passing through the processing chamber.

18. A method for manufacturing a semiconductor device, comprising: a first step including: (a1) a step of storing a process gas in a storage section; and a second step including: performing a cycle including the steps of: (b1) a step of storing the process gas in the storage section; and (b2) a step of supplying at least a portion of the process gas in the storage section to a substrate placed in a processing chamber, a predetermined number of times after the first step.

19. A substrate processing apparatus comprising: a processing chamber in which a substrate is placed; a processing gas supply system including a storage section for storing a processing gas, the processing gas supply system storing the processing gas in the storage section and supplying the processing gas stored in the storage section to the substrate; and a control section configured to be capable of controlling the processing gas supply system to perform a first process including: (a1) a process of storing the processing gas in the storage section; (b1) a process of storing the processing gas in the storage section; and (b2) a process of supplying at least a portion of the processing gas in the storage section to the substrate, the second process being performed a predetermined number of times after the first process.

20. A program for causing a substrate processing apparatus to execute, by a computer, a first procedure including: (a1) a procedure for storing a processing gas in a storage section; and (b1) a procedure for storing the processing gas in the storage section; and (b2) a procedure for supplying at least a portion of the processing gas in the storage section to a substrate placed in a processing chamber, a cycle of the above steps being performed a predetermined number of times after the first procedure.

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