Method of processing substrate

Abstract

To improve uniformity of a film formed over a substrate and controlling a step coverage.SOLUTION: A substrate processing apparatus 10 includes a reaction tube storage chamber 206b, and includes, inside the reaction tube storage chamber, a cylindrical reaction tube 210 having a process chamber 201 that is a section to process a substrate S and extending in the vertical direction, a heater 211 serving as a heating part (furnace body) provided around the outer periphery of the reaction tube, a gas supply structure 212 serving as a gas supplier, and a gas exhaust structure 213 serving as a gas exhauster. The gas supply structure is provided at an upstream side of the reaction tube in a gas flow direction, and a gas is supplied, from the gas supply structure into the reaction tube, to the substrate in the horizontal direction. The gas exhaust structure is provided at a downstream side of the reaction tube in the gas flow direction, and the gas inside the reaction tube is discharged from the gas exhaust structure. The gas supply structure, the interior of the reaction tube, and the gas exhaust structure are in communication with one another in the horizontal direction. An upstream gas guide 214 is provided at an upstream side of the reaction tube to regulate a flow of the gas supplied, and a downstream gas guide 215 is provided at a downstream side of the reaction tube to regulate a flow of the gas discharged.SELECTED DRAWING: Figure 1

Description

[Technical field]

[0001] The present disclosure relates to a method for processing a substrate. [Background technology]

[0002] As one step in the manufacturing process of a semiconductor device, there is a technique for supplying source gases and / or reactive gases at supply times that correspond to the concentration distribution of by-products formed on a substrate within the substrate surface (see, for example, Patent Document 1). [Prior art documents] [Patent documents]

[0003] [Patent Document 1] JP 2014-208883 A Summary of the Invention [Problem to be solved by the invention]

[0004] However, the uniformity of the film formed on the substrate may not meet the uniformity required for semiconductor device performance.

[0005] The present disclosure provides techniques that can improve the uniformity of a film formed on a substrate. [Means for solving the problem]

[0006] According to one aspect of the present disclosure, a) supplying a first process gas to the substrate; b) supplying a second process gas from a second process gas reservoir to the substrate; In b), a technique is provided that is implemented to reduce the time it takes for subsequent reactions of the second process gas on the substrate to occur. Effect of the Invention

[0007] According to the present disclosure, it is possible to improve the uniformity of a film formed on a substrate. [Brief description of the drawings]

[0008] [Figure 1] FIG. 1 is a schematic vertical cross-sectional view of a substrate processing apparatus according to an embodiment of the present disclosure. [Diagram 2] FIG. 2(A) is a diagram illustrating a first gas supply system in one embodiment of the present disclosure, FIG. 2(B) is a diagram illustrating a second gas supply system in one embodiment of the present disclosure, and FIG. 2(C) is a diagram illustrating a third gas supply system in one embodiment of the present disclosure. [Diagram 3] FIG. 3(A) is a diagram showing a processing chamber exhaust system in one embodiment of the present disclosure, and FIG. 3(B) is a diagram showing a transfer chamber exhaust system in one embodiment of the present disclosure. [Figure 4] FIG. 4 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. [Diagram 5] FIG. 5 is a diagram showing a substrate processing flow according to an embodiment of the present disclosure. [Figure 6] FIG. 6 is a diagram showing a substrate processing sequence in one embodiment of the present disclosure. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0009] Hereinafter, one embodiment of the present disclosure will be described mainly with reference to Figures 1 to 6. Note that all of the drawings used in the following description are schematic, and the dimensional relationships of the elements, the ratios of the elements, etc. shown in the drawings do not necessarily match the actual ones. Furthermore, the dimensional relationships of the elements, the ratios of the elements, etc. between multiple drawings do not necessarily match.

[0010] (1) Configuration of the substrate processing device The configuration of the substrate processing apparatus 10 will be described with reference to FIG.

[0011] The substrate processing apparatus 10 includes a reaction tube storage chamber 206b, and includes a cylindrical reaction tube 210 extending vertically in the reaction tube storage chamber 206b, a heater 211 as a heating unit (furnace body) installed on the outer periphery of 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 rectifier 214 and nozzles 223 and 224, which will be described later. The gas exhaust unit may include a downstream 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 may also be called a processing space in which the substrate S is disposed.

[0012] The gas supply structure 212 is provided upstream of the reaction tube 210 in the gas flow direction, and gas is supplied from the gas supply structure 212 into the reaction tube 210, and the gas is supplied horizontally to the substrate S. The gas exhaust structure 213 is provided downstream of the reaction tube 210 in the gas flow direction, and the gas inside the reaction tube 210 is exhausted from the gas exhaust structure 213. The gas supply structure 212, the inside of the reaction tube 210, and the gas exhaust structure 213 are horizontally connected to each other.

[0013] An upstream side of the reaction tube 210 between the reaction tube 210 and the gas supply structure 212 is provided with an upstream side straightening unit 214 for straightening the flow of the gas supplied from the gas supply structure 212. In addition, a downstream side of the reaction tube 210 between the reaction tube 210 and the gas exhaust structure 213 is provided with a downstream side of the reaction tube 210 for straightening the flow of the gas exhausted from the reaction tube 210. The lower end of the reaction tube 210 is supported by a manifold 216.

[0014] The reaction tube 210, the upstream rectifier 214, and the downstream rectifier 215 have a continuous structure and are made of materials such as quartz and SiC. These are made of a heat-transmitting material that transmits heat radiated from the heater 211. The heat from the heater 211 heats the substrate S and gas.

[0015] The gas supply structure 212 has a distribution section 225 to which the gas supply pipe 251 and the gas supply pipe 261 are connected and which distributes the gas supplied from each gas supply pipe. A plurality of nozzles 223 and nozzles 224 are provided downstream of the distribution section 225. The gas supply pipe 251 and the gas supply pipe 261 supply different types of gas as described below. The nozzles 223 and the nozzles 224 are arranged in a vertical relationship or a horizontal relationship. In this embodiment, the gas supply pipe 251 and the gas supply pipe 261 are also collectively referred to as the gas supply pipe 221. Each nozzle is also referred to as a gas discharge section. The distribution section 225 is configured so that the gas is supplied from the gas supply pipe 251 to the nozzle 223 and from the gas supply pipe 261 to the nozzle 224.

[0016] The upstream straightening section 214 has a housing 227 and a partition plate 226. The partition plate 226 extends in the horizontal direction and has a continuous structure without holes. The horizontal direction here means the direction toward the side wall of the housing 227 and the direction parallel to the surface of the substrate S in the reaction tube 210. A plurality of partition plates 226 are arranged in the vertical direction. The partition plate 226 is fixed to the side wall of the housing 227 and configured so that the gas does not move beyond the partition plate 226 to an adjacent area below or above.

[0017] Each partition plate 226 is provided at a position corresponding to each substrate S. Nozzles 223 and 224 are provided between the partition plates 226 and between the partition plate 226 and the housing 227. The gas discharged from the nozzles 223 and 224 has its flow adjusted by the partition plate 226 and is supplied to the surface of the substrate S. That is, when viewed from the substrate S, the gas is supplied from the side of the substrate S.

[0018] The downstream rectifier 215 is configured so that the ceiling is higher than the topmost substrate S when the substrate S is supported by a substrate support 300 (described later). , the bottom portion of the substrate support 300 is configured to be lower than the substrate S arranged at the bottom of the substrate support 300.

[0019] The downstream straightening section 215 has a housing 231 and a partition plate 232. The partition plate 232 extends in the horizontal direction and has a continuous structure without holes. The horizontal direction here is the same as the horizontal direction described above. Furthermore, a plurality of partition plates 232 are arranged in the vertical direction. The partition plate 232 is fixed to the side wall of the housing 231 and configured so that the gas does not move beyond the partition plate 232 downward or upward to an adjacent area. A flange 233 is provided on the side of the housing 231 that contacts the gas exhaust structure 213.

[0020] The partition plates 232 are provided at positions corresponding to the substrates S, respectively, at positions corresponding to the partition plates 226. It is desirable that the corresponding partition plates 226 and partition plates 232 have the same height. Furthermore, when processing the substrate S, it is desirable to align the height of the substrate S with the height of the partition plates 226 and partition plates 232.

[0021] By providing the partition plate 226 and the partition plate 232 in the positional relationship described above, the pressure loss in the vertical direction can be made uniform upstream and downstream of each substrate S. That is, as shown by the arrows in the figure, a horizontal gas flow can be reliably formed from the partition plate 226, over the substrate S, and to the partition plate 232, with the vertical flow being suppressed. Therefore, the difference in gas pressure over each substrate S can be reduced. This allows each substrate S to be processed uniformly.

[0022] The gas exhaust structure 213 is provided downstream of the downstream rectifier 215. The gas exhaust structure 213 is mainly composed of a housing 241 and an exhaust pipe connection part 242. A flange 243 is provided on the downstream rectifier 215 side of the housing 241. The housings 231 and 241 have a structure in which the heights of their ceilings and bottoms are continuous. An exhaust hole 244 is formed on the downstream side of the housing 241, below or in the horizontal direction, for exhausting gas that has passed through the downstream rectifier 215. The gas exhaust structure 213 is provided in the lateral direction of the reaction tube 210, and is a lateral exhaust structure for exhausting gas from the lateral direction of the substrate S.

[0023] The transfer chamber 217 is installed at the bottom of the reaction tube 210 via a manifold 216. In the transfer chamber 217, a substrate S is placed (mounted) on a substrate support (hereinafter, may be simply referred to as a boat) 300 by a vacuum transfer robot via a substrate carry-in port, and the substrate S is removed from the substrate support 300 by the vacuum transfer robot.

[0024] The transfer chamber 217 can accommodate the substrate support 300, the partition plate support 310, and a vertical drive mechanism 400 that drives the substrate support 300 and the partition plate support 310 (collectively referred to as the substrate holder) in the vertical and rotational directions. In FIG. 1, the substrate support 300 is shown raised by the vertical drive mechanism 400 and stored in the reaction tube 210.

[0025] The vertical direction drive mechanism 400 includes a rotation drive mechanism 430 for rotating the substrate support 300 and the partition plate support 310 together, and a boat up-down mechanism 420 for driving the substrate support 300 vertically relative to the partition plate support 310. The rotation drive mechanism 430 and the boat up-down mechanism 420 are fixed to a base flange 401 as a lid 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, and the inside of the reaction tube 210 can be kept airtight by being driven by a vertical drive motor 410 to raise the base flange 401 to a position where the upper surface of the base flange 401 is pressed against the transfer chamber 217 as shown in FIG. 1. The support 440 fixed to the partition plate support 310 and the support 441 fixed to the substrate support 300 are connected by a vacuum bellows 443.

[0026] Next, the substrate support portion will be described in detail with reference to FIG. The substrate support unit is composed of at least a substrate support 300 that supports a substrate S, and is stored in the reaction tube 210. The substrate S is disposed directly below the inner wall of the top plate of the reaction tube 210. The substrate support unit transfers the substrate S using a vacuum transfer robot through a substrate loading port (not shown) inside the transfer chamber 217, and transfers the transferred substrate S into the reaction tube 210 to perform a process of forming a thin film on the surface of the substrate S. The substrate loading port is provided, for example, in a side wall of the transfer chamber 217. The substrate support unit may also include a partition plate support unit 310.

[0027] On the substrate support 300, a plurality of substrates S are placed at predetermined intervals in the vertical direction by a plurality of support rods 315 supported by a base 311. The substrates S supported by the support rods 315 are partitioned by disk-shaped partitions 314 fixed (supported) at predetermined intervals on posts 313 supported by a partition support section 310. Here, the partitions 314 are disposed directly below the substrates S, and disposed above and / or below the substrates S. The partitions 314 separate the spaces between the substrates S. The predetermined intervals between the substrates S placed on the substrate support 300 are the same as the intervals between the top and bottom of the partitions 314 fixed to the partition support section 310. The diameter of the partitions 314 is formed to be larger than the diameter of the substrates S.

[0028] The base 311, the partition plate 314 and the multiple support rods 315 are formed of a material such as quartz or SiC. Note that, although an example in which five substrates S are supported by the substrate support 300 is shown here, the present invention is not limited to this. For example, the substrate support 300 may be configured to be capable of supporting approximately 5 to 50 substrates S. Note that the partition plate 314 is also called a separator.

[0029] In this specification, the expression of a numerical range such as "5 to 50 sheets" means that the lower limit and the upper limit are included in the range. Therefore, for example, "5 to 50 sheets" means "5 sheets or more and 50 sheets or less". The same applies to other numerical ranges.

[0030] In the process of forming a thin film on the substrate S, the partition plate 314 is preferably located at a height corresponding to the partition plate 226 and / or the partition plate 232. More preferably, the partition plate 314 is aligned in height with the partition plate 226 and the partition plate 232.

[0031] By using such a substrate support portion, it becomes easier to form a horizontal gas flow with vertical flow suppressed across the partition plate 226, over the substrates S, and across the partition plate 232. This makes the difference in gas pressure over each substrate S uniform, allowing each substrate S to be processed uniformly.

[0032] The partition plate support part 310 and the substrate support 300 are driven by a vertical drive mechanism part 400 in the vertical direction between the reaction tube 210 and the transfer chamber 217 and in the rotational direction around the center of the substrate S supported by the substrate support 300.

[0033] Next, the gas supply system will be described in detail with reference to Figures 2(A) to 2(C). As shown in Figure 2(A), a first gas source 252, a mass flow controller (MFC) 253 which is a flow rate controller (flow rate control section), a valve 275 which is an on-off valve, a tank 259 which is a first storage section for storing a first process gas, and a valve 254 which is an on-off valve are provided in gas supply pipe 251 in this order from the upstream direction.

[0034] The first gas source 252 is a source of a first gas containing a first element (also called a "first element-containing gas"). The first gas is a source gas, i.e., one of the process gases.

[0035] A first gas supply system 250 (also referred to as a source gas supply system or a process gas supply system) is mainly composed of the gas supply pipe 251, the MFC 253, the valve 275, the tank 259, and the valve 254. The first gas supply system 250 may include a first gas source 252.

[0036] A gas supply pipe 255 is connected between the valve 275 and the tank 259 in the gas supply pipe 251. An inert gas source 256, an MFC 257, and a valve 258 which is an on-off valve 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.

[0037] A first inert gas supply system is mainly composed of the gas supply pipe 255, the MFC 257, and the valve 258. In the substrate processing step, the inert gas supplied from the inert gas source 256 acts as a purge gas for purging gas remaining in the reaction tube 210. The inert gas source 256 may be included in the first inert gas supply system. The first inert gas supply system may be added to the first gas supply system 250.

[0038] As shown in FIG. 2B, the gas supply pipe 261 is provided with, in order from the upstream direction, a second gas source 262, an MFC 263, a valve 276, a tank 269 as a second storage unit for storing a second process gas, and a valve 264.

[0039] The second gas source 262 is a source of a second gas containing a second element (hereinafter also referred to as a "second element-containing gas"). The second gas is a gas different from the first gas, and may be one of the process gases. The second gas may be considered as a reaction gas that reacts with a precursor of the first gas, which is a raw material gas, or a modifying gas that modifies the surface of the substrate S.

[0040] A second gas supply system 260 (also referred to as a reactive gas supply system or a process gas supply system) is mainly composed of the gas supply pipe 261, the MFC 263, the valve 276, the tank 269, and the valve 264. The second gas supply system 260 may include a second gas source 262. Although one second gas supply system 260 is shown in Fig. 2(B), the present invention is not limited to this. A plurality of second gas supply systems 260 may be configured to be connectable in parallel.

[0041] A gas supply pipe 265 is connected between the valve 276 and the tank 269 in the gas supply pipe 261. An inert gas source 266, an MFC 267, and a valve 268 which is an on-off valve are provided in the gas supply pipe 265 in this order from the upstream direction. An inert gas is supplied from the inert gas source 266.

[0042] A second inert gas supply system is mainly composed of the gas supply pipe 265, the MFC 267, and the valve 268. In the substrate processing step, the inert gas supplied from the inert gas source 266 acts as a purge gas for purging gas remaining in the reaction tube 210. The inert gas source 266 may be included in the second inert gas supply system. The second inert gas supply system may be added to the second gas supply system 260.

[0043] 2(C), the gas supply pipe 271 is provided with a third gas source 272, an MFC 273, and a valve 274 in this order from the upstream direction. The gas supply pipe 271 is connected to the transfer chamber 217. When the transfer chamber 217 is made to have an inert gas atmosphere or is made to be in a vacuum state, an inert gas is supplied.

[0044] The third gas source 272 is an inert gas source. A third gas supply system 270 is mainly composed of the gas supply pipe 271, the MFC 273, and the valve 274. The third gas source 272 may be included in the third gas supply system 270. The third gas supply system 270 is also called a transfer chamber supply system.

[0045] Next, the exhaust system will be described with reference to Figures 3(A) and 3(B). The exhaust system 280, which exhausts the atmosphere in the reaction tube 210, has an exhaust pipe 281 communicating with the reaction tube 210, and is connected to the housing 241 via an exhaust pipe connector 242.

[0046] 3A, a vacuum pump 284 as a vacuum exhaust device is connected to the exhaust pipe 281 via a valve 282 and an APC (Auto Pressure Controller) valve 283 as a pressure regulator (pressure adjustment unit), and the reaction tube 210 is configured to be evacuated to a predetermined pressure (vacuum level). 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 processing chamber exhaust system. The exhaust system 280 may include the vacuum pump 284. An exhaust system 290 that exhausts the atmosphere of the transfer chamber 217 has an exhaust pipe 291 that is connected to the transfer chamber 217 and communicates with the inside thereof.

[0047] 3(B), a vacuum pump 294 is connected to the exhaust pipe 291 via a valve 292 and an APC valve 293, and is configured to evacuate the inside of the transfer chamber 217 to a predetermined pressure. The exhaust pipe 291, the valve 292, and the APC valve 293 are collectively referred to as an exhaust system 290. The exhaust system 290 is also referred to as a transfer chamber exhaust system. The exhaust system 290 may include the vacuum pump 294.

[0048] Next, a controller serving as a control section (control means) will be described with reference to Fig. 4. The substrate processing apparatus has a controller 600 that controls the operation of each section of the substrate processing apparatus .

[0049] 4 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.

[0050] The storage device 603 is composed of, for example, a flash memory, a HDD (Hard Disk Drive), etc. A control program for controlling the operation of the substrate processing apparatus 10, a process recipe in which procedures and conditions for substrate processing are described, etc. are readably stored in the storage device 603.

[0051] The process recipe is a combination of procedures in a substrate processing step, which will be described later, that are executed by the controller 600 to obtain a predetermined result, and functions as a program. Hereinafter, the process recipe and the control program are collectively referred to as simply a program. In addition, when the word program is used in this specification, it may include only a process recipe, only a control program, or both. The RAM 602 is configured as a memory area (work area) in which programs and data read by the CPU 601 are temporarily stored.

[0052] The I / O port 604 is connected to the above-mentioned vertical drive mechanism 400, heater 211, APC valves 283, 293, vacuum pumps 284, 294, MFCs 253, 257, 263, 267, 273, valves 254, 258, 264, 268, 274, 275, 276, rotation drive mechanism 430, etc.

[0053] 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 lifting and lowering operation of the substrate support 300 by the vertical direction drive mechanism 400, the heating operation by the heater 211, the opening and closing operation of the APC valves 283 and 293, the start and stop of the vacuum pumps 284 and 294, the flow rate adjustment operation of various gases by the MFCs 253, 257, 263, 267, and 273, the opening and closing operation of the valves 254, 258, 264, 268, 274, 275, and 276, the rotation of the substrate support 300 by the rotation drive mechanism 430, and the adjustment of the rotation speed, etc., in accordance with the contents of the read process recipe.

[0054] The controller 600 according to this embodiment can be configured by installing the program in the computer using an external storage device (for example, 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) 682 storing the above-mentioned program. The means for supplying the program to the computer is not limited to supplying it via the external storage device 682. For example, the program may be supplied without going through the external storage device 682 by using a communication means such as the Internet or a dedicated line. 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 simply as recording media. In this specification, when the term "recording medium" is used, it may include only the storage device 603 alone, only the external storage device 682 alone, or both.

[0055] Next, as one step in a semiconductor manufacturing process, a step of forming a thin film on a substrate S using the substrate processing apparatus 10 having the above-mentioned configuration will be described with reference to Figures 5 and 6. In the following description, the operation of each part constituting the substrate processing apparatus 10 is controlled by a controller 600.

[0056] Here, a film forming process is described in which a film is formed in a recess such as a trench or hole of a substrate S using a first gas and a second gas. For example, a gas containing a halogen element can be used as the first gas. Hexachloride disilane (Si2Cl6, hexachlorodisilane, abbreviated as HCDS) gas can be used.

[0057] The term "substrate" used in this specification may mean the substrate itself or 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 mean the surface of the substrate itself or 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".

[0058] (S102) The transfer chamber pressure adjustment step S102 will now be described. Here, the pressure inside the transfer chamber 217 is adjusted to the same level as that of a vacuum transfer chamber (not shown) adjacent to the transfer chamber 217. Specifically, the exhaust system 290 is operated to exhaust the atmosphere in the transfer chamber 217 so that the atmosphere in the transfer chamber 217 is at a vacuum level.

[0059] (S104) Next, the substrate carrying-in step S104 will be described. When the transfer chamber 217 reaches a vacuum level, the transfer of the substrate S begins. When the substrate S arrives at the vacuum transfer chamber, the gate valve is opened and the vacuum transfer robot carries the substrate S into the transfer chamber 217.

[0060] At this time, the substrate support 300 is on standby in the transfer chamber 217, and the substrates S are transferred to the substrate support 300. When a predetermined number of substrates S have been transferred to the substrate support 300, the vacuum transport robot is retreated, and the substrate support 300 is raised by the vertical drive mechanism 400 to move the substrates S into the reaction tube 210. At this time, the substrates S are positioned so that their surfaces are flush with the heights of the partition plates 226 and 232.

[0061] (S106) Next, the heating step S106 will be described. After the substrate S is carried into the reaction tube 210, the pressure inside the reaction tube 210 is controlled to be a predetermined pressure, and the surface temperature of the substrate S is controlled to be a predetermined temperature. When HCDS gas, for example, is used as the first gas, the temperature of the heater 211 is controlled so that the temperature of the substrate S is, for example, 100°C to 1500°C, preferably 200°C to 1000°C, and more preferably 400°C to 800°C. The pressure inside the reaction tube 210 may be, for example, 0.01 Pa to 1 kPa.

[0062] (S108) Next, the film treatment step S108 will be described. In the film treatment step S108, a first gas supply step of flush-supplying a first gas to the substrate S and a second gas supply step of flush-supplying a second gas to the substrate S are performed one or more times in accordance with a process recipe to form a predetermined film on the substrate S having a recess on its surface.

[0063] <First gas supply step, step S1> In this step, the first gas is flush-supplied to the processing chamber 201 inside which the substrate S is placed. Here, flush supply refers to supplying a large flow rate of gas into the reaction tube 210 in a short period of time.

[0064] Specifically, in this step, a first gas is stored in advance in a tank 259 provided in the gas supply pipe 251. When, for example, HCDS gas is used as the first gas, the pressure inside the tank 259 at this time is, for example, 0.01 to 100 kPa, preferably 0.1 to 1.0 kPa.

[0065] When the first gas is supplied, the valve 254 provided downstream of the tank 259 between the tank 259 and the nozzle 223 is opened, and the first gas is supplied into the gas supply pipe 251 from the tank 259 in which the first gas is stored in advance. At this time, the pressure (total pressure) inside the processing chamber 201 is set to, for example, 0.01 to 100 kPa, preferably 0.1 to 1.0 kPa. Then, after a predetermined time has elapsed since the supply of the first gas was started, the valve 254 is closed to stop the supply of the first gas into the gas supply pipe 251. When, for example, HCDS gas is used as the first gas, the valve 254 is closed to stop the supply of the first gas into the gas supply pipe 251 after a time within a range of, for example, 0.01 to 10 seconds has elapsed.

[0066] The first gas is supplied in large quantities from the gas supply structure 212 into the reaction tube 210 in a short time via the upstream rectifier 214. Thereafter, the first gas is exhausted through the space above the substrate S, the downstream rectifier 215, the gas exhaust structure 213, and the exhaust pipe 281. At this time, the valve 282 and the APC valve 283 are in an open state. Here, while the first gas is being supplied into the processing chamber 201, the valve 275 may be in an open state or a closed state.

[0067] At this time, it is preferable to supply the first gas into the processing chamber 201 so that the decomposition rate of the first gas in the processing chamber 201 becomes small.

[0068] In addition, when forming a film in a recess (or groove, trench, or hole) formed on the substrate S, the higher the reactivity of the gas, the easier it is to adsorb to the opening side of the recess and the harder it is to adsorb to the deep side of the recess. Therefore, when forming a film in a recess using a gas that generates a more reactive substance by decomposition (for example, HCDS gas) as the first gas, the shorter the residence time τ of the first gas and / or the higher the flow rate v of the first gas, the lower the decomposition rate X, and the better the step coverage. It is preferable to control the residence time τ of the first gas and / or the flow rate v of the first gas so that the decomposition rate X of the first gas is 0%, in order to improve the step coverage. As a method of shortening the residence time τ of the first gas and increasing the flow rate v of the first gas, there is a method of supplying the first gas by increasing the opening of the APC valve 283 using the tank 259.

[0069] When using, for example, HCDS gas as the first gas, by setting the flow rate of the first gas to, for example, 10 m / sec or more, the decomposition rate X can be set to a relatively low value of 0% to 25%, which is advantageous for improving step coverage. Also, by setting the flow rate of the first gas to, for example, 15 m / sec or more, the decomposition rate can be set to an even lower value within the range of 0% to 15%, which is preferable for improving step coverage. Also, by controlling the flow rate to 20.0 m / sec or more, the decomposition rate can be set to 0%, that is, the first gas can be left undecomposed, which is even more preferable for improving step coverage.

[0070] That is, in this step, the first gas is flush-supplied, thereby making it possible to change the decomposition rate X of the first gas supplied to the substrate S. Also, in this step, the first gas is flush-supplied, thereby controlling the flow rate of the first gas, thereby controlling the residence time of the first gas in the processing chamber 201, and making it possible to control the decomposition rate X of the first gas.

[0071] In addition, in this step, the supply amount of the first gas can be increased at the start of supply of the first gas by flushing the first gas. When, for example, HCDS gas is used as the first gas, the supply amount of the first gas per unit time per one substrate S may be, for example, 0.001 to 15 slm, preferably 0.05 to 10 slm, and more preferably 0.010 to 5 slm. If it is less than 0.001 slm, the partial pressure of the first gas in the process chamber 201 may be lowered, and the film formation rate may be reduced. If it is more than 15 slm, the partial pressure of the first gas in the process chamber 201 may increase, and decomposition of the first gas may proceed excessively. If it is 0.001 to 15 slm, the flow rate can be changed by controlling the flow rate of the first gas while suppressing a decrease in the film formation rate and excessive decomposition of the first gas. If it is 0.05 to 10 slm, the flow rate can be changed by controlling the flow rate of the first gas while further suppressing a decrease in the film formation rate and decomposition of the first gas. When the flow rate is set to 0.010 to 5 slm, the flow velocity can be changed by controlling the flow rate of the first gas while sufficiently suppressing a decrease in the film formation rate and excessive decomposition of the first gas.

[0072] Furthermore, by flush-supplying the first gas, the first gas whose pressure has been increased (boosted) in the tank 259 can be supplied into the processing chamber 201. This makes it possible to increase the flow rate of the first gas at the start of supply.

[0073] As described above, in this step, the valve 282 and the APC valve 283 are in an open state, and the reaction tube 210 is evacuated by the vacuum pump 284 while the first gas is being supplied into the processing chamber 201. This reduces the pressure in the processing chamber 201, increases the flow rate of the first gas, and shortens the residence time τ of the first gas in the processing chamber 201.

[0074] During the supply of the first gas into the processing chamber 201, the valve 258 may be opened to supply an inert gas into the gas supply pipe 251 via the gas supply pipe 255. As the inert gas, for example, nitrogen (N2), helium (He), argon (Ar), etc. may be used. As the inert gas, one or more of these may be used. This also applies to each step described later.

[0075] Furthermore, prior to this step and before starting the supply of the first gas into the processing chamber 201, the APC valve 283 may be adjusted to evacuate the reaction tube 210 using the vacuum pump 284. This increases the flow rate of the first gas, particularly the flow rate at the start of the supply, and shortens the residence time τ of the first gas in the processing chamber 201.

[0076] The temperature in the process chamber 201 in this step may be set to be higher than the decomposition temperature of the first gas, which increases the reactivity of the first gas to improve the film formation rate, and also reduces the residence time of the first gas in the process chamber 201, thereby preventing the decomposition rate of the first gas from becoming high.

[0077] This step may be performed so that at least a portion of the adsorption sites on the surface of the substrate S becomes first element sites to which a first element-containing substance, which is a substance containing a first element contained in the first gas, is chemically adsorbed.

[0078] In the above-mentioned embodiment, the first element may be, for example, silicon (Si) or germanium (Ge) which is a group 14 element, or aluminum (Al), gallium (Ga), or indium (In) which is a group 13 element. In addition, for example, a transition metal element may be the first element. As the transition metal element, for example, the first element may be titanium (Ti), zirconium (Zr), or hafnium (Hf) which is a group 4 element, niobium (Nb) or tantalum (Ta) which is a group 5 element, molybdenum (Mo) or tungsten (W) which is a group 6 element, manganese (Mn) which is a group 7 element, ruthenium (Ru) which is a group 8 element, cobalt (Co) which is a group 9 element, or nickel (Ni) which is a group 10 element.

[0079] As the first gas, for example, a Si-containing gas containing Si as the first element can be used. As the Si-containing gas, for example, a gas containing Si and chlorine (Cl) can be used. As the Si- and Cl-containing gas, for example, a source gas containing Si-Si bonds, such as HCDS gas, can be used. As the Si- and Cl-containing gas, for example, 1,1,2,2-tetrachloro-1,2-dimethyldisilane ((CH3)2Si2Cl4, abbreviated as TCDMDS) or 1,2-dichloro-1,1,2,2-tetramethyldisilane ((CH3)4Si2Cl2, abbreviated as DCTMDS) may be used. TCDMDS has a Si-Si bond and further includes a chloro group and an alkylene group. Furthermore, DCTMDS has a Si-Si bond and further includes a chloro group and an alkylene group. As the first gas, one or more of these can be used.

[0080] In the case where HCDS gas is used as the first gas, for example, when the HCDS gas is decomposed and the bonds between the Si bonds are broken, SiCl4 and SiCl2, which have higher reactivity than HCDS gas, are generated. That is, HCDS gas is decomposed as shown below.

[0081] HCDS(Si2Cl6) →SiCl4+SiCl2

[0082] Since SiCl4 and SiCl2 are more reactive than HCDS, the decomposition rate of HCDS is high, and the more HCDS decomposes, the more the reaction proceeds. When ammonia (NH3) gas is used as the second gas described below, SiCl2 and SiCl4 react with NH groups described below to form a SiN layer, and at this time, reaction by-products such as hydrogen chloride (HCl) are generated.

[0083] At least some of the adsorption sites on the surface of the substrate S become Si sites where Si-containing substances, which are Si-containing substances, are chemically adsorbed, but reaction by-products such as HCl are adsorbed to the adsorption sites on the substrate S and inhibit the adsorption of the Si-containing substances. In this step, by flushing the first gas, a large amount of the first gas is supplied to the substrate S in a short time after the start of the supply, so that the adsorption sites on the substrate S for reaction by-products such as HCl can be reduced and the amount of adsorption of the Si-containing substances can be increased. This makes it possible to improve the step coverage performance while improving the film formation rate.

[0084] <Purge, step S2> In this step, a purge gas is supplied to the process chamber 201 in which the substrate S is placed. That is, after the flush supply of the first gas in step S1, Si-containing substances that have not been adsorbed on the adsorption sites and reaction by-products that have been re-adsorbed on the surface of the substrate S are desorbed and removed from the reaction tube 210.

[0085] Specifically, while valve 254 is open, valve 275 is closed, and valves 258, 268, and 264 are opened to supply an inert gas as a purge gas into gas supply pipes 251 and 261 via gas supply pipes 255 and 265, while valve 282 and APC valve 283 of exhaust pipe 281 are kept open and the reaction tube 210 is evacuated to a vacuum by vacuum pump 284.

[0086] <Second gas supply process, step S3> Next, a second gas that reacts with the first gas is supplied to the processing chamber 201 in which the substrate S is disposed. Specifically, in this step, the second gas is stored in advance in a tank 269 provided in the gas supply pipe 261. Then, when the second gas is supplied, a valve 264 provided downstream of the tank 269 between the tank 269 and the nozzle 224 is opened, and the second gas is supplied from the tank 269 in which the second gas is stored in advance into the gas supply pipe 261. Then, after a predetermined time has elapsed since the start of the supply of the second gas, the valve 264 is closed to stop the supply of the second gas into the gas supply pipe 261.

[0087] The second gas is supplied in a large amount from the gas supply structure 212 into the reaction tube 210 through the upstream rectifier 214 in a short time, and then exhausted through the space above the substrate S, the downstream rectifier 215, the gas exhaust structure 213, and the exhaust pipe 281. At this time, the valve 282 is in an open state. The APC valve 283 is in a state adjusted to a predetermined opening degree. Here, while the second gas is supplied into the processing chamber 201, the valve 276 may be in an open state or a closed state. Preferably, the valve 276 is in an open state. Also, the valve 268 may be opened to allow an inert gas to flow into the gas supply pipe 261 through the gas supply pipe 265. Also, in order to prevent the second gas from entering the gas supply pipe 251, the valves 258 and 254 may be opened to allow an inert gas to flow into the gas supply pipe 251. At this time, a large amount of the second gas is supplied at once from the side of the substrate S in a horizontal direction to the substrate S through the gas supply structure 212 that is in communication with the reaction tube 210.

[0088] In this step, the second gas is flush-supplied. By supplying the second gas, the pressure of which is increased in the tank 269, into the processing chamber 201, the second gas can be uniformly supplied to the surface of the substrate S. In particular, when a recess that will become a semiconductor device structure is formed in the substrate S, the second gas can be supplied to the bottom of the recess.

[0089] In this step, the APC valve 283 is adjusted to a predetermined opening, and the reaction tube 210 is evacuated by the vacuum pump 284 while the second gas is being supplied into the processing chamber 201. This allows the inside of the processing chamber 201 to reach a predetermined pressure. Also, the inside of the processing chamber 201 can be maintained at the predetermined pressure.

[0090] Specifically, in this step, the second gas is stored in advance in the tank 269 provided in the gas supply pipe 261. When, for example, NH3 gas is used as the second gas, the pressure inside the tank 269 at this time is, for example, 0.01 to 100 kPa, preferably 0.1 to 50 kPa.

[0091] When the second gas is supplied, the valve 264 (also called the downstream valve) provided on the downstream side of the tank 269 is opened, and the second gas is supplied from the tank 269 into the gas supply pipe 261. At this time, the pressure (total pressure) inside the process chamber 201 is set to, for example, 0.1 to 100 kPa, preferably 300 to 5 kPa, more preferably 300 to 3 kPa, and more preferably 2 kPa to 2.6 kPa. Then, after a predetermined time has elapsed since the start of the supply of the second gas, the valve 264 is closed to stop the supply of the second gas into the gas supply pipe 261. In addition, in this step, the valve 276 (also called the upstream valve) on the upstream side of the tank 269 may be opened. Here, the time for supplying the second gas is about 0.1 to 5 seconds, preferably 2 to 5 seconds, and more preferably 2 to 4 seconds.

[0092] The second gas is supplied in a large amount in a short time from the gas supply structure 212 through the upstream rectifier 214 into the reaction tube 210. Thereafter, the second gas is exhausted through the space above the substrate S, the downstream rectifier 215, the gas exhaust structure 213, and the exhaust pipe 281.

[0093] The temperature inside the process chamber 201 at this time may be set to be higher than the decomposition temperature of the second gas. In this step, similarly to step S1 described above, the decomposition rate X of the second gas may be controlled by setting the residence time τ of the second gas based on a predetermined relationship between the decomposition rate X of the second gas in the process chamber 201 and the residence time τ of the second gas in the process chamber 201.

[0094] The second gas may be, for example, a gas containing a second element different from the first gas. The second element is, for example, any one of N, oxygen (O), and carbon (C). The second gas may be, for example, a hydrogen (H) and N-containing gas. The H and N-containing gas may be, for example, a hydrogen nitride gas containing an NH bond, such as ammonia (NH3) gas, diazene (N2H2) gas, hydrazine (N2H4) gas, or N3H8 gas. The second gas may be one or more of these.

[0095] When a hydrogen nitride gas containing an NH bond, such as NH3 or N2H4, in which multiple hydrogen atoms are bonded to nitrogen, is used as the second gas, the following successive reactions may occur on the surface of the substrate S. In the following model, x, y, and z are integers, and there is a relationship of x>y>z, and a reaction in which H is released from an NH bond molecule (ligand) may occur until z becomes 1. NHx, NHy, H, and the like (also referred to as released products in this disclosure) may be released until z becomes 1. This release may occur not only in this step S3 but also in other steps.

[0096] Sequential reaction model: NHx→NHy→NHz

[0097] In a film formation process in which such successive reactions occur, it may be difficult to improve the uniformity of the properties of the film formed on the substrate S. In particular, when a recess is formed on the substrate S, a problem occurs in that the film properties of the film formed on the top of the recess differ from the film formed on the bottom of the recess. Here, the film properties include the film thickness, the amount of nitrogen vacancy, the refractive index, etc.

[0098] The above-mentioned desorbed material may be generated not only in this step S3 but also in other steps. For example, if the desorbed material is generated in step S1 performed after step S3, the desorbed material may react with the first gas (gas phase reaction). If such a gas phase reaction occurs, an unintended film may be formed, and the uniformity of the film characteristics of the substrate S may not be improved. For example, it may be difficult to improve the step coverage (S / C) of the film formed in the recess.

[0099] To address such issues, in step S3 of the present disclosure, the second gas is flush-supplied under the above-mentioned conditions, thereby shortening the time until the above-mentioned successive reactions converge, and solving the above-mentioned issues caused by the successive reactions. In particular, in a substrate S having a recess formed therein, it is possible to bring the S / C ratio of the film formed in the recess close to 100%. Also, in the case where the film formed in the recess is a nitrogen-containing film, the amount of nitrogen vacancies in the film is 2.5×10 18 pieces / cm 3 The above-described film can be formed from the top to the bottom of the recess.

[0100] Moreover, it is preferable that the supply conditions (pressure, time, etc.) of the second gas described above be adjusted in accordance with the aspect ratio of the recess formed in the substrate S.

[0101] In addition, in the film formation process having the above-mentioned successive reaction model, it is preferable to supply the second gas for a longer time than the first gas. This allows the second gas to be supplied to every corner of the surface of the substrate S. In particular, a sufficient amount of the second gas can be supplied to the bottom of the recess.

[0102] In the film formation process having the above-mentioned successive reaction model, it is preferable that the opening degree of the APC valve 283 when supplying the second gas is smaller than the opening degree of the APC valve 283 when supplying the first gas. This allows the second gas to be supplied to every corner of the surface of the substrate S. In particular, a sufficient amount of the second gas can be supplied to the bottom of the recess.

[0103] In addition, in the film formation process having the above-mentioned successive reaction model, it is preferable to set the pressure in the process chamber 201 when the second gas is supplied higher than the pressure in the process chamber 201 when the first gas is supplied. This allows the second gas to be supplied to every corner of the surface of the substrate S. In particular, a sufficient amount of the second gas can be supplied to the bottom of the recess.

[0104] In addition, in the film formation process having the above-mentioned successive reaction model, it is preferable to supply the second gas in a larger amount than the first gas. This allows the second gas to be supplied to every corner of the surface of the substrate S. In particular, a sufficient amount of the second gas can be supplied to the bottom of the recess. Here, the supply amount of each gas refers to one or more of pressure, time, tank capacity, tank pressure, etc.

[0105] In addition, in the film formation process having the above-mentioned successive reaction model, it is desirable to shorten the time for the successive reaction to converge. In addition, when a recess is formed in the substrate S, it is preferable to make the time for the successive reaction to converge uniform between the top (opening side) and the bottom (rear side) of the recess. As a method for achieving this, the second gas may be flush-supplied under the above-mentioned conditions.

[0106] <Purge, step S4> In this step, a purge gas is supplied to the process chamber 201 in which the substrate S is placed by the same process procedure as in step S2. That is, after the flush supply of the second gas in step S3, the second gas that has not been adsorbed to the adsorption sites and the reaction by-products that have been generated by reaction with the second gas and re-adsorbed on the surface of the substrate S are desorbed and removed from the reaction tube 210.

[0107] Specifically, while the valve 264 is open, the valve 276 is closed, and the valves 268, 258, and 254 are opened to supply an inert gas as a purge gas into the gas supply pipes 251 and 261 through the gas supply pipes 255 and 265, and the valve 282 and the APC valve 283 of the exhaust pipe 281 are kept open, and the reaction tube 210 is evacuated to a vacuum by the vacuum pump 284. This makes it possible to suppress the reaction between the first gas and the second gas in the gas phase present in the reaction tube 210.

[0108] (Performed a set number of times) A film of a predetermined thickness is formed on the substrate S having a recess by performing a cycle of sequentially and non-simultaneously performing the above-mentioned first gas supply step and second gas supply step a predetermined number of times (n times, n is an integer of 1 or more). For example, when HCDS gas is used as the first gas and a gas containing H and N is used as the second gas, a SiN film is formed. This allows a film to be formed on the substrate S having a recess with improved step coverage performance and an improved film formation rate.

[0109] (S110) Next, the substrate unloading step S110 will be described. In S110, the processed substrate S is unloaded from the transfer chamber 217 in the reverse order to the substrate loading step S104 described above.

[0110] (S112) Next, judgment S112 will be described. Here, it is judged whether or not the substrate has been processed the predetermined number of times. If it is judged that the substrate has not been processed the predetermined number of times, the process returns to the substrate loading step S104, and the next substrate S is processed. If it is judged that the substrate has been processed the predetermined number of times, the process ends.

[0111] Although the gas flow is described above as being horizontal, it is sufficient that the main gas flow is formed in a horizontal direction overall, and the gas flow may be diffused in a vertical direction as long as this does not affect uniform processing of multiple substrates.

[0112] Furthermore, in the above, expressions such as "to the same extent," "equivalent," and "equal" are used, but it goes without saying that these include things that are substantially the same.

[0113] (Other embodiments) Although the embodiment of the present invention has been specifically described above, the present invention is not limited thereto, and various modifications are possible without departing from the spirit of the present invention.

[0114] In the above embodiment, the tank 259 is provided in the first gas supply system 250, but the embodiment is not limited to this. That is, the tank 259 may not be provided in the first gas supply system 250, and the first gas may be supplied by a method other than flush supply. Even in this case, the same effects as those of the above embodiment can be obtained.

[0115] Similarly, although the above-mentioned second gas supply system 260 is described using a case where the tank 269 is provided, the present embodiment is not limited to this. That is, the second gas supply system 260 may not include the tank 269, and the second gas may be supplied by a method other than flush supply. Even in this case, the same effects as those of the above-mentioned embodiment can be obtained.

[0116] In the above embodiment, the film forming process performed by the substrate processing apparatus is performed by using the first gas and the second gas to form a film on the substrate S, but the embodiment is not limited to this. That is, other types of gases may be used as the processing gases used in the film forming process to form other types of thin films. Furthermore, the embodiment can be applied even when three or more types of processing gases are used.

[0117] In the above-described embodiment, the film formation process is taken as an example of the process performed by the substrate processing apparatus, but the present embodiment is not limited thereto. That is, the present embodiment can be applied to film formation processes other than the film formation processes taken as examples in the above-described embodiment.

[0118] In the above-mentioned 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-mentioned embodiment, and can be suitably applied to, for example, a case where a film is formed using a single-wafer type substrate processing apparatus that processes one or several substrates at a time. In the above-mentioned embodiment, an example of forming a film using a substrate processing apparatus having a hot-wall type processing furnace has been described. The present disclosure is not limited to the above-mentioned embodiment, and can be suitably applied to, for example, a case where a film is formed using a substrate processing apparatus having a cold-wall type processing furnace.

[0119] When using these substrate processing apparatuses, each process can be performed according to the same process procedures and under the same process conditions as in the above-described aspects and modifications, and the same effects as in the above-described aspects and modifications can be obtained.

[0120] The above-mentioned aspects and modifications may be used in appropriate combination. The processing procedures and processing conditions in such a case may be the same as those of the above-mentioned aspects and modifications. Explanation of symbols

[0121] S-substrate 201 Processing Room

Claims

1. a) supplying a first process gas to the substrate; b) supplying a second process gas from a second reservoir to the substrate; c) shortening the time it takes for the sequential reactions of the second process gas on the substrate to converge in b); A substrate processing method comprising the steps of:

2. 2. The substrate processing method according to claim 1, wherein in b), a pressure in the area where the substrate exists is set to 300 to 3000 Pa, and a time for supplying the second processing gas is set to 2 to 5 seconds.

3. 2. The substrate processing method according to claim 1, wherein in b), a pressure in the area where the substrate exists is set to 2000 to 2600 Pa, and a time for supplying the second processing gas is set to 2 to 4 seconds.

4. In step a), the first process gas is supplied from a first reservoir. The method of claim 1 .

5. A plurality of the second storage sections are provided, The substrate processing method of claim 1 , wherein in b), the second process gas is supplied from the plurality of second reservoirs.

6. The substrate processing method according to claim 1 or 5, wherein the method is performed in a state where an upstream valve and a downstream valve of the second reservoir are open.

7. the first process gas and the second process gas are supplied from a gas supply unit protruding in a horizontal direction of the substrate at a side of a process vessel that accommodates the substrate, 2. The substrate processing method according to claim 1, wherein the gas is exhausted from an exhaust unit facing the gas supply unit.

8. the substrate has a recess; c) further modifying the pressure of b) based on the aspect ratio of the recess. The substrate processing method according to claim 2 .

9. The substrate has a recess, In the case of b), the nitrogen deficiency amount of the nitrogen-containing film formed in the recess is 2.5×10 １８ pieces / cm ３ and supplying a second process gas from a second reservoir to the substrate so as to achieve the above. The method of claim 1 .

10. In step b), a second process gas is supplied from a second reservoir to the substrate for a time period longer than the time period for which the first process gas is supplied. The method of claim 1 .

11. In step b), the opening of an exhaust valve for exhausting the area in which the substrate is present is controlled by: Make the opening larger than that in a). The method of claim 1 .

12. The pressure in the area where the substrate is present during the step b) is made higher than the pressure during the step a). The method of claim 1 .

13. In step b), the supply amount of the second process gas is made larger than the supply amount of the first process gas. The method of claim 1 .

14. the substrate has a recess; In step b), the second process gas is supplied so that the successive reactions occurring at the top of the recess and the successive reactions occurring at the bottom of the recess are completed simultaneously. The method of claim 1 .

15. a) supplying a first process gas to the substrate; b) supplying a second process gas from a second reservoir to the substrate; c) shortening the time it takes for the sequential reactions of the second process gas on the substrate to converge in b); A method for manufacturing a semiconductor device having the above structure.

16. a) supplying a first process gas to the substrate; b) delivering a second process gas from a second reservoir to the substrate; c) reducing the time it takes for the sequential reactions of the second process gas on the substrate to converge; A program for causing a computer to execute the above in a substrate processing apparatus.

17. a first gas supply system that supplies a first process gas to the substrate; a second gas supply system having a second reservoir and configured to supply a second process gas to the substrate; a) supplying the first process gas to the substrate; b) supplying the second process gas from the second reservoir to the substrate; c) reducing the time it takes for the sequential reactions of the second process gas on the substrate to converge; a control unit configured to be able to control the first gas supply system and the second gas supply system to perform the above-mentioned A substrate processing apparatus comprising:

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