Control methods for gasification systems, manufacturing methods for semiconductor devices, substrate processing equipment, gasification systems and programs

Abstract

This invention can suppress the poor vaporization of liquid raw materials that may occur when liquid raw materials are injected into a gas container. The present invention provides a technique comprising the following steps: (a) supplying the liquid raw material to a vaporization container in which the liquid raw material is vaporized; (b) at the end of (a) or after a predetermined time having elapsed from that point, adjusting the pressure to reduce the pressure in the vaporization container; (c) after (b), maintaining the vaporization container in a state where the pressure adjustment has been stopped; and (d) after (c), supplying the vaporized gas generated by vaporizing the liquid raw material in the vaporization container to a processing container for processing a substrate.

Description

Control Method of Vaporization System, Manufacturing Method of Semiconductor Device, Substrate Processing Apparatus, Vaporization System, and Program The present invention relates to a control method of a vaporization system, a manufacturing method of a semiconductor device, a substrate processing apparatus, a vaporization system, and a program. In Patent Document 1, a vaporization system that generates a vaporized gas by vaporizing a liquid raw material stored in a vaporization container, and a substrate processing apparatus that performs substrate processing using the generated vaporized gas are disclosed. [Prior Art Documents] [Patent Documents] Patent Document 1: WO2018 / 056346 (Problems to be Solved by the Invention) When the liquid raw material stored in the vaporization container decreases, there is a case where it is necessary to replenish the liquid raw material into the vaporization container. However, pressure fluctuations in the vaporization container generated when injecting the liquid raw material into the vaporization container, etc., tend to cause poor vaporization of the liquid raw material. The present invention provides a technique that can suppress poor vaporization of the liquid raw material that may occur due to the injection of the liquid raw material into the gas container. (Technical Means for Solving the Problem) The present invention provides a technique that performs the following steps: (a) a step of supplying the liquid raw material into a vaporization container that vaporizes the liquid raw material inside; (b) a step of performing pressure adjustment to decompress the vaporization container at the time point when (a) ends, or after a first predetermined time has elapsed from that time point; (c) a step of maintaining the state where pressure adjustment in the vaporization container has stopped after (b); and (d) a step of supplying the vaporized gas generated by vaporizing the liquid raw material in the vaporization container into a processing container that processes a substrate after (c). (Effects Compared with the Prior Art) According to the present invention, it is possible to suppress poor vaporization of the liquid raw material that may occur due to the injection of the liquid raw material into the gas container. <Aspect of the Present Invention> Hereinafter, an aspect of the present invention will be mainly described with reference to FIGS. 1 to 6 and FIG. 8. Furthermore, the drawings used in the following description are all schematic, and the dimensional relationships of each component shown in the drawings, the ratios of each component, etc. are not necessarily the same as the actual ones. In addition, among the plurality of drawings, the dimensional relationships of each component, the ratios of each component, etc. are not necessarily the same. (1) Configuration of Substrate Processing Apparatus As shown in FIG. 1, a substrate processing apparatus 10 having a vaporization system (refer to FIG. 3) as described later has a processing furnace 202 that processes a wafer 200 as a substrate. The processing furnace 202 has a cylindrical heater 207 that extends in the vertical direction of the apparatus, and the heater 207 is supported by a heater base (not shown) that serves as a holding plate. Moreover, the heater 207 heats the inside of a processing chamber 201 described later to a predetermined temperature. Furthermore, inside the heater 207, a processing tube 203 serving as a processing unit and having a concentric cylindrical shape with the heater 207 is disposed. Moreover, inside the processing tube 203, a processing chamber 201 for processing a plurality of wafers 200 is formed. Specifically, by means of a boat 217 serving as a substrate support, a plurality of wafers 200 (for example, 25 to 200 wafers) are stacked in the vertical direction, and the plurality of wafers 200 in a state of being stacked by the boat 217 are disposed inside the processing chamber 201. Below the boat 217, a cylindrical heat insulating cylinder 218 is disposed. In addition, below the processing tube 203, a manifold (inlet flange) 209 having a concentric cylindrical shape with the processing tube 203 is disposed. The upper end of the manifold 209 faces the lower end of the processing tube 203, and the manifold 209 supports the processing tube 203 via an O-ring 220 serving as a sealing member. In addition, in the processing chamber 201, between the wall surface of the processing tube 203 and the plurality of wafers 200 stacked by the boat 217, nozzles 410 and 420 extending in the vertical direction are disposed. Furthermore, in the nozzles 410 and 420, within a range facing the wafers 200 in the horizontal direction, a plurality of gas supply holes 410a and 420a for supplying gas are respectively formed. Thereby, the gas ejected from the gas supply holes 410a and 420a can flow toward the wafers 200. Furthermore, the lower end side portions of the nozzles 410 and 420 are bent to penetrate the side walls of the manifold 209, and the end portions of the lower end sides of the nozzles 410 and 420 protrude outside the manifold 209. Moreover, at the end portions of the lower end sides of the nozzles 410 and 420, gas supply pipes 310 and 320 serving as gas supply pipelines are respectively connected. Thereby, it can supply a plurality of types of gas to the processing chamber 201. In the gas supply pipes 310 and 320, from the upstream side in the flow direction of the gas flowing in the gas supply pipes 310 and 320 (hereinafter referred to as "gas flow direction"), mass flow controllers (flow control units) i.e., mass flow controllers (MFCs) 312 and 322, and on-off valves i.e., valves 314 and 324 are respectively provided in sequence. In addition, in the gas supply pipes 310 and 320, at portions on the downstream side in the gas flow direction with respect to the valves 314 and 324, the ends of gas supply pipes 510 and 520 serving as gas supply pipelines for supplying inert gas are respectively connected. In the gas supply pipes 510 and 520, from the upstream side in the flow direction of the gas flowing in the gas supply pipes 510 and 520, mass flow controllers (flow control units) i.e., MFCs 512 and 522, and on-off valves i.e., valves 514 and 524 are respectively provided in sequence. The raw material gas, which is a processing gas generated by vaporizing a liquid raw material in a storage tank 610 described later, is supplied from a gas supply pipe 310 to the processing chamber 201 via an MFC 312, a valve 314, and a nozzle 410. The raw material gas supply system is composed of the gas supply pipe 310, the MFC 312, and the valve 314. It is also possible to consider including the nozzle 410 in the raw material gas supply system. In addition, it is also possible to consider including a vaporization system 500 described later in the raw material gas supply system. The raw material gas supply system may also be referred to as a raw material supply system or a vaporized gas supply system. In contrast, the reaction gas, which is a processing gas, is supplied from a gas supply pipe 320 to the processing chamber 201 via an MFC 322, a valve 324, and a nozzle 420. When supplying a reaction gas (reactant) from the gas supply pipe 320, the reaction gas supply system (reactant supply system) is mainly composed of the gas supply pipe 320, the MFC 322, and the valve 324. It is also possible to consider including the nozzle 420 in the reaction gas supply system. When the reaction gas flows out from the nozzle 420, the nozzle 420 may also be referred to as a reaction gas nozzle. Furthermore, the inert gas is supplied from gas supply pipes 510 and 520 to the processing chamber 201 via MFCs 512 and 522, valves 514 and 524, and nozzles 410 and 420. The inert gas supply system is mainly composed of the gas supply pipes 510 and 520, the MFCs 512 and 522, and the valves 514 and 524. On the other hand, one end of an exhaust pipe 231, which is an exhaust flow path for discharging the ambient gas of the processing chamber 201, is connected to the wall surface of the manifold 209. An APC (Auto Pressure Controller) valve 243, which is an exhaust valve (pressure adjustment unit) for detecting the pressure inside the processing chamber 201, and a pressure sensor 245 are installed on the exhaust pipe 231. A vacuum pump 246, which is a vacuum exhaust device, is installed at the end of the exhaust pipe 231. The APC valve 243 is configured as a valve that opens and closes the valve in a state where the vacuum pump 246 is operating, thereby enabling vacuum exhaust and stopping of vacuum exhaust in the processing chamber 201. Furthermore, in a state where the vacuum pump 246 is operating, the valve opening degree is adjusted according to the pressure information detected by the pressure sensor 245, thereby enabling adjustment of the pressure in the processing chamber 201. The exhaust system is mainly composed of the exhaust pipe 231, the APC valve 243, and the pressure sensor 245. It is also possible to consider including the vacuum pump 246 in the exhaust system. Below the manifold 209, a sealing cover 219 serving as a furnace port cover that can hermetically seal the lower end opening of the manifold 209 is provided. The sealing cover 219 is configured to abut against the lower end of the manifold 209 from the lower side in the vertical direction. On the upper surface of the sealing cover 219, an O-ring 220 serving as a sealing member that abuts against the lower end of the manifold 209 is provided. On the opposite side of the processing chamber 201 with respect to the sealing cover 219, a rotation mechanism 267 for rotating a susceptor 217 described later is provided. The rotation shaft 255 of the rotation mechanism 267 penetrates the sealing cover 219 and is connected to the susceptor 217. The rotation mechanism 267 is configured to rotate the wafer 200 by rotating the susceptor 217. The sealing cover 219 is configured to be lifted and lowered in the vertical direction by a susceptor elevator 115 serving as a lifting mechanism that is vertically provided outside the processing tube 203. The susceptor elevator 115 is configured to be able to carry the susceptor 217 into and out of the processing chamber 201 by lifting and lowering the sealing cover 219. The susceptor elevator 115 is configured as a transfer device (transfer mechanism) that transfers the susceptor 217, that is, the wafer 200, into and out of the processing chamber 201. In addition, below the manifold 209, a gate 219s serving as a furnace port cover is provided, which can hermetically seal the lower end opening of the manifold 209 during the lowering of the sealing cover 219 by the susceptor elevator 115. On the upper surface of the gate 219s, an O-ring 220c serving as a sealing member that abuts against the lower end of the manifold 209 is provided. The opening and closing operation (lifting and lowering operation or rotating operation, etc.) of the gate 219s is controlled by a gate opening and closing mechanism 115s. In addition, in the processing chamber 201, a temperature sensor 263 serving as a temperature detector is disposed. It adjusts the energization state to the heater 207 based on the temperature information detected by the temperature sensor 263, thereby making the temperature in the processing chamber 201 a desired temperature distribution. The temperature sensor 263 is provided along the inner wall of the processing tube 203 in the same manner as the nozzles 410 and 420. [Vaporization System] Next, the vaporization system 500 will be described with reference to FIG. 3. The vaporization system 500 is a system that vaporizes a liquid raw material stored in a storage tank 610 to generate a vaporized gas as a raw material gas, and supplies the vaporized gas into the processing chamber 201 via a gas supply pipe 310. The vaporization system 500 includes a vaporization unit 600, a replenishment unit 700, and a pressure adjustment unit 800 described later. The vaporization system 500 can also be regarded as including at least a part of a raw material gas supply system. [Vaporization Unit 600] The vaporization unit 600 includes: a storage tank 610 serving as a vaporization container that stores a liquid raw material that becomes a raw material gas by vaporization; a heater 630 serving as a heating unit (heating device) that vaporizes the stored liquid raw material by heating the storage tank 610; and a pressure sensor 640 that detects the pressure inside the storage tank 610. The storage tank 610 is formed, for example, in the shape of a rectangular parallelepiped or a cylinder. The storage space formed inside the storage tank 610 is a sealed space isolated from the outside by closing the valves 620 and 720. The lower end side of the gas supply pipe 310 is connected so as to penetrate the top wall portion of the storage tank 610 and communicate with the inside of the storage space. In a state where the valves 620 and 720 are closed, the liquid raw material is vaporized inside the storage tank 610, and the vaporized gas is filled in the storage tank 610. The filled vaporized gas is pressed toward the gas supply pipe 310 by the pressure inside the storage tank 610. Furthermore, in the vaporization unit 600 of the present embodiment, other gases such as carrier gas are not supplied into the storage tank 610. Therefore, the pressure rise inside the storage tank 610 is mainly caused by the vaporized gas generated by the vaporization of the liquid raw material and the supply (refilling) of the liquid raw material into the storage tank 610, which will be described later. [Refilling unit 700] The refilling unit 700 of the liquid raw material supply system is a device that refills the liquid raw material pumped from the refill tank 760 into the storage tank 610, and includes: a liquid supply pipe 754 as a liquid raw material supply pipeline through which the liquid raw material flows; and an on-off valve, that is, a valve 720. In addition, the refill tank 760 as a supply source of the liquid raw material may be included in the refilling unit 700. In addition, the valve 720 may be configured to control the opening degree by the control unit 121, not limited to performing an opening / closing operation (fully open / fully closed operation), thereby adjusting the flow rate (or pumping pressure) of the liquid raw material. The valve 720 is closed when the liquid raw material is not refilled. The liquid supply pipe 754 is connected so as to penetrate the top wall portion of the storage tank 610, and one end thereof communicates with the inside of the storage tank 610. By opening the valve 720, the liquid raw material in the liquid supply pipe 754 can be pumped into the storage tank 610. At this time, the valve 620 is closed, and the liquid raw material is pumped into the storage tank 610 that has become a sealed space, and this may cause the pressure inside the storage tank 610 to rise rapidly. The refill tank 760 is disposed outside the storage tank 610 and is connected to the other end of the liquid supply pipe 754. A pumping pipe 761 is connected to the upper part of the refill tank 760. The pumping gas is sent into the refill tank 760 from the pumping pipe 761, and the liquid raw material stored in the refill tank 760 is pumped into the liquid supply pipe 754 by the pumping pressure inside the refill tank 760. Furthermore, the pumping pressure inside the refill tank 760 is greater than the pressure inside the storage tank 610. For example, the pressure inside the storage tank 610 is exemplified as 100 to 10,000 Pa, and the pumping pressure from the refill tank 760 is exemplified as 0.1 to 10 MPa, etc. [Pressure Adjustment Unit 800] The pressure adjustment unit 800 includes: an exhaust pipe 810 as an exhaust pipeline, one end of which is directly or indirectly connected to the storage tank 610; an on-off valve, i.e., valve 820, which is provided in the exhaust pipe 810; and an exhaust pump 830 as an exhaust device, which is connected to the exhaust pipe 810 on the downstream side of the valve 820. In this embodiment, the exhaust pipe 810 is connected to the downstream side of the valve 620 of the gas supply pipe 310 and is connected so as to communicate with the inside of the storage tank 610 via the gas supply pipe 310. In this case, the valve 620 can also be regarded as a component constituting the pressure adjustment unit 800. Furthermore, as another aspect, as shown in FIG. 9, the exhaust pipe 810 can also be arranged to be directly connected to the storage tank 610 without passing through the gas supply pipe 310. In addition, it can also be that, instead of having the vacuum pump 830, the exhaust pipe 810 is connected to the exhaust pipe 231 (downstream side of the APC valve 245), and the exhaust is carried out from the exhaust pipe 810 by the vacuum pump 246. In addition, it can also be that, instead of having the vacuum pump 830, the exhaust pipe 810 is connected to the exhaust pipeline provided in the facility where the substrate processing device 10 is installed, and the exhaust is carried out from the exhaust pipe 810 via this exhaust pipeline. In addition, the valve 820 can also be configured such that, not limited to the opening and closing operation (fully open / fully closed operation), its opening degree can be controlled by the control unit 121, thereby adjusting the exhaust flow rate (exhaust speed). When the pressure adjustment in the storage tank 610 is not performed as described later, the valve 820 is closed. In addition, in the exhaust pipe 810, in addition to the valve 820, an MFC configured to be able to adjust the exhaust flow rate in the exhaust pipe 810 can also be further provided. By controlling the flow rate of this MFC by the control unit 121, it can adjust the exhaust speed when performing the pressure adjustment in the storage tank 610. Next, the control unit 121 as a control unit provided in the substrate processing device 10 will be described. As shown in FIG. 4, the control unit 121 is configured as a computer, and it includes a CPU (Central Processing Unit) 121a, a RAM (Random Access Memory) 121b, a memory device 121c, and an I / O port 121d. The RAM 121b, the memory device 121c, and the I / O port 121d are configured to be able to exchange data with the CPU 121a via the internal bus 121e. An input / output device 122 configured as a touch panel or the like is connected to the control unit 121, for example. The memory device 121c is constituted by, for example, a flash memory, an HDD (Hard Disk Drive), etc. In the memory device 121c, various programs such as a control program for controlling the operation of the control board processing device, a liquid raw material replenishment program described later, etc., and data for executing each program are stored in a readable manner. The RAM 121b is configured as a memory area (working area) that temporarily holds programs or data read out by the CPU 121a. The I / O port 121d is connected to the MFCs 312, 322, 512, 522, valves 314, 324, 514, 524, 620, 720, 820, pressure sensors 245, 640, APC valve 243, vacuum pump 246, 830, temperature sensor 263, heater 207, 630, rotation mechanism 267, susceptor elevator 115, gate opening / closing mechanism 115s, etc. The CPU 121a is configured to read out a control program from the memory device 121c for execution, and read out data from the memory device 121c in response to the input of an operation instruction from the input / output device 122, etc. The CPU 121a is configured to control, according to the content of the read data, various gas flow adjustment operations performed by the MFCs 312, 322, 512, 522, opening / closing operations of the valves 314, 324, 514, 524, 620, 720, 820, opening / closing operation of the APC valve 243, pressure adjustment operation of the APC valve 243 according to the pressure sensor 245, opening / closing operation of the valves 620, 820 according to the pressure sensor 640, start and stop of the vacuum pumps 246, 830, temperature adjustment operation of the heater 207 according to the temperature sensor 263, rotation and rotation speed adjustment operation of the susceptor 217 performed by the rotation mechanism 267, lifting operation of the susceptor 217 performed by the susceptor elevator 115, opening / closing operation of the gate 219s performed by the gate opening / closing mechanism 115s, etc. Furthermore, another control unit may be separately provided apart from the control unit 121, which is configured to control the above-described controlled elements constituting the vaporization system 500. The control unit 121 can be constituted by installing a program stored in an external memory device (such as a magnetic disk such as a magnetic tape, a floppy disk, or a hard disk, an optical disk such as a CD or a DVD, a magneto-optical disk such as an MO (magneto-optical disc), a semiconductor memory such as a USB memory or a memory card) 123 into a computer. The memory device 121c or the external memory device 123 is configured as a computer-readable recording medium. Hereinafter, these are collectively referred to simply as the recording medium. When the term recording medium is used in this specification, it may include only the memory device 121c alone, only the external memory device 123 alone, or both. Furthermore, the program may be provided to the computer without using the external memory device 123, but by using communication means such as the Internet or a dedicated line. (2) Substrate Processing Step Next, as a step in the manufacturing process of the semiconductor device, a substrate processing method for the step of processing the substrate using the substrate processing apparatus 10 will be described. Also, as a step in the step of processing the substrate, a control method for the vaporization system 500 for the step of replenishing the liquid raw material into the storage tank 610 will be described. Furthermore, the operations of the respective parts constituting the substrate processing apparatus 10 are controlled by the control unit 121. First, a timing example of forming a film on the wafer 200 using the substrate processing apparatus 10 will be described with reference to FIG. 5. In the present embodiment, the processing chamber 201 containing a plurality of wafers 200 in a stacked state is heated to a predetermined temperature. Then, the raw material gas supply step and the reaction gas supply step are performed a predetermined number of times (n times, where n is an integer of 1 or more); in the raw material gas supply step, a raw material gas containing a predetermined element is supplied to the processing chamber 201 from the supply hole 410a of the nozzle 410; in the reaction gas supply step, a reaction gas is supplied to the processing chamber 201 from the supply hole 420a of the nozzle 420. Thereby, a film containing a predetermined element is formed on the wafer 200. The predetermined number of times (n times) here is one batch process in the film formation process, which has been preset. [Loading, Loading In] First, a plurality of wafers 200 are loaded on the susceptor 217 (wafer loading). The gate 219s is moved by the gate opening / closing mechanism 115s to open the lower end opening of the manifold 209 (gate opening). Next, as shown in FIG. 1, the susceptor 217 on which a plurality of wafers 200 are loaded is lifted by the susceptor elevator 115 and loaded into the processing chamber 201 (susceptor loading). In this state, the seal cover 219 seals the lower end of the manifold 209 via the O-ring 220b. [Pressure, Temperature Adjustment] Next, vacuum exhaust is performed by the vacuum pump 246 to make the processing chamber 201 reach a desired pressure (vacuum degree). At this time, the pressure in the processing chamber 201 is measured by the pressure sensor 245, and the APC valve 243 performs feedback control (pressure adjustment) based on the measured pressure information. The vacuum pump 246 remains in an operating state at least until the processing of the wafer 200 is completed. In addition, the heater 207 is used for heating to make the processing chamber 201 reach the desired temperature. The heating of the processing chamber 201 by the heater 207 continues at least during the period until the processing of the wafer 200 is completed. Furthermore, the susceptor 217 and the wafer 200 are rotated by the rotation mechanism 267. The rotation of the susceptor 217 and the wafer 200 by the rotation mechanism 267 continues at least during the period until the processing of the wafer 200 is completed. [Film formation process (an example of substrate processing)] [Raw material gas supply step] Next, the valves 314 and 620 are opened, and the vaporized gas in the storage tank 610, that is, the raw material gas, is supplied into the processing chamber 201 through the gas supply pipe 310. As the raw material gas, one or more of the gases obtained by vaporizing the liquid raw material in the storage tank 610 can be used. Furthermore, during the period when the subsequent liquid raw material replenishment step is not performed, the valve 820 of the pressure adjustment unit 800 is always closed. Here, the storage tank 610 and the stored liquid raw material are heated by the heater 630. Due to being heated, the liquid raw material vaporizes to generate the raw material gas (vaporized gas). Before the raw material gas is about to be supplied to the processing chamber 201, the valve 620 is closed, and the storage tank 610 is in a state filled with the raw material gas. The pressure in the storage tank 610 decreases during the period of supplying the raw material gas (that is, the period when the valves 314 and 620 are opened), and rises due to the vaporization of the liquid raw material during the period of stopping the supply of the raw material gas (that is, the period when the valves 314 and 620 are closed). FIG. 6 shows the state of the pressure in the storage tank 610 over time in this embodiment. For example, as shown in the pressure change state before time T0 in FIG. 6, during the period of one batch process in the film formation process, the pressure decreases a predetermined number of times (n times) due to the supply of the raw material gas, and the pressure rises due to the stop of the supply of the raw material gas. In this way, by repeating the vaporization and supply of the liquid raw material one or multiple times, the liquid raw material in the storage tank 610 is consumed. In this embodiment, for each batch process, the liquid raw material is replenished into the storage tank 610 (replenishment step). However, the liquid raw material replenishment step can also be set to be performed in each of the multiple batch processes. The raw material gas supplied from the storage tank 610 is adjusted in flow rate by the MFC 312 and supplied into the processing chamber 201 from the supply hole 410a of the nozzle 410. At the same time, the valve 514 is opened to allow the carrier gas to flow into the gas supply pipe 510. The carrier gas is adjusted in flow rate by the MFC 512, and is supplied into the processing chamber 201 together with the raw material gas from the supply hole 410a of the nozzle 410, and is discharged from the exhaust pipe 231. Furthermore, in order to prevent the raw material gas from invading toward the nozzle 420 (prevent backflow), the valve 524 is opened to allow the carrier gas to flow into the gas supply pipe 520. The carrier gas is supplied toward the processing chamber 201 via the gas supply pipe 520 and the nozzle 420, and is discharged from the exhaust pipe 231. At this time, the APC valve 243 is appropriately adjusted to set the pressure in the processing chamber 201 to a pressure within a range of, for example, 1 to 1000 Pa. Furthermore, in this specification, regarding the range of numerical values, for example, when it is described as 1 to 1000 Pa, it means 1 Pa or more and 1000 Pa or less. That is, 1 Pa and 1000 Pa are included within the range of its numerical values. The same applies to other numerical value ranges described in this specification. The supply flow rate of the raw material gas controlled by the MFC 312 is, for example, set within a range of 10 to 2000 sccm, preferably within a range of 50 to 1000 sccm, and more preferably within a range of 100 to 500 sccm. The time for supplying the raw material gas to the wafer 200 is, for example, set within a range of 1 to 60 seconds. The heater 207 is controlled to bring the temperature of the wafer 200 to, for example, within a range of 400 to 600 °C. When supplying the raw material gas to the processing chamber 201 under the above conditions, a containing layer containing a predetermined element in the raw material gas is formed on the outermost surface of the wafer 200. An inert gas can be, for example, nitrogen (N 2 ), or noble gases such as argon (Ar), helium (He), neon (Ne), xenon (Xe), etc. One or more of these gases can be used as the inert gas. The same applies to each of the steps described later. In addition, the raw material gas is, for example, a gas containing a semiconductor element such as silicon (Si), or a gas containing a predetermined element such as metal elements titanium (Ti), zirconium (Zr), hafnium (Hf), tantalum (Ta), aluminum (Al), molybdenum (Mo), tungsten (W), etc., and a gas that has a liquid state at normal temperature and pressure (i.e., liquid raw material) can be used. By vaporizing the liquid raw material of these gases in the storage tank 610, the raw material gas can be obtained. For example, liquid raw materials such as the following gases can be used: monochlorosilane (SiH 3 Cl) gas, dichlorosilane (SiH 2 Cl 2 ) gas, trichlorosilane (SiHCl 3 ) gas, tetrachlorosilane (SiCl 4 ) gas, hexachlorodisilane (Si 2 Cl 6 ) Gas, octachlorotrisilane (Si 3 Cl 8 ) Gas, 1,2-bis(trichlorosilyl)ethane ((SiCl 3 ) 2 C 2 H 4 ) Gas, bis(trichlorosilyl)methane ((SiCl 3 ) 2 CH 2 ) Gas, 1,1,2,2-tetrachloro-1,2-dimethyldisilane ((CH 3 ) 2 Si 2 Cl 4 ) Gas, 1,2-dichloro-1,1,2,2-tetramethyldisilane ((CH 3 ) 4 Si 2 Cl 2 ) Gas, 1-monochloro-1,1,2,2,2-pentamethyldisilane ((CH 3 ) 5 Si 2 Cl) Gas, trifluorosilane (SiHF 3 ) Gas, tetrafluorosilane (SiF 4 ) Gas, tribromosilane (SiHBr 3 ) Gas, tetrabromosilane (SiBr 4 ) Gas and other halogenated silane raw material gases; trisilane (Si 3 H 8 ) Gas, tetrasilane (Si 4 H 10 ) Gas, pentasilane (Si 5 H 12 ) Gas, hexasilane (Si 6 H 14 ) Gas and other inorganic silane raw material gases; tetrakis(dimethylamino)silane (Si[N(CH 3 ) 2 4 ) Gas, tris(dimethylamino)silane (Si[N(CH 3 ) 2 3 H) gas, bis(diethylamino)silane (Si[N(C 2 H 5 ) 2 2 H 2 ) and bis(tert-butylamino)silane (SiH 2 [NH(C 4 H 9 )] 2 ) gas and various amino silane raw material gases; 1,4-disilabutane (Si 2 C 2 H 10 ) gas and other organic silane raw material gases. In addition, for example, liquid raw materials such as the following gases can be used: tetra(dimethylamino)titanium (Ti[N(CH 3 ) 2 4 )(Gas, titanium tetrachloride (TiCl 4 )(Gas; tetra(ethylmethylamido)hafnium (Hf[N(C 2 H 5 )(CH 3 )] 4 )(Gas, hafnium tetrachloride (HfCl 4 )(Gas; tetra(ethylmethylamido)zirconium (Zr[N(C 2 H 5 )(CH 3 )] 4 )(Gas; trimethylaluminum (Al(CH 3 ) 3 )(Gas; pentaethoxytantalum (Ta(OC 2 H 5 ) 5 ), triethylmethylamido-tert-butylimido tantalum (Ta[NC(CH 3 ) 3 [N(C 2 H 5 )CH 3 3 ), pentaethoxytantalum (Ta(OC 2 H 5 ) 5 ) gas. [Residual Gas Removal Step] After forming a layer containing a predetermined element, valves 314 and 620 are closed to stop the supply of the source gas. At this time, with the APC valve 243 kept open, the processing chamber 201 is evacuated by the vacuum pump 246 to remove the unreacted source gas remaining in the processing chamber 201 or the source gas after assisting in forming the layer containing the predetermined element from the processing chamber 201. With valves 514 and 524 open, a carrier gas is continuously supplied to the processing chamber 201. The carrier gas acts as a purge gas, which can enhance the effect of removing the unreacted source gas remaining in the processing chamber 201 or the source gas after assisting in forming the layer containing the predetermined element from within the processing chamber 201. [Reaction Gas Supply Step] After removing the residual gas in the processing chamber 201, valve 324 is opened to allow the reaction gas to flow into the gas supply pipe 320. The reaction gas contains, for example, oxygen (O), and an oxygen-containing gas (oxidizing gas, oxidant) that can be used as a reaction gas (reactant) for reacting with the predetermined element contained in the source gas can be used. The oxygen-containing gas can be, for example, oxygen gas (O 2 ), ozone (O 3 ), plasma-excited O 2 gas (O 2 *), O 2 gas + hydrogen gas (H 2 ), water vapor (H 2 O gas), hydrogen peroxide (H 2 O 2 ), nitrous oxide (N 2 O) gas, nitric oxide (NO) gas, nitrogen dioxide (NO 2 ) gas, carbon monoxide (CO) gas, carbon dioxide (CO 2 ) gas, etc. One or more of these gases can be used as the reaction gas. The flow rate of the reaction gas is adjusted by the MFC 322, supplied from the supply hole 420a of the nozzle 420 to the wafer 200 in the processing chamber 201, and discharged from the exhaust pipe 231. That is, the wafer 200 is exposed to the reaction gas. At this time, valve 524 is opened to allow the carrier gas to flow into gas supply pipe 520. The carrier gas is adjusted in flow rate by MFC 522, supplied into processing chamber 201 together with the reaction gas, and discharged from exhaust pipe 231. At this time, in order to prevent the reaction gas from invading into nozzle 410 (prevent backflow), valve 514 is opened to allow the carrier gas to flow into gas supply pipe 510. The carrier gas is supplied into processing chamber 201 via gas supply pipe 510 and nozzle 410, and discharged from exhaust pipe 231. At this time, APC valve 243 is appropriately adjusted to set the pressure in processing chamber 201 to a pressure within the range of, for example, 1 to 1000 Pa. The supply flow rate of the reaction gas controlled by MFC 322 is set, for example, within the range of 5 to 40 slm, preferably within the range of 5 to 30 slm, and more preferably within the range of 10 to 20 slm. The time for supplying the reaction gas to wafer 200 is set, for example, within the range of 1 to 60 seconds. Other processing conditions are set to the same processing conditions as those in the aforementioned raw material gas supply step. When an oxygen-containing gas is supplied as the reaction gas to processing chamber 201 under the aforementioned conditions, in the reaction gas supply step, the reaction gas reacts with at least a part of the containing layer of the predetermined element formed on wafer 200 to oxidize the containing layer of the predetermined element, and an oxide layer containing the predetermined element and O is formed. That is, the containing layer of the predetermined element is modified into an oxide layer containing the predetermined element. [Residual gas removal step] After the oxide layer is formed, valve 324 is closed to stop the supply of the reaction gas. Moreover, by the same processing procedure as the residual gas removal step after the raw material gas supply step, the unreacted reaction gas or the reaction gas or reaction by-products after assisting in the formation of the oxide layer remaining in processing chamber 201 are removed from processing chamber 201. The cycles of the vaporization step, raw material gas supply step, residual gas removal step, reaction gas supply step, and residual gas removal step described above are sequentially performed, and a predetermined number of times (n times) are executed. Thus, by performing a plurality of steps a predetermined number of times in one batch process, an oxide film obtained by forming a laminated oxide layer on wafer 200 is formed. Furthermore, the so-called batch process refers to the following process: The cycles of the raw material gas supply step, residual gas removal step, reaction gas supply step, and residual gas removal step are sequentially performed, and a predetermined number of times (n times) are executed to form a film with a predetermined thickness on wafer 200. Moreover, in one batch, a film with a predetermined thickness is formed on wafer 200. [Exhaust, Pressure Adjustment] A film of a predetermined thickness is formed on the wafer 200. After the residual gas removal step is completed, valves 514 and 524 are opened, and a carrier gas is supplied from each of the gas supply pipes 310 and 320 toward the processing chamber 201, and is discharged from the exhaust pipe 231. The carrier gas functions as a purge gas, and the gas or reaction by-products remaining in the processing chamber 201 are removed from the processing chamber 201 (post-purge). Then, the ambient gas in the processing chamber 201 is replaced with the carrier gas, and the pressure in the processing chamber 201 is restored to normal pressure (atmospheric pressure restoration). [Unloading, Removal] Then, the sealing lid 219 is lowered by the susceptor elevator 115 to open the lower end of the manifold 209, and the processed wafer 200 is unloaded from the lower end of the manifold 209 to the outside of the processing tube 203 while being supported by the susceptor 217 (susceptor unloading). After unloading, the gate 219s is moved, and the lower end opening of the manifold 209 is sealed by the gate 219s (gate closing). After the processed wafer 200 is unloaded to the outside of the processing tube 203, it is removed from the susceptor 217 (wafer removal). Furthermore, in this embodiment, for each batch, the wafer 200 is loaded into and unloaded from the processing tube 203 (processing chamber 201). As described above, after the wafer 200 on which a film of a predetermined thickness has been formed through each process (step) is taken out, when a film is to be formed on another wafer 200, "loading, loading-in", "pressure, temperature adjustment", "film formation process", "exhaust, pressure adjustment", and "unloading, removal" are performed again. That is, the batch process for the wafer 200 is performed again. Through the above film formation process, an oxide film containing a predetermined element in the source gas can be formed on the wafer 200. For example, using the above source gas, an oxide film such as a titanium oxide film (TiO film), a zirconium oxide film (ZrO film), a hafnium oxide film (HfO film), a tantalum oxide film (TaO film), an aluminum oxide film (AlO film), a molybdenum oxide film (MoO film), a tungsten oxide film (WO film), etc. can be formed. In addition, for example, a nitride film such as a titanium nitride film (TiN film), a zirconium nitride film (ZrN film), a hafnium nitride film (HfN film), a tantalum nitride film (TaN film), an aluminum nitride film (AlN film), a molybdenum nitride film (MoN film), a tungsten nitride film (WN film), etc. can be formed by using a nitrogen-containing gas (nitriding gas, nitriding agent) instead of an oxygen-containing gas as the reaction gas. [Liquid Raw Material Supplement Step] After the raw material gas supply step in one batch process is completed, the liquid raw material is replenished into the storage tank 610 (replenishment step). The replenishment step is carried out during the period from when the valves 314 and 620 are closed after the raw material gas supply step in one batch process is completed to when the valves 314 and 620 are opened at the start of the raw material gas supply step in the next batch process. The replenishment step can be carried out simultaneously with other steps in one batch process, and in addition, it can also be carried out simultaneously with steps other than that. Furthermore, in this embodiment, the replenishment step is carried out for each batch, but as described above, the replenishment step can also be carried out once for every plural batches. (Step A: Liquid Raw Material Supply Step) After the raw material gas supply step is completed, with the valve 620 closed, by opening the valve 720, the liquid raw material in the liquid supply pipe 754 can be pressed into the storage tank 610. By opening the valve 720 for a predetermined period of time and then closing it, a predetermined amount of liquid raw material can be supplied (replenished) into the storage tank 610. At this time, as described above, with the valve 620 closed, when the liquid raw material is pressed into the storage tank 610 which is a sealed space, the pressure in the storage tank 610 may rise rapidly. As an example, in FIG. 6, when the supply of the liquid raw material starts at time T0 and stops at time T1, the pressure in the storage tank 610 rises to the pressure Pf. Here, the pressure in the storage tank 610 at time T1 becomes high, resulting in a state where it is easy for the liquid raw material to have poor vaporization. In particular, when the pressure rises to a value exceeding the saturated vapor pressure of the liquid raw material (the temperature at this time point), it will significantly easily cause poor vaporization of the liquid raw material, and in addition, there is also a possibility that a part of the vaporized gas in the storage tank 610 will liquefy. When the fine droplets generated due to poor vaporization are supplied into the processing chamber 201 together with the raw material gas in the raw material gas supply step, they will adhere to the surface of the wafer 200 etc., and become the main cause for reducing the quality of the product. Here, in this embodiment, in the next step B, the pressure in the storage tank 610 is adjusted. (Step B: First Pressure Adjustment Step) After step A is completed, with the valve 314 closed, by opening the valves 620 and 820, the ambient gas in the storage tank 610 is exhausted through the exhaust pipe 810 to adjust the pressure by reducing the pressure in the storage tank 610. The vacuum pump 830 is maintained in an operating state at least during the implementation of this step. In this embodiment, as shown in the example of FIG. 6, at the time point when step A ends (i.e., time T1), or immediately thereafter, pressure adjustment is started and pressure adjustment is performed during a predetermined time (the first pressure adjustment time). That is, pressure adjustment is performed during the period from time T1 to T2. By the pressure adjustment, the pressure in the storage tank 610 is reduced to the first predetermined pressure, i.e., pressure Pt. At time T2, by closing the valves 620 and 820, this step (i.e., pressure adjustment) is ended. In this step, by reducing the pressure in the storage tank 610, the possibility of poor vaporization of the liquid raw material can be reduced. Further, preferably, the pressure Pt after depressurization is less than the saturated vapor pressure of the liquid raw material (the temperature at this time point). By reducing the pressure in the storage tank 610 to less than the saturated vapor pressure, the possibility of poor vaporization of the liquid raw material can be significantly reduced. Furthermore, the pressure adjustment in this step is not limited to the aspect of ending after a predetermined time as described above, and it can also be set to end at the time point when the pressure in the storage tank 610 detected by the pressure sensor 640 becomes below a predetermined pressure (for example, at the time point when it becomes the predetermined pressure). In this case, the predetermined pressure is preferably also set to a pressure less than the saturated vapor pressure of the liquid raw material. Furthermore, the time point to start this step is not limited to the time point when step A ends or immediately after it as shown in the example of FIG. 6. As shown in the example of FIG. 7, it can also be set to the time point (time T1-2) after a predetermined time has elapsed from the time point (time T1-1) when step A ends. In this way, starting from the end of step A, pressure adjustment is performed after setting a fixed time interval, whereby it is possible to suppress the situation where minute droplets or the like that may occur in the storage tank 610 during pressure adjustment adhere to the gas supply pipe 310 and cause corrosion or the like. Furthermore, this predetermined time (the time from time T1-1 to time T1-2) is preferably shorter than the time for performing the subsequent pressure stabilization step (step C) (the time from time T2 to time T3). When this predetermined time is equal to or longer than the time for performing the pressure stabilization step, the period from time T1-1 to time T1-2 when the poor vaporization state is likely to occur becomes longer, and the effect of this step (pressure adjustment) for suppressing the occurrence of poor vaporization cannot be obtained sufficiently. (Step C: Pressure Stabilization Step) After step B ends, by closing the valve 620, the inside of the storage tank 610 is set to a closed state. Inside the storage tank 610 that has become a closed state, the liquid raw material is heated and vaporized, thereby increasing (restoring) the pressure in the storage tank 610. By fully obtaining the duration of this step, the temperature of the liquid raw material in the storage tank 610 can be stabilized, and then the pressure in the storage tank 610 can be increased to the pressure Ps near the saturated vapor pressure of the liquid raw material at the (stable temperature). This step ends according to the time point when the next batch process starts to execute. For example, starting from the time point when the raw material gas supply step in the next batch process begins, the time for executing the subsequent step D (the second pressure adjustment step) and step E (the pressure increase step) is traced back, and this step ends at that time point. More specifically, for example, this step ends at the time point after tracing back the above time starting from the start time of the raw material gas supply step in the next batch process set in advance, or from the start time of the raw material gas supply step in the next batch process instructed by the user to the control unit 121. In addition, this step can also be set to, for example, continue until the change rate of the pressure value (the slope of the change of the pressure value with respect to time) in the storage tank 610 becomes below a predetermined value. In addition, this step can also be set to continue for at least a predetermined time (i.e., the third predetermined time) set in advance. This predetermined time is set to be the time when the change rate of the pressure value becomes small enough, which can be obtained, for example, through prior experiments, etc. In addition, this step can also be set to continue until the pressure value in the storage tank 610 rises to a predetermined pressure (i.e., the second predetermined pressure) set in advance. This predetermined pressure is set to be the pressure when the change rate of the pressure value becomes small enough, which can be obtained, for example, through prior experiments, etc. (Step D: The second pressure adjustment step) After step C ends, similar to step B, with the valve 314 closed, the ambient gas in the storage tank 610 is discharged through the exhaust pipe 810 to perform pressure adjustment, and the storage tank 610 is depressurized as a pre-step for the raw material gas supply step in the next batch process. The vacuum pump 830 is maintained in an operating state at least during the implementation of this step. In this embodiment, as shown in the example of FIG. 6, at the time point (i.e., time T3) when step C ends, or immediately after that, pressure adjustment starts and is performed for a predetermined time (the second pressure adjustment time). That is, pressure adjustment is performed during the period from time T3 to T4. By pressure adjustment, the pressure in the storage tank 610 is reduced to the pressure Pu. At time T4, the valves 620 and 820 are closed, thereby ending this step (i.e., pressure adjustment). Here, the time for performing step B (the first pressure adjustment step) is longer than the time for performing step D (the second pressure adjustment step). The pressure Pf in the storage tank 610 at the time point when step B starts is higher than the pressure Ps at the time point when step D starts. Therefore, by setting the time for decompression in step B to be longer, the pressure in the storage tank 610 can be surely reduced to the desired pressure. For example, each step is performed in such a way that the time Tb for performing step B and the time Td for performing step D satisfy 1 < Tb / Td ≤ 20. In addition, it can also be that by adjusting the opening degree of the valve 820, the exhaust speed of the storage tank 610 in step B is made smaller than the exhaust speed of the storage tank 610 in step D. By adjusting the exhaust speed in this way, it can easily control that the pressure in the storage tank 610 in step B does not decrease excessively. Furthermore, it can also be that in step B (the first pressure adjustment step) and step D (the second pressure adjustment step), by adjusting the opening degree of the valve 820, the exhaust speed of the storage tank 610 in step B is made smaller than the exhaust speed of the storage tank 610 in step D. By adjusting the exhaust speed in this way, the following situation can be suppressed: the pressure in the storage tank 610 in step B decreases excessively, resulting in the rapid gasification of the liquid raw material, being discharged and consumed, etc. Furthermore, the adjustment of the exhaust speed can also be set to be performed by the MFC provided in the exhaust pipe 810. (Step E: Pressure increase step) After step D is completed, similar to step C, by closing the valve 620, the inside of the storage tank 610 is made airtight. Inside the airtight storage tank 610, the liquid raw material is heated and gasified, thereby increasing (restoring) the pressure in the storage tank 610 to the pressure at which the required amount of raw material gas can be supplied in the raw material gas supply step. After this step, by opening the valves 314 and 620, the raw material gas supply step in the next batch process is started. (3) Comparison with the comparative example Here, as a comparative example with respect to this embodiment, the situation where step B (the first pressure adjustment step) and step D (the second pressure adjustment step) are not performed is described. FIG. 8 shows an example of the change in the pressure in the storage tank 610 over time in the comparative example. In the comparative example, after the pressure in the storage tank 610 rises to the pressure Pf' in step A, no pressure adjustment is performed, and the state of closing the valve 620 is maintained during the period from time T1' to time T3'. During this period, the pressure in the storage tank 610 changes in the direction of decreasing to the saturated vapor pressure of the liquid raw material, and becomes stable at the pressure Ps'. However, in the case of the comparative example, during the period of change in the pressure decreasing direction, the pressure exceeds the saturated vapor pressure, and the state where gasification failure is likely to occur continuously. Therefore, after T3', when the raw material gas supply step starts in the next batch process, the possibility that mists of the liquid raw material generated due to gasification failure and the raw material gas are supplied into the processing chamber 201 together becomes high. On the other hand, in the embodiment of the present invention, as shown in FIG. 6, in step B, the pressure in the storage tank 610 is particularly reduced to a pressure lower than the saturated vapor pressure of the liquid raw material. Thereby, in step C, the pressure changes in the direction of rising to the saturated vapor pressure and tends to be stable. Thus, in the embodiment of the present invention, by making the pressure approach saturation while rising, it can maintain a state where gasification failure of the liquid raw material is not likely to occur while stabilizing the pressure. Furthermore, in the embodiment of the present invention, in step D, the pressure in the storage tank 610 is reduced as a pre-step of the raw material gas supply step in the next batch process, whereby the possibility that the vaporized gas supplied into the processing chamber 201 in the raw material gas supply step contains mists generated due to gasification failure of the liquid raw material can be further reduced. <Other aspects of the present invention> As described above, the aspects of the present invention have been specifically described. However, the present invention is not limited to the above aspects, and various changes can be made without departing from the spirit of the present invention. In the above embodiment, the case where the pressure in the storage tank 610 is increased in step A of the liquid raw material replenishment step and then the pressure is adjusted in step B has been described. However, the present invention is not limited to such an aspect. For example, it may also be that at least either the pumping pressure or the supply flow rate of the liquid raw material supplied in step A is adjusted to a value below the saturated vapor pressure of the liquid raw material at which the pressure in the storage tank 610 at the end of step A becomes a predetermined pressure. More specifically, it may be set to adjust the opening degree of the valve 720 in step A so that at least either the pumping pressure or the supply flow rate becomes the above value. In addition, it may also be set to further provide a liquid MFC in the liquid supply pipe 754, and by controlling the liquid MFC, at least either the pumping pressure or the supply flow rate is adjusted. In addition, it can also be set to provide an orifice portion (aperture portion) in the liquid supply pipe 754, or provide a nozzle having an aperture portion at the front end of the liquid supply pipe 754, thereby making at least one of the pressure for pumping the liquid raw material or the supply flow rate be below the above value. In this way, by adjusting the pressure in the storage tank 610 at the end of step A to a value below the saturated vapor pressure of the liquid raw material, it is possible to suppress the occurrence of poor vaporization due to the increase in pressure in the storage tank 610 in the same manner as in the above embodiment. Preferably, the recipes for each process are prepared individually corresponding to the process content, and are pre-recorded and stored in the memory device 121c via an electrical communication line or an external memory device 123. Moreover, preferably, at the start of each process, the CPU 121a appropriately selects a suitable recipe corresponding to the process content from a plurality of recipes recorded and stored in the memory device 121c. Thereby, it can reproducibly form films of various film types, composition ratios, film qualities, and film thicknesses by one substrate processing apparatus. In addition, it can also reduce the burden on the operator, avoid operation errors, and quickly start various processes. The above recipes are not limited to the case of re-production. For example, they can also be prepared by changing the existing recipes already installed in the substrate processing apparatus. When changing the recipe, it can also be set to install the changed recipe in the substrate processing apparatus via an electrical communication line or a recording medium recording the recipe. In addition, it can also be set to directly change the existing recipe installed in the substrate processing apparatus by operating the input / output device 122 provided in the existing substrate processing apparatus. In the above aspect, an example of forming a film using a batch-type substrate processing apparatus that processes a plurality of substrates at one time has been described. However, the present invention is not limited to the above aspect. For example, it can also be suitably applied to the case of forming a film using a single-substrate processing apparatus that processes one or several substrates at one time. In addition, in the above aspect, an example of forming a film using a substrate processing apparatus having a hot-wall type processing furnace has been described. However, the present invention is not limited to the above aspect, and it can also be suitably applied to the case of forming a film using a substrate processing apparatus having a cold-wall type processing furnace. When using these substrate processing apparatuses, each process can also be performed using the same processing procedures and processing conditions as in the above aspect or modification example, and the same effects as in the above aspect or modification example can be obtained. The above aspect or modification example can be suitably combined and used. The processing procedures and processing conditions at this time can be set to be the same as the processing procedures and processing conditions of the above aspect or modification example, for example. 10: Substrate processing apparatus 115: Cassette elevator 115s: Gate opening / closing mechanism 121: Control unit (controller) 121a: CPU 121b: RAM 121c: Memory device 121d: I / O port 121e: Internal bus 122: Input / output device 123: External memory device 200: Wafer 201: Processing chamber 202: Processing furnace 203: Processing tube 207, 630: Heater 209: Manifold 217: Cassette 218: Heat insulating cylinder 219: Sealing lid 219s: Gate 220, 220b, 220c: O-ring 231, 810: Exhaust pipe 243: APC valve 245, 640: Pressure sensor 246: Vacuum pump 255: Rotating shaft 263: Temperature sensor 267: Rotating mechanism 310, 320, 510, 520: Gas supply pipe 312, 322, 512, 522: Mass flow controller (MFC) 314, 324, 325, 514, 524, 620, 720, 820: Valve 410, 420: Nozzle 410a, 420a: Supply hole 500: Vaporization system 600: Vaporization section 610: Storage tank 700: Refilling section 754: Liquid supply pipe 760: Refilling tank 761: Pressurizing pipe 800: Pressure adjustment section 830: Exhaust pump (vacuum pump) FIG. 1 is a schematic configuration diagram of a vertical processing furnace of a substrate processing apparatus that can be suitably used in one aspect of the present invention, and is a diagram showing a part of the processing furnace 202 in a longitudinal sectional view. FIG. 2 is a schematic configuration diagram of a vertical processing furnace of a substrate processing apparatus that can be suitably used in one aspect of the present invention, and is a diagram showing a part of the processing furnace 202 in a sectional view taken along line L in FIG. 1. FIG. 3 is a configuration diagram showing a vaporization system provided in a substrate processing apparatus that can be suitably used in one aspect of the present invention. FIG. 4 is a schematic configuration diagram of a controller 121 of a substrate processing apparatus that can be suitably used in one aspect of the present invention, and is a diagram showing a control system of the controller 121 in a block diagram. FIG. 5 is a diagram showing a film formation timing when film formation is performed on a wafer in one aspect of the present invention. FIG. 6 is a diagram showing the relationship between the passage of time and the pressure in the vaporization container in one aspect of the present invention. FIG. 7 is a diagram showing the relationship between the passage of time and the pressure in the vaporization container in another aspect of the present invention. FIG. 8 is a diagram showing the relationship between the passage of time and the pressure in the vaporization container in a comparative example of the present invention. FIG. 9 is a configuration diagram showing a vaporization system provided in a substrate processing apparatus that can be suitably used in another aspect of the present invention. 121: Control unit (controller) 310: Gas supply pipe 500: Vaporization system 600: Vaporization section 610: Storage tank 620, 720, 820: Valve 630: Heater 640: Pressure sensor 700: Refilling section 754: Liquid supply pipe 760: Refilling tank 761: Pressurized piping 800: Pressure adjustment section 810: Exhaust pipe 830: Exhaust pump (vacuum pump)

Claims

1. A method for controlling a vaporization system, comprising the following steps: (a) supplying a liquid raw material to a vaporization container that is set to a closed state; (b) adjusting the pressure at the end of (a) or after a predetermined time from that point to reduce the pressure in the vaporization container; (c) after (b) vaporizing the liquid raw material without supplying a carrier gas to the vaporization container while maintaining the state in which the pressure adjustment in the vaporization container has been stopped, which is set to a closed state; and (d) after (c) supplying the vaporized gas generated by vaporizing the liquid raw material in the vaporization container to a processing container for processing a substrate.

2. The control method for the gasification system of claim 1 further includes the following steps: (e) adjusting the pressure between (c) and (d) to reduce the pressure inside the gasification container.

3. The control method for the gasification system as described in claim 2, wherein, The time required for pressure adjustment in (b) is longer than the time required for pressure adjustment in (e).

4. The control method for the gasification system as described in claim 2, wherein, The exhaust velocity in the vaporization container in (b) is lower than the exhaust velocity in the vaporization container in (e).

5. The control method for the gasification system of claim 2 further includes the following steps: (f) maintaining the state in which the pressure adjustment in the gasification container has been stopped between (e) and (d).

6. The control method for the gasification system as described in Request 1, wherein, During the period from start (a) to start (d), the supply of the aforementioned vaporized gas to the aforementioned processing container shall not be carried out.

7. The control method for the gasification system as described in Request 1, wherein, In (b), pressure is adjusted until the pressure inside the vaporization container becomes the saturated vapor pressure of the liquid raw material inside the vaporization container.

8. The control method for the gasification system as described in Request 1, wherein, In (b), pressure adjustment is performed during the period up to the second predetermined time.

9. The control method for the gasification system as described in claim 1, wherein, In (b), pressure adjustment is performed until the pressure inside the vaporization container is reduced to the first predetermined pressure.

10. The control method for the gasification system as described in claim 1, wherein, In (a), the liquid raw material is supplied to the vaporization container in a closed state.

11. A method for manufacturing a semiconductor device, comprising the following steps: (a) supplying a liquid raw material to a vaporization container that is set to a sealed state; (b) adjusting the pressure at the end of (a) or after a predetermined time from that point to reduce the pressure in the vaporization container; (c) after (b) vaporizing the liquid raw material without supplying a carrier gas to the vaporization container while maintaining the state in which the pressure adjustment in the vaporization container has been stopped, which is set to a sealed state; and (d) after (c) supplying the vaporized gas generated by vaporizing the liquid raw material in the vaporization container to a processing container for processing a substrate.

12. The method for manufacturing a semiconductor device as claimed in claim 11 further comprises the following steps: (e) before (d), a step of moving the substrate into the processing container; and (f) after (d), a step of removing the substrate from the processing container; wherein (a), (b) and (c) are performed at least once each time (e) and (f) are performed.

13. The method for manufacturing a semiconductor device according to claim 11 further comprises the following steps: (e) before (d), a step of moving the substrate into the processing container; and (f) after (d), a step of removing the substrate from the processing container; and (a), (b) and (c) are performed at least once each time (e) and (f) are performed.

14. A substrate processing apparatus comprising: a vaporization container for vaporizing a liquid raw material inside; a liquid raw material supply system for supplying the liquid raw material to the vaporization container; a vaporization gas supply system for supplying vaporized gas generated by vaporizing the liquid raw material in the vaporization container to a processing container for processing the substrate; a pressure adjustment unit for adjusting the pressure inside the vaporization container; a heating unit for heating the liquid raw material inside the vaporization container; and a control unit configured to control the liquid raw material supply system, the vaporization gas supply system, the pressure adjustment unit, and the heating unit to perform the following processes: (a) supplying the liquid raw material to the vaporization container, which is in a sealed state; (b) adjusting the pressure at the end of (a) or after a first predetermined time from that point to reduce the pressure inside the vaporization container; (c) ... After (b), the liquid raw material is vaporized without supplying carrier gas to the vaporization container, while maintaining the state in which the pressure adjustment in the vaporization container has been stopped and is set to a sealed state; and (d) after (c), the vaporized gas is supplied to the processing container.

15. The substrate processing apparatus of claim 14, wherein, The pressure regulating unit is composed of: an exhaust pipe, one end of which is directly or indirectly connected to the vaporization container and the other end of which is connected to the exhaust device; and a first on / off valve, which is provided on the exhaust pipe; the control unit is in (b) and reduces the pressure in the vaporization container by controlling at least one of the opening or closing or opening degree of the first on / off valve.

16. The substrate processing apparatus as claimed in claim 15, wherein, The pressure adjustment system further includes: a flow controller, which is installed on the exhaust pipe; the control system in (b) adjusts the flow rate in the exhaust pipe by controlling the flow controller.

17. The substrate processing apparatus of claim 14, wherein, The liquid raw material supply system is composed of the following: a liquid raw material supply pipe, one end of which is connected to the vaporization container and the other end of which is connected to the liquid raw material supply source; and a second on / off valve, which is provided on the liquid raw material supply pipe; the control unit is in (a) that supplies the liquid raw material into the vaporization container by controlling at least one of the opening or closing or opening degree of the second on / off valve.

18. The substrate processing apparatus of claim 14, wherein, The aforementioned vaporized gas supply system comprises: a vaporized gas supply pipe, one end of which is directly or indirectly connected to the vaporization container and the other end of which is connected to the processing container; and a third on / off valve disposed on the vaporized gas supply pipe; the aforementioned control unit is configured to supply the vaporized gas from the vaporization container to the processing container by controlling at least one of the opening or closing or the opening degree of the third on / off valve.

19. The substrate processing apparatus as claimed in claim 14, wherein, The aforementioned liquid raw material supply system includes a liquid raw material supply pipe, one end of which is connected to the aforementioned vaporization container and the other end of which is connected to the aforementioned liquid raw material supply source. An orifice is provided in the aforementioned liquid raw material supply pipe or at least at one of the aforementioned front ends of the aforementioned liquid raw material supply pipe.

20. A vaporization system comprising: a vaporization container for vaporizing a liquid raw material inside; a liquid raw material supply system for supplying the liquid raw material to the vaporization container; a vaporization gas supply system for supplying vaporized gas generated by vaporizing the liquid raw material in the vaporization container to a processing container for processing a substrate; a pressure regulating unit for adjusting the pressure inside the vaporization container; a heating unit for heating the liquid raw material inside the vaporization container; and a control unit configured to control the liquid raw material supply system, the vaporization gas supply system, the pressure regulating unit, and the heating unit to perform the following processes: (a) supplying the liquid raw material to the vaporization container, which is in a sealed state; (b) adjusting the pressure at the end of (a) or after a first predetermined time from that point to reduce the pressure inside the vaporization container; (c) ... After (b), the liquid raw material is vaporized without supplying carrier gas to the vaporization container, while maintaining the state in which the pressure adjustment in the vaporization container has been stopped and is set to a sealed state; and (d) after (c), the vaporized gas is supplied to the processing container.

21. A program for executing a program by a computer on a substrate processing apparatus, the program comprising: (a) supplying a liquid raw material to a vaporization container that is in a sealed state; (b) adjusting the pressure at the end of (a) or after a predetermined time from that point to reduce the pressure in the vaporization container; (c) after (b) vaporizing the liquid raw material without supplying a carrier gas to the vaporization container while maintaining the sealed state in which the pressure adjustment has ceased; and (d) after (c) supplying the vaporized gas generated by vaporizing the liquid raw material in the vaporization container to a processing container for processing the substrate.

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