Raw material feeding device

Abstract

To provide a technique by which a solid raw material can be fed to a treatment container at a large flow rate in subliming and feeding the material.SOLUTION: A raw material feeding device generates reactive gas from solution formed by dissolving a solid raw material into solvent or a dispersal system in which a solid raw material is dispersed into dispersant. The feeding device has: a container which has a first wall surface forming an internal space; a spray nozzle which sprays the solution or the dispersed system into the internal space; and a wall structure which is provided for the internal space, and has a second wall surface extending in a vertical direction.SELECTED DRAWING: Figure 1

Description

[Technical Field]

[0001] The present disclosure relates to a raw material supply device. [Background technology]

[0002] A known technique involves dissolving a solid raw material in a solvent and spraying the solution into a processing chamber, then heating the processing chamber to remove the solvent and leave the solid raw material, and subsequently heating the processing chamber to sublimate the solid raw material and generate a corresponding gas (see, for example, Patent Documents 1 and 2). [Prior art documents] [Patent documents]

[0003] [Patent Document 1] Japanese Patent Application Laid-Open No. 2004-115831 [Patent Document 2] Japanese Patent Application Laid-Open No. 2009-170800 Summary of the Invention [Problem to be solved by the invention]

[0004] The present disclosure provides a technique that allows a solid source to be sublimated and supplied to a processing vessel at a large flow rate. [Means for solving the problem]

[0005] A raw material supply device according to one aspect of the present disclosure is a raw material supply device that generates a reactive gas from a solution in which a solid raw material is dissolved in a solvent or a dispersion in which a solid raw material is dispersed in a dispersion medium, and includes: a container having a first wall surface that forms an internal space; a spray nozzle that sprays the solution or the dispersion into the internal space; and a wall structure that is provided in the internal space and has a second wall surface that extends in a vertical direction. The wall structure includes a columnar body having an axial direction in the vertical direction, the columnar body has a through hole formed therethrough in the axial direction, the second wall surface is an inner wall surface of the through hole, and the inner wall surface of the through hole has an uneven shape. . [Effects of the Invention]

[0006] According to the present disclosure, a solid source can be sublimated and supplied to a processing vessel at a large flow rate. [Brief explanation of the drawings]

[0007] [Figure 1] FIG. 1 is a diagram showing an example of a raw material supply system according to an embodiment. [Figure 2] A diagram showing an example of a raw material supply device [Figure 3] Diagram (1) explaining the operation of the raw material supply system of FIG. [Figure 4] Diagram (2) explaining the operation of the raw material supply system of Figure 1 [Figure 5] 1 is a diagram illustrating a spraying step of a raw material supply method according to an embodiment; [Figure 6] 1 is a diagram illustrating a drying process of a raw material supply method according to an embodiment; [Figure 7] 1 is a diagram illustrating a sublimation process of a raw material supply method according to an embodiment; [Figure 8] FIG. 10 is a diagram showing a first modified example of the raw material supply device. [Figure 9] FIG. 2 shows a second modified example of the raw material supply device. DETAILED DESCRIPTION OF THE INVENTION

[0008] Hereinafter, non-limiting exemplary embodiments of the present disclosure will be described with reference to the accompanying drawings. In all the accompanying drawings, the same or corresponding reference numerals are used to designate the same or corresponding members or components, and redundant descriptions will be omitted.

[0009] [Raw material supply system] A raw material supply system according to an embodiment will be described with reference to FIGS.

[0010] The raw material supply system 1 is a system that generates a reactive gas by sublimating a second solid raw material formed by removing the solvent from a solution (hereinafter simply referred to as "solution") in which a first solid raw material is dissolved in a solvent, and then uses the generated reactive gas to form a film in a processing device.

[0011] The first solid source material is not particularly limited, and may be, for example, an organometallic complex containing a metal element such as strontium (Sr), molybdenum (Mo), ruthenium (Ru), zirconium (Zr), hafnium (Hf), tungsten (W), aluminum (Al), etc., or a chloride containing a metal element such as tungsten (W), aluminum (Al), etc. The solvent may be any solvent capable of dissolving the first solid source material to produce a solution, and may be, for example, hexane.

[0012] The raw material supply system 1 includes a raw material supply source 10, raw material supply devices 30 and 40, a processing device 50, and a control device 90.

[0013] The raw material supply source 10 supplies the solution M1 to the raw material supply devices 30 and 40. The raw material supply source 10 is disposed in, for example, a sub-fab. In this embodiment, the raw material supply source 10 includes a tank 11 and a float sensor 12. The tank 11 is filled with the solution M1. The float sensor 12 detects the amount of the solution M1 filled in the tank 11.

[0014] One end of a pipe L1 is inserted into the raw material supply source 10 from above the tank 11. The other end of the pipe L1 is connected to a carrier gas supply source G1, and the carrier gas is supplied from the supply source G1 into the tank 11 via the pipe L1. The carrier gas may be an inert gas such as nitrogen (N2) or argon (Ar). A valve V1 is provided in the pipe L1. When the valve V1 is opened, the carrier gas is supplied from the supply source G1 to the raw material supply source 10, and when the valve V1 is closed, the supply of the carrier gas from the supply source G1 to the raw material supply source 10 is cut off. A pressure sensor P1 is provided in the pipe L1 to detect the pressure inside the pipe L1. The detection value of the pressure sensor P1 is transmitted to the control device 90. In addition, a flow rate controller (not shown) for controlling the flow rate of the carrier gas flowing through the pipe L1, an additional valve, etc. may be provided in the pipe L1.

[0015] The raw material supply source 10 is connected to the raw material supply device 30 via pipes L2 and L3, and supplies the solution M1 to the raw material supply device 30 via the pipes L2 and L3. Valves V2 and V3 are provided in the pipes L2 and L3, respectively. When the valves V2 and V3 are opened, the solution M1 is supplied from the raw material supply source 10 to the raw material supply device 30, and when the valves V2 and V3 are closed, the supply of the solution M1 from the raw material supply source 10 to the raw material supply device 30 is stopped. In addition, the pipe L3 may be provided with a flow rate controller (not shown) for controlling the flow rate of the solution M1 flowing through the pipe L3, an additional valve, etc.

[0016] Furthermore, the raw material supply source 10 is connected to the raw material supply device 40 via pipes L2 and L4, and supplies the solution M1 to the raw material supply device 40 via the pipes L2 and L4. A valve V4 is provided in the pipe L4. When the valves V2 and V4 are opened, the solution M1 is supplied from the raw material supply source 10 to the raw material supply device 40, and when the valves V2 and V4 are closed, the supply of the solution M1 from the raw material supply source 10 to the raw material supply device 40 is stopped. Furthermore, a flow rate controller (not shown) for controlling the flow rate of the solution M1 flowing through the pipe L4, an additional valve, etc. may be provided in the pipe L4.

[0017] The raw material supply device 30 stores the solution M1 transported from the raw material supply source 10. In this embodiment, the raw material supply device 30 includes a container 31, an injection part 32, an exhaust port 33, a heating part , a filter 35, and a columnar body .

[0018] The container 31 has an inner wall 31s that forms an internal space, and stores the solution M1 transported from the raw material supply source 10 in the internal space.

[0019] The injection unit 32 sprays the solution M1 supplied from the raw material supply source 10 via pipes L2 and L3 and injects it into the container 31. By spraying the solution M1, the injection unit 32 deposits the solution M1 as a raw material mist MM inside the container 31 without removing the solvent from the solution M1. The injection unit 32 may be, for example, a spray nozzle. The spray nozzle is attached to the ceiling of the container 31. However, the spray nozzle may also be attached to the side wall of the container 31. The spray nozzle may also be attached to the ceiling of the container 31 so that the direction of the nozzle center axis can be changed.

[0020] The exhaust port 33 is provided below the container 31 and exhausts the inside of the container 31. The processing device 50 is connected to the exhaust port 33 via pipes L10 and L12. The exhaust port 33 is also connected to an exhaust device E1 via pipes L10 and L14.

[0021] The heating unit 34 includes a heater disposed around the outer periphery of the container 31. However, the heating unit 34 may also include a heater disposed at the bottom or ceiling of the container 31. The heating unit 34 heats the container 31 to various temperatures, such as the spraying temperature, drying temperature, and sublimation temperature. The spraying temperature is a temperature at which the solution M1 sprayed into the container 31 from the injection unit 32 can be deposited on the inside of the container 31 as mist raw material MM. The drying temperature is a temperature at which a solid raw material can be formed by removing the solvent from the mist raw material MM deposited on the inside of the container 31. The drying temperature is determined, for example, according to the vapor pressure of the solvent contained in the mist raw material MM. Hereinafter, the solid raw material formed by removing the solvent from the mist raw material MM will be referred to as the second solid raw material. The sublimation temperature is a temperature at which the second solid raw material can be sublimated to generate a reactive gas. The sublimation temperature is determined, for example, according to the vapor pressure of the second solid raw material. The magnitude relationship among the spraying temperature, drying temperature, and sublimation temperature may be, for example, spraying temperature < drying temperature < sublimation temperature.

[0022] The filter 35 is disposed substantially horizontally within the container 31 and divides the container 31 into a first region 31a and a second region 31b. The first region 31a is provided with an inlet 32. The second region 31b is located below the first region 31a. The second region 31b is provided with an exhaust port 33. The filter 35 is formed of a material that is permeable to reactive gases and captures the mist raw material MM, the second solid raw material, and impurities such as particles. This prevents the solution M1 sprayed from the inlet 32 ​​from flowing out of the container 31 through the exhaust port 33. The filter 35 is formed of, for example, a porous material. The porous material may be, for example, a porous metal material such as sintered stainless steel, or a porous ceramic material. The filter 35 may not be provided.

[0023] The pillar 36 is provided below the injection part 32 in the first region 31a. The pillar 36 is formed separately from the container 31. However, the pillar 36 may be formed integrally with the container 31. The pillar 36 has a cylindrical shape with its axial direction aligned in the vertical direction, and its outer wall surface is joined to the inner wall 31s of the container 31. The pillar 36 is formed from, for example, stainless steel, aluminum, or a nickel alloy.

[0024] The columnar body 36 has a plurality of (for example, four) through-holes 36h formed therethrough in the axial direction. The plurality of through-holes 36h are formed, for example, at intervals along the circumferential direction of the columnar body 36. The solution M1 sprayed from the injection part 32 adheres to the inner wall surface 36s of each through-hole 36h as mist raw material MM. The amount of mist raw material MM adhering to the inside of the container 31 increases as the surface area of ​​the inside of the container 31 increases. For this reason, it is preferable that the columnar body 36 has a plurality of through-holes 36h formed therein. However, the number of through-holes 36h may be one.

[0025] Each through hole 36h has a circular shape in a planar view. However, each through hole 36h may have a polygonal shape in a planar view. The through axis of each through hole 36h is parallel to the vertical direction. However, the through axis of each through hole 36h may be inclined with respect to the vertical direction. When the through axis of each through hole 36h is inclined, the surface area of ​​the inner wall surface 36s is larger than when the through axis of each through hole 36h is not inclined, and therefore a larger amount of mist raw material MM adheres to the inner wall surface 36s. It is preferable that a fine uneven shape is formed on the inner wall surface 36s. This increases the surface area of ​​the inner wall surface 36s, and therefore a larger amount of mist raw material MM adheres to the inner wall surface 36s. The uneven shape is formed, for example, by blasting.

[0026] One end of pipe L8 is connected to the pipe L3 downstream of valve V3. The other end of pipe L8 is connected to carrier gas supply source G7 via pipe L7, and carrier gas is supplied from supply source G7 into container 31 via pipes L7, L8, and L3. The carrier gas may be an inert gas such as N2 or Ar. Valves V8a and V8b are installed in pipe L8 in this order from the supply source G7 side. When valves V8a and V8b are opened, carrier gas is supplied from supply source G7 to raw material supply device 30, and when valves V8a and V8b are closed, the supply of carrier gas from supply source G7 to raw material supply device 30 is stopped. A flow rate controller F7 is installed in pipe L7 to control the flow rate of carrier gas flowing through pipe L7. In this embodiment, flow rate controller F7 is a mass flow controller (MFC).

[0027] The raw material supply device 30 is connected to the processing device 50 via pipes L10 and L12, and supplies a reactive gas to the processing device 50 via the pipes L10 and L12. Valves V10a to V10c are installed in the pipe L10 in this order from the raw material supply device 30 side. When the valves V10a to V10c are opened, the reactive gas is supplied from the raw material supply device 30 to the processing device 50, and when the valves V10a to V10c are closed, the supply of the reactive gas from the raw material supply device 30 to the processing device 50 is stopped. The pipe L10 is provided with a pressure sensor P10 that detects the pressure inside the pipe L10. The detected value of the pressure sensor P10 is sent to the control device 90.

[0028] One end of pipe L13 is connected between valve V10a and valve V10b of pipe L10. The other end of pipe L13 is connected between valve V8a and valve V8b of pipe L8. Pipe L13 functions as a bypass pipe that connects pipe L8 and pipe L10 without passing through raw material supply device 30. Valve V13 is provided in pipe L13. When valve V13 is opened, pipe L8 and pipe L10 communicate with each other, and when valve V13 is closed, communication between pipe L8 and pipe L10 is blocked.

[0029] One end of pipe L14 is connected between valves V10b and V10c of pipe L10. The other end of pipe L14 is connected to an exhaust device E1, such as a vacuum pump. A pressure control valve V14 is provided in pipe L14. When the pressure control valve V14 is opened with valves V10a and V10b open, the inside of container 31 is exhausted, which can promote removal of the solvent from the mist raw material MM adhering to the inside of container 31. Furthermore, the pressure inside container 31 can be controlled by adjusting the opening of pressure control valve V14.

[0030] The raw material supply device 40 stores the solution M1 transported from the raw material supply source 10. The raw material supply device 40 is provided in parallel with the raw material supply device 30. In this embodiment, the raw material supply device 40 includes a container 41, an injection unit 42, an exhaust port 43, a heating unit 44, a filter 45, and a columnar body 46.

[0031] The container 41 has an inner wall 41s that forms an internal space, and stores the solution M1 transported from the raw material supply source 10 in the internal space.

[0032] The injection unit 42 sprays the solution M1 supplied from the raw material supply source 10 via pipes L2 and L4 and injects it into the container 41. By spraying the solution M1, the injection unit 42 deposits the solution M1 as a raw material mist MM inside the container 41 without removing the solvent from the solution M1. The injection unit 42 may have the same configuration as the injection unit 32, for example.

[0033] The exhaust port 43 is provided below the container 41 and exhausts air from the container 41. The exhaust port 43 is connected to the processing device 50 via pipes L11 and L12. The exhaust port 43 is also connected to the exhaust device E2 via pipes L11 and L16.

[0034] The heating unit 44 includes a heater arranged to cover the outer periphery of the container 41. However, the heating unit 44 may also include a heater arranged on the bottom or ceiling of the container 41. Similar to the heating unit 34, the heating unit 44 heats the container 41 to various temperatures, such as the spray temperature, drying temperature, and sublimation temperature.

[0035] The filter 45 is disposed substantially horizontally within the container 41, dividing the container 41 into a first region 41a and a second region 41b. The first region 41a is provided with an injection section 42. The second region 41b is located below the first region 41a. The second region 41b is provided with an exhaust port 43. The filter 45 is formed of a material that is permeable to reactive gases and captures the mist raw material MM, the second solid raw material, and impurities such as particles. This prevents the solution M1 sprayed from the injection section 42 from flowing out of the container 41 via the exhaust port 43. The filter 45 is formed of, for example, the same material as the filter 35. Note that the filter 45 does not necessarily have to be provided.

[0036] The pillars 46 are provided in the first region 41a below the injection portion 42. The pillars 46 may have the same configuration as the pillars 36, for example.

[0037] One end of pipe L9 is connected to pipe L4 downstream of valve V4. The other end of pipe L9 is connected to carrier gas supply source G7 via pipe L7, and carrier gas is supplied from supply source G7 into container 41 via pipes L7, L9, and L4. The carrier gas may be an inert gas such as N2 or Ar. Valves V9a and V9b are installed in pipe L9 in this order from the supply source G7 side. When valves V9a and V9b are opened, carrier gas is supplied from supply source G7 to raw material supply device 40, and when valves V9a and V9b are closed, the supply of carrier gas from supply source G7 to raw material supply device 40 is blocked.

[0038] The raw material supply device 40 is connected to the processing device 50 via pipes L11 and L12, and supplies a reactive gas to the processing device 50 via the pipes L11 and L12. Valves V11a to V11c are installed in the pipe L11 in this order from the raw material supply device 40 side. When the valves V11a to V11c are opened, the reactive gas is supplied from the raw material supply device 40 to the processing device 50, and when the valves V11a to V11c are closed, the supply of the reactive gas from the raw material supply device 40 to the processing device 50 is stopped. The pipe L11 is provided with a pressure sensor P11 that detects the pressure inside the pipe L11. The detected value of the pressure sensor P11 is sent to the control device 90.

[0039] One end of pipe L15 is connected between valve V11a and valve V11b of pipe L11. The other end of pipe L15 is connected between valve V9a and valve V9b of pipe L9. Pipe L15 functions as a bypass pipe that connects pipe L9 and pipe L11 without passing through raw material supply device 40. Valve V15 is provided in pipe L15. When valve V15 is opened, pipe L9 and pipe L11 communicate with each other, and when valve V15 is closed, communication between pipe L9 and pipe L11 is blocked.

[0040] One end of the pipe L16 is connected between the valves V11b and V11c of the pipe L11. The other end of the pipe L16 is connected to an exhaust device E2, such as a vacuum pump. A pressure control valve V16 is provided in the pipe L16. When the pressure control valve V16 is opened with the valves V11a and V11b open, the inside of the container 41 is exhausted, which can promote the removal of the solvent from the mist raw material MM adhering to the inside of the container 41. Furthermore, the pressure inside the container 41 can be controlled by adjusting the opening of the pressure control valve V16.

[0041] Processing device 50 is connected to raw material supply device 30 via pipes L10 and L12, and is supplied with a reactive gas generated by heating and sublimating the second solid raw material in raw material supply device 30. Processing device 50 is also connected to raw material supply device 40 via pipes L11 and L12, and is supplied with a reactive gas generated by heating and sublimating the second solid raw material in raw material supply device 40.

[0042] The processing apparatus 50 performs various processes, such as film formation processes, on substrates, such as semiconductor wafers, using reactive gas supplied from the source supply apparatuses 30 and 40. In this embodiment, the processing apparatus 50 includes a processing vessel 51, a flow meter 52, a storage tank 53, a pressure sensor 54, and a valve V12. The processing vessel 51 accommodates one or more substrates. In this embodiment, the flow meter 52 is a mass flow meter (MFM). The flow meter 52 is installed in the pipe L12 and measures the flow rate of the reactive gas flowing through the pipe L12. The storage tank 53 temporarily stores the reactive gas. The installation of the storage tank 53 allows a large flow rate of reactive gas to be supplied into the processing vessel 51 in a short period of time. The storage tank 53 is also referred to as a buffer tank or a fill tank. The pressure sensor 54 detects the pressure in the storage tank 53. The pressure sensor 54 is, for example, a capacitance manometer. The valve V12 is installed in the pipe L12. When the valve V12 is opened, reactive gas is supplied from the source supply devices 30 and 40 to the processing vessel 51, and when the valve V12 is closed, the supply of reactive gas from the source supply devices 30 and 40 to the processing vessel 51 is stopped.

[0043] The control device 90 is an example of a control unit, and controls each part of the raw material supply system 1. For example, the control device 90 controls the operation of the raw material supply source 10, raw material supply devices 30 and 40, processing device 50, etc. The control device 90 also controls the opening and closing of various valves. The control device 90 may be, for example, a computer.

[0044] [Raw material supply method] 3 to 7, an example of a raw material supply method carried out in raw material supply system 1 will be described. In raw material supply system 1, control device 90 controls the opening and closing of various valves, so that one of two parallel raw material supply devices 30, 40 supplies reactive gas to processing device 50, and the other charges solid raw material. An example of the operation of raw material supply system 1 will be specifically described below.

[0045] (Supply of reactive gas by raw material supply device 30) 3 and 5 to 7, a case will be described in which a reactive gas is supplied to processing equipment 50 by raw material supply device 30 in raw material supply system 1. In this case, in raw material supply system 1, raw material supply device 40 performs the spraying step and the drying step, and raw material supply device 30 performs the sublimation step.

[0046] 3, pipes through which the carrier gas, solution M1, and reactive gas flow are indicated by thick solid lines, and pipes through which the carrier gas, solution M1, and reactive gas do not flow are indicated by thin solid lines. Also, in FIG. 3, open valves are indicated by outlined symbols, and closed valves are indicated by filled symbols. The raw material supply system 1 will be described assuming that, in its initial state, all valves are closed, as shown in FIG. 1, and that the second solid raw material M2 is stored in the raw material supply device 30.

[0047] The spraying process is a process of spraying a solution M1, in which a first solid raw material is dissolved in a solvent, into the container 41, and is a process of attaching the solution M1 to the inside of the container 41 as a raw material mist MM without removing the solvent from the solution M1. For example, in the spraying process, the control device 90 opens valves V1, V2, and V4. As a result, a carrier gas is supplied from the supply source G1 to the raw material supply source 10, and the solution M1 is transported from the raw material supply source 10 to the raw material supply device 40 via pipes L2 and L4. The control device 90 also opens valves V11a and V11b and adjusts the aperture of the pressure control valve V16. As a result, the inside of the container 41 is evacuated by the exhaust device E2, and the inside of the container 41 is depressurized to a first pressure. The control device 90 also controls the heating unit 44 to heat the container 41 to the spray temperature. 5, the solution M1 transported to the raw material supply device 40 and sprayed into the container 41 from the injector 42 adheres to the inner wall 41s, the filter 45, and the inner wall surface 46s as a raw mist MM without removing the solvent. Note that the pressure inside the container 41 does not need to be reduced in the spraying step. However, from the viewpoint of allowing the raw mist MM to adhere to a wider area of ​​the inner wall 41s, the filter 45, and the inner wall surface 46s, it is preferable to reduce the pressure inside the container 41 in the spraying step.

[0048] The drying process follows the spraying process. The drying process is a process of forming a second solid raw material M2 by removing the solvent from the mist raw material MM adhering to the inner wall 41s, the filter 45, and the inner wall surface 46s. For example, in the drying process, the control device 90 closes valves V1, V2, and V4. This stops the supply of the solution M1 from the raw material supply source 10 into the container 41. The control device 90 also adjusts the aperture of the pressure control valve V16 to reduce the pressure inside the container 41 to a second pressure while keeping the valves V11a and V11b open, and controls the heating unit 44 to heat the container 41 to a drying temperature. As a result, as shown in FIG. 6, the solvent is removed from the mist raw material MM adhering to the inner wall 41s, the filter 45, and the inner wall surface 46s to form the second solid raw material M2. The solvent removed from the mist raw material MM is then exhausted by the exhaust device E2. In the drying process, since the mist raw material MM adheres to a wide area of ​​the inner wall 41s, the filter 45, and the inner wall surface 46s in the spraying process, after the solvent is removed from the mist raw material MM, the second solid raw material M2 is formed over a wide area of ​​the inner wall 41s, the filter 45, and the inner wall surface 46s. The second pressure may be, for example, lower than the first pressure. The drying temperature is, for example, higher than the spraying temperature. However, if the solvent can be removed from the mist raw material MM by setting the second pressure lower than the first pressure, the drying temperature may be the same as the spraying temperature.

[0049] The sublimation process is a process in which the second solid source material M2 formed in the container 31 is heated to sublimate the second solid source material M2 and generate a reactive gas. For example, in the sublimation process, the controller 90 controls the heater 34 to heat the container 31 to a sublimation temperature. As a result, as shown in FIG. 7, the second solid source material M2 formed on the inner wall 31s, the filter 35, and the inner wall surface 36s is sublimated to generate a reactive gas. The controller 90 also opens valves V8a, V8b, V10a-V10c, and V12. As a result, a carrier gas is injected into the container 31 from the supply source G7 via pipes L7 and L8, and the reactive gas generated in the container 31 together with the carrier gas is supplied to the processing container 51 via pipes L10 and L12. In the sublimation process, the second solid source material M2 is formed over a wide area of ​​the inner wall 31s, the filter 35, and the inner wall surface 36s during the drying process, so the specific surface area of ​​the second solid source material M2 is large. This increases the sublimation rate of the second solid source material M2, thereby enabling a large flow rate of reactive gas to be supplied to the processing vessel 51. The sublimation temperature is higher than, for example, the drying temperature.

[0050] (Supply of reactive gas by raw material supply device 40) 4 to 7, a case will be described in which a reactive gas is supplied to processing equipment 50 by raw material supply device 40 in raw material supply system 1. In this case, in raw material supply system 1, raw material supply device 30 performs the spraying step and the drying step, and raw material supply device 40 performs the sublimation step.

[0051] 4, pipes through which the carrier gas, solution M1, and reactive gas flow are indicated by thick solid lines, and pipes through which the carrier gas, solution M1, and reactive gas do not flow are indicated by thin solid lines. Also, in FIG. 4, open valves are indicated by outlined symbols, and closed valves are indicated by filled symbols. The raw material supply system 1 will be described assuming that, in its initial state, all valves are closed, as shown in FIG. 1, and that the second solid raw material M2 is stored in the raw material supply device 40.

[0052] The spraying process is a process of spraying a solution M1, in which a first solid raw material is dissolved in a solvent, into the container 31, and is a process of attaching the solution M1 to the inside of the container 31 as a mist raw material without removing the solvent from the solution M1. In the spraying process, the control device 90 opens valves V1, V2, and V3. As a result, a carrier gas is supplied from the supply source G1 to the raw material supply source 10, and the solution M1 is transported from the raw material supply source 10 to the raw material supply device 30 via pipes L2 and L3. The control device 90 also opens valves V10a and V10b and adjusts the aperture of the pressure control valve V14. As a result, the inside of the container 31 is evacuated by the exhaust device E1, and the inside of the container 31 is depressurized to a first pressure. The control device 90 also controls the heating unit 34 to heat the container 31 to the spray temperature. 5, the solution M1 transported to the raw material supply device 30 and sprayed into the container 31 from the injector 32 adheres to the inner wall 31s, the filter 35, and the inner wall surface 36s as a raw mist MM without the solvent being removed. As a result, the raw mist MM adheres over a wide area of ​​the inner wall 31s, the filter 35, and the inner wall surface 36s. Note that the pressure inside the container 31 does not need to be reduced in the spraying step. However, from the viewpoint of allowing the raw mist MM to adhere over a wider area of ​​the inner wall 31s, the filter 35, and the inner wall surface 36s, it is preferable to reduce the pressure inside the container 31 in the spraying step.

[0053] The drying process follows the spraying process. The drying process involves removing the solvent from the mist raw material MM adhering to the inner wall 31s, filter 35, and inner wall surface 36s to form a second solid raw material M2. For example, in the drying process, the control device 90 closes valves V1, V2, and V3. This stops the supply of the solution M1 from the raw material supply source 10 into the container 31. The control device 90 also maintains valves V10a and V10b open while adjusting the aperture of the pressure control valve V14 to reduce the pressure inside the container 31 to a second pressure and controls the heating unit 34 to heat the container 31 to a drying temperature. As a result, as shown in FIG. 6, the solvent is removed from the mist raw material MM adhering to the inner wall 31s, filter 35, and inner wall surface 36s to form a second solid raw material M2, and the solvent removed from the mist raw material MM is exhausted by the exhaust device E1. In the drying step, since the mist raw material MM adheres to a wide area of ​​the inner wall 31s, the filter 35, and the inner wall surface 36s in the spraying step, after the solvent is removed from the mist raw material MM, the second solid raw material M2 is formed over a wide area of ​​the inner wall 31s, the filter 35, and the inner wall surface 36s. The second pressure may be, for example, lower than the first pressure. The drying temperature is, for example, higher than the spraying temperature. However, if the solvent can be removed from the mist raw material MM by setting the second pressure lower than the first pressure, the drying temperature may be the same as the spraying temperature.

[0054] The sublimation process is a process in which the second solid source material M2 formed in the container 41 is heated to sublimate the second solid source material M2 and generate a reactive gas. For example, in the sublimation process, the control device 90 controls the heating unit 44 to heat the container 41 to a sublimation temperature. As a result, as shown in FIG. 7, the second solid source material M2 formed on the inner wall 41s, the filter 45, and the inner wall surface 46s is sublimated to generate a reactive gas. The control device 90 also opens valves V9a, V9b, V11a-V11c, and V12. As a result, a carrier gas is injected into the container 41 from the supply source G7 via pipes L7 and L9, and the reactive gas generated in the container 41 together with the carrier gas is supplied to the processing container 51 via pipes L11 and L12. In the sublimation process, the second solid source material M2 is formed over a wide area of ​​the inner wall 41s, the filter 45, and the inner wall surface 46s during the drying process, so the specific surface area of ​​the second solid source material M2 is large. This increases the sublimation rate of the second solid source material M2, thereby enabling a large flow rate of reactive gas to be supplied to the processing vessel 51. The sublimation temperature is higher than, for example, the drying temperature.

[0055] As described above, according to the embodiment, control device 90 controls the opening and closing of the valves, so that one of two raw material supply devices 30, 40 supplies reactive gas to processing device 50, and the other charges solid raw material. This enables raw material supply devices 30, 40 to be automatically replenished with raw material, improving the continuous operation capability of processing device 50 and the availability rate of processing device 50.

[0056] Furthermore, according to the embodiment, in the spraying step, when the solution M1 is sprayed from the inlet 32, 42 into the container 31, 41, the solvent of the solution M1 is not removed, and the solution M1 adheres to the inner walls 31s, 41s, the filters 35, 45, and the inner wall surfaces 36s, 46s as mist raw material MM. Then, in the drying step, the solvent is removed from the mist raw material MM adhering to the inner walls 31s, 41s, the filters 35, 45, and the inner wall surfaces 36s, 46s to form a second solid raw material M2. Then, in the sublimation step, the second solid raw material M2 formed on the inner walls 31s, 41s, the filters 35, 45, and the inner wall surfaces 36s, 46s is sublimated to generate a reactive gas. Thus, according to the embodiment, the mist raw material MM can be adhered over a wide area within the container 31, 41 in the spraying step, and therefore the second solid raw material M2 is formed over a wide area within the container 31, 41 in the drying step. Therefore, the sublimation rate of the second solid source material M2 can be increased in the sublimation step, and as a result, the reactive gas can be supplied to the processing chamber 51 at a large flow rate.

[0057] [Modification of the raw material supply device] (First Modification) A first modified example of the raw material supplying device 30 will be described with reference to Fig. 8. Fig. 8(a) is a schematic cross-sectional view showing the first modified example of the raw material supplying device 30, and Fig. 8(b) is a cross-sectional view taken along line 8B-8B in Fig. 8(a).

[0058] The raw material supply device 130 of the first modified example differs from the raw material supply device 30 in that it includes a plurality of fins 136 (eight in the illustrated example) instead of the pillars 36. Note that other features may be the same as the raw material supply device 30. The following description will focus on the differences from the raw material supply device 30.

[0059] The multiple fins 136 are provided radially in the first region 31a in a plan view. The solution M1 sprayed from the injection part 32 adheres to the plate surfaces 136s of the multiple fins 136 as mist raw material MM. The amount of mist raw material MM adhering to the inside of the container 31 increases as the surface area of ​​the inside of the container 31 increases. For this reason, it is preferable to have multiple fins 136. However, the number of fins 136 may be one.

[0060] Each fin 136 is formed separately from the container 31. However, each fin 136 may be formed integrally with the container 31. Each fin 136 has a base end joined to the inner wall 31s of the container 31 and a plate-like tip extending from the inner wall 31s of the container 31 toward the center of the container 31. Each fin 136 is joined to the inner wall 31s of the container 31 so that the plate surface 136s is parallel to the vertical direction. However, each fin 136 may also be joined to the inner wall 31s of the container 31 so that the plate surface 136s is inclined with respect to the vertical direction. Each fin 136 is formed from, for example, stainless steel, aluminum, or a nickel alloy.

[0061] It is preferable that the plate surface 136s has a fine uneven shape formed thereon. This increases the surface area of ​​the plate surface 136s, and therefore increases the amount of mist raw material MM that adheres to the plate surface 136s. The uneven shape is formed by, for example, blast processing.

[0062] According to the raw material supply device 130, when the solution M1 is sprayed into the container 31 from the inlet 32 ​​in the spraying process, the solution M1 adheres to the inner wall 31s, the filter 35, and the plate surface 136s as a mist raw material MM without removing the solvent from the solution M1. Then, in the drying process, the solvent is removed from the mist raw material MM adhering to the inner wall 31s, the filter 35, and the plate surface 136s to form a second solid raw material M2. Then, in the sublimation process, the second solid raw material M2 formed on the inner wall 31s, the filter 35, and the plate surface 136s is sublimated to generate a reactive gas. Thus, according to the raw material supply device 30 of the first modification, the mist raw material MM can be adhered over a wide area within the container 31 in the spraying process, and therefore the second solid raw material M2 is formed over a wide area within the container 31 in the drying process. Therefore, the sublimation rate of the second solid raw material M2 can be increased in the sublimation process, resulting in a high flow rate of a reactive gas being supplied to the processing container 51.

[0063] Although the raw material supplying device 130, which is a first modified example of the raw material supplying device 30, has been described in FIG. 8, the raw material supplying device 40 can also have a similar configuration.

[0064] (Second Modification) A second modified example of the raw material supply device will be described with reference to Figure 9. Figure 9(a) is a schematic cross-sectional view showing the second modified example of the raw material supply device, Figure 9(b) is a cross-sectional view taken along line 9B-9B in Figure 9(a), and Figure 9(c) is a cross-sectional view taken along line 9C-9C in Figure 9(a).

[0065] The raw material supply device 230 of the second modified example differs from the raw material supply device 130 of the first modified example in that it further includes a heat transfer unit 37. Note that other features may be the same as the raw material supply device 130. The following description will focus on the differences from the raw material supply device 130.

[0066] The heat transfer unit 37 includes a shaft member 37a and a plate-shaped member 37b. The shaft member 37a has a cylindrical shape, and its outer wall surface is joined to the tips of the multiple fins 136. The plate-shaped member 37b has a plate-like shape with its plate surface parallel to the horizontal direction, and its upper plate surface is joined to the lower end of the shaft member 37a. In this manner, the heat transfer unit 37 connects the tips of the multiple fins 136 to the inner wall 31s of the container 31 via the shaft member 37a and the plate-shaped member 37b. The shaft member 37a and the plate-shaped member 37b are made of a heat-conducting material, such as stainless steel, aluminum, or a nickel alloy. As a result, the heat transfer unit 37 transfers heat between the tips of the multiple fins 136 and the inner wall 31s of the container 31 via the shaft member 37a and the plate-shaped member 37b.

[0067] The material forming the shaft member 37a and the plate-like member 37b may be the same as that of the fins 136. In this case, even if a temperature change (heat cycle) occurs due to the repetition of the spraying process, drying process, and sublimation process, the fins 136, the shaft member 37a, and the plate-like member 37b have the same thermal expansion coefficient, so that damage at the joints of the members due to the difference in thermal expansion coefficient can be prevented.

[0068] Furthermore, the material forming the shaft member 37a and the plate-like member 37b may be a material having a higher thermal conductivity than, for example, the material forming the fins 136. In this case, heat is efficiently transferred between the tips of the fins 136 and the inner wall 31s of the container 31, and the tips of the fins 136 are efficiently heated. For example, when the fins 136 are made of stainless steel or a nickel alloy, the shaft member 37a and the plate-like member 37b can be made of aluminum.

[0069] The raw material supply device 230 includes multiple fins 136, similar to the raw material supply device 130, and therefore can increase the sublimation rate of the second solid raw material M2 in the sublimation process, thereby enabling a large flow rate of reactive gas to be supplied to the processing vessel 51.

[0070] Furthermore, the raw material supply device 230 has a heat transfer section 37 that connects the tips of the multiple fins 136 to the inner wall 31s and transfers heat between the tips and the inner wall 31s. This allows heat to be transferred between the tips of the multiple fins 136 and the inner wall 31s via the heat transfer section 37, heating the tips of the multiple fins 136. This improves the temperature uniformity in the surface direction of the plate surface 136s of each fin 136. As a result, during the spraying process, the raw material mist MM adheres uniformly to the surface direction of the plate surface 136s of each fin 136.

[0071] Although the raw material supplying device 230, which is a second modified example of the raw material supplying device 30, has been described in FIG. 9, the raw material supplying device 40 can also be configured in a similar manner.

[0072] In the above embodiment, the pillars 36, 46 and the fins 136 are an example of a wall structure, the inner wall 31s is an example of a first wall surface, and the inner wall surfaces 36s, 46s and the plate surface 136s are an example of a second wall surface.

[0073] The embodiments disclosed herein should be considered to be illustrative in all respects and not restrictive, and the above-described embodiments may be omitted, substituted, or modified in various ways without departing from the scope and spirit of the appended claims.

[0074] In the above embodiment, the raw material supply system 1 has been described as having two raw material supply devices 30, 40 arranged in parallel, but the present disclosure is not limited to this. For example, the raw material supply device may be one, or three or more raw material supply devices may be arranged in parallel. However, from the viewpoint of eliminating downtime associated with filling with the solution M1, it is preferable to have two or more raw material supply devices.

[0075] In the above embodiment, the injection units 32, 42 are spray nozzles, but the present disclosure is not limited to this. For example, the injection units 32, 42 may be spray nozzles that spray and inject the solution M1 into the containers 31, 41.

[0076] In the above embodiment, a system has been described in which a reactive gas is generated by sublimating a second solid source material M2 formed by removing a solvent from a solution M1, and the generated reactive gas is used to form a film in a processing device 50. However, the present disclosure is not limited to this. For example, instead of the solution M1, a dispersion such as a slurry in which a first solid source material is dispersed in a dispersion medium, or a colloidal solution in which a first solid source material is dispersed in a dispersion medium, can be used. For example, by using a colloidal solution, it is possible to fill a precursor at a higher concentration than by using the solution M1 or a slurry. The term "dispersion" includes the subconcepts of slurry and colloid. A slurry is also referred to as a suspension. A subconcept of colloid is a subconcept of a colloidal solution. A colloidal solution is also referred to as a sol. [Explanation of symbols]

[0077] 30,40 Raw material supply equipment 31,41 container 32,42 Injection part 36,46 columnar body 136 Finn

Claims

1. A raw material supply device for generating a reactive gas from a solution in which a solid raw material is dissolved in a solvent or a dispersion system in which a solid raw material is dispersed in a dispersion medium, a container having a first wall surface defining an interior space; a spray nozzle that sprays the solution or the dispersion into the internal space; a wall structure provided in the internal space and having a second wall surface extending in a vertical direction; and the wall structure includes a columnar body having an axial direction in the vertical direction, and a through-hole penetrating the columnar body in the axial direction is formed; the second wall surface is an inner wall surface of the through hole, The inner wall surface of the through hole has an uneven shape formed thereon. Raw material supply equipment.

2. The wall structure is formed separately from the container. The raw material supply device according to claim 1 .

3. The wall structure is integrally formed with the container. The raw material supply device according to claim 1 .

4. The through hole has a through axis parallel to the vertical direction. The raw material supply device according to any one of claims 1 to 3.

5. The through hole has a through axis inclined with respect to the vertical direction. The raw material supply device according to any one of claims 1 to 3.

6. A raw material supply device for generating a reactive gas from a solution in which a solid raw material is dissolved in a solvent or a dispersion system in which a solid raw material is dispersed in a dispersion medium, a container having a first wall surface defining an interior space; a spray nozzle that sprays the solution or the dispersion into the internal space; a wall structure provided in the internal space and having a second wall surface extending in a vertical direction; and The wall structure includes a plate-shaped fin extending from the first wall surface toward the center of the container. Raw material supply equipment.

7. The plate surface of the fin has irregularities formed thereon. The raw material supply device according to claim 6.

8. The fin has a plate surface parallel to the vertical direction. The raw material supply device according to claim 6 or 7.

9. The fin has a plate surface inclined with respect to the vertical direction. The raw material supply device according to claim 6 or 7.

10. The fins are provided in a plurality of radial directions. The raw material supply device according to any one of claims 6 to 9.

11. a heat transfer portion that connects the tip portion of the fin and the first wall surface and transfers heat between the tip portion and the first wall surface; The raw material supply device according to any one of claims 6 to 10.

12. The heat transfer unit includes a plate-shaped member whose plate surface is parallel to the horizontal direction. The raw material supply device according to claim 11.

13. A raw material supply device for generating a reactive gas from a solution in which a solid raw material is dissolved in a solvent or a dispersion system in which a solid raw material is dispersed in a dispersion medium, a container having a first wall surface defining an interior space; a spray nozzle that sprays the solution or the dispersion into the internal space; a wall structure provided in the internal space and having a second wall surface extending in a vertical direction; and the wall structure includes a columnar body having an axial direction in the vertical direction, and a through-hole penetrating the columnar body in the axial direction is formed; the second wall surface is an inner wall surface of the through hole, The inner wall surface of the through hole has an uneven shape formed thereon. Raw material supply equipment.

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