Evaporation raw material container and solid vaporization supply system

Abstract

To provide a container for an evaporation raw material to stably evaporate the evaporation raw material at an almost constant evaporation speed.SOLUTION: A container for an evaporation raw material according to the present invention is a container 100 for storing and evaporating a raw evaporation material S, and comprises: an inner container 1 housed in an outer container 2 and forming a double wall structure together with the outer container 2; a lid body 3 having an inner lid 3a detachably provided to the inner container 1 and an outer lid 3b detachably provided to the outer container 2; and a gas introduction pipe 5 linked with a carrier gas introduction port 14 arranged on the lid body 3. A partition wall 13 for parting an inside of the container into two upper and lower spaces is provided to the inner container 1. When the evaporation raw material is evaporated, average surface temperature of the partition wall 13 is higher than average surface temperature of a side wall 1a of the inner container 1 by 50°C or more.SELECTED DRAWING: Figure 1

Description

[Technical Field]

[0001] The present invention relates to a container for evaporation material that is highly corrosion-resistant, and a solid vaporization and supply system that uses the container for evaporation material. [Background technology]

[0002] In the chemical vapor deposition (CVD) film deposition method, a solid vaporization supply system that uses evaporation has traditionally been used. In this system, the outer surfaces (sides and bottom) of a container filled with the evaporation source (evaporation source container) are heated, so that the inner surface of the container becomes the heat source, and evaporation begins from the evaporation source that comes into contact with the inner surface of the container.

[0003] Patent Document 1 listed below discloses a typical evaporation raw material container capable of transferring heat to the filled evaporation raw material, for example, an evaporator in which the contact area between the inner surface serving as a heat source and the evaporation raw material is increased by increasing the heated surface area inside the container. Specifically, this evaporator has a structure in which the evaporation raw material comes into contact with a heated gas introduction tube, a structure in which multiple internal containers (holders) filled with the evaporation raw material are stacked inside the evaporator to increase the contact area of ​​the evaporation raw material, and a structure in which the evaporation raw material comes into contact with a heated tube by providing a tube with a gas diffusion through-hole on the bottom surface of the holder. [Prior art documents] [Patent documents]

[0004] [Patent Document 1] Japanese Patent Application Laid-Open No. 2016-866 Summary of the Invention [Problem to be solved by the invention]

[0005] In the evaporator described in Patent Document 1, the contact between the bottom part of the holder (internal container), which is the heat source, and the evaporation raw material continues due to the evaporation raw material falling under its own weight (falling under its own weight) as it evaporates. However, as for the contact between the side part of the holder, which is the other heat source, the gas introduction tube, and the gas diffusion tube, and the evaporation raw material, the distance between the wall surface and the evaporation raw material gradually increases as the evaporation of the evaporation raw material progresses, which reduces the heat transfer efficiency and gradually reduces the amount of evaporation.

[0006] That is, in the evaporator described in Patent Document 1, the bottom surface of the holder is the main heat source for the evaporation raw material, and over time, the heat from the side surface of the holder, the gas introduction tube, and the gas diffusion tube becomes difficult to transfer to the evaporation raw material, so the evaporation amount tends to gradually decrease. Then, as the evaporation of the evaporation raw material progresses and the evaporation rate decreases significantly, it becomes difficult to ensure a stable film formation rate in the film formation process performed using the evaporated evaporation raw material.

[0007] In recent years, the use of evaporation sources with lower vapor pressures for thin film formation has led to a tendency for the evaporation rate to decrease significantly as the evaporation rate of the source material increases. As a result, the problem of film formation speeds not being able to be ensured has become more pronounced. Meanwhile, there is a demand for ever higher performance in semiconductor products, and as a result, uniformity in the film's in-plane distribution (thickness, electrical properties) is desired. Furthermore, when forming films using atomic layer deposition (ALD), the film must be defect-free and uniform at the atomic level, so the film formation speed must be kept as constant as possible. Therefore, measures to stabilize the evaporation rate of source materials will become even more important in the future.

[0008] The present invention has been made in consideration of the problems of the prior art as described above, and aims to provide a container for evaporation raw material that continues to stably vaporize the evaporation raw material at an approximately constant evaporation rate, and a solid vaporization and supply system that uses such a container for evaporation raw material. [Means for solving the problem]

[0009] The evaporation raw material container of the present invention is a container for storing and evaporating an evaporation raw material, and includes, for example, an inner container housed in an outer container and forming a double-wall structure together with the outer container, a lid body having an inner lid detachably attached to the inner container and an outer lid detachably attached to the outer container, and a gas inlet pipe connected to a carrier gas inlet arranged in the lid body.

[0010] The inner container is further provided with a partition wall for dividing the interior thereof into two spaces, an evaporation raw material storage space on the inner lid side constituting the top wall of the inner container, and a carrier gas diffusion space on the bottom wall side of the inner container, and the evaporation raw material is stored on the upper surface of this partition wall. The partition wall also has one or more through holes formed therein, and the tip of a gas introduction pipe penetrates the partition wall and extends to a position directly above the bottom wall of the inner container.

[0011] The evaporation raw material container according to the present invention configured as described above is characterized in that the carrier gas supplied through the carrier gas inlet is released from the tip of the gas inlet pipe into the carrier gas diffusion space, the carrier gas diffused in the carrier gas diffusion space is released through the through-hole into the evaporation raw material storage space, the evaporation raw material evaporated in the evaporation raw material storage space by heating is mixed with the carrier gas diffused in the evaporation raw material storage space, and a mixed gas is released from a mixed gas outlet disposed in the lid, and when evaporating the evaporation raw material, the average surface temperature of the partition wall is 50°C or more higher than the average surface temperature of the side wall of the inner container. Alternatively, when evaporating the evaporation raw material, the heat flow rate due to heat transfer from the partition wall is 80% or more of the total heat flow rate due to heat transfer from all container walls constituting the inner container.

[0012] According to the evaporation raw material container of the present invention, the partition wall is used as a heat source for the evaporation raw material, and the evaporation raw material is continuously brought into contact with the partition wall due to its own weight falling as it evaporates, so that the evaporation raw material can continue to evaporate stably at an approximately constant evaporation rate without reducing its evaporation rate.

[0013] Furthermore, in the evaporation raw material container of the present invention, it is preferable that the second area, which is the contact area between the partition wall and the evaporation raw material, is 80% or more of the first area, which is the contact area between all container walls constituting the inner container and the evaporation raw material.

[0014] In the evaporation material container according to the present invention, the partition wall serves as a heat source for the evaporation material by installing a heater for heating the evaporation material on the outside bottom side of the outer container, by installing a heat shield between the inner wall of the outer container and the outer wall of the inner container, or by creating a vacuum in the space between the inner wall of the outer container and the outer wall of the inner container. Furthermore, the partition wall may serve as a heat source for the evaporation material by providing multiple protrusions of the same length on the inner wall of the outer container or the outer wall of the inner container, forming gaps at regular intervals between the inner wall of the outer container and the outer wall of the inner container, and by making the "length of the gap" > the "length in the height direction of the carrier gas diffusion space."

[0015] Furthermore, in the evaporation material container according to the present invention, it is desirable that the parts of the inner container, inner lid, and gas inlet pipe that come into contact with the evaporation material in gaseous and solid states are made of the same metal material as the metal that constitutes the evaporation material and that has a purity of 2N to 6N, thereby obtaining excellent thermal conductivity and corrosion resistance.

[0016] Furthermore, the evaporation raw material container of the present invention is equipped with a fastening member for fixing the outer container and the outer lid, and the fastening member is composed of a bolt member inserted into a bolt insertion hole provided in the outer container and the outer lid, and a nut member that can be screwed onto this bolt member to fasten them.

[0017] Furthermore, the evaporation source container according to the present invention is characterized in that, when a thin-film-forming metal halide compound is used as the evaporation source, the thin-film-forming metal halide compound is a compound that can be represented by the general formula: MXn, where M represents a metal element constituting the thin-film-forming metal halide compound, X represents a halogen element, and n represents the number of Xs.

[0018] Furthermore, the evaporation source container according to the present invention can store an evaporation source used for film formation by chemical vapor deposition (CVD) or an evaporation source used for film formation by atomic layer deposition (ALD).

[0019] Furthermore, the evaporation raw material container according to the present invention heats the carrier gas diffused in the carrier gas diffusion space, and mixes the evaporation raw material evaporated by heating with the heated carrier gas to generate a mixed gas.

[0020] The present invention also provides a solid vaporization and supply system comprising the evaporation source container and the evaporation source, and further comprising a carrier gas supply means for supplying a carrier gas into the evaporation source container from a carrier gas inlet. [Effects of the Invention]

[0021] According to the present invention, it is possible to provide a container for evaporation material that has excellent thermal conductivity and corrosion resistance, and that continues to stably vaporize the evaporation material at a substantially constant evaporation rate. [Brief explanation of the drawings]

[0022] [Figure 1] FIG. 1 is a cross-sectional view schematically showing a first embodiment of an evaporation material container according to the present invention. [Figure 2] FIG. 2 is a plan view showing an example of the structure of the partition wall. [Figure 3] FIG. 3 is a cross-sectional view schematically showing a second embodiment of the evaporation material container according to the present invention. [Figure 4] FIG. 4 is a cross-sectional view schematically showing a third embodiment of the evaporation material container according to the present invention. [Figure 5] FIG. 5 is a cross-sectional view schematically showing a fourth embodiment of the evaporation material container according to the present invention. DETAILED DESCRIPTION OF THE INVENTION

[0023] Hereinafter, embodiments of the evaporation source container and solid vaporization supply system according to the present invention will be described in detail with reference to the drawings. However, the present invention is not limited to these embodiments. In other words, appropriate modifications and improvements to the following embodiments based on the ordinary knowledge of those skilled in the art are also within the scope of the present invention, provided they do not deviate from the spirit of the present invention. Furthermore, in the specification and drawings of this application, elements that can be similarly described may be designated by the same reference numerals, and redundant description may be omitted.

[0024] First Embodiment A first embodiment of an evaporation material container and a solid vaporization and supply system according to the present invention will be described in detail with reference to the drawings.

[0025] <Overall structure> FIG. 1 is a cross-sectional view schematically illustrating a first embodiment of an evaporation source container according to the present invention, and is a diagram for explaining in detail the gas flows of a carrier gas G1, an evaporated evaporation source G2 (for example, an evaporated thin film-forming metal halide compound G2), and a mixed gas G3.

[0026] The evaporation raw material container 100 shown in Fig. 1 is a container for storing and evaporating the evaporation raw material S, and includes, for example, an inner container 1, an outer container 2, a lid body 3 having an inner lid 3a and an outer lid 3b, a fastening member 4, and a gas introduction pipe 5. As shown in Fig. 1, this evaporation raw material container 100 has a double-wall structure made up of the inner container 1 and the outer container 2, and the inner container 1 storing the evaporation raw material S essentially forms the container body. In this embodiment, a heater 6 is installed on the outside of the bottom side of the evaporation raw material container 100 (outside the bottom side of the outer container 2), and the evaporation raw material S is evaporated (vaporized) by heating the evaporation raw material container 100 from the outside of the bottom side.

[0027] In the evaporation source container 100 of this embodiment, the inner container 1 is, for example, a cylindrical container, and is provided with a side wall 1a and a bottom wall 1b that function as container walls that come into contact with the evaporation source S, the carrier gas G1, the evaporation source G2 vaporized by evaporation (hereinafter simply referred to as the evaporation source G2), and the mixed gas G3. The inner container 1 is also provided with a disk-shaped partition wall 13 (the partition wall 13 also functions as part of the container wall) that divides the interior into two spaces, an evaporation source storage space 11 and a carrier gas diffusion space 12. The evaporation source storage space 11 is a space formed between the upper surface of the partition wall 13 and the inner lid 3a that constitutes the upper wall of the inner container 1. In this embodiment, the evaporation source S is stored on the upper surface of the partition wall 13, i.e., in the evaporation source storage space 11 of the inner container 1. The carrier gas diffusion space 12 is a space formed between the lower surface of the partition wall 13 and the bottom wall 1b of the inner container 1.

[0028] 1, the evaporation source container 100 of this embodiment has a structure in which the tip of the gas introduction pipe 5 connected to the carrier gas introduction port 14 provided in the center of the lid 3 penetrates the center of the partition wall 13 and extends to a position directly above the bottom wall 1b of the inner container 1. In other words, the tip of the gas introduction pipe 5 does not abut against the bottom wall 1b of the inner container 1. As a result, the carrier gas G1 supplied from the outside flows inside the gas introduction pipe 5 and is released and diffused from its tip in the carrier gas diffusion space 12.

[0029] The partition wall 13 has one or more through holes 15 formed therein for supplying the carrier gas G1 diffused in the carrier gas diffusion space 12 to the evaporation raw material storage space 11. Fig. 2 is a plan view showing an example of the structure of the partition wall 13. That is, the carrier gas G1 diffused in the carrier gas diffusion space 12 passes through these through holes 15 and is released into the evaporation raw material storage space 11 (bottom blowing method). Then, a mixed gas G3 obtained by mixing the evaporation raw material G2 evaporated into gas in the evaporation raw material storage space 11 of the inner container 1 with the carrier gas G1 diffused in the evaporation raw material storage space 11 is released from the mixed gas outlet 16.

[0030] 2, the partition wall 13 preferably has a shower head structure in which a plurality of through holes 15 are formed. The shower head structure is a structure in which the plurality of through holes 15 serve as ejection holes for the carrier gas G1, thereby realizing a shower-like gas flow.

[0031] Furthermore, there are no particular limitations on the arrangement of the multiple through holes 15 formed in the partition wall 13, and for example, the through holes 15 may be arranged evenly as shown in Fig. 2. Furthermore, although not shown, the multiple through holes 15 may be arranged, for example, so that the multiple through holes 15 are formed around the partition wall 13 and the trajectories of the multiple through holes 15 form a spiral.

[0032] The partition wall 13 may also be made of, for example, a porous material. In this case, the partition wall 13 does not need to have through-holes 15 as shown in FIG. 2 . The porous material allows the carrier gas G1 that flows into the carrier gas diffusion space 12 to be released into the evaporation raw material storage space 11 and diffused. Then, gas flows of the carrier gas G1, evaporation raw material G2, and mixed gas G3 occur within the evaporation raw material storage space 11. Furthermore, the porous material functions as a filter, so that particles generated within the carrier gas diffusion space 12 can be collected and removed here. Examples of porous materials that can be used for the partition wall 13 of this embodiment include ceramics.

[0033] Furthermore, by configuring the gas introduction pipe 5 as described above, when the evaporation raw material container 100 (outer container 2) is heated from the outside of the bottom surface side, the carrier gas G1 diffused in the carrier gas diffusion space 12 can also be heated at the same time, and this heated carrier gas G1 can be released into the evaporation raw material storage space 11 through the through-holes 15 in the partition wall 13. Therefore, the heated carrier gas G1 can be brought into contact with the evaporation raw material S, and the evaporation raw material S can be vaporized stably and at a high flow rate.

[0034] The partition wall 13 constitutes a part of the inner container 1, and may be, for example, an integral structure with the inner container 1, or may be a structure that is removable from the inner container 1 as needed. Furthermore, when the partition wall 13 is a removable structure, the attachment position of the partition wall 13 is not particularly limited, and can be adjusted as appropriate as long as it can be locked and fixed inside the inner container 1, for example.

[0035] In the evaporation source container 100 of this embodiment, the outer container 2 is a container formed in the same cylindrical shape as the inner container 1, but slightly larger than the inner container 1. In this embodiment, the inner container 1 is housed inside the outer container 2, thereby forming a container with the above-mentioned double-wall structure. The outer container 2 is provided at its upper end with an annular flange 2a formed so as to be able to tightly fit with the outer lid 3b. The shapes of these two containers (1, 2) are not limited to a cylindrical shape as long as they facilitate gas diffusion of the carrier gas G1, evaporation source G2, and mixed gas G3.

[0036] In the evaporation source container 100 of this embodiment, the inner lid 3a is provided in close contact with and detachably attached to the upper periphery of the inner container 1, and the outer lid 3b is provided in a detachable manner with respect to the outer container 2 and in close contact with the inner lid 3a, and these two lids form a lid body 3. The lid body 3 is provided with a carrier gas inlet 14 for supplying a carrier gas G1 into the inner container 1 and a mixed gas outlet 16 for discharging a mixed gas G3 obtained by mixing the evaporation source G2 and the carrier gas G1 to the outside. In this embodiment, as an example, the carrier gas inlet 14 is provided in the center of the disk-shaped lid body 3 (inner lid 3a, outer lid 3b) so as to be penetrable, and the mixed gas outlet 16 is provided in a position other than the center of the lid body 3 so as to be penetrable. As a result, in this embodiment, carrier gas G1 supplied from the outside flows into carrier gas diffusion space 12 inside inner container 1 through gas inlet pipe 5 connected to carrier gas inlet 14, and diffuses in evaporation raw material storage space 11 inside inner container 1 through through-holes 15 formed in partition wall 13. Then, mixed gas G3 obtained by mixing evaporation raw material G2 evaporated into gas in evaporation raw material storage space 11 with carrier gas G1 diffused in evaporation raw material storage space 11 is released from mixed gas outlet 16.

[0037] In addition, in the evaporation raw material container 100 of this embodiment, the fastening member 4 is a member for fixing the outer container 2 and the outer lid 3b, and is composed, for example, of a bolt member inserted into a bolt insertion hole provided in the flange portion 2a of the outer container 2 and the outer lid 3b, and a nut member that can be screwed onto this bolt member to fasten them.

[0038] In this embodiment, the heater 6 is installed on the outside of the bottom surface of the evaporation source container 100 (outer container 2) along the bottom of the outer container 2, as shown in FIG. 1 . By heating the evaporation source container 100 from the outside of the bottom surface, the partition wall 13 becomes a heat source via the bottom wall 1b of the inner container 1 and the carrier gas diffusion space 12, and the evaporation source S in contact with the partition wall 13 is evaporated (vaporized). When evaporating the evaporation source S, the heater 6 is controlled so that the average surface temperature of the partition wall 13 is 50°C or more higher than the average surface temperature of the side wall 1a of the inner container 1. If the temperature difference between the average surface temperature of the partition wall 13 and the average surface temperature of the side wall 1a of the inner container 1 is less than 50°C, the side wall 1a of the inner container 1 becomes a heat source, which promotes evaporation of the evaporation source S in contact with the side wall 1a of the inner container 1, which is not preferable.

[0039] As mentioned above, a typical vaporization method involves heating the container from the bottom and sides to vaporize the evaporation raw material S. In this vaporization method, the evaporation raw material S in contact with the bottom, which is one of the heat sources, continues to vaporize stably due to its own weight as it vaporizes, but the evaporation raw material S in contact with the side, which is the other heat source, moves away from the wall as evaporation progresses, and the amount of evaporation gradually decreases. In other words, as evaporation progresses, the evaporation rate of the evaporation raw material S decreases over time.

[0040] On the other hand, in this embodiment, the heater 6 is installed outside the bottom side of the evaporation source container 100 along the bottom of the outer container 2, and only the partition wall 13 of the inner container 1 serves as a heat source for the evaporation source S. By using the partition wall 13 as a heat source for the evaporation source S, the evaporation source S is continuously brought into contact with the partition wall 13 by falling under its own weight as it vaporizes. As a result, the evaporation source container 100 of this embodiment can continue to vaporize the evaporation source S without reducing the evaporation rate of the evaporation source S, that is, while always maintaining a constant evaporation amount. Furthermore, by maintaining a constant evaporation amount by the evaporation source container 100, a stable film formation rate can be ensured in the film formation process, and further, uniformity in the in-plane distribution (film thickness, electrical properties) of the film can be achieved.

[0041] In addition, the evaporation raw material container 100 of this embodiment may further be provided with a coupling member (not shown) for connecting the carrier gas inlet 14 provided in the lid body 3 to a gas piping (not shown) for flowing the carrier gas G1 toward the carrier gas inlet 14, and a coupling member (not shown) for connecting the mixed gas outlet 16 also provided in the lid body 3 to a gas piping (not shown) for flowing the mixed gas G3 released from the mixed gas outlet 16.

[0042] In addition, in this embodiment, from the viewpoint of further suppressing evaporation of the evaporation raw material S in contact with the side wall 1a of the inner container 1, it is preferable that the second area, which is the contact area between the partition wall 13 and the evaporation raw material S, is 80% or more of the first area (total contact area), which is the contact area between all container walls constituting the inner container 1 and the evaporation raw material S.

[0043] Furthermore, in this embodiment, the heater 6 is controlled so that the average surface temperature of the partition wall 13 is 50° C. or more higher than the average surface temperature of the side wall 1a of the inner container 1 when evaporating the evaporation raw material S, but this is not limited thereto. For example, the heater 6 may be controlled so that the heat flow rate due to heat transfer from the partition wall 13 of the inner container 1 is 80% or more of the total heat flow rate due to heat transfer from all container walls that constitute the inner container 1 when evaporating the evaporation raw material S. If the proportion of the heat flow rate due to heat transfer from the partition wall 13 to the total heat flow rate is less than 80%, this is not preferable because it promotes evaporation of the evaporation raw material S that comes into contact with the side wall 1a of the inner container 1.

[0044] <Materials for each component> In the evaporation source container 100 of this embodiment, the container wall of the inner container 1 and the gas inlet pipe 5 are made of the same metal material as the evaporation source S, and are made of a high-purity metal material, such as copper with a purity of 99 to 99.9999% (2N to 6N), aluminum with a purity of 99 to 99.9999% (2N to 6N), or titanium with a purity of 99 to 99.9999% (2N to 6N). This results in a container with excellent thermal conductivity. Note that "purity" refers to the proportion (weight ratio) of the main component in the sample determined by quantitative analysis. For example, if the purity of the copper, aluminum, or titanium constituting the container wall of the inner container 1 and the gas inlet pipe 5 is less than 99%, the thermal conductivity of these components will decrease, which is undesirable. Furthermore, if the purity of the copper, aluminum, or titanium constituting the container wall of the inner container 1 and the gas inlet pipe 5 exceeds 99.9999%, the strength of these components will decrease, which is undesirable.

[0045] The vessel walls of the inner vessel 1 include the side wall 1a, the bottom wall 1b, the partition wall 13, and the steam contact surface (corresponding to the steam contact surface of the inner lid 3a) of the lid body 3 that constitutes the upper wall of the inner vessel 1. In other words, when the evaporation raw material S is introduced into the vessel 100 for evaporation raw material, all of the walls in the inner vessel 1 that come into contact with the evaporation raw material G2 are vessel walls.

[0046] For example, if the evaporation raw material is aluminum chloride, the aluminum chloride will react with moisture to generate oxidizing gases such as hydrochloric acid inside the inner container 1. However, if aluminum with a purity of 99.9% is used for the container wall of the inner container 1 and the gas inlet tube 5, even if corrosion occurs inside the inner container 1 due to this hydrochloric acid gas, the aluminum will be eluted, and the mixed gas G3 obtained by mixing the carrier gas G1 and the evaporated gas G2 of the aluminum chloride will not be contaminated with elements other than aluminum.

[0047] The material of the parts of the inner container 1 other than the container wall (including the parts of the inner lid 3a other than the vapor contact surface) is not particularly limited, but from the viewpoint of manufacturing, it is preferable that they be made of the same metal material as above.

[0048] Furthermore, the materials for the outer container 2, outer lid 3b, and fastening member 4 are not particularly limited. However, from the viewpoint of manufacturing and use (the strength required to hold and protect the entire container, including the inner container 1 and outer container 2, during handling and transportation), it is preferable to use, for example, aluminum, copper, titanium, nickel alloy, aluminum alloy, super stainless steel, stainless steel, etc. Of these, aluminum, copper, and titanium preferably have a purity of 99% or more, and more preferably a purity of 99 to 99.9999%. As the nickel alloy, for example, Hastelloy or Inconel can be used, and Hastelloy and Inconel are alloys containing Ni and Mo. As the aluminum alloy, for example, an aluminum-copper alloy or an aluminum-magnesium alloy can be used, but the alloy is not limited to these alloys.

[0049] The composition of Hastelloy can be determined as appropriate, but specifically, it contains 40 to 60 mass % of Ni and 30 to 50 mass % of Mo.

[0050] The composition of Inconel can also be determined as appropriate, but specifically, it is 20 to 50 mass % Ni and 70 to 50 mass % Mo.

[0051] In addition, super stainless steel is a stainless steel with enhanced corrosion resistance that contains 17.00 to 19.50 mass% Ni, 19.00 to 21.00 mass% Cr, 5.50 to 6.50 mass% Mo, 0.16 to 0.24 mass% N, 0.50 to 1.00 mass% Cu, and further contains 0.020 mass% or less C, 0.80 mass% or less Si, 1.00 mass% or less Mn, 0.030 mass% or less P, and 0.015 mass% or less S.

[0052] <Carrier gas and evaporation material> In the evaporation raw material container 100 of this embodiment, the carrier gas G1 may be, for example, hydrogen, helium, nitrogen, oxygen, argon, carbon monoxide, or carbon dioxide. Specifically, it is preferable to use helium or argon. However, the use of hydrogen, nitrogen, oxygen, carbon monoxide, or carbon dioxide is permitted as long as it does not affect the reaction with the evaporation raw material.

[0053] Furthermore, when a metal halide compound for forming a thin film is used as a more reactive evaporation source, the evaporation source S is preferably a compound that can be represented by the following general formula.

[0054] General formula: MXn In the above general formula, M represents any one of Al, Cu, Ti, Hf, Zr, Ta, and W. X represents a halogen element. n represents the number of Xs.

[0055] Examples of compounds that can be represented by the above general formula when X is chlorine (Cl) include aluminum chloride (AlCl3), copper chloride (CuCl or CuCl2), titanium chloride (TiCl3), hafnium chloride (HfCl4), zirconium chloride (ZrCl4), tantalum chloride (TaCl5), tungsten pentachloride (WCl5), and tungsten hexachloride (WCl6).

[0056] The evaporation raw material container 100 of this embodiment can store even highly corrosive evaporation raw materials such as the compounds that can be represented by the general formula above, and can greatly reduce the proportion of impurities present in the evaporation raw material. Furthermore, the evaporation raw material container 100 keeps the evaporation raw material in the container in either a gas (G2) or solid (S) state.

[0057] Furthermore, the evaporation source container 100 of this embodiment can be used as a container for storing evaporation sources used in film formation by chemical vapor deposition (CVD), metalorganic chemical vapor deposition (MOCVD), and atomic layer deposition (ALD). For example, it is preferable to use it as a container for storing evaporation sources used in film formation by atomic layer deposition (ALD). Specifically, atomic layer deposition (ALD) is a method capable of forming films thinner than those formed by chemical vapor deposition (CVD), and can form very thin films of about several nanometers. However, on the other hand, the accuracy of the film is easily affected by impurities contained in the evaporation source. Therefore, in this embodiment, by using the evaporation source container 100, the amount of impurities contained in the evaporation source is kept to an extremely small amount.

[0058] <Method of manufacturing the evaporation material container> The evaporation source container 100 of this embodiment is manufactured, for example, as follows. First, the outer container 2 having the flange 2a is manufactured by hollowing out a material or welding a roll-shaped workpiece using a known method. Next, the inner container 1 constituting the container body is manufactured. This inner container 1 is made of the same metal material as the metal constituting the evaporation source S, and is made of a high-purity metal material such as copper with a purity of 99 to 99.9999%, aluminum with a purity of 99 to 99.9999%, or titanium with a purity of 99 to 99.9999%. Then, a double-walled container is manufactured by placing the inner container 1 inside the outer container 2. Next, the lid 3 is manufactured. Specifically, an inner lid 3a that is detachable from the inner container 1 and an outer lid 3b that is detachable from the outer container 2 are manufactured. At least the vapor-contacting surface of the inner lid 3a constituting the upper wall of the inner container 1 is made of the same metal material as the metal constituting the evaporation source S, similar to the inner container 1, and is made of a high-purity metal material such as copper with a purity of 99 to 99.9999%, aluminum with a purity of 99 to 99.9999%, or titanium with a purity of 99 to 99.9999%. Furthermore, the flange 2a of the outer container 2 and the outer lid 3b are formed with bolt insertion holes for threading fastening members 4, and fastening members 4 (bolts and nuts) that fit these bolt insertion holes are prepared. A gas inlet pipe 5 connected to the carrier gas inlet 14 provided in the lid 3, and various joint members (not shown) that connect to the carrier gas inlet 14 and the mixed gas outlet 16 provided in the lid 3 are also prepared. Similarly to the inner vessel 1, the gas introduction pipe 5 is also made of the same metal material as that constituting the evaporation raw material S, and is made of a high-purity metal material such as copper with a purity of 99 to 99.9999%, aluminum with a purity of 99 to 99.9999%, or titanium with a purity of 99 to 99.9999%. In this way, the various components constituting the evaporation raw material vessel 100 are obtained (preparation step).

[0059] Thereafter, the components obtained in the preparation step are assembled to produce the evaporation raw material container 100 (assembly step). Note that the method for producing the evaporation raw material container 100 of this embodiment is not limited to the above method.

[0060] <How to use the evaporation material container> In this embodiment, first, the carrier gas inlet 14 of the evaporation raw material container 100 is connected to a carrier gas tank (not shown) via a joint member or the like, and further, the mixed gas outlet 16 is connected to semiconductor processing equipment (not shown) via a joint member or the like.

[0061] Next, the evaporation raw material S is charged into the inner container 1 (above the partition wall 13) of the evaporation raw material container 100, and then the inner container 1 is closed with the lid body 3 (inner lid 3a, outer lid 3b), and the flange 2a of the outer container 2 and the outer lid 3b are fixed with the fastening member 4 to hermetically seal the inner container 1. Then, a heater 6 is installed along the bottom of the outer container 2 on the outside of the bottom side of the evaporation raw material container 100.

[0062] Next, the heater 6 is used to heat the evaporation source container 100 (outer container 2) from the outside of the bottom surface, and a carrier gas G1 is supplied from a carrier gas tank (not shown) into the inner container 1 of the evaporation source container 100. Specifically, the carrier gas G1 flows through the gas inlet pipe 5 and is released and diffused from its tip in the carrier gas diffusion space 12. The carrier gas G1 diffused in the carrier gas diffusion space 12 passes through the through-holes 15 in the partition wall 13 and is released into the evaporation source storage space 11. As a result, the evaporation source S in contact with the partition wall 13, which serves as the heat source, can continue to stably vaporize at a substantially constant evaporation rate due to its own weight as it vaporizes. A mixed gas G3, which is a mixture of the evaporation source G2 vaporized in the evaporation source storage space 11 and the carrier gas G1 diffused in the evaporation source storage space 11, is released from the mixed gas outlet 16. The evaporation source S is evaporated (vaporized) by heating to become a source gas.

[0063] Then, in a semiconductor processing facility (not shown), a film is formed by chemical vapor deposition (CVD), metalorganic chemical vapor deposition (MOCVD), or atomic layer deposition (ALD). The semiconductor processing facility is a facility (e.g., a reaction chamber of a CVD apparatus) where a substrate to be film-formed is placed, and a desired thin film is formed on the substrate placed in the semiconductor processing facility.

[0064] As a result, the evaporation source container 100 of this embodiment can significantly reduce the proportion of impurities originating from the container in the evaporation source, and therefore can supply a high-purity mixed gas G3 to a semiconductor processing facility (not shown). Furthermore, as described above, the evaporation source container 100 of this embodiment can stably continue vaporizing the evaporation source at a substantially constant evaporation rate, that is, can maintain a constant evaporation amount, thereby ensuring a stable film formation rate in the film formation process and further realizing uniformity in the in-plane distribution (film thickness, electrical properties) of the film.

[0065] As described above, the evaporation source container 100 of this embodiment is a container used for gasifying the material into a gas phase in CVD, ALD, MOCVD, etc., and is used, for example, as a pressure container for supplying the mixed gas G3 to semiconductor processing equipment.

[0066] <Solid Vaporization Supply System> Next, a solid vaporization and supply system using the evaporation raw material container 100 of this embodiment will be described. The solid vaporization and supply system of this embodiment includes the evaporation raw material container 100 described above and the evaporation raw material S stored in the inner container 1. Note that this solid vaporization and supply system may further include a carrier gas supply means (not shown) for supplying a carrier gas G1 into the inner container 1.

[0067] In the solid vaporization and supply system of this embodiment, a carrier gas G1 supplied from a carrier gas inlet 14 flows into an evaporation source container 100, and a mixed gas G3 obtained by mixing the evaporation source G2 evaporated in the evaporation source container 100 by heating from the outside of the bottom side of the evaporation source container 100 with the carrier gas G1 is released from a mixed gas outlet 16. As a result, in the solid vaporization and supply system of this embodiment, an evaporation source of higher purity can be supplied to semiconductor processing equipment (not shown) at a substantially constant evaporation rate.

[0068] Specifically, the solid vaporization and supply system of this embodiment is preferably configured as follows. First, the evaporation source material S is introduced into the inner vessel 1 (above the partition wall 13) of the evaporation source material container 100. Next, the evaporation source material container 100 is heated from the outside on the bottom side, using the partition wall 13 as a heat source to heat the evaporation source material S, and the carrier gas G1 flowing in through the gas inlet pipe 5 is released and diffused into the inner vessel 1. Then, the evaporation source material G2 evaporated in the inner vessel 1 by heating is mixed with the carrier gas G1 diffused in the inner vessel 1 to generate a mixed gas G3. As a result, the evaporation source material S falls by its own weight onto the partition wall 13 as it vaporizes, allowing stable evaporation to continue at an approximately constant evaporation rate. In other words, a constant evaporation amount can be maintained. This ensures a stable film formation rate in the film formation process and also achieves uniformity in the in-plane distribution (film thickness, electrical properties) of the film.

[0069] <Second embodiment> Next, a second embodiment of the evaporation source container and solid vaporization supply system according to the present invention will be described in detail with reference to the drawings. Note that the present invention is not limited to this embodiment. Furthermore, elements that can be explained in the same way as in the first embodiment will be given the same reference numerals and will not be explained again.

[0070] <Overall structure> 3 is a cross-sectional view showing a second embodiment of the evaporation source container according to the present invention, specifically showing the gas flows of the carrier gas G1, evaporation source G2, and mixed gas G3. In this embodiment, similar to the first embodiment, the heater 6 is installed outside the bottom side of the outer container 2, and a heater 21 is also installed so as to surround the side surface of the outer container 2.

[0071] The evaporation raw material container 200 shown in Fig. 3 is a container for storing and evaporating the evaporation raw material S, and includes, for example, two containers forming a double-walled structure: an inner container 1 and an outer container 2; a lid body 3 having an inner lid 3a and an outer lid 3b; a fastening member 4 for fastening the outer container 2 and the outer lid 3b together; and a gas inlet pipe 5 for discharging a carrier gas G1 supplied from the outside into the inner container 1. Furthermore, the evaporation raw material container 200 is provided with a heat shield 22 between the inner wall of the outer container 2 and the outer wall of the inner container 1 to suppress evaporation of the evaporation raw material S due to heating from the side of the outer container 2 (heater 21), i.e., to suppress the heat flow from the heater 21 to the evaporation raw material S. When evaporating the evaporation raw material S, the action of the heat shield 22 and control of the heater make the average surface temperature of the partition wall 13 50°C or more higher than the average surface temperature of the side wall 1a of the inner container 1. The configuration is the same as that of the evaporation material vessel 100 of the first embodiment described above, except that a heat shield 22 is provided between the inner wall of the outer vessel 2 and the outer wall of the inner vessel 1.

[0072] Furthermore, the materials of each component, carrier gas, and evaporation raw material used in the evaporation raw material container 200 can be explained in the same way as for the evaporation raw material container 100 of the first embodiment described above, so duplicate explanations will be omitted.

[0073] Furthermore, the manufacturing method of the evaporation raw material container 200 is the same as the first embodiment (manufacturing method of the evaporation raw material container 100) described above, except that when the inner container 1 is placed inside the outer container 2, a heat shield 22 is installed between the inner wall of the outer container 2 and the outer wall of the inner container 1.

[0074] <How to use the evaporation material container> In this embodiment, as in the first embodiment, first, the carrier gas inlet 14 of the evaporation raw material container 200 is connected to a carrier gas tank (not shown) via a joint member or the like, and further, the mixed gas outlet 16 is connected to semiconductor processing equipment (not shown) via a joint member or the like.

[0075] Next, the evaporation raw material S is charged into the inner container 1 (above the partition wall 13) of the evaporation raw material container 200, and then the inner container 1 is closed with the lid body 3 (inner lid 3a, outer lid 3b), and the flange 2a of the outer container 2 and the outer lid 3b are fixed with the fastening member 4 to seal the inner container 1. Then, a heater 6 is installed outside the bottom side of the evaporation raw material container 200, and a heater 21 is installed so as to surround the side surface of the outer container 2.

[0076] Next, the evaporation source container 200 (outer container 2) is heated from the outside using the heater 6 and the heater 21, and a carrier gas G1 is supplied from a carrier gas tank (not shown) into the inner container 1 of the evaporation source container 200. Specifically, the carrier gas G1 flows through the gas inlet pipe 5 and is released and diffused from its tip in the carrier gas diffusion space 12. The carrier gas G1 diffused in the carrier gas diffusion space 12 passes through the through-hole 15 in the partition wall 13 and is released into the evaporation source storage space 11. At this time, the evaporation source container 200 suppresses the heat flow from the heater 21 to the evaporation source S due to the action of the heat shield 22, so that evaporation of the evaporation source S due to heating from the heater 21 can be suppressed. In other words, the side wall 1a of the inner container 1 can be prevented from becoming a heat source for the evaporation source S. As a result, the evaporation raw material S that comes into contact with the partition wall 13, which is the heat source, can continue to evaporate stably at an approximately constant evaporation rate due to its own weight falling as it evaporates, and a mixed gas G3, which is a mixture of the evaporation raw material G2 evaporated in the evaporation raw material storage space 11 and the carrier gas G1 diffused in the evaporation raw material storage space 11, is released from the mixed gas outlet 16.

[0077] Other methods of using the evaporation raw material container 200 are the same as those of the first embodiment (method of using the evaporation raw material container 100).

[0078] The solid vaporization and supply system using the evaporation raw material container 200 of this embodiment is similar to the solid vaporization and supply system of the first embodiment described above, except that the evaporation raw material container 200 (outer container 2) is heated from the outside using the heating heater 6 and the heating heater 21, and the evaporation of the evaporation raw material S due to heating from the heating heater 21 is suppressed by the action of the heat shield 22.

[0079] <Third embodiment> Next, a third embodiment of the evaporation source container and solid vaporization supply system according to the present invention will be described in detail with reference to the drawings. Note that the present invention is not limited to this embodiment. Furthermore, elements that can be explained in the same way as in the first embodiment will be given the same reference numerals and will not be explained again.

[0080] <Overall structure> 4 is a cross-sectional view showing a third embodiment of the evaporation source container according to the present invention, specifically showing the gas flows of the carrier gas G1, evaporation source G2, and mixed gas G3. In this embodiment, as in the second embodiment, the heater 6 is installed outside the bottom surface of the outer container 2, and a heater 21 is also installed so as to surround the side surface of the outer container 2.

[0081] The evaporation raw material container 300 shown in FIG. 4 is a container for storing and evaporating the evaporation raw material S, and includes, for example, two containers forming a double-walled structure: an inner container 1 and an outer container 2; a lid 3 having an inner lid 3a and an outer lid 3b; a fastening member 4 for fastening the outer container 2 and the outer lid 3b; and a gas inlet pipe 5 for discharging a carrier gas G1 supplied from outside into the inner container 1. In the evaporation raw material container 300 configured in this manner, when heating the evaporation raw material S, a space 31 between the inner wall of the outer container 2 and the outer wall of the inner container 1 is evacuated. This makes it possible to suppress the heat flow from the heater 21, which is installed to surround the side of the outer container 2, to the evaporation raw material S. When evaporating the evaporation raw material S, the average surface temperature of the partition wall 13 is made 50°C or more higher than the average surface temperature of the side wall 1a of the inner container 1 by the effect of the evacuated space 31 and control of the heater. The configuration is the same as that of the evaporation material container 100 of the first embodiment described above, except that the space 31 between the outer container 2 and the inner container 1 is in a vacuum state.

[0082] Furthermore, the materials of each component, carrier gas, and evaporation raw material used in the evaporation raw material container 300 can be explained in the same way as for the evaporation raw material container 100 of the first embodiment described above, so duplicate explanations will be omitted.

[0083] <Method of manufacturing the evaporation material container> The method for manufacturing the evaporation material container 300 is the same as that of the first embodiment (the method for manufacturing the evaporation material container 100) described above, except that the space 31 between the outer container 2 and the inner container 1 is evacuated.

[0084] One method that can be used to evacuate the space 31 is to form a vacuum-forming hole 2b in the bottom or side of the double-walled evaporation raw material container 300 (outer container 2), place the evaporation raw material container 300 in a vacuum chamber, and fill the hole in the vacuum state. There are no particular restrictions on the material that can be used to fill the hole, but it is desirable that the material be highly heat-resistant and have the same strength as the outer container 2.

[0085] <How to use the evaporation material container> In this embodiment, as in the first embodiment, first, the carrier gas inlet 14 of the evaporation raw material container 300 is connected to a carrier gas tank (not shown) via a joint member or the like, and further, the mixed gas outlet 16 is connected to semiconductor processing equipment (not shown) via a joint member or the like.

[0086] Next, the evaporation raw material S is charged into the inner container 1 (above the partition wall 13) of the evaporation raw material container 300, after which the inner container 1 is closed with the lid body 3 (inner lid 3a, outer lid 3b), and the flange 2a of the outer container 2 and the outer lid 3b are fixed with the fastening member 4 to seal the inner container 1 and evacuate the space 31 between the outer container 2 and the inner container 1. Then, a heater 6 is installed outside the bottom side of the evaporation raw material container 300, and a heater 21 is installed so as to surround the side surface of the outer container 2.

[0087] Next, the heater 6 and the heater 21 are used to heat the evaporation source container 300 (outer container 2) from the outside, and a carrier gas G1 is supplied from a carrier gas tank (not shown) into the inner container 1 of the evaporation source container 300. Specifically, the carrier gas G1 flows through the gas inlet pipe 5 and is released and diffused from its tip in the carrier gas diffusion space 12. The carrier gas G1 diffused in the carrier gas diffusion space 12 passes through the through-holes 15 in the partition wall 13 and is released into the evaporation source storage space 11. At this time, the space 31 between the outer container 2 and the inner container 1, which is formed in a vacuum state, acts to suppress the heat flow from the heater 21 to the evaporation source S, thereby suppressing the evaporation of the evaporation source S due to the heat from the heater 21. In other words, the side wall 1a of the inner container 1 can be prevented from becoming a heat source for the evaporation source S. As a result, the evaporation raw material S that comes into contact with the partition wall 13, which is the heat source, can continue to evaporate stably at an approximately constant evaporation rate due to its own weight falling as it evaporates, and a mixed gas G3, which is a mixture of the evaporation raw material G2 evaporated in the evaporation raw material storage space 11 and the carrier gas G1 diffused in the evaporation raw material storage space 11, is released from the mixed gas outlet 16.

[0088] Other methods of using the evaporation raw material container 300 are the same as those of the first embodiment (method of using the evaporation raw material container 100).

[0089] The solid vaporization supply system using the evaporation raw material container 300 of this embodiment is similar to the solid vaporization supply system of the first embodiment described above, except that the evaporation raw material container 300 (outer container 2) is heated from the outside using the heating heater 6 and the heating heater 21, and the evaporation of the evaporation raw material S due to heating from the heating heater 21 is suppressed by the action of the space 31 between the outer container 2 and the inner container 1, which is formed in a vacuum state.

[0090] <Fourth embodiment> Next, a fourth embodiment of the evaporation source container and solid vaporization supply system according to the present invention will be described in detail with reference to the drawings. Note that the present invention is not limited to this embodiment. Furthermore, elements that can be explained in the same way as in the first embodiment will be given the same reference numerals and will not be explained again.

[0091] <Overall structure> 5 is a cross-sectional view showing a fourth embodiment of the evaporation source container according to the present invention, specifically showing the gas flows of the carrier gas G1, evaporation source G2, and mixed gas G3. In this embodiment, as in the second and third embodiments, the heater 6 is installed outside the bottom surface of the outer container 2, and a heater 21 is also installed so as to surround the side surface of the outer container 2.

[0092] The evaporation material container 400 shown in FIG. 5 is a container for storing and evaporating the evaporation material S, and includes, for example, an inner container 1 and an outer container 2, which are two containers forming a double-walled structure; a lid body 3 having an inner lid 3a and an outer lid 3b; a fastening member 4 for fastening the outer container 2 and the outer lid 3b; and a gas inlet pipe 5 for discharging a carrier gas G1 supplied from the outside into the inner container 1. Furthermore, the evaporation material container 400 has a plurality of protrusions 41, each having the same length L, on the inner wall of the outer container 2 or the outer wall of the inner container 1. Specifically, the protrusions 41 are arranged so that the distance between the outer wall of the inner container 1 and the outer wall of the outer container 2 is maintained at length L around the entire circumference. In other words, a constant gap is formed between the inner wall of the outer container 2 and the outer wall of the inner container 1. FIG. 5 illustrates, as an example, a case in which the protrusions 41 are provided on the inner wall of the outer container 2. The protrusions 41 are provided so that their length L (the distance between the outer wall of the inner container 1 and the inner wall of the outer container 2) is longer than the height H of the carrier gas diffusion space 12 (L>H) so that the average surface temperature of the partition wall 13 is 50°C or more higher than the average surface temperature of the side wall 1a of the inner container 1 when evaporating the evaporation raw material S. From a manufacturing standpoint, it is preferable to use a material of the same quality as that of the inner container 1 or the outer container 2. This is because the protrusions 41 are bonded to the inner container 1 or the outer container 2. This reduces the heat flow from the heater 21, which is installed to surround the side surface of the outer container 2, to the evaporation raw material S. Note that, except for the provision of the protrusions 41 on the inner wall of the outer container 2 or the outer wall of the inner container 1, this is the same as the evaporation raw material container 100 of the first embodiment described above.

[0093] Furthermore, the materials of each component other than the protrusion 41 used in the evaporation raw material container 400, the carrier gas, and the evaporation raw material can be explained in the same way as for the evaporation raw material container 100 of the first embodiment described above, so duplicate explanations will be omitted.

[0094] The manufacturing method of the evaporation material container 400 is the same as that of the first embodiment (the manufacturing method of the evaporation material container 100) described above, except that protrusions 41 are provided on the inner wall of the outer container 2 or the outer wall of the inner container 1.

[0095] <How to use the evaporation material container> In this embodiment, first, the carrier gas inlet 14 of the evaporation raw material container 400 is connected to a carrier gas tank (not shown) via a joint member or the like, and further, the mixed gas outlet 16 is connected to semiconductor processing equipment (not shown) via a joint member or the like.

[0096] Next, the evaporation raw material S is charged into the inner container 1 (above the partition wall 13) of the evaporation raw material container 400, and then the inner container 1 is closed with the lid body 3 (inner lid 3a, outer lid 3b), and the flange 2a of the outer container 2 and the outer lid 3b are fixed with the fastening member 4 to seal the inner container 1. Then, a heater 6 is installed outside the bottom side of the evaporation raw material container 400, and a heater 21 is installed so as to surround the side surface of the outer container 2.

[0097] Next, the heater 6 and the heater 21 are used to heat the evaporation source container 400 (outer container 2) from the outside, and a carrier gas G1 is supplied from a carrier gas tank (not shown) into the inner container 1 of the evaporation source container 400. Specifically, the carrier gas G1 flows through the gas inlet pipe 5 and is released and diffused from its tip in the carrier gas diffusion space 12. The carrier gas G1 diffused in the carrier gas diffusion space 12 passes through the through-holes 15 in the partition wall 13 and is released into the evaporation source storage space 11. At this time, the difference between the length L of the protrusions 41 and the height H of the carrier gas diffusion space 12 (L>H) in the evaporation source container 400 suppresses the heat flow from the heater 21 to the evaporation source S, thereby suppressing the evaporation of the evaporation source S due to heating from the heater 21. In other words, the side wall 1a of the inner container 1 can be prevented from becoming a heat source for the evaporation source S. As a result, the evaporation raw material S that comes into contact with the partition wall 13, which is the heat source, can continue to evaporate stably at an approximately constant evaporation rate due to its own weight falling as it evaporates, and a mixed gas G3, which is a mixture of the evaporation raw material G2 evaporated in the evaporation raw material storage space 11 and the carrier gas G1 diffused in the evaporation raw material storage space 11, is released from the mixed gas outlet 16.

[0098] Other methods of using the evaporation raw material container 400 are the same as those of the first embodiment (method of using the evaporation raw material container 100).

[0099] The solid vaporization supply system using the evaporation raw material container 400 of this embodiment is similar to the solid vaporization supply system of the first embodiment described above, except that the evaporation raw material container 400 (outer container 2) is heated from the outside using the heating heater 6 and the heating heater 21, and that the evaporation of the evaporation raw material S due to heating from the heating heater 21 is suppressed by providing protrusions 41 on the inner wall of the outer container 2 or the outer wall of the inner container 1.

[0100] First to Fourth Embodiments In the evaporation raw material containers (100-400) of the first to fourth embodiments described above, the contact parts with the evaporation raw material S in gas and solid state are made of the same metal material as the metal constituting the evaporation raw material S and have a purity of 99 to 99.9999% (2N to 6N). However, from the viewpoint of thermal conductivity and strength, it is more preferable to make the contact parts of the same metal material as the metal constituting the evaporation raw material S and have a purity of 99.99 to 99.999% (4N to 5N). [Example]

[0101] The evaporation material container according to the present invention will be described in more detail below with reference to examples and comparative examples, although the present invention is not limited thereto.

[0102] <Examples 1 to 24> In Examples 1 to 24, evaporation source containers 100 to 400 were fabricated, each including an inner container 1, an outer container 2, a lid 3, a fastening member 4, a gas inlet pipe 5, and other components constituting the container (including joint members (not shown)). Specifically, in Examples 1 to 6, an evaporation source container 100 was fabricated having a "container wall and gas inlet pipe" (corresponding to the "inner container wall" in the table) made of materials with the "materials" and "purity (%)" shown in Table 1. In addition, in Examples 7 to 12, an evaporation source container 200 was fabricated having a "container wall and gas inlet pipe" made of materials with the "materials" and "purity (%)" shown in Table 2. In addition, in Examples 13 to 18, an evaporation source container 300 was fabricated having a "container wall and gas inlet pipe" made of materials with the "materials" and "purity (%)" shown in Table 3. In Examples 19 to 24, the evaporation material container 400 having the "container wall and gas introduction pipe" made of the materials with the "materials" and "purity (%)" shown in Table 4 was produced.

[0103] <Comparative Examples 1 to 11> On the other hand, in Comparative Examples 1 to 6, the evaporation raw material containers were fabricated under the conditions shown in Table 5. Specifically, the "container wall and gas inlet pipe" were fabricated using materials with the "materials" and "purity (%)" shown in Table 5. The structure of the evaporation raw material containers fabricated in the Comparative Examples was the same as the evaporation raw material container 100. In other words, only the materials of the "container wall and gas inlet pipe" were different from those in Examples 1 to 6.

[0104] In each of the examples and comparative examples, a valve with a CV value (water displacement) of 1.5 was installed downstream of the mixed gas outlet, and mixed gas G3 was supplied through this valve.

[0105] <Method of Example> The thin film-forming metal halide compound S shown in the "Evaporation Raw Material" column in Tables 1 to 5 was placed into the evaporation raw material containers of Examples 1 to 24 and Comparative Examples 1 to 6, and a carrier gas G1 was supplied into the inner container to generate a mixed gas G3 by mixing the evaporated thin film-forming metal halide compound G2 with the carrier gas G1. Specifically, 3 kg of the thin film-forming metal halide compound S was heated for 20 hours to evaporate (vaporize).

[0106] In the evaporation source containers of Examples 1 to 24, the heater was controlled so that the average surface temperature of the partition wall was 50°C to 60°C higher than the average surface temperature of the side wall of the inner container when evaporating the thin film-forming metal halide compound S. On the other hand, in Comparative Examples 1 to 6, the heater was controlled so that the average surface temperature was 35°C to 45°C higher than the average surface temperature.

[0107] The resulting mixed gas G3 was used to form a film by atomic layer deposition (ALD), and the evaporation rate (g / min) was measured using a mass flow meter at the beginning (1 h after heating), middle (10 h after heating), and end (18 h after heating).

[0108] <Other Examples> Next, the evaporation material container according to the present invention will be described more specifically with reference to other examples.

[0109] <Examples 25 to 30> In Examples 25 to 30, the same evaporation raw material container 100 as in Examples 1 to 6 described above (the evaporation raw material container 100 having a "container wall and gas inlet pipe" made of materials with the "material" and "purity (%)" shown in Table 6) was manufactured, and a valve with a CV value (water displacement) of 1.5 was installed downstream of the mixed gas outlet, and mixed gas G3 was supplied through this valve.

[0110] <Method of Example> The thin film-forming metal halide compound S shown in the "evaporation raw material" column of Table 6 was placed in the evaporation raw material container of Examples 25 to 30, and carrier gas G1 was supplied into the inner container to generate mixed gas G3 by mixing evaporated thin film-forming metal halide compound G2 with carrier gas G1. Specifically, 3 kg of thin film-forming metal halide compound S was heated for 20 hours to evaporate (vaporize).

[0111] In addition, for the evaporation raw material containers of Examples 25 to 30, when evaporating the metal halide compound S for forming a thin film, the heater was controlled so that the heat flow rate due to heat transfer from the partition wall of the inner container was 80% to 90% or more of the total heat flow rate due to heat transfer from all container walls that make up the inner container.

[0112] The resulting mixed gas G3 was used to form a film by atomic layer deposition (ALD), and the evaporation rate (g / min) was measured using a mass flow meter at the beginning (1 h after heating), middle (10 h after heating), and end (18 h after heating).

[0113] Next, using evaporation source containers 100 (Examples 31 to 46) in which the "container wall and gas inlet tube" were made of materials with the "materials" and "purity (%)" shown in Table 7, and evaporation source containers in which the "container wall and gas inlet tube" were made of stainless steel shown in Table 8 (Comparative Examples 7 to 16: the same as the evaporation source container 100 except for the material of the "inner container wall"), the "amount of impurities in the evaporation source," "internal surface roughness," and "growth rate" after forming an ALD film by atomic layer deposition (ALD) were evaluated.

[0114] Tables 7 and 8 show the "amount of impurities in the evaporated raw material," "internal surface roughness," and "growth rate" after the ALD film was formed by atomic layer deposition (ALD).

[0115] The amount of impurities (12 elements shown in Tables 7 and 8) in the evaporation raw materials after film formation was measured using an ICPMS (inductively coupled plasma mass spectrometer). Note that the amount of impurities (12 elements shown in Tables 7 and 8) in the evaporation raw materials before film formation is listed in the "Before film formation" column of Table 7.

[0116] The amount of impurities was measured by the following method. First, after film formation, the residue of the evaporation source material S remaining in the inner container was collected. Next, a predetermined amount of the collected material was dissolved using aqua regia in an ICPMS (inductively coupled plasma mass spectrometry) device, and this was heated to 120°C on a hot plate to evaporate and dry. Thereafter, the evaporated and dried material was diluted to obtain a measurement sample. Then, the metal impurities in the measurement sample were measured using the above-mentioned analyzer.

[0117] In addition, the surface roughness of the inner surface of the inner container was measured before and after the film formation using an AFM (atomic force microscope) analyzer (manufactured by HORIBA Corporation). This surface roughness was measured multiple times and the average value was calculated. The surface roughness before film formation was designated B, and the surface roughness after film formation was designated A, and the value A / B was calculated by dividing A by B. The calculated "A / B" values ​​are shown in the "Internal surface roughness" column of Tables 7 and 8.

[0118] In addition, the growth rate (GPC: Growth Per Cycle) was measured during film formation using the atomic layer deposition (ALD) method. Specifically, during the above-mentioned film formation, a valve was opened and closed once every 0.2 seconds to introduce mixed gas G3 containing the evaporation source material into the film formation chamber. Each 0.2 seconds, during which the valve was opened and closed, was counted as one cycle. The film thickness formed on an 8-inch silicon wafer was measured, and the film growth rate per unit time (one cycle) was calculated.

[0119] [Table 1]

[0120] [Table 2]

[0121] [Table 3]

[0122] [Table 4]

[0123] [Table 5]

[0124] [Table 6]

[0125] [Table 7]

[0126] [Table 8]

[0127] <Evaluation> As shown in Tables 1 to 5, the evaporation raw material containers (100, 200, 300, 400) of Examples 1 to 24 showed a smaller decrease in evaporation rate at the end of the evaporation period of the evaporation raw material compared to the evaporation raw material containers of Comparative Examples 1 to 6. Furthermore, as shown in Table 6, the evaporation raw material containers 100 of Examples 25 to 30 also showed a smaller decrease in evaporation rate at the end of the evaporation period of the evaporation raw material, similar to the evaporation raw material containers of Examples 1 to 24.

[0128] Furthermore, as can be seen from the results of Tables 7 and 8, the evaporation source containers of Examples 31 to 46 were found to have a smaller amount of impurities than the evaporation source containers of Comparative Examples 7 to 16. Furthermore, the evaporation source containers of Examples 31 to 46 had an "A / B" value for "internal surface roughness" close to 1, indicating a small difference in surface roughness before and after film formation. This small difference in surface roughness indicates that the degree of corrosion caused by the evaporation source was small, and thus the corrosion resistance can be said to be high. From these results, it can be said that the evaporation source containers of Examples 31 to 46 have excellent corrosion resistance. Additionally, the evaporation source containers of Examples 31 to 46 also had a fast growth rate. [Explanation of symbols]

[0129] 100,200,300,400 Evaporation raw material container 1 Inner container 1a side wall 1b bottom wall 2 Outer container 2a Tsuba 2b Hole 3 Lid 3a Inner lid 3b Outer lid 4 Fastening members 5 Gas inlet pipe 6,21 Heating heater 11 Evaporation raw material storage space 12 Carrier gas diffusion space 13 Partition Wall 14 Carrier gas inlet 15 through holes 16 Mixed gas outlet 22 Heat Shield 31 Space 41 Protrusion G1 Carrier Gas G2,S Evaporation raw material (metal halide compound for thin film formation) G3 mixed gas

Claims

1. An evaporation raw material container for storing and evaporating an evaporation raw material, an inner container housed in an outer container and forming a double-wall structure together with the outer container; a lid body having an inner lid detachably attached to the inner container and an outer lid detachably attached to the outer container; a gas introduction pipe connected to a carrier gas introduction port disposed in the lid; Equipped with Furthermore, the inner container is provided with a partition wall for dividing the interior thereof into two spaces, namely, an evaporation raw material storage space on the inner lid side constituting the upper wall of the inner container and a carrier gas diffusion space on the bottom wall side of the inner container, and the evaporation raw material is stored on the upper surface of the partition wall; The partition wall has one or more through holes formed therein, The tip of the gas introduction pipe has a structure that penetrates the partition wall and extends to a position directly above the bottom wall of the inner container, the carrier gas supplied through the carrier gas inlet is released from a tip of the gas inlet pipe into the carrier gas diffusion space, the carrier gas diffused in the carrier gas diffusion space is released into the evaporation raw material storage space through the through-hole, and a mixed gas obtained by mixing the evaporation raw material evaporated in the evaporation raw material storage space by heating and the carrier gas diffused in the evaporation raw material storage space is released from a mixed gas outlet disposed in the lid body, When evaporating the evaporation raw material, the average surface temperature of the partition wall is higher than the average surface temperature of the side wall of the inner container by 50°C or more, a second area, which is a contact area between the partition wall and the evaporation raw material, being 80% or more of a first area, which is a contact area between all of the container walls constituting the inner container and the evaporation raw material; A container for evaporation raw material.

2. a heater for heating the evaporation raw material is installed on the outside of the bottom surface of the outer container; 2. The evaporation material container according to claim 1, wherein the evaporation material container is a container for evaporating a raw material.

3. a heat shield disposed between the inner wall of the outer container and the outer wall of the inner container; 2. The evaporation material container according to claim 1, wherein the evaporation material container is a container for evaporating a raw material.

4. A space between the inner wall of the outer container and the outer wall of the inner container is evacuated.

2. The evaporation material container according to claim 1, wherein the evaporation material container is a container for evaporating a raw material.

5. A plurality of protrusions of the same length are provided on the inner wall of the outer container or the outer wall of the inner container, forming a gap at a constant interval between the inner wall of the outer container and the outer wall of the inner container, and the "length of the gap" is greater than the "length in the height direction of the carrier gas diffusion space." 2. The evaporation material container according to claim 1, wherein the evaporation material container is a container for evaporating a raw material.

6. An evaporation raw material container for storing and evaporating an evaporation raw material, an inner container housed in an outer container and forming a double-wall structure together with the outer container; a lid body having an inner lid detachably attached to the inner container and an outer lid detachably attached to the outer container; a gas introduction pipe connected to a carrier gas introduction port disposed in the lid; Equipped with Furthermore, the inner container is provided with a partition wall for dividing the interior thereof into two spaces, namely, an evaporation raw material storage space on the inner lid side constituting the upper wall of the inner container and a carrier gas diffusion space on the bottom wall side of the inner container, and the evaporation raw material is stored on the upper surface of the partition wall; The partition wall has one or more through holes formed therein, The tip of the gas introduction pipe has a structure that penetrates the partition wall and extends to a position directly above the bottom wall of the inner container, the carrier gas supplied through the carrier gas inlet is released from a tip of the gas inlet pipe into the carrier gas diffusion space, the carrier gas diffused in the carrier gas diffusion space is released into the evaporation raw material storage space through the through-hole, and a mixed gas obtained by mixing the evaporation raw material evaporated in the evaporation raw material storage space by heating and the carrier gas diffused in the evaporation raw material storage space is released from a mixed gas outlet disposed in the lid body, when evaporating the evaporation raw material, the heat flow rate due to heat transfer from the partition wall is 80% or more of the total heat flow rate due to heat transfer from all container walls constituting the inner container; a second area, which is a contact area between the partition wall and the evaporation raw material, being 80% or more of a first area, which is a contact area between all of the container walls constituting the inner container and the evaporation raw material; A container for evaporation raw material.

7. a heater for heating the evaporation raw material is installed on the outside of the bottom surface of the outer container; 7. The evaporation material container according to claim 6.

8. a heat shield disposed between the inner wall of the outer container and the outer wall of the inner container; 7. The evaporation material container according to claim 6.

9. A space between the inner wall of the outer container and the outer wall of the inner container is evacuated.

7. The evaporation material container according to claim 6.

10. A plurality of protrusions of the same length are provided on the inner wall of the outer container or the outer wall of the inner container, forming a gap at a constant interval between the inner wall of the outer container and the outer wall of the inner container, and the "length of the gap" is greater than the "length in the height direction of the carrier gas diffusion space." 7. The evaporation material container according to claim 6.

11. The inner container, the inner lid and the gas inlet pipe are configured such that the contact portions with the evaporation raw material in gaseous and solid states are made of the same metal material as the metal constituting the evaporation raw material and have a purity of 2N to 6N.

11. The evaporation material container according to claim 1, wherein the evaporation material container is a container for evaporating a material.

12. moreover, a fastening member for fastening the outer container and the outer lid; Equipped with The fastening member is composed of a bolt member inserted into a bolt insertion hole provided in the outer container and the outer lid, and a nut member that can be threadedly fastened to the bolt member.

12. The evaporation material container according to claim 11.

13. When using a metal halide compound for thin film formation as the evaporation source, The thin film-forming metal halide compound is a compound that can be represented by the general formula: MXn, M represents a metal element constituting the thin film-forming metal halide compound, X represents a halogen element, and n represents the number of Xs; 12. The evaporation material container according to claim 11.

14. Stores evaporated raw materials used in film formation by chemical vapor deposition (CVD).

12. The evaporation material container according to claim 11.

15. Store the evaporated raw materials used in film formation by atomic layer deposition (ALD).

12. The evaporation material container according to claim 11.

16. heating the carrier gas diffused in the carrier gas diffusion space; mixing the evaporated raw material with a heated carrier gas to generate a mixed gas; 12. The evaporation material container according to claim 11.

17. An evaporation material container according to any one of claims 1 to 10; an evaporation source; Equipped with A solid vaporization supply system.

18. moreover, a carrier gas supply means for supplying a carrier gas from a carrier gas inlet into the evaporation material container; Equipped with 18. The solid vaporization delivery system of claim 17.

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