JP4585182B2 - Trimethylindium filling method and filling container - Google Patents

Description

  The present invention relates to a filling method of a solid organometallic compound into a filling vessel and a filling vessel of a solid organometallic compound filled by the filling method. More specifically, a solid organometallic compound that is a material for vapor phase epitaxial growth by a Metalorganic Chemical Vapor Deposition (hereinafter abbreviated as “MOCVD”) method used when manufacturing materials for electronic industry such as compound semiconductors, The present invention relates to a filling method of a solid organometallic compound into a filling vessel that can be stably supplied to a vapor phase epitaxial growth apparatus at a constant concentration for a long period of time, and a filling vessel filled with the solid organometallic compound by the filling method.

  Organometallic compounds such as trimethylindium are widely used as raw materials for producing materials for electronic industry.

  In recent years, vapor phase epitaxial growth by the MOCVD method or the like is frequently used as a method for producing materials for electronic industry using an organometallic compound. For example, a thin film of a compound semiconductor is manufactured by the MOCVD method, and an organic metal compound such as trimethylaluminum, trimethylgallium, or trimethylindium is used as a raw material.

  When these organometallic compounds are used in the MOCVD method, when the organometallic compounds are solid under the conditions used, the organometallic compounds are usually separated into a carrier gas inlet (2a) and a carrier gas outlet as shown in FIG. (3a) is filled in a filling container (hereinafter referred to as filling container A), a carrier gas such as hydrogen gas is introduced into the container through the carrier gas inlet (2a), and from the carrier gas outlet (3a). A method is used in which the organometallic compound is taken out as a gas saturated in the carrier gas and supplied to the MOCVD apparatus.

  In this case, when the organometallic compound is solid at the temperature used in the above supply, the carrier gas passes through the solid organometallic compound in the filled container A without making sufficient contact with the solid organometallic compound. It is difficult to maintain a uniform contact state between the carrier gas and the solid organometallic compound due to the formation of a flow path, and the carrier gas is stably solid from the filling container A to the MOCVD apparatus at a constant concentration for a long period of time. There is a problem that it is difficult to supply the organometallic compound. In addition, in the supply of the solid organometallic compound by the method using the carrier gas as described above, if the amount of the solid organometallic compound filled in the filling container A is increased, it can be stably supplied to the MOCVD apparatus. The proportion of the amount of the solid organometallic compound is reduced with respect to the amount of the filled solid organometallic compound, and as a result, the remaining amount of the solid organometallic compound in the filling container increases and the solid organometallic compound cannot be used effectively. There is a problem.

  In order to solve these problems, various proposals have been made regarding methods for filling a solid container A with a solid organometallic compound. For example, Patent Literature 1, Patent Literature 2, Patent Literature 3, Patent Literature 4 and Patent Literature 5 propose a method of filling a solid container with a solid organometallic compound together with a filler. For example, Patent Document 6 proposes a method in which a solid organometallic compound is coated on an inert carrier and filled in a filling container A.

  In addition to the above, various proposals have been made for the structure of the filling container itself filled with the solid organometallic compound in the method for solving the above-mentioned problems. For example, in Patent Document 7 and the like, as shown in FIG. 34, a diffuser (20a) for homogenizing the gas is provided at the carrier gas inlet, and the carrier gas is uniformly distributed to the solid organometallic compound. A filling container (hereinafter referred to as filling container B) has been proposed.

  For example, Patent Document 8 proposes a filling container (hereinafter referred to as filling container C) having a solid organometallic compound arrangement chamber (21a) having air permeability as shown in FIG.

  Further, for example, Patent Document 9 proposes a filling container (hereinafter referred to as filling container D) in which a porous inlet chamber as shown in FIG. 36 is used as a filling portion of a solid organometallic compound.

On the other hand, in Patent Document 10 and the like, a method for controlling the particle diameter in the case of using a ruthenium compound has been proposed for stabilizing the supply of a solid organometallic compound.
Japanese Patent Publication No. 5-39915 Japanese Patent Publication No.6-20051 JP 7-58023 A JP-A-8-250440 JP-A-8-299778 Japanese Patent No. 2651530 Japanese Patent Publication No. 2-12496 JP-A-10-223540 JP 2002-83777 A JP 2003-160865 A

  However, in the proposal of the filling method and the filling container in Patent Documents 1 to 9, the particle size of the solid organometallic compound itself to be filled in the filling container has not been studied.

  In addition, although the effect of the control of the particle size of the ruthenium compound on the supply stability in Patent Document 10 or the like has been described by several times of film formation, the effect of the initial supply state is described, but the ruthenium compound is constant for a long time. It is not clear about the effect which supplies stably with the density | concentration of. As a result of studies by the present inventors, it has been found that there is a particle size control method for obtaining not only initial stability but also long-term stability in the supply of a solid organometallic compound using a carrier gas.

  The present invention solves the above-mentioned problems, and the problem to be solved by the present invention is that a solid organometallic compound is stably supplied to a vapor phase epitaxial growth apparatus such as an MOCVD apparatus at a constant concentration for a long period of time. It is to provide a filling method of a solid organometallic compound in a filling vessel for a solid organometallic compound that can be supplied, and a filling container filled with the solid organometallic compound by the filling method.

  As a result of studies by the present inventors in order to solve the above-mentioned problems, a solid organometallic compound is supplied at a constant concentration for a long period of time by filling a filled container with a solid organometallic compound and circulating a carrier gas. Therefore, when filling the solid organometallic compound into the filling container for the solid organometallic compound, the initial supply stability is controlled by controlling the particle diameter of the solid organometallic compound to a certain particle size or less. As a result, the present inventors have found that the supply stability can be maintained for a long period of time, and the present invention has been completed.

  That is, when filling the solid organometallic compound into the filling container for the solid organometallic compound, the particle diameter of the solid organometallic compound is 8 mm or less, and further particles having a particle diameter of 2.5 to 6 mm are contained in the solid organometallic compound. It is related with the filling method of the solid organometallic compound to the filling container for solid organometallic compounds characterized by including as an essential component.

Furthermore, in the filling method of the present invention, the filler can be used together with the solid organometallic compound whose particle size is controlled as described above.
That is, in the method of filling a solid organometallic compound into a filling vessel for a solid organometallic compound, the solid organometallic compound is a particle having a particle size of 8 mm or less, and further a particle having a particle size of 2.5 to 6 mm It is related with the filling method of the solid organometallic compound to the filling container for solid organometallic compounds characterized by including as an essential in.

  Furthermore, in the filling method of the solid organometallic compound into the filled container for the solid organometallic compound according to the present invention, the filling material is filled together with the solid organometallic compound, and the size of the filler is 0.8 to 8 mm. use.

  Further, in the solid organometallic compound filling method of the solid organometallic compound filling container of the present invention, the solid organometallic compound filling container is for a solid organometallic compound having a carrier gas inlet and a carrier gas outlet. The filling container has a structure in which the inside of the filling container is divided into a plurality of vertical spaces, and the carrier gas introduced from the carrier gas introduction port flows through each vertical space and is discharged from the carrier gas discharge port. It is characterized by being a filling container for solid organometallic compounds.

  Furthermore, in the method for filling a solid organic metal compound into the solid organic metal compound filling container of the present invention, the solid organic metal compound filling container can have the requirements (a) to (c).

(a) The inside of the filling container is vertically divided by at least one partition wall, and the inside of the filling container is divided into at least two spaces.
(b) The space inside the filling container formed by partitioning with a partition wall has a space having a carrier gas inlet and a space having a carrier gas outlet.
(c) The partition inside the filling container has a partition having an opening for flowing the carrier gas from the carrier gas inlet to the carrier gas outlet through each space in the filling container.

  In the method for filling a solid organometallic compound into the solid organometallic compound filling container of the present invention, the solid organometallic compound filling container having the requirements (a) to (c) includes the opening. In the case where the opening is disposed at the lower part of the partition wall, the container has a height of 1/3 or less of the inner height of the container from the inner bottom surface of the filling container. It is characterized in that each opening is installed at a position more than 2/3 of the internal height.

  Furthermore, in the method for filling a solid organometallic compound into the filled container for a solid organometallic compound of the present invention, the filling vessel for a solid organometallic compound having the requirements (a) to (c), It has a filling port for filling a solid organometallic compound into the space inside the filling container formed by partitioning with a partition wall.

  Further, in the solid organometallic compound filling method of the present invention, the solid organometallic compound filling container has a solid organometallic compound filling container having a carrier gas inlet and a carrier gas outlet. In the container, the inside of the filling container is divided into a plurality of vertical spaces, and the carrier gas introduced from the carrier gas inlet is circulated as a downward flow in each vertical space by the carrier gas flow direction reversing means, and the carrier gas is discharged. It is a filling container for a solid organometallic compound having a structure discharged from an outlet.

  Furthermore, in the method of filling a solid organometallic compound into the solid organometallic compound filling container of the present invention, the solid organometallic compound filling container can have the requirements (d) to (h).

(d) The inside of the filling container is vertically divided by at least one partition wall, and the inside of the filling container is partitioned into at least two spaces.
(e) The space inside the filling container formed by partitioning with a partition wall has a space having a carrier gas inlet and a space having a carrier gas outlet.
(f) In the partition wall inside the filling container, a communication channel having a lower opening and an upper opening for allowing the carrier gas to flow from the carrier gas inlet to the carrier gas outlet through each space in the filling container is provided. Having a partition
(g) In the communication channel, the carrier gas introduced into the filling container is introduced from the lower opening of the communication channel and discharged to the upper opening.
(h) A solid organic metal compound filling container having a discharge channel having a lower opening through which a carrier gas is discharged from a lower portion of a space having a carrier gas discharge port to a carrier gas discharge port.

  Furthermore, in the method of filling the solid organometallic compound into the solid organometallic compound filling container of the present invention, the solid organometallic compound filling container having the requirements (d) to (h), In the communication channel, the lower opening of the communication channel is 1/3 or less of the inner height of the container from the inner bottom surface of the filling container, and the upper opening of the communication channel is 2 of the inner height of the container from the inner bottom surface of the filling container. The lower opening of the discharge channel is installed at a position of 1/3 or less of the inner height of the container from the inner bottom surface of the filling container. To do.

  Furthermore, in the method of filling the solid organometallic compound into the solid organometallic compound filling container of the present invention, the solid organometallic compound filling container having the requirements (d) to (h), It has a filling port for filling a solid organometallic compound into the space inside the filling container formed by partitioning with a partition wall.

  Moreover, in the method for filling a solid organometallic compound into the filled container for a solid organometallic compound according to the present invention, the filling vessel for a solid organometallic compound having the requirements (d) to (h) includes a partition wall. It is characterized by having a filling port for filling a solid organometallic compound in the space inside the filling container formed by partitioning with (3).

  In the method for filling a solid organometallic compound into the solid organometallic compound filling container of the present invention, trimethylindium can be used as the solid organometallic compound.

  Moreover, this invention relates to the filling container for solid organometallic compounds filled with the solid organometallic compound by said filling method of this invention.

  According to the present invention, when the solid organometallic compound is filled into the filling container for the solid organometallic compound, the initial stability is ensured by including particles of a certain size as the essential particle size of the solid organometallic compound. In addition, the solid organometallic compound can be stably supplied to a vapor phase epitaxial growth apparatus such as an MOCVD apparatus for a long period of time.

  The filling method of the present invention and the filling container filled with the solid organometallic compound by the filling method will be described in more detail below.

  In the filling method of the present invention, when the solid organometallic compound is filled into the filling vessel for the solid organometallic compound, the particle diameter of the solid organometallic compound is 8 mm or less, and further, particles having a particle diameter of 2.5 to 6 mm. Is contained as an essential component in the solid organometallic compound.

  In the present invention, as the size of the solid organometallic compound particles, for example, when filling the filling container with solid, it is assumed that the size passes through the opening of the filling port provided in the filling container. Usually, 8 mm or less, preferably 6 mm or less, more preferably 5 mm or less can be used, and particles having a particle size of 2.5 to 6 mm are included as essential in the solid organometallic compound. To do.

  When the solid organometallic compound exceeds 8 mm, when the carrier gas flow rate is increased, the contact area where the carrier gas contacts the solid organometallic compound is reduced, so that sufficient time to reach saturation cannot be obtained. Therefore, long-term supply stability cannot be obtained.

  The abundance ratio of 2.5 to 6 mm particles per solid organometallic compound is, for example, 30 to 100%, preferably 40 to 100%, and more preferably 50 to 100%.

  The reason for this is that when the proportion of particles of 2.5 to 6 mm per solid organometallic compound is small, for example, when many particles larger than 6 mm are included, the carrier gas flow rate increases as described above and the carrier gas It is considered that sufficient contact between the solid organic metal compound particles and the solid organometallic compound particles cannot be obtained, and long-term supply stability cannot be obtained. For example, in the case where many particles smaller than 2.5 mm are contained, the carrier Although the contact area between the gas and the particles becomes large, good initial supply stability can be obtained, but as long-term use, the solid organometallic compound is supplied to the carrier gas as saturated vapor and consumed. The phenomenon that the particles become finer, the carrier gas does not easily pass between the fine particles, and the carrier gas passes between the larger particles, It is considered that a flow path through which the organometallic compound and the carrier gas pass without sufficient contact is likely to be formed, and that supply stability is not obtained in long-term use. It is done.

  The method for molding the particles of the solid organometallic compound is not particularly limited, and a known molding method can be used as it is. As an example of this forming method, for example, a method of pulverizing a mass of a solid organometallic compound, or a method of liquefying and solidifying a solid organometallic compound can be used.

  Further, the method for controlling the particle diameter of the solid organometallic compound is not particularly limited, and a conventionally known method for adjusting the particle diameter can be used as it is. As a method for controlling the particle size, for example, in a method of pulverizing a mass of a solid organometallic compound, after pulverizing a solid organometallic compound, a method of collecting a sieve that has passed through a sieve having a certain size, etc. In addition, for example, as a method for liquefying a solid organometallic compound and solidifying it, a method for controlling the weight of a droplet or a method for controlling the shape of a liquid by the size of the mold is used. I can do it.

  In order to obtain the above-mentioned method, the solid organometallic compound has a particle size of 8 mm or less, and further contains particles having a particle size of 2.5 to 6 mm as essential components in the solid organometallic compound. The method is not particularly limited, and specifically, for example, a suitably pulverized solid organometallic compound is screened into one that does not pass through a sieve having a sieve size of 8 mm and one that does not pass through. The particles of the solid organometallic compound having a size of 8 mm or less that have been sieved are further pulverized to pass through a sieve having a 6 mm sieve and not passing through a 2.5 mm sieve. After obtaining the solid organometallic compound having a particle size of 2.5 to 6 mm, the particle having a particle size of 2.5 to 6 mm is used as an essential component, and the mesh size is 8 mm. 8mm or less solid obtained by passing through a sieve having A method of mixing the metal compound particles, or a solid organometallic compound that has been simply pulverized so as to include particles having a particle size of 2.5 to 6 mm, and a sieve mesh having a size of 2.5 to 6 mm. A method can be used in which the entire amount passed through the sieve is collected.

  Thus, in the method of filling a solid container with a solid organometallic compound and circulating a carrier gas, the solid organometallic compound has a particle size of 8 mm or less, and further, particles having a particle size of 2.5 to 6 mm are solid organic. The reason why the effect of being able to supply the solid organometallic compound at a constant concentration over a long period of time by including it as an essential component in the metal compound is as follows: In the space formed from the particles of that size, it is considered that the carrier gas is likely to be circulated, and when the solid organometallic compound does not include particles having a particle size of 2.5 to 6 mm In the space formed from these grains, although the carrier gas can sufficiently contact the solid organometallic compound in the solid organometallic compound in the initial stage of supply of the solid organometallic compound, The carrier gas in the course of use of the period is considered to be because the flow path sufficient contact with the solid organic metal compound will pass through without obtained is easily formed.

  Accordingly, in the supply of the solid organometallic compound using the carrier gas, if the particle diameter of the solid organometallic compound does not include particles having a particle diameter of 2.5 to 6 mm, there is no problem in the initial supply stability, but long There is a problem with the stability of the period. As in the present invention, by using the solid organic metal compound having a particle size of 2.5 to 6 mm as essential in the solid organic metal compound, the flow path is not easily formed, and the supply amount is short-term. It is considered that the carrier gas can circulate through the packed bed of the solid organometallic compound stably for a long period of time, and the supply stability of the solid organometallic compound is improved.

  In the filling method of the present invention, the structure of the usable filling container for the solid organometallic compound is not particularly limited, and for example, the containers known so far as described above can be used as they are.

  Furthermore, in the filling method of the present invention, in addition to the solid organic metal compound filling container having the above-described structure, in the solid organic metal compound filling container having a carrier gas introduction port and a carrier gas discharge port, the inside of the filling container includes a plurality of Filling container for solid organometallic compound characterized in that carrier gas divided into vertical space and introduced from carrier gas introduction port circulates in each vertical space and is discharged from carrier gas discharge port Can be used.

  An example of this filled container for a solid organometallic compound is shown in FIGS. As shown in FIGS. 1-4, the filling container for solid organometallic compounds used with the filling method of this invention partitions the inside of a filling container into the vertical direction by at least 1 or more partition (1), and is at least 2 or more. The structure is divided into two spaces. The partitioning method of the space by the partition wall (1) includes, for example, a structure in which the space is partitioned as shown in FIGS.

  The outer shape of the filling container can be, for example, a prismatic container such as a triangular prism, a quadrangular prism, a pentagonal prism, and a hexagonal prism in addition to a cylindrical container as shown in FIGS.

  Furthermore, the filling container for a solid organometallic compound used in the filling method of the present invention has a carrier gas inlet (2) leading to one space inside the filling container formed by partitioning with the partition wall (1), and the rest A structure having a carrier gas discharge port (3) leading to one of the spaces, for example, the structure shown in FIGS. The carrier gas is introduced into the filled container filled with the solid organometallic compound from the carrier gas inlet (2), and the inside of the filled container is circulated, and the organometallic compound is saturated in the carrier gas from the carrier gas outlet (3). It is taken out as gas and supplied to the MOCVD apparatus. The installation positions of the carrier gas introduction port (2) and the carrier gas discharge port (3) in the filling container are, for example, the filling container according to the way of dividing the space by the partition wall (1), the form of use of the filling container, and the like. There is a structure having a carrier gas introduction port (2) and a carrier gas discharge port (3) in the upper part of the container, and a structure having them on the side surface of the filling container, for example.

  In the partition wall (1) inside the filling container used in the present invention, as shown in FIGS. 1 to 4, the carrier gas is discharged from the carrier gas introduction port (2) through each space in the filling container (3). It has the partition (1) which comprises the opening part (30) for making it distribute | circulate to).

  As an example of the partition wall (1) having the opening (30), for example, the structure of FIGS.

  The positions of these openings (30) are such that the carrier gas is sufficiently circulated from the carrier gas inlet (2) to the carrier gas outlet (3) through the space filled with the solid organometallic compound, and the solid filled at that time. There is no particular limitation as long as the organometallic compound is in sufficient contact with the carrier gas and does not interfere with the stable supply of the organometallic compound, but the filled solid organometallic compound and the carrier gas are not particularly limited. In order to make saturation contact effectively, in the opening (30) for flowing the carrier gas, when the opening (30) is disposed at the lower part of the partition wall (1), the height inside the container from the inner bottom surface of the filling container. When the opening (30) is installed at a position of 1/3 or less, preferably 1/5 or less, more preferably 1/10 or less, and the opening (30) is arranged above the partition wall (1). The filling container Part bottom two thirds of the container inner height from, preferably 4/5 or more, more preferably installing opening (30) to 9/10 or more positions.

  In the filling container used in the filling method of the present invention, the carrier gas is circulated through each partitioned space due to the above structure, and is discharged from the carrier gas discharge port (3).

  In the filling container used in the present invention, as an example of the partition wall (1) having the opening (30), as an example in the case of one partition wall (1), for example, a structure as shown in FIG. As an example in the case where there are two partition walls (1), for example, a structure as shown in FIG. 2 is shown, and further, an example in which there are three or more partition walls (1). For example, the structure shown in FIG. 3 or 4 can be shown.

  Further, depending on the position of the opening (30) provided in the partition wall (1), the carrier gas is circulated through the space from the carrier gas introduction port (2) through the opening (30) to the carrier gas discharge port (3). In order to make it circulate, it can be set as the structure which provided the flow path (31) in each of the carrier gas introduction port (2) and the carrier gas discharge port (3). As an example of a filling container having a structure in which a flow path (31) is provided in each of the carrier gas introduction port (2) and the carrier gas discharge port (3), for example, one having a structure as shown in FIGS. I can do it.

  The flow path (31) is, for example, a tubular shape as shown in FIG. 9 or a flow path lower opening (32) at the lower part of the structure partitioned by the partition wall (1) as shown in FIG. 10 or FIG. It is possible to use those having The flow path (5) may be a combination of those having a tubular structure or a structure having a flow path lower opening (32) in the lower part of the structure partitioned by the partition wall (1).

  The position of the flow path lower opening (32) of the flow path (31) is 1/3 or less, preferably 1/5 or less, more preferably 1/10 or less of the container internal height from the inner bottom surface of the filling container. It is desirable to install in the position.

  The flow mode of the carrier gas in the filling container used in the filling method of the present invention will be described with reference to FIG. First, the carrier gas is introduced from the carrier gas inlet (2) and circulates in the space having the carrier gas inlet (2). The carrier gas flows through each space through the opening (4), is discharged from the carrier gas discharge port (3), and is supplied to the MOCVD apparatus. In addition, although the distribution | circulation form of carrier gas was demonstrated based on FIG. 1, when the inside of a filling container was divided into three or more space like FIGS. 2-4, it was provided in each partition (1). The carrier gas flows through the opening (30).

  In this flow form, in the structure in which the flow path (31) is provided in each of the carrier gas inlet (2) and the carrier gas outlet (3) as shown in FIG. 7, the carrier gas is the carrier gas inlet (2 ) And circulates in the space having the carrier gas inlet (2) after flowing through the flow path (31). The carrier gas flows through each space through the opening (30), flows through the flow path (31) provided in the carrier gas discharge port (3), is discharged from the carrier gas discharge port (3), and is supplied to the MOCVD apparatus. The

  Furthermore, in the filling container for solid organometallic compounds used in the filling method of the present invention, a filling port (9) for filling the space inside the filling container formed by partitioning with the partition wall (1) with the solid organometallic compound. Can also be provided. By providing this filling port (9), the solid organometallic compound can be charged as it is. In this invention, the filling port of a filling container can be provided in the upper part of a filling container, for example like FIGS. Further, the carrier gas introduction port (2) and / or the carrier gas discharge port (3) can be separated from the filling container, so that the carrier gas introduction port (2) and / or the carrier gas discharge port (3) can be separated. And a filling port (9). The separated carrier gas introduction port (2) and / or carrier gas discharge port (3) and the filling container are used together again through the connecting part (26). As an example of this structure, for example, as shown in FIG. 12, a connecting part (26) that can be separated as a filling port is provided between the carrier gas introduction port (2) and the filling container, and the connection parts are joined together via this. What is used.

  In addition, in the filling container used with the filling method of this invention, the valve | bulb (22) which can be opened and closed is provided in a carrier gas introduction port (2) and a carrier gas discharge port (3) like FIG. When the carrier gas is circulated, the valve (22) is used with the valve open, and when the organometallic compound is not supplied, the solid organometallic compound is usually contaminated or filled with the valve closed. Prevents evaporation from sublimating outside the container.

  As described above, the filling container used in the filling method of the present invention is divided into a plurality of spaces by the partition wall (1) inside the filling container, and the carrier gas introduced from the carrier gas inlet (2) is in each container space. In all the spaces in the filled solid organometallic compound, the structure passes from the upper part of the space to the lower part of the space and flows to the carrier gas discharge port (3). As described above, since the inside of the container is partitioned by the partition wall (1) and divided into a plurality of spaces, the cross-sectional area of each space is reduced and the contact between the carrier gas and the solid organometallic compound is sufficiently performed. The contact state between the carrier gas and the solid organometallic compound can be kept uniform without the formation of a flow path, and the solid organometallic compound can be stably transferred from the filling container to the MOCVD apparatus at a constant concentration for a long time by the carrier gas. It becomes possible to supply, and by filling the container with a solid organometallic compound with a controlled particle size, the effect of controlling the particle size can be more effectively brought out.

  Furthermore, in the filling method of the present invention, in addition to the solid organic metal compound filling container having the above-described structure, in the solid organic metal compound filling container having a carrier gas introduction port and a carrier gas discharge port, the inside of the filling container includes a plurality of The carrier gas is divided into vertical spaces and has a structure in which the carrier gas introduced from the carrier gas inlet by the carrier gas flow direction reversing means flows through each vertical space as a downward flow and is discharged from the carrier gas outlet. It is possible to use a filled container for a solid organometallic compound characterized by the following.

  The structure of the filling container that can be used in the present invention is not particularly limited as long as the internal space is divided into a plurality of vertical spaces, and the carrier gas flows through each vertical space as a downward flow.

  The carrier gas flow direction reversing means of the present invention reverses the flow direction of the carrier gas that flows through the fractionated vertical space as a downward flow, and supplies the carrier gas as a downward flow above the adjacent vertical space. Means. Specific examples of the carrier gas flow reversal means include those in which a connecting channel is provided in the partition as shown in FIGS. 13 to 20, and the partition in the connecting channel as shown in FIGS. As shown in FIG. 23 and FIG. 24, there may be mentioned what constitutes the communication flow path with the partition walls, but it is not limited thereto.

  An example of the filling container for a solid organometallic compound used in the present invention is shown in FIGS. As shown in FIGS. 13-16, the filling container for solid organometallic compounds used with the filling method of this invention partitions the inside of a filling container into the vertical direction by at least 1 or more partition (1), and is at least 2 or more. The structure is divided into two spaces. The partitioning method of the space by the partition wall (1) includes, for example, a structure in which the space is partitioned as shown in FIGS.

  The outer shape of the filling container can be, for example, a prismatic container such as a triangular prism, a quadrangular prism, a pentagonal prism, and a hexagonal prism, in addition to a cylindrical container as shown in FIGS.

  Furthermore, the filling container for a solid organometallic compound used in the filling method of the present invention has a carrier gas inlet (2) leading to one space inside the filling container formed by partitioning with the partition wall (1), and the rest A structure having a carrier gas discharge port (3) leading to one of the spaces, for example, the structure shown in FIGS. The carrier gas is introduced into the filled container filled with the solid organometallic compound from the carrier gas inlet (2), and the inside of the filled container is circulated, and the organometallic compound is saturated in the carrier gas from the carrier gas outlet (3). It is taken out as gas and supplied to the MOCVD apparatus. The installation positions of the carrier gas introduction port (2) and the carrier gas discharge port (3) in the filling container are, for example, the filling container according to the way of dividing the space by the partition wall (1), the form of use of the filling container, and the like. There is a structure having a carrier gas introduction port (2) and a carrier gas discharge port (3) in the upper part of the container, and a structure having them on the side surface of the filling container, for example.

  In the partition wall (1) inside the filling container of the present invention, as shown in FIGS. 13 to 16, the carrier gas is supplied from the carrier gas inlet (2) to the carrier gas outlet (3) through each space in the filling container. It has a partition wall (1) comprising a communication channel (6) having a lower opening (4) and an upper opening (5) for circulation.

  Moreover, as shown to FIGS. 13-16, the carrier gas introduce | transduced inside the filling container is introduce | transduced from the lower opening part (4) of a connection flow path (6), and the filling container of this invention is an upper opening part (5). ).

  Since the filling container of the present invention includes the flow channel having the above structure, the carrier gas flows through each partitioned space and is discharged from the carrier gas discharge port (3).

  Furthermore, as shown to FIGS. 13-16, the filling container of this invention is a lower opening part (7) which discharges carrier gas to a carrier gas discharge port (3) from the lower part of the space which has a carrier gas discharge port (3). A discharge channel (8) having

  In the filling container of the present invention, examples of the communication channel (6) and the channel (8) include a structure as shown in FIG. 13 as an example of a single partition wall (1). As an example of the case where there are two partition walls (1), for example, a structure as shown in FIG. 14 is shown, and further, as an example when there are three or more partition walls (1), For example, the structure of FIG. 15 or FIG. 16 can be shown.

  In the filled container for a solid organometallic compound of the present invention, the communication channel (6) can be provided with one or a plurality of tubular ones as shown in FIGS.

  A carrier gas distribution mode in the filling container of the present invention will be described with reference to FIG. First, the carrier gas is introduced from the carrier gas inlet (2) and descends in the space having the carrier gas inlet (2). The carrier gas flows in from the lower opening (4) of the communication channel (6) as the carrier gas flow direction reversing means in the vicinity of the bottom of the container, flows through the communication channel (6) as an upward flow, and discharges the carrier gas. It is supplied to the upper part of the space having the outlet (3). The carrier gas supplied to the upper part of the space having the carrier gas discharge port (3) descends. The discharge channel (8) rises from the lower opening (7) of the discharge channel (8) near the lower part of the space having the carrier gas discharge port (3), and is discharged from the carrier gas discharge port (3). And supplied to the MOCVD apparatus. In addition, although the distribution | circulation form of carrier gas was demonstrated based on FIG. 13, when the inside of a filling container was divided into three or more spaces as shown in FIGS. 14-16, it was provided in each partition (1). By the communication channel (6), the carrier gas flows through each space as a downward flow from the upper side to the lower side.

  For example, the same effect is achieved even in a structure in which the partition wall (1) also serves as the communication channel (6) as shown in FIGS. As these structures, for example, as shown in FIG. 21, the tubular structures are arranged in the longitudinal direction of the container, and the gaps are closed so that the tubular structures are in contact with each other, or as shown in FIG. In the structure, the gap between the tubular structures is closed by the partition wall (1), and an opening is provided in the lower part of the space-side tubular structure on the upstream side with respect to the carrier gas flow direction, and this is used as the lower opening (4). An opening is provided in the upper part of the tubular structure on the downstream space side, and this is used as the upper opening (5). Also, as shown in FIG. 23 or FIG. An opening is provided in the lower part of the partition wall (1) on the upstream side with respect to the lower opening part (4), and an opening is provided in the lower part of the partition wall (1) on the downstream side. It is good also as an opening part (5). The connecting channel (6) may be a combination of those having a tubular structure or a structure in which the partition wall (1) also serves as the connecting passage (6).

  Further, in the filling container of the present invention, the discharge channel (8) having the lower opening (7) for discharging the carrier gas to the carrier gas discharge port (3) from the lower part of the space having the carrier gas discharge port (3). For example, the lower opening (7) is formed in the lower part of the structure having a tubular structure having an opening in the lower part as shown in FIG. 25 or the structure partitioned by the partition wall (1) as shown in FIG. It can be used. The discharge channel (8) may be a combination of those having a tubular structure or those having a lower opening (7) at the lower part of the structure partitioned by the partition wall (1).

  Furthermore, in the filling container for solid organometallic compounds of the present invention, the communication channel (6) having the lower opening (4) and the upper opening (5) for flowing each carrier gas, and the carrier gas discharge port (3) ) In a discharge flow path (8) having a lower opening (7) for discharging the carrier gas to the carrier gas discharge port (3) from the lower part of the space having the upper opening (5) and the lower opening ( 4) is a discharge flow path (7) having a space filled with a solid organometallic compound, a communication flow path (6), and a lower opening (7) through which the carrier gas is discharged to the carrier gas discharge port (3). 8) The carrier gas sufficiently flows from the carrier gas inlet (2) to the carrier gas outlet (3) through 8), and the filled solid organometallic compound is sufficiently in contact with the carrier gas. Is not particularly limited as long as it does not hinder the effective supply, but in particular, the lower opening for flowing the carrier gas in order to effectively bring the filled solid organometallic compound and the carrier gas into saturation contact. In the communication channel (6) having the part (4) and the upper opening (5), the lower opening (4) is 1/3 or less, preferably 1/5 or less of the height inside the container from the inner bottom surface of the filling container. More preferably, it is installed at a position of 1/10 or less, and the upper opening (5) is 2/3 or more, preferably 4/5 or more, more preferably 9/10 of the inner height of the container from the inner bottom surface of the filling container. The lower portion of the discharge channel (8) having the lower opening (7) that is installed at the above position and discharges the carrier gas to the carrier gas discharge port (3) from the lower portion of the space having the carrier gas discharge port (3). Opening (7) is filled Vessels 1/3 from the interior bottom surface of the container interior height less, preferably 1/5 or less, still more preferably installed in the position of 1/10 or less.

  When the solid organometallic compound is filled in the filling container of the present invention and used for supplying the organometallic compound to the MOCVD apparatus, the space inside the filling container is filled with the solid organometallic compound.

  Furthermore, in the filling container for solid organometallic compounds of the present invention, a filling port (9) for filling the solid organometallic compound in the space inside the filling container formed by partitioning with the partition wall (1) may be provided. it can. By providing this filling port (9), the solid organometallic compound can be charged as it is. In this invention, the filling port of a filling container can be provided in the upper part of a filling container, for example like FIGS. Further, the carrier gas introduction port (2) and / or the carrier gas discharge port (3) can be separated from the filling container, so that the carrier gas introduction port (2) and / or the carrier gas discharge port (3) can be separated. And a filling port (9). The separated carrier gas introduction port (2) and / or carrier gas discharge port (3) and the filling container are used together again through the connecting part (26). At that time, the flow path (8) connected to the carrier gas discharge port (3) can also be removed to facilitate filling of the solid organometallic compound. As an example of this structure, for example, as shown in FIG. 28, a connecting part (26) that can be separated as a filling port is provided between the carrier gas introduction port (2) and the filling container, and the connection parts are joined together again through this. What is used.

  In the filling container of the present invention, for example, as shown in FIGS. 13 to 16, the carrier gas inlet (2) and the carrier gas outlet (3) can be provided with a valve (22) that can be opened and closed, When the carrier gas is circulated, the valve (22) is opened, and when the organometallic compound is not supplied, the solid organometallic compound is usually contaminated from the outside with the valve closed, or sublimated outside the filling container. To prevent transpiration.

  Thus, the filling container used for the filling method of the present invention is divided into a plurality of spaces by the partition wall (1) inside the filling container, and the carrier gas introduced from the carrier gas inlet (2) is in each container space. In all the spaces in the filled solid organometallic compound, the structure passes from the upper part of the space to the lower part of the space and flows to the carrier gas discharge port (3). As described above, since the inside of the container is partitioned by the partition wall (1) and divided into a plurality of spaces, the cross-sectional area of each space is reduced and the contact between the carrier gas and the solid organometallic compound is sufficiently performed. The contact state between the carrier gas and the solid organometallic compound can be kept uniform without the formation of a flow path, and the solid organometallic compound can be stably transferred from the filling container to the MOCVD apparatus at a constant concentration for a long time by the carrier gas. It becomes possible to supply, and by filling the container with a solid organometallic compound having a controlled particle size, the effect of controlling the particle size can be further effectively extracted.

  When the solid organometallic compound is filled into the filling vessel by the method for filling the solid organometallic compound into the filling vessel for the solid organometallic compound of the present invention and used for supplying the organometallic compound to the MOCVD apparatus, the inside of the filling vessel The space is filled with a solid organometallic compound.

  In the method for filling a solid organometallic compound into a filling vessel for a solid organometallic compound according to the present invention, as a method for filling a solid organometallic compound into a space inside the filling vessel, a known method is used as it is. For example, a method of introducing and filling a solid organometallic compound into a filling container by sublimation, or a method of introducing and filling an organometallic compound into a filling container as a saturated vapor in a carrier gas, for example. In addition, for example, a method in which an organometallic compound is heated to a melting point or higher to be liquefied and introduced into a filled container can be used, but these methods are difficult to control the particle size of the solid organometallic compound. There are many cases.

  Usually, the filling of the solid organometallic compound with a controlled particle size of the present invention into the filling vessel for the solid organometallic compound does not require the special operation as described above, and the solid organometallic compound is not contained in the space inside the filling vessel. By using a filling container provided with a filling port for filling the solid organic metal compound whose particle size is controlled outside the filling container can be charged as a solid.

  For example, when the solid organometallic compound is a substance that ignites in air, the filling operation from the filling port of the solid organometallic compound is performed on, for example, a solid organometallic compound such as nitrogen, argon, or helium. In an inert gas atmosphere.

  Regarding the solid organometallic compound that can be used by filling the filling container of the present invention, not only the solid organometallic compound used in the filling container known so far, but also other solid organometallic compounds may be used. It is possible to apply a carrier gas having a saturated vapor pressure sufficient for a desired supply and a solid under supply conditions at a use temperature and pressure using the carrier gas. Representative examples of these solid organometallic compounds include alkyl metal compounds, metallocene compounds, β-diketone complexes, and adduct compounds. Specifically, for example, trimethylindium, dimethylchloroindium, triphenylaluminum, triphenylbismuth, alkyl metal compounds such as tert-butyllithium, metallocene compounds such as cyclopentadienylindium, biscyclopentadienylmagnesium, biscyclopentadienylmanganese, ferrocene, barium acetylacetonate complex, strontium acetylacetonate complex, copper acetyl Acetonate complex, calcium acetylacetonate complex, barium dipivaloylmethanate complex, strontium dipivaloylmethanate complex, copper dipivaloylmethanate complex, Β-diketone complexes such as thorium dipivaloylmethanate complex, calcium dipivaloylmethanate complex, trimethylindium trimethylarsine adduct, trimethylindium trimethylphosphine adduct, barium dipivaloylmethanate 1,10 -Adduct compounds, such as a phenanthroline adduct, etc. are mentioned.

  Further, the pressure when using a filling container filled with a solid organometallic compound in the filling method of the present invention can be used without changing the conditions used in the filling containers known so far. There is no particular limitation as long as the solid organometallic compound is stably supplied to the MOCVD apparatus for a period of time, and any of pressurization, normal pressure, and reduced pressure can be used. use.

  Furthermore, the temperature at the time of using the filling container filled with the solid organometallic compound in the filling method of the present invention can be applied without changing the conditions used in the filling containers known so far, A condition in which a normally used solid organometallic compound has a saturated vapor pressure sufficient for a desired supply to the carrier gas and is solid under the supply conditions is applicable.

  In the filling container filled with the solid organometallic compound by the filling method of the present invention, all the carrier gas used in the known filling containers can be used, for example, nitrogen, argon, helium, etc. An inert gas or hydrogen gas is used.

  In addition, in the filling container filled with the solid organometallic compound by the filling method of the present invention, it is possible to use a known filler that is used by being filled together with the solid organometallic compound in the known filling container. it can. As the filler, for example, stainless steel, glass, ceramics, fluororesin or the like is used, and stainless steel can be preferably used. In addition, as the shape of the filler, various shapes such as a round shape, a square shape, a cylindrical shape, a coil shape, a spring shape, and a spherical shape can be used. For example, various packings for distillation such as Dixon packing, Helipak, Fenceke etc. can be used. A fibrous filler can also be used.

  In the present invention, the size of the filler may be a size that passes through the size of the opening of the filling port provided in the filling container, and is usually 0.8 to 8 mm, preferably 0.8 to 6 mm, more preferably 0.8-5 mm can be used.

  These fillers can be used in the filling container of the present invention together with the solid organometallic compound after filling the filling container by a known method.

  The filling method of the present invention can be used not only for solid organic metal compounds, but also for filling other general solid substances such as solid inorganic compounds, solid organic compounds, or solid metals having vapor pressure. Thus, the filling method of the present invention can also be used as a filling method for taking out another solid substance as a gas saturated with a carrier gas using a carrier gas instead of the solid organometallic compound.

  Hereinafter, the present invention will be described in detail by way of examples.

  Trimethylindium was used as the solid organometallic compound.

  Trimethylindium was pulverized in a nitrogen atmosphere, and a sieve having a 4.75 mm mesh was used to obtain particles having a particle size of trimethylindium of 4.75 mm or less. Further, from the particles of trimethylindium having a particle diameter of 4.75 mm or less that passed through this sieve, the particles having a particle diameter of 1 mm or less were cut using a sieve having a 1 mm mesh, and particles having a particle diameter of 4.75 mm or less were cut. Trimethylindium having a diameter was prepared.

  When the particle diameter of the trimethylindium particles was confirmed, 50% or more of them were 2.5 to 4.75 mm in size.

  The supply stability was tested using trimethylindium containing particles having a particle size of 2.5 to 4.75 mm obtained in this manner.

  The supply stability test was conducted by the following method.

  In a nitrogen atmosphere, as shown in FIG. 28, in a SUS filled container having an outer diameter of 60.5 mmφ, 200 g of trimethylindium whose particle size was controlled by the above-described method and 0.9 mm × 1.8 mm × 1.8 mm stainless steel The filler 263g and the stainless steel filler 97g of 2.5 mm x 5.0 mm x 5.0 mm were filled from the filling port (9). In this filling operation, it was cut off at the connecting part (26) and filled as a filling port (9).

  Next, the carrier gas outlet (3) was connected to a trap cooled with dry ice-methanol for collecting trimethylindium. The pipe connecting the carrier gas discharge port (3) and the trap cooled with dry ice-methanol was heated so that trimethylindium did not precipitate in the pipe. A filling container containing trimethylindium and a filler is attached to a thermostatic bath at 25 ° C., and nitrogen is supplied from the carrier gas inlet (2) of the filling container under the condition that the pressure in the apparatus system of the supply stability test is close to atmospheric pressure. The gas was flowed at 500 cc per minute, and the weight of trimethylindium collected in a trap cooled with dry ice-methanol every 8 hours was measured. In addition, the gas phase gas concentration of the carrier gas containing trimethylindium vapor was measured with an ultrasonic gas concentration meter (trade name Epison: manufactured by Thomas Swan).

  The result is shown in FIG. The vertical axis of the graph shown in FIG. 29 shows the supply amount of trimethylindium per hour, and the horizontal axis shows the use ratio of the supplied trimethylindium in weight%.

  As a result of the supply stability test, when the filling method of the present invention was used, the supply rate of trimethylindium was stable up to 91% by weight of the usage ratio.

  Thus, by using the solid organometallic compound having a particle size of 2.5 to 4.75 mm, the solid organometallic compound can be stably supplied at a constant concentration. In addition, it is possible to increase the proportion of the solid organometallic compound used under conditions where a stable supply rate is obtained. As a result, the period during which the solid organometallic compound is stably supplied can be improved.

Comparative Example 1

  In Example 1, trimethylindium was pulverized in a nitrogen atmosphere, a sieve having a mesh size of 2.36 mm was used, and trimethylindium was changed to a particle having a particle size of 2.36 mm or less. The operation was performed to test the supply stability of the solid organometallic compound. The result is shown in FIG. The vertical axis of the graph shown in FIG. 30 shows the supply amount of trimethylindium per hour, and the horizontal axis shows the usage ratio of the supplied trimethylindium in weight%. As a result of the supply stability test, the supply rate of trimethylindium containing no particles having a particle size of 2.5 to 6 mm was stable up to 77% by weight of the use ratio.

  In this way, when filled with trimethylindium that does not contain particles of trimethylindium having a particle size of 2.5 to 6 mm, the supply rate can be stably obtained for a long period of time as in Example 1. There wasn't.

  In Example 1, the filling container is a SUS filling container having an outer diameter of 76 mm as shown in FIG. 28, and 400 g of trimethylindium with a controlled particle diameter and 394 g of a 0.9 mm × 1.8 mm × 1.8 mm stainless steel filling material. The same operation as in Example 1 was conducted except that 78 g of stainless steel filler of 2.5 mm × 5.0 mm × 5.0 mm was used, and the supply stability of the solid organometallic compound was tested. The result is shown in FIG. The vertical axis of the graph shown in FIG. 31 shows the supply amount of trimethylindium per hour, and the horizontal axis shows the usage ratio of the supplied trimethylindium in weight%. As a result of the supply stability test, the supply rate of trimethylindium containing particles having a particle size of 2.5 to 6 mm was stable up to 85% by weight of the use ratio.

  In Example 1, a filled container made of glass having an outer diameter of 35 mmφ having a structure in which the diffuser (20a) was removed from a container having a structure as shown in FIG. 34, and 100 g of trimethylindium having a controlled particle diameter was used. Except for the above, the same operation as in Example 1 was performed to test the supply stability of the solid organometallic compound. As a result of the supply stability test, the supply rate of trimethylindium containing particles having a particle size of 2.8 to 4.75 mm was stable up to 76% by weight of the use ratio.

Comparative Example 2

  In Example 2, trimethylindium was pulverized in a nitrogen atmosphere, and a sieve having a mesh size of 2.36 mm was used, and trimethylindium was made particles having a particle size of 2.36 mm or less. The operation was performed to test the supply stability of the solid organometallic compound. The result is shown in FIG. The vertical axis of the graph shown in FIG. 32 shows the supply amount of trimethylindium per hour, and the horizontal axis shows the usage ratio of the supplied trimethylindium in weight%. As a result of the supply stability test, the supply rate of trimethylindium containing no particles having a particle size of 2.5 to 6 mm was stable up to 59% by weight of the use ratio.

  In this way, when filled with trimethylindium that does not contain particles of 2.5 to 6 mm in particle size, the supply rate can be stably obtained for a long period of time as in Example 2. There wasn't.

Comparative Example 3

  In Example 3, trimethylindium was pulverized under a nitrogen atmosphere, and the same operation as in Example 3 was performed except that trimethylindium was made into particles having a particle size of 0.1 to 0.3 mm. Supply stability was tested. As a result of the supply stability test, the supply rate of trimethylindium having a particle diameter of 0.1 to 0.3 mm was stable up to 20% by weight of the use ratio.

  As described above, when trimethylindium having a particle diameter of 0.1 to 0.3 mm was filled and used, the supply rate could not be stably obtained for a long period of time as in Example 3.

  According to the present invention, when the solid organometallic compound is filled into the filling container for the solid organometallic compound, the initial stability is ensured by including particles of a certain size as the essential particle size of the solid organometallic compound. In addition, the solid organometallic compound can be stably supplied to a vapor phase epitaxial growth apparatus such as an MOCVD apparatus for a long period of time.

It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) is a top view, (C) shows a perspective view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) shows a top view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) shows a top view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) shows a top view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) is a top view, (C) shows a perspective view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) is a top view, (C) shows a perspective view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) is a top view, (C) shows a perspective view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) is a top view, (C) shows a perspective view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) shows a top view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) shows a top view. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is sectional drawing, (B) shows a top view. It is a perspective view which shows one Embodiment of the filling container of this invention. It is a perspective view which shows one Embodiment of the filling container of this invention. It is a perspective view which shows one Embodiment of the filling container of this invention. It is a perspective view which shows one Embodiment of the filling container of this invention. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows one Embodiment of the filling container of this invention, (A) is a perspective view, (B) shows sectional drawing. It is a schematic diagram which shows the filling container used in the present Example 1, (A) is sectional drawing, (B) is a top view, (C) shows a perspective view. The figure which shows the result (The relationship between the usage-ratio of the supplied trimethylindium, and the supply amount of the trimethylindium per hour) of the supply stability test of the trimethylindium in the present Example 1. FIG. The figure which shows the result (the relationship between the usage-amount of the supplied trimethylindium and the supply amount of the trimethylindium per hour) of the supply stability test of the trimethylindium in the comparative example 1. The figure which shows the result (The relationship between the usage-amount of the supplied trimethylindium and the supply amount of the trimethylindium per hour) of the supply stability test of the trimethylindium in the present Example 2. FIG. The figure which shows the result (the relationship between the usage-ratio of the supplied trimethylindium, and the supply amount of the trimethylindium per hour) of the supply stability test of the trimethylindium in the comparative example 2. The schematic cross section which shows the conventional filling container A. FIG. The schematic cross section which shows the conventional filling container B. FIG. The schematic cross section which shows the conventional filling container C. FIG. The schematic cross section which shows the conventional filling container D. FIG.

Explanation of symbols

2: Carrier gas introduction port 3: Carrier gas discharge port 9: Filling port 22: Valve 26: Connection part 2a: Carrier gas introduction port 3a: Carrier gas discharge port 7a: Lower opening 8a: Channel 9a: Filling port 20a: Diffuser 21a: Solid organometallic compound arrangement chamber 22a: Valve 23a: Column type container 24a: Filter 25a: Inlet chamber 27a: Porous member

Claims (14)

In a method of filling a trimethylindium filling container for supplying trimethylindium to a vapor phase epitaxial growth apparatus, particles made of only trimethylindium are particles having a particle size of 8 mm or less, and particles having a particle size of 2.5 to 6 mm A method for filling trimethylindium into a filling vessel for trimethylindium for supplying to an apparatus for vapor phase epitaxial growth characterized in that trimethylindium is contained as an essential component in trimethylindium.   The method for filling trimethylindium according to claim 1, further comprising causing a filler to coexist with the trimethylindium.   The filling method of trimethylindium according to claim 2, wherein the size of the filler is 0.8 to 8 mm.   The trimethylindium filling container has a carrier gas introduction port and a carrier gas discharge port, and the inside of the filling container is divided into a plurality of vertical spaces and introduced from the carrier gas introduction port. 4. The trimethylindium filling container according to claim 1, wherein the container is configured to flow through each vertical space and to be discharged from a carrier gas discharge port. 5. Filling method of trimethylindium. In the filled container for trimethylindium,
(a) The inside of the filling container is vertically divided by at least one partition wall, and the inside of the filling container is divided into at least two spaces.
(b) The space inside the filling container formed by partitioning with a partition wall has a space having a carrier gas inlet and a space having a carrier gas outlet.
(c) A trimethylindium filled container having a partition wall having an opening for flowing the carrier gas from the carrier gas inlet to the carrier gas outlet through each space in the filled container in the partition wall inside the filled container. The method for filling trimethylindium according to claim 4.   In the opening, when the opening is arranged at the lower part of the partition wall, it is 1/3 or less of the container inner height from the inner bottom surface of the filling container, and when the opening is arranged at the upper part of the partition wall, the inner bottom surface of the filling container 6. The method for filling trimethylindium according to claim 5, wherein the openings are respectively installed at positions of 2/3 or more of the inner height of the container.   6. The method for filling trimethylindium according to claim 4 or 5, further comprising a filling port for filling trimethylindium into a space inside the filling container formed by partitioning with a partition wall.   The trimethylindium filling container is a trimethylindium filling container having a carrier gas introduction port and a carrier gas discharge port, and the inside of the filling container is divided into a plurality of vertical spaces. 4. A filling container for trimethylindium having a structure in which a carrier gas introduced from an introduction port flows through each vertical space as a downward flow and is discharged from the carrier gas discharge port. The method of filling trimethylindium according to claim 1. In the filled container for trimethylindium,
(d) The inside of the filling container is vertically divided by at least one partition wall, and the inside of the filling container is divided into at least two spaces.
(e) The space inside the filling container formed by partitioning with a partition wall has a space having a carrier gas inlet and a space having a carrier gas outlet.
(f) In the partition wall inside the filling container, a communication channel having a lower opening and an upper opening for allowing the carrier gas to flow from the carrier gas inlet to the carrier gas outlet through each space in the filling container is provided. Having a partition
(g) In the communication channel, the carrier gas introduced into the filling container is introduced from the lower opening of the communication channel and discharged to the upper opening.
(h) A trimethylindium filling container comprising a discharge channel having a lower opening through which a carrier gas is discharged from a lower portion of a space having a carrier gas discharge port to a carrier gas discharge port. The filling method of trimethylindium as described.   In the communication channel, the lower opening of the communication channel is 1/3 or less of the inner height of the container from the inner bottom surface of the filling container, and the upper opening of the communication channel is 2 The lower opening of the discharge channel is installed at a position of 1/3 or less of the inner height of the container from the inner bottom surface of the filling container. The method for filling trimethylindium according to claim 8.   The filling method for trimethylindium according to claim 8 or 10, further comprising a filling port for filling trimethylindium into a space inside the filling container formed by partitioning with a partition wall.   The method for filling trimethylindium according to claim 8 or 9, further comprising a filling port for filling trimethylindium into a space inside the filling container formed by partitioning with a partition wall.   A filling container for trimethylindium filled with trimethylindium by the filling method according to any one of claims 1 to 3. The filled container for trimethylindium according to claim 13, wherein the filled container for trimethylindium is a filled container for trimethylindium having the structure according to claims 4 to 12.

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