JP2006297251A - Film forming apparatus and film forming method using the film forming apparatus - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a film forming apparatus for adjusting an amount of fine particles sprayed from a nozzle to obtain a stable and highly uniform film formed. <P>SOLUTION: The film forming apparatus comprises: an aerosol forming means for forming an aerosol containing particles of a film forming material; and a nozzle for spraying the aerosol formed by the aerosol forming means, wherein the aerosol forming means includes a detection means for detecting the amount of particles of a film forming material, and a means for controlling the amount of particles of a film forming material contained in the aerosol formed based on a detection result of the detection means. <P>COPYRIGHT: (C)2007,JPO&INPIT

Description

  The present invention is a film forming method in which a film containing ceramics or metal is formed on a substrate by spraying an aerosol containing particles of a film forming material such as ceramics or metal at high speed from a nozzle toward the substrate which is a member to be processed. The present invention relates to an apparatus and a film forming method.

  In an apparatus and manufacturing method for forming a structure or film made of ceramics or metal, an aerosol containing particles of a film forming material such as ceramics or metal is sprayed from a nozzle toward the substrate, and the film containing ceramics or metal is formed on the substrate. A method and apparatus have been proposed which are performed by depositing on top. In such a film forming apparatus, it is a big problem to perform film formation by stabilizing the supply amount of aerosol containing particles of a material to be formed over time. An example of the ceramic is piezoelectric ceramic. Examples of the piezoelectric ceramic include lead zirconate titanate (hereinafter abbreviated as “PZT”) and sodium bismuth titanate (hereinafter abbreviated as “BNT”).

  To address this problem, as disclosed in Patent Document 1, the amount of film forming material particles in the aerosol is sensed by a sensor, and the height of the ceramic structure is adjusted using the sensed sensor signal. There is. In the case of this method, the amount of fine particles ejected from the nozzle is measured, and the measurement data is fed back to the aerosol generation source to adjust the aerosol generation amount.

  FIG. 1 shows the outline of a ceramic structure manufacturing apparatus according to the above method. Conventionally, a carrier gas is introduced into the aerosol forming unit 29 filled with powder from the gas cylinder 11 in some form, and the aerosolized fine particles are conveyed to the film forming chamber through the carrier tube 4 and injected from the nozzle 5. Thus, a ceramic structure is produced. At this time, the classifier 31 may be incorporated into the conveyance path via the disperser 30 in order to make the particle diameters of the conveyance fine particles uniform.

Further, in Patent Document 1, the amount of fine particles in the aerosol is sensed by a sensor 32 in order to stabilize the amount of aerosol generated, and the drive unit of the aerosol generation unit 29 or the carrier gas supply cylinder is fed through the feedback control circuit 9 and the wiring 10. The correction data is transmitted to 11, and the aerosol supply amount is adjusted using the correction data. At this time, the aerosol supply amount adjusting means includes gas flow rate adjustment, gas flow rate adjustment, gas temperature adjustment, or aerosolization unit drive adjustment.
JP 2001-348659 A

  However, even if the amount of fine particles in the aerosol is evaluated after being ejected from the nozzle, and the aerosol generation amount is controlled in the aerosol generation source after that, it is not reflected in the amount of fine particles in the aerosol that is already being conveyed, The amount of fine particles cannot be adjusted. That is, the reaction speed of the adjusting mechanism is slow, and as a result, the injection amount of the fine particles cannot be controlled with high accuracy. Moreover, even if it is going to form into a film using a particle | grain (primary particle) with a small particle size, such a primary particle tends to raise | generate aggregation. Therefore, when film formation is performed using an aerosol in which particles (secondary particles) formed by agglomerating multiple primary particles are mixed, even if the supply amount of particles can be controlled, it is stable and uniform. High film formation was difficult. Furthermore, when the dispersibility of the particles in the aerosol is lowered, it is difficult to form a film with high uniformity because the thickness of the formed film is uneven. The present invention has been made in view of these problems, and aims to control the supply rate of fine particles with high accuracy. Furthermore, by performing classification and dispersion of fine particles, a highly uniform and stable composition is achieved. It is also aimed to realize a membrane.

  In order to solve the above problems, a first invention includes an aerosol forming unit that forms an aerosol containing particles of a film forming material, and a nozzle that jets the aerosol formed by the aerosol forming unit. In the membrane apparatus, the aerosol forming means includes a supply means for supplying particles of the film forming material, a detecting means for detecting the amount of particles of the film forming material, and an aerosol to be formed based on a detection result of the detecting means. Control means for controlling the amount of particles of the film-forming material contained therein, the supply means comprises a container for containing particles of the film-forming material, and the detection means The film forming apparatus is characterized in that the amount of film forming material particles contained in the aerosol to be formed is detected by measuring the weight of the container in a state in which the particles are contained.

  Further, the film forming apparatus of the first aspect of the invention is “the control means is means for controlling the amount of particles of the film forming material supplied from the supply means”, “the container is the film forming material. A filter having a plurality of openings through which the particles pass through, “the container further includes a brush that contacts and moves the filter,” “the aerosol forming means further includes the particles. Among them, a crushing means for crushing particles formed by agglomeration of a large number of particles into a plurality of particles ”,“ the crushing means includes a first transport pipe through which the formed aerosol flows. , Including a second carrier tube in which the tip of the first carrier tube is inserted and gas is allowed to flow along with the aerosol discharged from the tip, “the flow velocity of the aerosol emitted from the tip Alongside the aerosol As the flow rate of the gas is different to, also the gas and is flowed "it and the aerosol is to its features.

  In order to solve the above problems, a second invention comprises an aerosol forming means for forming an aerosol containing particles of a film forming material, and a nozzle for injecting the aerosol formed by the aerosol forming means. In the membrane device, the aerosol forming means includes a first carrier tube and a second carrier tube in which a tip of the first carrier tube is inserted and gas flows along with the aerosol discharged from the tip. And a film forming apparatus characterized by comprising:

  And, the film forming apparatus of the second invention is “the aerosol and the gas are caused to flow so that the flow velocity of the aerosol released from the tip and the flow velocity of the gas flowing along with the aerosol are different”. This is also a feature.

  Further, a third aspect of the present invention is a film forming method for forming a film containing the film forming material by injecting the aerosol toward a substrate using the film forming apparatus.

  As described above, the particles of the film forming material are classified to a predetermined particle size or less, and the supply amount of the classified particles is fed back to the drive unit of the immediate supply device, thereby stably supplying the particles over time. Further, by crushing and / or dispersing the supplied particles, it is possible to stably obtain fine particles having an optimum diameter suitable for film formation, and thus the film formation stability can be improved.

  Embodiments of the present invention will be described below.

  A first example of the film forming apparatus of the present invention is shown in FIG. 2, and a second example is shown in a conceptual diagram in FIG. In addition, the film-forming apparatus of this invention is not restricted to the example shown by FIG. 2, FIG. 3, A various modified example is applicable.

  The film forming apparatus of the present invention includes an aerosol forming means 100 (shown surrounded by a dotted line in FIGS. 2 and 3) for generating (forming) an aerosol containing particles of a film forming material, and an aerosol forming means 100. And at least a nozzle 5 for injecting the generated (formed) aerosol. Then, the aerosol formed by the aerosol forming means 100 is guided to the nozzle 5 through the transport pipe 4. The nozzle 5 is introduced into a film forming chamber (chamber) 6. A substrate 7 that is a film forming member is disposed in the film forming chamber 6, and aerosol is jetted from the nozzle 5 toward the substrate 7. The substrate is typically a substrate. The substrate 7 is fixed on the stage 8. The stage 8 may be an XY stage movable in the X direction and the Y direction. If such an XY stage is used, a film having a desired pattern can be formed on the substrate 7.

  The aerosol forming unit 100 includes at least a supply unit 1 for supplying particles of the film forming material into the gas. The supply unit 1 supplies the particles of the film forming material supplied into the gas for forming the aerosol. The amount (supply amount) can be controlled to a desired amount.

  As the supply means 1, for example, a container containing particles of a film forming material within a desired particle size range is provided. The container can also be provided with means (for example, a feeder) capable of supplying a predetermined amount of particles. When such a supply means 1 is used, it is preferable that the aerosol forming means 100 supply particles from the supply means 1 in the gas flow (see FIG. 11, details will be described in Example 4). To do). Alternatively, the supply means 1 includes a container containing particles of a film forming material within a desired particle size range, and a means for injecting gas (blowing gas) into the container, and is accommodated in the container. It is also possible to use supply means for supplying particles by blowing gas onto the particles (preferably gas is injected from a lower part of the container through a filter having an opening), causing particles of the film forming material to rise in the container (FIG. 10). See details in Example 3).

  And the aerosol formation means 100 in this invention is provided with the detection means 2 which detects the quantity of the particle | grains of the film-forming material supplied from the supply means 1, before an aerosol is injected from the nozzle 5 preferably. By this detection means 2, the amount of particles of the film forming material supplied from the supply means 1 can be detected (measured).

  Based on the detection result (detection value) of the detection means 2, the control means (feedback control circuit) 9 supplies from the supply means 1 so that the amount of particles contained in the aerosol becomes a desired value. Control the amount of particles to the desired amount.

  It is most preferable to always detect the supply amount of particles by the detection means 2, but it can also be performed intermittently within an allowable range. Note that the example described in FIG. 3 is an example in which the amount of film forming material particles supplied from the supply unit 1 is measured for each container containing particles. In this example, the supply means 1 includes a container for storing particles, and detects the amount of particles discharged (supplied) from the container (the amount of particles supplied) by a change in the weight of the container storing the particles. Can be monitored. And it is an example which controls the supply amount of particle | grains by the control means 9 based on this detected value. In this example, a filter having a plurality of openings can be provided as a classifying means for classifying the particles in a container for containing the particles. In this way, the particle size of the film forming material supplied from the supply means 1 can be made uniform to some extent in advance. Furthermore, in order to send particles to the opening of the filter, a brush that contacts and moves the filter can be provided. Moreover, as such a movable brush, it is preferable to use, for example, a brush that rotates while being in contact with the filter. In this way, a desired amount of particles of the film forming material can be supplied from the supply means 1 stably and with high accuracy.

  In the film forming apparatus of the present invention, more preferably, the aerosol forming unit 100 disintegrates particles contained in the formed aerosol (or may be considered as particles supplied from the supplying unit 1). A crushing means (which may further have a function of improving the dispersibility of particles in the gas) 3 is provided.

  The particles supplied from the supply device 100 often include secondary particles formed by aggregation of a large number of particles. Therefore, a lump of particles (typically secondary particles) formed by aggregating a large number of particles by providing the crushing means 3 (or sometimes called “crushing / dispersing means 3”). And the number of primary particles can be increased. Furthermore, the dispersibility of the particles in the carrier gas can be improved.

  As a result, highly uniform film formation can be realized. Further, if particles that are not aggregated are supplied to the crushing means 3, they are not crushed, but the dispersibility of the particles in the carrier gas can be improved. In this sense, the “disintegration means 3” of the present invention can also be called “disintegration / dispersion means 3”. Even if the particles are agglomerated, even when they are not crushed by the crushing means 3, the dispersibility of the particles can be improved.

  In the film forming apparatus of the present invention, the aerosol passes through the transport pipe 4 and is sprayed from the tip of the nozzle 5 toward the base 7 fixed on the XY stage 8.

  The supply apparatus 100 can further include a classification unit for classifying supplied particles. As the classifying means, practically, any means can be used as long as it can classify to a particle size of 2000 μm or less, preferably 100 μm or less.

  The lower limit of the particle diameter is practically 0.5 μm or more. The supply means may be practically such that the particles can be supplied at a rate of 0.1 g / h or more, and preferably can be supplied at a rate of 500 g / h or less.

  For example, the classifying means includes a container (a “mesh member”) or a container having a desired mesh diameter (preferably 0.5 μm to 2000 μm) disposed at the bottom of the container for storing (storing) particles. And a member (for example, a brush) that can move relative to the mesh body (including rotation and vibration) while contacting the mesh body. be able to. Particles having a desired particle diameter can be extracted (classifying particles having a desired particle diameter) by sieving the particles through the mesh body by rotating the brush. As described above, such a classifying means can be provided in a container in which the particles of the film forming material constituting the supplying means 1 shown in FIG. 3 are accommodated.

  As the classifying means, the aerosol transport path (transport pipe 4) is configured in a non-linear manner, and an opening serving as a particle outlet is provided in a part of the transport path, whereby the mass depending on the particle size of the particles. By using the difference, it is possible to use one that removes particles having a predetermined particle size or more. Alternatively, by charging the particles and generating an electric field or magnetic field on the transport path, the particles larger than a predetermined particle size are removed using the difference in deflection force due to the electric and magnetic fields applied to the charged particles. Can also be used. Thus, a classification means is not specifically limited, A well-known classification means can be applied.

  The supply unit 1 and the classification unit are not particularly limited as long as the supply amount of particles and the particle size of particles can be controlled to a desired value (desired range).

  In the film forming apparatus of the present invention, the pressure in the chamber 6 is maintained in a reduced pressure state by an exhaust device (vacuum pump) 12 or the like. That is, the pressure in the chamber 6 is set lower than the pressure on the supply device 1 side (the pressure on the supply device 100 side is set higher than the pressure on the chamber 6 side of the transport pipe 4). The particles supplied from the apparatus 100 are ejected from the nozzle 5 toward the surface of the substrate 7 fixed on the stage 8. As a result, particles contained in the aerosol collide with the surface of the substrate 7 and deposit, whereby a film is formed on the surface of the substrate 7.

  In the first example of the film forming apparatus of the present invention shown in FIG. 2, a cylinder 11 for supplying carrier gas is connected to the supply means 1.

  In this example, the supply apparatus 100 includes a supply amount detection unit 2 that detects the amount of particles contained in the aerosol supplied from the supply unit 1 to the carrier tube 4. Then, based on the value detected by the detection unit 2, the amount of particles supplied from the supply unit 1 can be appropriately controlled to a desired amount.

  On the other hand, in the second example of the film forming apparatus of the present invention shown in FIG. 3, an electronic balance 13 is used as the supply amount detection means 2 and supplied for each particle supply means 1 (every container containing particles). This is an example of measuring the weight of particles. This example is preferable because the weight of the supplied particles can be calculated and the amount of particles supplied from the supply means 1 can be controlled based on the calculated data. By using such an apparatus, the amount of particles to be supplied can be controlled with high accuracy.

  In the present invention, the weight measurement method is not limited as long as the mechanism can measure the supply amount of particles and control the amount of particles supplied from the supply device based on the measured data. For example, an apparatus that optically measures the supply amount of particles can be preferably employed as the supply amount detection means. However, in order to measure with higher accuracy, it is preferable to employ the supply amount detection means 2 having the configuration shown in FIG.

  The supply unit 1 supplies the particles 15 to the crushing unit 3 (crushing / dispersing unit 3). In the form shown in FIG. 3, the space between the supply unit 1 and the crushing unit 3 may be open to the atmosphere, but may be covered with a structure. When covered with a structure, the inside may be maintained in a reduced pressure state. For example, in the form shown in FIG. 2, since the supply means 1 and the crushing means 3 are connected by the conveyance pipe, the space between the supply means 1 and the crushing means 3 is covered with the conveyance pipe. This can also be said (the supply means 1 and the crushing means 3 are connected by a transport pipe). Then, the particles that have passed through the crushing means 3 are guided to the nozzle 5 through the transport pipe 4 and are jetted together with the transport gas from the tip of the nozzle 5 toward the base body 7.

  As the crushing means 3 (crushing / dispersing means 3) in the present invention, specifically, for example, a structure as shown in FIG. 4 or FIG. 5 can be adopted.

  In the example shown in FIG. 4, the first transport pipe 4-1 to which the particles 24 are supplied from the supply device 100 and the second transport pipe 4 into which the tip of the first transport pipe 4-1 is inserted. -2. In addition, it is preferable that the first transport pipe and the second transport pipe are preferably disposed so that the center of the first transport pipe substantially coincides with the center of the second transport pipe.

  The second transport pipe 4-2 is provided with a second introduction port 19 for introducing the second gas, and the first transport pipe 4-1 is provided with a first gas for introducing the first gas. May be provided. The first introduction port 18 is connected to a control valve 21 for controlling the flow rate of the first gas introduced into the first transfer pipe 4-1. Similarly, a control valve 22 for controlling the flow rate of the second gas introduced into the second transport pipe 4-2 is connected to the second introduction port 19. In addition, when the aerosol state is formed before the particle | grains 24 are guide | induced to the 1st conveyance pipe 4-1, the 1st inlet 18 and the control valve 21 for introducing 1st gas are not necessarily required. do not need.

  By doing so, the direction in which the first gas (aerosol) flows and the direction in which the second gas flows can be made substantially the same. More specifically, although depending on the flow velocity, the central axis of the first transport pipe 4-1 is substantially the same as the central axis of the second transport pipe from the tip to a predetermined distance. By doing so, the direction in which the first gas (aerosol) flows and the direction in which the second gas flows can be made substantially the same. In other words, the flow of the first gas (aerosol) discharged from the tip of the first transfer pipe 4-1 into the second transfer pipe 4-2 is aligned with the flow of the second gas (so as to follow). To). In particular, by preventing the tip of the first transfer tube 4-1 from coming into contact with the inner wall of the second transfer tube 4-2, the second transfer can be performed from the tip of the first transfer tube 4-1. The flow of the first gas (aerosol) released into the tube 4-2 can be surrounded by the flow of the second gas.

  In the structure of FIG. 5, in addition to the structure of FIG. 4, it is an example provided with the 3rd conveyance pipe 4-3 in which the front-end | tip of the 2nd conveyance pipe 4-2 is inserted. The third transfer pipe 4-3 is provided with a third introduction port 20 for introducing a third gas, and the third introduction port 20 has a third transfer of the third gas. A control valve 23 is connected to control the flow rate introduced into the pipe 4-3.

  In the present invention, the diameter of the tip of the first transport pipe 4-1 is set to be smaller than the inner diameter of the second transport pipe 4-2. And the front-end | tip of the 1st conveyance pipe 4-1 is inserted in the 2nd conveyance pipe 4-2. And preferably, it arrange | positions so that the front-end | tip of the 1st conveyance pipe 4-1 may not contact the inner wall of a 2nd conveyance pipe.

  Further, in the form shown in FIG. 5, in addition to the form shown in FIG. 4, the diameter of the tip of the second transport pipe 4-2 is smaller than the inner diameter of 4-3 of the third transport pipe. It is set and the tip of the 2nd conveyance pipe 4-2 is inserted in the 3rd conveyance pipe 4-3. Preferably, the tip of the second transport pipe 4-2 is disposed so as not to contact the inner wall of the third transport pipe 4-3.

  In this way, in addition to the gas flow described for the configuration of FIG. 4, the flow direction of the second gas (the mixed gas of the second gas and the first gas) and the flow of the third gas The direction can be almost the same.

  In FIG. 5, the position of the tip of the second transport pipe 4-2 and the position of the tip of the first transport pipe 4-1 are substantially the same position in the third transport pipe 4-3. The case where it is inserted is shown.

  However, in the present invention, for example, the front end of the first transport pipe 4-1 can be arranged at a position farther from the nozzle 5 than the front end of the second transport pipe 4-2. That is, after the first gas and the second gas are sufficiently mixed, a mixed gas (including particles) of the first gas and the second gas is introduced from the tip of the second transfer tube 4-2. In addition, it is possible to adopt a configuration in which the gas is introduced into the third gas flow. If it is such a form, the effect of disperse | distributing the particle | grains in gas and the effect of pulverizing the aggregated particle | grain can be improved further.

  4 and FIG. 5, the case where the 1st-3rd conveyance pipe was used as the crushing / dispersing means 3 was shown. However, in the present invention, it is also possible to increase the number of transport pipes (the number of gas inlets) in order to further improve the above-described effects, or in accordance with the particle size distribution and the degree of dispersion of the particles to be finally obtained. It is.

  Next, the operation of the crushing means 3 (crushing / dispersing means 3) will be described below with reference to the structure of FIG.

  First, the particles 24 supplied from the supply device 100 are introduced into a first gas that flows at a first velocity (substantially no problem replacing the “first flow velocity”), and the particles 24 have a first velocity. Set to Next, the first gas including the particles 24 is aligned with the second gas flowing at a second speed (second flow rate) different from the first speed (adjacent to the second gas). Washed away. In other words, the first gas including the particles 24 and having the first flow rate is brought into contact with the second gas having the second flow rate different from the first flow rate.

  In this way, the particles 24 existing near the boundary between the first gas flowing at the first velocity (first flow velocity) and the second gas flowing at the second velocity (second flow velocity) Force (for example, shearing force) acts. As a result, ideally, the particles 24 are crushed and into the gas of the particles 25 formed by pulverizing the particles 24 (in the mixed gas of the first gas and the second gas). Is distributed.

  In order to further obtain the effect of the force acting on the particles 24, in particular, as shown in FIGS. 4 and 5, the outer diameter of the tip of the first transport pipe 4-1 is the second transport pipe 4-2. It is preferable that the inner diameter of the first conveying pipe 4-1 is set so as not to contact the inner wall of the second conveying pipe 4-2. By doing in this way, the aerosol discharge | released from the front-end | tip of the 1st conveyance pipe 4-1 can be surrounded by the flow of 2nd gas, As a result, the above-mentioned force can be efficiently used for particle | grains 24. Can act on.

  As described above, in the present invention, it is only necessary to apply a force to the particles 24 so as to crush and / or disperse the particles 24 in the vicinity of the boundary between the first gas and the second gas. Therefore, the present invention does not exclude other than the form in which the first gas and the second gas flow through the transfer pipe in a completely laminar flow state, and the boundary between the first gas and the second gas is Including unclear states.

  Note that the first speed and the second speed are preferably substantially aligned in directions. However, as long as the flow velocity is not significantly reduced, the case where the directions of the respective gas flows intersect is allowed.

  In addition, the “first gas including the particles 24” obtained by introducing the particles 24 supplied from the supply device 100 into the first gas can be referred to as “first aerosol”.

  After passing through the crushing / dispersing means 3, the particles 25 are present in the mixed gas of the second gas and the first gas (in the example of FIG. It will be present in the mixed gas of the third gas). Therefore, the gas containing such particles 25 can also be referred to as a “second aerosol”.

  In the above description, for the sake of convenience, “first gas” and “second gas” are distinguished from each other. However, this expression allows different types of gas and different partial pressures of gas, but does not exclude that they are the same gas.

  In addition to the structure of the crushing means 3 shown in FIG. 4, FIG. 5 further includes a transport pipe 4-3 provided with a third gas introduction path 20 for creating a third gas flow. It is another example of a form of the present invention. In this embodiment, at least a part of the second transport pipe 4-2 is inserted into the third transport pipe 4-3. The inner diameter of the third transfer pipe 4-3 is set larger than the outer diameter of the second transfer pipe 4-2, and the tip of the second transfer pipe 4-2 is the third transfer pipe 4- 3 is set so as not to contact the inner wall. In this way, the second gas released from the tip of the transport pipe 4-2 is surrounded by the third gas.

  The crushing / dispersing means 3 shown in FIG. 5 allows the third gas to flow from the third gas introduction path 20. The third gas is allowed to have a flow rate different from the flow rate of the first gas and / or the flow rate of the second gas. If it is the form shown in FIG. 5, it suppresses that the particle | grains 25 disintegrated and disperse | distributed by the force produced by the difference of the flow velocity of 1st gas and the flow velocity of 2nd gas adhere to the inner wall of a conveyance pipe. And / or further dispersion of the particles 25 can be performed. The “third gas” allows the gas type and the partial pressure of the gas to be different from the “first gas” and the “second gas”, but is the same gas. It is not excluded.

  Thus, as the crushing / dispersing means 3 in the present invention, it is possible to employ a configuration in which a large number (two or more) of gases having different flow velocities are used depending on the target particle size and flow velocity.

  The supplied particles 24 by the crushing / dispersing means 3 of the present invention are preferably arranged in a practical range to particles 25 having a particle size of 0.1 μm or more and 500 μm or less. When particles having such a particle size range are used, a film having excellent film thickness uniformity can be formed on the substrate 7.

  In order to effectively apply a force for performing crushing or the like to the particles 24 and / or to improve the dispersibility of the particles 25, the second gas is surrounded by the flow of the first gas containing the particles 24. It is preferable to flow. Therefore, the crushing / dispersing means 3 shown in FIG. 4 has the tip of the first transport pipe 4-1 disposed near the center of the second transport pipe 4-2. And the situation where the flow of the second gas surrounds the flow of the first gas containing particles by introducing the particles 24 from the supply device 100 together with the first gas into the flow of the second gas. Can be made. For the same reason, in the embodiment shown in FIG. 5, the tip of the first transport pipe 4-1 is disposed near the center of the second transport pipe 4-2, The tip of the transport pipe is arranged near the center of the third transport pipe 4-3.

  It can be said that when the particles 24 are introduced into the first gas, the particles 24 are dispersed in the first gas, and an aerosol is formed. Then, the second gas introduced from the second introduction port 19 and the gas introduced from the introduction port 18 merge, and the particles 25 are dispersed in the merged gas to form an aerosol. The formed aerosol is guided to the nozzle 5 by the above-described differential pressure, and the particles 25 are ejected from the nozzle 5 together with the carrier gas (a mixed gas of the first gas and the second gas).

  As described above, according to the film forming apparatus of the present invention, it is possible to form an aerosol in which particles having a controlled particle size are highly uniform in the gas and the change in the degree of dispersion over time is small. As a result, the amount of particles ejected from the nozzle 5 varies little over time and the particle size distribution of the ejected particles is narrow, so that highly uniform film formation can be performed.

  In the present invention, the substrate 7 can be moved by the stage 8 in a direction substantially perpendicular to the flying direction of the particles ejected from the nozzle 5. Therefore, a film having a desired shape can be formed. Since the relative position between the injection nozzle 5 and the substrate 7 only needs to be changed, the nozzle 5 may be movable instead of the substrate 7.

Example 1
In this example, film formation was performed using the film formation apparatus having the configuration shown in FIG.

  50 g of untreated PZT powder was charged as particles into the supply means 1 having classification means. A container in which particles (PZT powder) are loaded in the supply means 1, a mesh body (mesh) having a fixed opening disposed at the bottom of the container, and a brush that can rotate in contact with the mesh body A supply means consisting of was used. The PZT powder is passed through a mesh body by rotation of a brush and sieved, and only particles having a predetermined particle size or less are supplied.

  In addition, by using a mesh having a fixed mesh size of 400 μm, particles classified to 400 μm or less were supplied to the crushing / dispersing means 3 at a rate of 1 g / h. The particle supply rate is calculated by calculating the weight of the particles to be supplied by measuring the weight of the supply means 1 using the electronic balance 13 and adjusting the rotation speed of the brush based on the calculated data. Controlled.

  The supply amount of PZT powder by this control changed substantially linearly as shown in FIG. The supply amount error at the time when 500 mg was supplied as measured by the electronic balance 13 was within ± 5%. Further, when the particle size distribution of the PZT powder at the time of supply was measured, the peak was in the range of 80 μm or more and 100 μm or less as shown in FIG.

  The PZT particles classified to 400 μm or less and supplied at a rate of 1 g / h are supplied to the crushing / dispersing means 3. The internal structure of the crushing / dispersing means 3 is the same as that shown in FIG. PZT particles having a particle diameter of 400 μm or less (there are many agglomerated particles) 24 were supplied from above in FIG.

  The first gas introduction pipe 18 and the gas valve 21 attached thereto were opened to the atmosphere, and the pressure of the second gas introduced from the second gas introduction pipe 19 was adjusted to 0.3 MPa by adjusting the valve 22. At this time, the flow velocity 26 of the first gas containing the supplied PZT particles is different from the flow velocity 27 of the second gas supplied from the second gas introduction pipe 19. Therefore, a shearing force is generated on the particles 24 in the vicinity of the boundary between the gas flow 26 and the gas flow 27, and the aggregated particles 24 in a range of 400 μm or less are crushed and dispersed. The particle size of the PZT particles 25 after pulverization is determined by the difference in flow velocity between the gas flow 26 and the gas flow 27 and can be appropriately adjusted according to the target particle size. In this case, the particle size distribution after pulverization was as shown in FIG. 8, and had a peak in the range of 1 μm ± 0.5 μm, and the particle size could be 3 μm or less.

  The PZT particles classified, supplied, crushed and dispersed using the above-described means are jetted from the jet nozzle 5 toward the substrate 7 through the transport pipe 4. The substrate 7 is fixed to a stage 8 that can move in the XY directions, and a PZT film was formed by scanning the stage 8.

  The formed PZT film had a film thickness error (variation) within ± 6% of the average film thickness. As described above, according to the film forming apparatus of the present invention, it was possible to perform film formation with high uniformity and good reproducibility. Here, PZT particles are used as the particles. However, in the present invention, even when particles of other materials are used, the film can be formed with good reproducibility.

(Example 2)
In this example, film formation was performed using the film formation apparatus having the configuration shown in FIG.

  As the supply device 100, a method was used in which a gas (first gas) was sprayed onto the powder (particles) filled in the container and the soared particles were transported together with the sprayed gas (first gas). A more detailed configuration of the supply apparatus 100 is shown in FIG. The container 1 is filled with PZT powder (PZT particles), and a gas introduction pipe 33 for directly blowing gas onto the filled powder and an aerosol formed by blowing the gas (introduced from the gas introduction pipe 33). A transport pipe 34 that transports the aerosol formed by dispersing PZT particles in the gas (first gas) to the outside of the container 1 is provided. A supply amount detection means 2 for detecting the supply amount of particles is provided at the tip of the transport pipe 34.

  Here, an optical method was used to detect the supply amount of the particles. Based on the detected data, the flow rate of the gas blown into the container was controlled to control the supply amount of particles to a desired amount. Further, by changing the relative positions of the gas introduction pipe 33 and the conveyance pipe 34, the average particle size of the particles carried out from the container 1 through the conveyance pipe 34 was set to 400 μm or less.

  The PZT particles classified to 400 μm or less are supplied to the crushing / dispersing means 3. The structure of the crushing / dispersing means 3 is the same as that shown in FIG. The average particle diameter of the particles 24 supplied to the crushing / dispersing means 3 is 400 μm or less. The pulverizing / dispersing means 3 is supplied with PZT particles 24 (including secondary particles composed of a large number of PZT particles) together with the gas flow 26 introduced from the gas introduction pipe 33.

  In this embodiment, the gas introduction pipe 18 and the valve 21 attached thereto are completely sealed.

  The pressure of the second gas introduced from the second gas introduction pipe 19 was adjusted to 0.3 MPa by adjusting the valve 22. At this time, the flow velocity of the particles (flow velocity corresponding to the flow velocity of the first gas) 26 and the flow velocity 27 of the second gas supplied from the second gas introduction pipe 19 are different. While being crushed, it is dispersed in a mixed gas of the first gas and the second gas. The particle size distribution of the particle size of the PZT particles after pulverization is as shown in FIG. 8, which is a particle size of 4 μm or less, and was pulverized to a peak between 0.5 μm and 1.5 μm.

  The film thickness error of the PZT film formed using the film forming apparatus of the present example (the range of fluctuation of the film thickness with respect to the average film thickness) is within ± 8%, and highly uniform film formation was realized.

(Example 3)
In this example, film formation was performed using the film formation apparatus having the configuration shown in FIG. The supply device 100 including classification means includes a container for filling powder and a mechanism for introducing gas with high uniformity from the lower part of the powder in the container. Then, the particles that have been raised are transported.

  A more detailed configuration of the supply device 100 of this embodiment is shown in FIG. A mesh-like filter (a member having a large number of holes through which gas can pass) 36 is disposed on the bottom of the container 1 so that the first gas can be introduced into the container 1 from the lower part of the filter 36. ing. The first gas is supplied from the cylinder 11 to the bottom of the container 1 through the filter 36 through the transport pipe 33 connected to the container 1. 30 g of PZT powder (particles) was filled (placed) on the filter 36. A second transfer pipe 34 was installed on the top of the container 1.

  A supply amount detection means 2 for detecting the supply amount of particles is provided at the tip of the transport pipe 34. Further, the crushing / dispersing means 3 to be described later is arranged further ahead of the transport pipe 34.

  The feedback of the supply amount of the particles was performed by measuring the amount of particles using an optical method and controlling the flow rate of the first gas based on the measurement data.

  Further, the position of the transport pipe 34, that is, the suction height of the aerosol was changed, and classification was performed so that the average particle diameter of the particles supplied to the supply amount detection means 2 would be 400 μm or less. Further, the variation with time of the supply amount of the particles at this time was within ± 8%.

  The internal structure of the crushing / dispersing means 3 is schematically shown in FIG. In this embodiment, the gas introduction pipe 18 and the gas valve 21 attached thereto are completely sealed. The pressure of the second gas introduced from the second gas introduction pipe 19 was adjusted to 0.3 MPa by adjusting the valve 22.

  By doing in this way, the flow velocity 26 which the powder (secondary particle comprised when many PZT particle | grains aggregated) 24 injected from the front-end | tip of the 1st conveyance pipe 4-1, and the 1st Since the flow velocity 27 of the second gas flowing in the vicinity of the tip of the transport pipe 4-1 is different, a force such as a shearing force acts on the particles 24 existing in the vicinity of the boundary between the gas flow 26 and the gas flow 27 and aggregates. Particles are crushed and dispersed.

  The particle size distribution of the PZT particles after pulverization is as shown in FIG. 8, and has a peak in the range of 0.5 μm to 1.5 μm, and the maximum particle size is pulverized to 4 μm or less.

  When the PZT film was formed using the apparatus as described above, the error (variation) of the thickness of the PZT film was within ± 9% of the average film thickness. According to the film forming apparatus of the present embodiment, the supply amount of particles can be stabilized, and particles having a small number of secondary particles and a narrow particle size distribution can be used. It was possible to form with good properties and high homogeneity.

Example 4
In the film forming apparatus of this example, film formation was performed using the film forming apparatus having the configuration shown in FIG.

  A feeder 37 was used as the supply device 100. In the third embodiment, the powder is disposed in advance in the container (aerosolization chamber) 1, but in this embodiment, the first mechanism passes through the mesh 36 disposed below in the aerosolization chamber 1 by the same mechanism as in the third embodiment. The aerosol was formed by supplying the powder into the aerosol chamber 1 little by little while introducing the above gas into the container 1. Then, the formed aerosol was led out from the container 1 through the transport pipe 34.

  FIG. 11 schematically shows a more detailed structure of the supply apparatus 100 used in this example.

  A mesh-like filter 36 is disposed on the bottom of the container (aerosolization chamber) 1 so that the first gas can be uniformly introduced from the lower part of the filter. This structure is the same as that of the third embodiment.

  PZT powder (PZT particles) was fed into the container 1 from the feeder 37 through the conveying pipe 38 at a rate of 1 g / h. The introduced powder is aerosolized by the first gas and conveyed by the conveying tube 34.

  In the present embodiment, the feedback mechanism for the supply amount of the particles measures the supply amount of the particles by an optical method, and the first gas so as to obtain a desired value (supply amount) based on the measured data. And the drive of the feeder 37 were controlled.

  In addition, the position of the transport pipe 34, that is, the suction height of the aerosol was changed to control the average particle diameter of the transported particles to be 300 μm or less.

  The PZT particles 24 classified to 300 μm or less are supplied to the crushing / dispersing means 3.

  The inside of the crushing / dispersing means 3 has a structure as shown in FIG. In the present embodiment, the first gas introduction pipe 18 and the gas valve 21 attached thereto are completely sealed. The pressure of the second gas introduced from the second gas introduction pipe 19 was adjusted to 0.4 MPa by adjusting the valve 22. At this time, the flow velocity 26 of the first gas discharged from the tip of the first transfer pipe 4-1, and the second gas supplied from the second gas introduction pipe 19 into the second transfer pipe 4-2. The gas flow rate 27 is different. Therefore, a force sufficient to break up the agglomerated particles 24 such as shear force is applied to the particles 24 existing in the vicinity of the boundary between the gas flow 26 and the gas flow 27, and the agglomerated powder 24 is crushed and dispersed. Is done.

  The particle size distribution of the PZT particles 25 after pulverization had a peak in the range of 0.7 μm or more and 1.3 μm or less, and the particle size was 3 μm or less. The particle size distribution of the crushed word can be controlled by the relative velocity between the flow rate of the first gas and the flow rate of the second gas. Generally, if the relative speed is large, the minimum value of the particle size after crushing tends to be small.

  When the PZT film was formed using the apparatus as described above, the error (variation) of the PZT film was within ± 7% of the average film thickness. According to the film forming apparatus of the present embodiment, the supply amount of particles can be stabilized, and particles having a small number of secondary particles and a narrow particle size distribution can be used. It was possible to form with good properties and high homogeneity. When PZT was replaced with BNT and a BNT film was formed using the film forming apparatus of this example, a film having good shape characteristics as in PZT could be formed.

Schematic diagram of conventional film deposition equipment The schematic view of the film forming apparatus of the present invention. Embodiment 1 of the present invention Enlarged view of the injector part 1 Enlarged view of the injector part 2 Particle supply Particle size distribution after classification Particle size distribution after crushing Aerosol forming means in embodiment 2 Aerosol forming means in Example 3 Aerosol forming means in Example 4

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Supply means 2 Supply amount detection means 3 Crushing means 4 Conveying pipe 5 Nozzle 6 Deposition chamber (chamber)
7 Substrate 8 Stage 9 Feedback Control Circuit 13 Electronic Balance 24 Aggregated Particles 25 Crushed Particles 26 First Gas Flow 27 Second Gas Flow 28 Third Gas Flow 100 Aerosol Forming Device

Claims (10)

In a film forming apparatus having an aerosol forming means for forming an aerosol containing particles of a film forming material, and a nozzle for injecting the aerosol formed by the aerosol forming means,
The aerosol forming means includes a supply means for supplying particles of the film forming material, a detecting means for detecting the amount of particles of the film forming material, and a film formed in the aerosol to be formed based on the detection result of the detecting means. Control means for controlling the amount of particles of the material,
The supply means includes a container for storing particles of a film forming material,
The detecting means detects the amount of film forming material particles contained in the aerosol to be formed by measuring the weight of the container in a state in which the film forming material particles are contained. A film forming apparatus.   The film forming apparatus according to claim 1, wherein the control unit controls the amount of particles of the film forming material supplied from the supply unit.   The film forming apparatus according to claim 1, wherein the container includes a filter having a plurality of openings through which particles of the film forming material are passed.   The film forming apparatus according to claim 3, wherein the container further includes a brush that moves in contact with the filter.   The aerosol forming means further comprises a crushing means for crushing particles formed by aggregation of a large number of particles among the particles into a plurality of particles. 2. The film forming apparatus according to 1.   The crushing means includes a first transport pipe through which the formed aerosol flows and a tip of the first transport pipe inserted therein so that the gas flows along with the aerosol discharged from the tip. The film forming apparatus according to claim 5, further comprising: a transfer pipe.   The film forming apparatus according to claim 6, wherein the aerosol and the gas are flowed so that a flow rate of the aerosol released from the tip and a flow rate of the gas flowing along with the aerosol are different. In a film forming apparatus having an aerosol forming means for forming an aerosol containing particles of a film forming material, and a nozzle for injecting the aerosol formed by the aerosol forming means,
The aerosol forming means includes a first transport pipe, and a second transport pipe into which a gas flows along with the aerosol that is inserted from the tip of the first transport pipe and discharged from the tip. A film forming apparatus.   The film forming apparatus according to claim 8, wherein the aerosol and the gas are caused to flow such that a flow rate of the aerosol released from the tip and a flow rate of the gas flowing along with the aerosol are different.   A film forming method comprising: forming a film containing the film forming material by spraying the aerosol toward a base using the film forming apparatus according to claim 1. .

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