JP4590594B2 - Aerosol deposition system - Google Patents

Description

  The present invention relates to an aerosol deposition film forming apparatus for forming a film using an aerosolized fine particle material.

  Aiming for a ubiquitous society, development of portable wearable mobile electronic devices is desired in the fields of personal computers, mobile phones, and other mobile devices. In order to realize such miniaturization, high performance, and multi-functionality of such an electronic device, it is important to integrate and form materials having various functions in the same space. Up to now, in the development of circuit boards, semiconductor elements, and passive electronic components, it is possible to develop devices that meet the requirements by forming a structure with a combination of resin and metal materials, and ceramic and metal materials. I did it.

  However, the structure formed by a combination of a resin material and a ceramic material has different process temperatures. Therefore, there is a limitation on the composite, and there has been no method that sufficiently exhibits both characteristics. As one of the methods, a method of mixing a ceramic powder in a resin to make a composite has been tried, but the current situation is that the required characteristics are not sufficiently satisfied. For example, even in a combination of a high dielectric constant ceramic and a resin for achieving a high dielectric constant, the filling rate of the ceramic in the resin is limited, and only a material having a relative dielectric constant of several tens can be obtained. For this reason, development of ceramics that can be formed at a low process temperature or a resin material having a high heat-resistant temperature is desired.

  Therefore, the so-called aerosol deposition method in which an inorganic material film is formed on a substrate by transporting an aerosol in which fine particles of inorganic material are dispersed in a gas and colliding with the substrate can form a ceramic film near room temperature. For this reason, it is expected that composite and integration with resin materials will be possible without impairing the original characteristics of the materials, and research and development in this field is starting to become active.

The aerosol deposition film forming apparatus sprays aerosol obtained by blowing a gas into ceramic particles onto a substrate from a nozzle to form a ceramic film on the substrate. This is because aerobic deposition occurs when individual ceramic particles that are injected collide with the substrate or other particles, causing the plastic deformation of the particle surface or crushing of the particles, and close contact with the substrate or other particles. A film is formed.
JP 2003-277948 A JP 2001-348658 A JP-T-2001-513697

  By the way, since ceramic particles are fine particles of about several tens of nm to several hundreds of nm, they easily aggregate. Aggregated particles are difficult to separate because a plurality of primary particles are adsorbed to each other by an electrostatic force or the like. If a film is formed as it is, the adhesion strength between the particles is reduced, and pores are formed to form a fragile aerodynamic device. A position film is formed. Further, even if primary particles are formed by impact of collision, the energy of collision that can be used for primary particleization is reduced. As a result, there is a problem in that the amount of strain on the particle surface for bringing the particles into close contact with each other is insufficient, and sufficient adhesion strength and denseness cannot be ensured. In addition, since the entire particle surface is not activated, there is a problem in adhesion strength and denseness in this respect as well.

  When forming an aerosol, the primary particle treatment is performed by applying vibration or ultrasonic waves, but this is not always sufficient, and the above problem is included because there is a material that easily aggregates even with a fine particle material.

  Accordingly, the present invention has been made in view of the above problems, and an object of the present invention is to provide an aerosol deposition film forming apparatus capable of forming a dense film with high film adhesion.

According to one aspect of the present invention, aerosol forming means for forming an aerosol made of fine particles made of an inorganic material and a carrier gas, and film forming means for forming an inorganic material film on a substrate by spraying the aerosol with a spray nozzle. And a primary particle forming means for dispersing fine particles contained in the aerosol between the aerosol forming means and the film forming means, and the primary particle forming means comprises a barrier portion disposed in the aerosol flow path. The fine particles contained in the aerosol collide with the barrier portion to disperse the primary particle forming means, the first barrier member disposed in the aerosol flow path, and the downstream side thereof. was made from the second barrier member, a portion of the first barrier member and a second barrier member, it wherein an opening for passing the aerosol is respectively provided Aero Rudepojisshon film-forming apparatus is provided.

  According to the present invention, before spraying the aerosol from the spray nozzle, primary particle forming means for dispersing the fine particles forming the aerosol is provided, and the fine particle aggregate in which the primary particles of the fine particles are aggregated is converted into primary particles. By spraying the aerosol composed of primary particles in this way with an injection nozzle, sufficient impact can be formed on the surface of each fine particle due to the impact when colliding with the substrate, and the adhesion between the fine particles and the fine particles The adhesion between the substrate and the substrate is improved, and an aerosol deposition film having high density and high film adhesion can be formed. Further, since the fine particles are converted into primary particles in an aerosol state, reaggregation of the fine particles can be avoided. In the present specification and claims, “primary particle formation” ideally means that fine particle aggregates in which fine particles of primary particles are aggregated are completely separated into individual primary particles. This includes the case where individual primary particles are not completely separated and some aggregates remain.

  The primary particle forming means may include a barrier portion disposed in the aerosol flow path, and the fine particles contained in the aerosol may collide with the barrier portion to be dispersed. Before injecting the aerosol from the injection nozzle, a barrier part that blocks part of the aerosol flow path is provided, and the kinetic energy of the fine particles generated by the aerosol flow is used to cause the fine particles to collide with the barrier part to be converted into primary particles. . Thus, the fine particles can be made into primary particles by means of primary particles that have a simple structure.

  The primary particle forming means includes a pair of electrodes provided in an aerosol flow path and an AC power source for applying an AC voltage between the pair of electrodes, and charges the fine particles contained in the aerosol, The fine particles may be dispersed by colliding with each other by electrical attraction. Before injecting the aerosol from the injection nozzle, the fine particle aggregate in which the primary particles forming the aerosol are aggregated by the primary particle forming means is charged by an alternating voltage applied between the pair of electrodes. Then, the fine particle aggregates are mechanically separated by the impact received at the time of collision by attracting and colliding the fine particle aggregates to each electrode by an electric attraction generated by an alternating voltage and an electric field alternating with the electric field direction. Particleize. By controlling the magnitude of the AC voltage to be applied, the speed at which the fine particles collide with the electrode can be controlled independently of the flow velocity of the aerosol, so that the fine particles can be made primary particles reliably.

  ADVANTAGE OF THE INVENTION According to this invention, the aerosol deposition film-forming apparatus which can form a precise | minute and film | membrane with high film | membrane adhesiveness can be provided.

  Embodiments will be specifically described below with reference to the drawings.

(First embodiment)
The aerosol deposition film forming apparatus according to the first embodiment includes a primary particle formation mechanism that disperses fine particles using kinetic energy of fine particles generated by the flow of the aerosol before the aerosol is injected from the injection nozzle. Has the main features.

  FIG. 1 is a schematic configuration diagram of an aerosol deposition film forming apparatus according to a first embodiment of the present invention.

  Referring to FIG. 1, an aerosol deposition (hereinafter abbreviated as “AD”) film forming apparatus 10 generally includes an aerosol forming unit 20 that aerosolizes fine particles 27 of a film forming material, and fine particles 27 in an aerosol 29. Primary particle formation mechanism 30, aerosol 29 is sprayed toward substrate 43 to form AD film 46, and exhaust system 50 that keeps film formation part 40 in a reduced-pressure atmosphere. The

  The AD film forming apparatus 10 causes the primary particle forming mechanism 30 to bring the fine particles 27 in the aerosol 29 ideally into a state where the primary particles of the fine particles 27 are individually dispersed. The primary particle formation mechanism 30 is provided with an aerosol flow path barrier portion (a first barrier plate 31 and a second barrier plate 32, which will be described in detail later with reference to FIG. 2), and the aggregates of the fine particles 27 collide with the barrier portion. And mechanically separate. When the aerosol 29 composed of the primary particles 27 is injected from the injection nozzle 42 onto the substrate, most of the energy when the particles 27 collide with the substrate 43 or the surface of the already formed AD film 46 is fine particles. 27 is consumed as energy that induces strain on the surface of 27. Therefore, sufficient strain is induced on the surface of the fine particles 27 to ensure adhesion. As a result, the adhesion between the fine particles 27 and the substrate 43 and the adhesion between the fine particles are improved, and a dense AD film 46 with high film adhesion is formed. Hereinafter, a specific configuration of the AD film forming apparatus 10 will be described.

  The aerosol forming unit 20 includes an aerosol generator 21, a gas cylinder 22 that supplies a compressed carrier gas to the aerosol generator 21, a compressor 23, a mass flow controller 24, and pipes 25 and 28.

  The aerosol generator 21 has a container 26 filled with fine particles 27 of a film forming material. The aerosol generator 21 includes a pipe 25 for introducing a carrier gas into the fine particles 27 and a pipe 28 for sending an aerosol 29 formed by the carrier gas and the fine particles 27 that have risen into the container 26 by the carrier gas to the primary particle formation mechanism 30. And are connected. In the aerosol generator 21, by introducing the carrier gas into the container 26, the fine particles 27 rise in the space inside the container 26 and an aerosol 29 is formed.

  The aerosol generator 21 may be provided with a vibrator for applying ultrasonic vibration, electromagnetic vibration, and mechanical vibration to the fine particles 27. A homogeneous AD film can be formed by mechanically separating the aggregation of the fine particles 27 with a vibrator. The aerosol generator 21 may be provided with a heater such as a heater for drying the fine particles 27.

  Further, the container 27 is connected to the vacuum system 50 via a pipe 56 and a valve 56b in order to set the inside of the aerosol generator 21 in a reduced pressure atmosphere in advance. When drying the aerosol generator 21, particularly when drying the fine particles 27, the vacuum system 50 is operated and the valve 56 b is opened to evacuate the container 26. At that time, vibration may be applied to the fine particles 27 with a vibrator or may be heated with a heater.

The fine particles 27 are made of an inorganic material, and the average particle diameter is preferably set in the range of, for example, 10 nm to 500 nm. The fine particles 27 are not particularly limited as long as they are inorganic materials. For example, when forming an interlayer insulating layer of a circuit board or a semiconductor device, MgO, TiO ₂ , ZrO _{2 is used} from the viewpoint of low dielectric loss at high frequencies. _{, SiO 2, Al 2 O 3} , BaTiO 3, BaZrO 3, ZrSnTiO 4, BaTi 4 O 9, Ba 2 Ti 9 O 20, MgTiO 3, MgZrO 3, Ba (Zn 1/3 Ta 2/3) O 3, Ba (Zn _1/3 Nb _2/3 ) O ₃ , Ba (Mg _1/3 Ta _2/3 ) O ₃ , Ba (Co _1/3 Ta _2/3 ) O ₃ , Ba (Co _1/3 Nb _{2 / 3} ) O ₃ , Ba (Ni _1/3 Ta _2/3 ) O ₃ , SrTiO ₃ , SrZrO ₃ , Nd ₂ Ti ₂ O ₇ , (BaSr) TiO ₃ , Ba (TiZr) O ₃ , PbZrTiO ₃ , PbTiO _{3 3, PbZrO 3, Pb (Mg} 1/3 Nb 2/3) O 3, Pb (Ni 1/3 Nb 2/3) _{3, Pb (Zn 1/3 Nb 2/3} ) O 3, 3Al 2 O 3 · 2SiO 2 ( _{mullite), MgO · Al 2 O 3} ( spinel), 2MgO · SiO ₂ (forsterite), 2Al ₂ O ₃ · 2MgO · 5SiO ₂ (cordierite), CaO · SiO _{2 (wollastonite), CaO · Al 2 O 3} · 2SiO 2 ( _{anorthite), CaO · MgO · 2SiO 2} ( diopside), 2CaO · Al ₂ O Ceramic powders such as ₃ · SiO ₂ (gerenite) and mixtures of one or more ceramic powders selected from these are preferred.

  In the case of forming a wiring pattern of a circuit board or a semiconductor device, examples of the fine particles 27 include a metal material containing Cu, Ag, Au, Pt, Pd, W, Al, or an alloy made of these elements. Further, as the fine particles 27, these metal materials and a mixture of one or more metal materials selected from them are suitable. The fine particles 27 are preferably filled in the container 26 after sufficient dehumidification.

  The gas cylinder 22 is filled with a carrier gas. As the carrier gas, an inert gas such as helium, neon, xenon, krypton, or nitrogen can be used in addition to the argon gas. When oxide ceramics having a perovskite structure is used for the fine particles 27, the carrier gas may be an oxidizing gas such as oxygen gas or air, and these gases may be added to the inert gas. Oxygen deficiency of the oxide ceramic fine particle material can be suppressed.

  The compressor 23 controls the pressure of the carrier gas to control the amount of fine particles 27 filled in the aerosol generator 21, that is, the amount of fine particles in the aerosol. If the gas pressure in the cylinder 23 is sufficiently high instead of the compressor 23, a cylinder gas regulator may be used. When the compressor 23 is used, the carrier gas supply source may be a vaporized carrier gas such as liquid nitrogen instead of the gas cylinder 23. In the case of nitrogen gas or oxygen gas, the carrier gas is recovered and purified from the air. May be.

  The mass flow controller 24 controls the flow rate of the carrier gas and the flow rate of the aerosol formed by the aerosol generator 21.

  As described above, in the aerosol generator 21, the carrier gas is introduced into the fine particles 27 serving as a film forming material, or the fine particles 27 are caused to rise into the carrier gas by using a vibrator or a heater. 29 is formed, and the aerosol 29 is delivered to the primary particle formation mechanism 30 through the pipe 28.

  FIG. 2 is a configuration diagram of a primary particle forming mechanism constituting the aerosol deposition film forming apparatus according to the first embodiment. Referring to FIG. 2, the primary particle formation mechanism 30 is disposed in the pipe 28 so as to substantially block the aerosol flow path, and is disposed downstream of the first barrier plate 31 so as to face the first barrier plate 31. The second barrier plate 32 is formed. Openings 31a and 32a are formed in the first barrier plate 31 and the second barrier plate 32, respectively.

  By configuring the primary particleizing mechanism 30 in this way, the aerosol 29 flows in the pipe 28 from the aerosol forming unit 20 shown in FIG. 1 and first collides with the upstream surface 31b of the first barrier plate 31, or Then, it passes through the opening 31 a of the first barrier plate 31 and collides with the upstream surface 32 b of the second barrier plate 32. The fine particle aggregate 27a forming the aerosol 29 is mechanically separated by the force received from the first barrier plate 31 or the second barrier plate 32 at the time of the collision, and primary particleization proceeds. Further, the aerosol 29 repeatedly collides with the downstream surface 31c of the first barrier plate 31 and the upstream surface 32b of the second barrier plate 32 facing the first barrier plate 31, and the primary particles of the fine particle aggregate 27a further progress. The fine particles converted into primary particles pass through the opening 32a of the second barrier plate 32 along the flow of the carrier gas forming the aerosol, and are sent to the film forming unit 40.

  The cross-sectional area of the opening 31a of the first barrier plate 31 (the area of the surface orthogonal to the aerosol flow direction) is preferably as small as possible because the velocity of the aerosol passing therethrough is large, but the velocity of the aerosol is less than the speed of sound. The cross-sectional area of the opening 31a should be set. When the aerosol velocity reaches the sonic velocity, the aerosol velocity cannot be controlled even if the pressure upstream of the primary particle formation mechanism 30 or the pressure downstream of the primary particle formation mechanism 30 is controlled. Furthermore, when the velocity of the aerosol passing through the opening 31a is excessively high, the fine particles that have passed through the opening 31a are deposited on the upstream surface 32b of the second barrier plate 32. The cross-sectional area of the opening 31a of the first barrier plate 31 should be set large so as to reduce the speed.

  The distance between the downstream surface 31c of the first barrier plate 31 and the upstream surface 32b of the second barrier plate 32 is appropriately selected according to the speed of the aerosol in the pipe 28, and is set to about 30 mm, for example. If the distance is excessively large, it becomes difficult for the fine particles to repeatedly collide with the downstream surface 31c of the first barrier plate 31 and the upstream surface 32b of the second barrier plate 32, and the degree of primary particleization does not sufficiently advance.

  Returning to FIG. 1, the film forming unit 40 is disposed opposite to the injection nozzle 42, the film formation chamber 41, the injection nozzle 42 that is connected to the pipe 28 in the film formation chamber 41, and injects the aerosol 29. A substrate holding table 44 for holding the substrate, an XYZ stage 45 for controlling the position of the substrate 43 and the substrate holding table 44, and the like. In the film forming unit 40, the fine particles 27 of the aerosol 29 ejected from the ejection nozzle 42 collide with the surface of the substrate 43 or the AD film 46 already deposited on the substrate 43, and the fine particles 27 adhere firmly.

  The spray speed of the aerosol 29 is controlled by the pressure of the carrier gas, the pressure of the film forming chamber 41 (depressurized atmosphere), and the opening area of the spray nozzle 42. The jetting speed is preferably as large as possible because the denseness of the AD film becomes good. For example, the jetting speed is set to 50 m / s to 1000 m / s. The opening area of the injection nozzle 42 may be set smaller than the cross-sectional area of the flow path through which the aerosol 29 flows in the pipe, that is, may be tapered so as to narrow the flow path through which the aerosol 29 flows. The flow rate of the aerosol 29 can be increased.

  The XYZ stage 45 moves the substrate holder 43 along two directions (X direction and Y direction) perpendicular to the incident direction of the aerosol 29 and the incident direction (Z direction) of the aerosol. Further, the XYZ stage 45 may perform a constant speed / repetitive driving operation in the X direction and the Y direction. By causing the substrate holder 43 to be driven at a constant speed and repeatedly, the AD film 46 having a large area or a constant film thickness can be formed.

  The exhaust system 50 is connected to the film forming chamber 41, and includes a mechanical booster 51 for setting the pressure in the film forming chamber 41 to a reduced pressure atmosphere, a vacuum pump 52, and pipes 53 and 54 for connecting them. . The exhaust system 50 increases the spraying speed of the aerosol 29 using the film forming chamber 41 as a reduced pressure atmosphere. As the vacuum pump 52, for example, a rotary pump, a diaphragm type vacuum pump, or the like can be used. A dust collector may be provided in the pipe 53 connecting the film forming chamber 41 and the mechanical booster 51 or the pipe 54 connecting the mechanical booster 51 and the vacuum pump 52.

  Next, a film forming method of the AD film 46 using the AD film forming apparatus 10 will be described with reference to FIGS. First, using the mechanical booster 51 and the vacuum pump 52, the film forming chamber 41, the inside of the container 26 of the aerosol generator 21, the inside of the pipes 25, 28, 56 and the like are evacuated to a reduced pressure atmosphere.

  Next, the valve 22b of the gas cylinder 22 is opened to deliver the carrier gas. The carrier gas pressure and flow rate are controlled by the compressor 23 and the mass flow controller 24 to introduce carrier gas into the fine particles 27 of the container 26 of the aerosol generator 21, and the fine particles 27 are aerosolized to form an aerosol 29. The concentration of the aerosol 29 is controlled by the pressure and flow rate of the carrier gas.

  Then, the aerosol 29 is sent to the primary particle formation mechanism 30 through the pipe 28, and as shown in FIG. 2, in the primary particle formation mechanism 30, the fine particles forming the aerosol 29 are on the downstream surface 31 c of the first barrier plate 31. And the collision with the upstream surface 32b of the second barrier plate 32 facing this is repeated, and the primary particle formation of the fine particle aggregate 27a proceeds. The primary particles 27b are sprayed from the spray nozzle 42 and deposited on the substrate 43 in an aerosol state. Sufficient distortion is induced on the surface of the fine particles due to the force applied at the time of collision, and the fine particles and the substrate or the fine particles are brought into close contact with each other, thus forming the dense AD film 46 with high film adhesion.

  According to the present embodiment, before injecting the aerosol from the injection nozzle 42, the primary particle formation mechanism 30 is provided with the first barrier plate 31 and the second barrier plate 32 that block the flow path of the aerosol to form the aerosol. The fine particles collide with the first barrier plate 31 and the second barrier plate 32. The fine particle aggregates are mechanically separated by the force received during the collision, and the fine particles are converted into primary particles. Therefore, by spraying the aerosol composed of the primary particles into the substrate by the injection nozzle, the adhesion between the particles and the adhesion between the particles 27 and the substrate 43 are improved, and the dense and high film adhesion AD. A film 46 can be formed.

  Next, three modified examples of the primary particle formation mechanism constituting the aerosol deposition film forming apparatus according to the first embodiment will be described.

  FIG. 3 is a configuration diagram of a first modification of the primary particle formation mechanism that constitutes the aerosol deposition film forming apparatus according to the first embodiment.

  Referring to FIG. 3, the primary particle formation mechanism 30 </ b> A includes barrier members 34-1 to 34-4 that are provided in the pipe 28 and prevent the flow of aerosol.

  One side end 34-1a of the barrier member 34-1 is fixed to the first inner wall 28a of the pipe, and the other side end 34-1b is separated from the second inner wall 28b facing the first inner wall 28a. Has been placed. The barrier member 34-2 disposed on the downstream side of the barrier member 34-1 has one side end 34-2a fixed to the second inner wall 28b and the other side end 34-2b extending from the first inner wall 28a. They are spaced apart. That is, the fine particle aggregate 27a that has passed through the opening between the side end 34-1b of the barrier member 34-1 and the second inner wall 28b collides with the barrier member 34-2 so as to collide. Furthermore, the barrier member 34-3 and the barrier member 34-4 disposed downstream of the barrier member 34-2 are disposed in the same manner as the barrier member 34-1 and the barrier member 34-2, respectively.

  By arranging the barrier members 34-1 to 34-4 in this way, aerosol fine particles flowing into the primary particle formation mechanism 30A collide with the barrier members 34-1 to 34-4, and at that time, the barrier member 34- The fine particle aggregate 27a is mechanically separated by the force received from 1 to 34-4. The fine particle aggregate 27a repeatedly collides with the barrier members 34-1 to 34-4 as it flows downstream through the openings of the barrier members 34-1 to 34-4 and the first inner wall 28a or the second inner wall 28b. As a result, an aerosol of the fine particles 27b that are primary particles is formed.

  Further, since the barrier members 34-1 to 34-4 are alternately arranged in the flow direction on the first inner wall 28a or the second inner wall 28b, the primary particles of the fine particle aggregate 27a can be efficiently formed with a simple structure. It is possible to reduce the size of the primary particle forming mechanism 30A.

  Moreover, the barrier members 34-1 to 34-4 are disposed obliquely along the aerosol flow direction. For example, the barrier member 34-1 is disposed obliquely toward the downstream side from the side end 34-1a fixed to the first inner wall 28a, and the other barrier members 34-2 to 34-4 are also disposed in the same manner. Yes. By arranging the barrier members 34-1 to 34-4 obliquely in this way, the fine particles 27a and 27b are hardly left and the cleaning maintenance cycle can be prolonged. Although illustration is omitted, in order to increase the force applied to the fine particles at the time of collision, the barrier members 34-1 to 34-4 may be arranged substantially perpendicular to the flow direction, or the flow direction May be tilted in the opposite direction.

  The number of barrier members 34-1 to 34-4 is not limited to four, and may be one to three, or five or more, and the degree of primary particle formation of aerosol fine particles that have passed through the primary particle formation mechanism 30A. May be determined as appropriate.

  The primary particle formation mechanism 30A of the first modification is provided with barrier members 34-1 to 34-4 so as to prevent the flow of aerosol, and the barrier member 34-1 as the fine particle aggregate 27a forming the aerosol flows downstream. The particle aggregate 27a receives force during the collision from the barrier members 34-1 to 34-4, mechanically separates and becomes primary particles. . Therefore, the fine particles forming the aerosol are converted into primary particles and the degree of activation of the surface is large, so that a dense AD film having high film adhesion can be formed.

  FIG. 4 is a configuration diagram of a second modification of the primary particle forming mechanism that constitutes the aerosol deposition film forming apparatus according to the first embodiment.

  Referring to FIG. 4, the primary particle formation mechanism 30 </ b> B includes a nozzle portion 36 provided in a pipe 28 and a barrier plate 38 disposed downstream thereof.

  The nozzle portion 36 has a tapered flow path 36a that gradually narrows the aerosol flow path along the flow direction, and a cross-sectional area (area of a surface orthogonal to the aerosol flow direction) connected to the tapered flow path 36a is constant. The flow path 36b is provided. The barrier plate 38 is provided so as to substantially block the flow path. The barrier plate 38 is provided with an opening 38a for allowing the aerosol to flow downstream. The opening 38 a is disposed in a region that is out of the position facing the opening of the flow path 36 b of the nozzle portion 36.

  By providing the nozzle portion 36 and the barrier plate 38 in this way, the aerosol that has flowed into the primary particleizing mechanism 30B is accelerated by the tapered flow path 36a and flows out from the flow path 36b toward the barrier plate 38. The fine particle aggregate 27a forming the aerosol collides with the upstream surface 38b of the barrier plate 38 and is mechanically separated by the force received at that time. Then, primary particles are repeatedly formed by repeatedly colliding with the downstream surface 36 c of the nozzle portion 36 and the upstream surface 38 b of the barrier plate 38. The fine particles 29 b that have been converted into primary particles pass through the opening 38 a of the barrier plate 38 and are sent to the film forming unit 40.

  The material of the nozzle portion 36 and the barrier plate 38 is not particularly limited, but the barrier plate 38 is preferably made of a material having a hardness higher than that of the fine particles in order to suppress wear due to the collision of the fine particles.

  The cross-sectional area of the opening of the flow path 36b of the nozzle section 36 is preferably as small as possible in order to increase the velocity of the aerosol passing therethrough. However, if it is excessively small, the fine particles that have passed through the flow path 36b are on the upstream surface of the barrier plate 38. It adheres to and deposits. Therefore, the cross-sectional area of the opening of the flow path 36b should be set to be smaller than the speed at which the fine particles are deposited. The cross-sectional area should be set so that the aerosol velocity is smaller than that.

  The distance between the downstream surface 36c of the nozzle portion 36 and the upstream surface 38b of the barrier plate 38 is appropriately selected according to the speed of the aerosol in the pipe 28, and is set to about 30 mm, for example. If the distance is excessively large, it is difficult for the fine particles to repeatedly collide with the downstream surface 36b of the nozzle portion 36 and the upstream surface 38b of the barrier plate 38.

  The primary particle formation mechanism 30B of the second modified example accelerates the aerosol by the nozzle portion 36, and causes the fine particle aggregate 27a that forms the aerosol to collide with the barrier plate 38 at a high speed. The fine particle aggregate 27a receives force from the barrier plate 38 due to collision and mechanically separates into primary particles. Furthermore, since the fine particle aggregate 27a collides at a high speed, the degree to which the surface of the fine particles is activated at the time of the collision increases. Therefore, the fine particles forming the aerosol are converted into primary particles and the degree of activation of the surface is large, so that a dense AD film having high film adhesion can be formed. In addition, it is not necessary to provide the flow path 36b in the nozzle part 36, that is, only the tapered flow path 36a may be provided in the nozzle part 36.

  FIG. 5 is a configuration diagram of a third modification of the primary particle forming mechanism that constitutes the aerosol deposition film forming apparatus according to the first embodiment.

  Referring to FIG. 5, the primary particle formation mechanism 30 </ b> C includes a shielding part 39 provided in the pipe 28, and the first flow path 39 a and the second flow path 39 b are parallel to the shielding part 39 on the upstream side. On the downstream side thereof, a joining portion 39c where the first passage 39a and the second passage 39b join, and a third passage 39d communicating with the joining portion 39c are provided on the downstream side. ing.

  When the flow path into which the aerosol 29 flows is, for example, a cylindrical shape whose central axis is the flow direction, the first flow path 39a and the second flow path 39b may be provided at positions that are substantially symmetric with respect to the central axis. preferable. By setting such a position, approximately the same amount of aerosol flows into each of the first flow path 39a and the second flow path 39b. In the merging portion 39c, the aerosol particles flowing in the first flow path 39a and the aerosol fine particles flowing in the second flow path 39b collide with each other. The fine particle aggregates 27a are mechanically separated from each other by the force received at the time of collision and advance into primary particles. The fine particles 29b converted into primary particles pass through the third flow path 39d and are sent to the film forming unit 40. .

  It is preferable that the first flow path 39a and the second flow path 39b have substantially the same shape, that is, their cross-sectional areas (areas of surfaces perpendicular to the flow direction of the aerosol) and lengths are approximately the same. By setting in this way, the flow from the junction 39c to the third flow path 39d becomes smooth.

  Further, in the confluence portion 39c, the first flow path 39a and the second flow path 39b cross each other, but the larger the crossing angle is, the more preferable is that the forces received by each other when the fine particle aggregates collide with each other. However, if the crossing angle exceeds 180 degrees, it becomes difficult to flow from the merging portion 39c to the third flow path 39d. Therefore, the crossing angle is preferably 180 degrees or less.

  Since the fine particle collides with each other in the junction 39c, the primary particle formation mechanism 30C of the third modification can advance the formation of fine particles into a primary particle while suppressing the mixing of the material of the barrier part 39 and the like. As a result, it is possible to form a dense AD film 46 with high film adhesion, and to form an AD film 46 with less mixing of materials other than the particulate material.

  2 to 5, the primary particle formation mechanisms 30 and 30A to 30C have been described by way of example in the case where they are provided in the flow path having the same cross-sectional area as the pipe 28 connected thereto. Alternatively, the primary particle formation mechanisms 30 and 30A to 30C may be provided in the flow path having a large cross-sectional area.

(Second Embodiment)
The aerosol deposition film forming apparatus according to the second embodiment is a primary particle in which fine particles are electrically polarized before the aerosol is jetted from the jet nozzle, and the fine particles are collided by an electric attractive force to disperse the fine particles. The main feature is the provision of the conversion mechanism.

  FIG. 6 is a configuration diagram of a primary particle forming mechanism constituting an AD film forming apparatus according to the second embodiment of the present invention. Since the configuration of the AD film forming apparatus other than the primary particle formation mechanism is the same as that of the AD film forming apparatus according to the first embodiment shown in FIG. 1, reference is made to FIG. .

  Referring to FIG. 6, the primary particle formation mechanism 60 constituting the AD film forming apparatus of the present embodiment includes a flat plate first electrode 61 provided in parallel with each other in the flow direction of the aerosol in the pipe 28, and The second electrode 62 and an AC power source 63 electrically connected to the first electrode 61 are configured, and the second electrode 62 and the AC power source 63 are each electrically grounded.

  The AC power source 63 applies a high AC voltage (for example, a frequency of 100 Hz) between the first electrode 61 and the second electrode 62. An electric field E is generated between the first electrode 61 and the second electrode 62 by applying an alternating voltage. The maximum electric field strength of the electric field E is set to 10 MV / m, for example. The aerosol fine particle aggregate 27a that has flowed into such an extremely high electric field comes to be positively charged by, for example, extracting electrons from the fine particle aggregate 27a by contact with the first electrode 61 or the second electrode 62. . When the first electrode 61 becomes a negative electrode, the fine particle aggregate 27a charged to the positive polarity is attracted by an electric attractive force proportional to the product of the charge amount and the electric field strength and collides with the first electrode 61. The fine particle aggregate 27a is mechanically separated from the first electrode 61 upon receiving a force upon collision. When the polarity of the AC voltage is reversed and the second electrode 62 becomes a negative electrode, the fine particle aggregate 27a is attracted to the second electrode 62 and collides with the second electrode 62, and further mechanically separated by the force at that time. . The fine particles 27b are repeatedly made into primary particles by repeating these collisions according to the reversal of the AC voltage while gradually moving downstream. The higher the voltage applied by the AC power source 63, the more the fine particle aggregates are accelerated.

  According to the present embodiment, before injecting the aerosol from the injection nozzle 42, the primary particle forming mechanism 60 charges the fine particle aggregate 27 a that forms the aerosol, so that the first electrode 61 and the second electrode 62 are not charged. By applying a high electric field strength to the first electrode 61 and the second electrode 62 by alternately attracting and colliding them with the first electrode 61 and the second electrode 62, and mechanically separating them by the force received during the collision, Fine particles are converted into primary particles. By forming primary particles in this way, the adhesion between the fine particles 27 and the substrate 43 and the adhesion between the fine particles are improved, and a dense and highly adhering AD film 46 can be formed.

  According to the present embodiment, by controlling the magnitude of the AC voltage to be applied, the speed at which the fine particles collide with the first electrode 61 and the second electrode 62 is controlled independently of the aerosol flow velocity. Primary particles.

  Further, according to the present embodiment, the fine particle aggregate 27a and the primary fine particles 27b flow downstream while alternately colliding with the first electrode 61 and the second electrode 62, so that the residual fine particles can be suppressed. The maintenance cycle for cleaning can be prolonged.

  A device for neutralizing the charging of the fine particles, for example, a neutralizer that generates thermoelectrons, may be provided on the downstream side of the primary particle forming mechanism 60. It is possible to suppress the fine particles from being electrically attached to the inner wall of the pipe.

  Further, the first electrode 61 and the second electrode 62 are not limited to parallel plate electrodes, and may be a cylindrical shape along the central axis of the flow path of the pipe 28. In this case, for example, the first electrode 61 is a cylindrical electrode, and the second electrode 62 is a columnar electrode coaxial with the central axis of the cylindrical electrode.

  Although not shown in FIG. 6, the first electrode 61 and the second electrode 62 and the pipe 28 are electrically insulated with an appropriate insulating material according to the magnitude of the AC voltage.

  FIG. 7 is a configuration diagram of a modified example of the primary particleizing mechanism constituting the aerosol deposition film forming apparatus according to the second embodiment.

  Referring to FIG. 7, the primary particle formation mechanism 60 </ b> A includes three first electrodes 61-1 to 61-3 that are flat plates provided in the flow path connected to the pipe 28 along the flow direction of the aerosol. It is composed of three second electrodes 62-1 to 62-3, an AC power source 63 and the like electrically connected to the first electrodes 61-1 to 61-3, and the second electrodes 62-1 to 62-3. The AC power supply 63 is electrically grounded. The three first electrodes 61-1 to 61-3 and the three second electrodes 62-1 to 62-3 are alternately arranged in pairs in a direction orthogonal to the flow direction of the aerosol. The action of the primary particle forming mechanism 60A is the same as that of the primary particle forming mechanism 60 shown in FIG. 6, and the aerosol fine particle aggregate 27a is passed through the first electrodes 61-1 to 61-3 and the second electrode. The charged fine particle aggregates 27a formed between the electrodes 62-1 to 62-3 are electrically attracted alternately to the first electrodes 61-1 to 61-3 and the second electrodes 62-1 to 62-3. The fine particle aggregate 27a is converted into primary particles by attracting and colliding with each other.

  In the primary particle formation mechanism 60A, the aerosol flowing in from the pipe 28 is divided into five flow paths 65-1 to 65-5, and the first electrodes 61-1 to 61- arranged on the downstream side of the respective flow paths. 3 and the second electrodes 62-1 to 62-3.

  The primary particle formation mechanism 60 </ b> A of this modification is configured so that the sum (total cross-sectional area) of the cross-sectional areas of the five flow paths 65-1 to 65-5 (area of the surface orthogonal to the aerosol flow direction) is Since it is larger than the cross-sectional area of the flow path, the flow velocity of the aerosol decreases. Therefore, it takes a long time for the fine particle aggregate 27a to pass through the primary particle forming mechanism 60A, and the number of collisions with the first electrodes 61-1 to 61-3 and the second electrodes 62-1 to 62-3 can be increased. Therefore, primary particle formation of the fine particle aggregate 27a can be promoted. As a result, an AD film with higher density and higher film adhesion can be formed.

  Next, Example 1 according to the first embodiment, Example 2 according to the second embodiment, and a comparative example not according to the present invention will be described.

[Example 1]
In Example 1, film formation was performed using the AD film formation apparatus according to the first embodiment shown in FIGS. 1 and 2.

First, as a pretreatment, BaTiO ₃ powder having an average particle size of 0.5 μm is placed in an aerosol generator container, the powder is heated to 150 ° C., and ultrasonic waves are applied to the entire container for 30 minutes by an exhaust system. The inside was evacuated and the BaTiO ₃ powder was dried. Further, the film forming chamber was evacuated in advance, and the degree of vacuum was set to 10 Pa or less.

Next, oxygen gas (purity: 99.9%, gas pressure: 2 kg / cm ² , gas flow rate: 4 l / min) was introduced into the container from the BaTiO ₃ powder thus obtained to form an aerosol.

  The aerosol obtained in this way was converted into primary particles of fine particles contained in the aerosol using the primary particle formation mechanism 30 shown in FIG. In addition, the diameter of the 1st barrier plate 31 and the 2nd barrier plate 32 was set to 10 mm, the diameter of each opening part 31a, 31b was set to 2 mm, and the distance of the 1st barrier plate 31 and the 2nd barrier plate 32 was set to 20 mm.

The aerosol thus obtained was sprayed from the spray nozzle toward the glass substrate for 20 minutes to form a BaTiO ₃ film having a thickness of 20 μm.

  During the film formation, the aerosol concentration was 8% by volume, and the variation in the aerosol concentration was 2%. Further, the pressure in the film formation chamber during film formation was 200 Pa, and the film formation rate was 1 μm / min ± 0.2 μm / min. The aerosol concentration and the variation in the aerosol concentration were measured using a laser type particle counter.

[Example 2]
In Example 2, film formation was performed using the AD film formation apparatus according to the second embodiment shown in FIGS. 1 and 6.

The pretreatment was carried out in the same manner as in Example 1, and BaTiO ₃ powder having an average particle size of 0.5 μm using oxygen gas (purity: 99.9%, gas pressure: 2 kg / cm ² , gas flow rate: 4 l / min). An aerosol was formed.

  The aerosol obtained in this manner is used to form an alternating electric field having a maximum electric field strength of 10 MV / m between the first electrode 61 and the second electrode 62 using the primary particle formation mechanism 60 shown in FIG. The fine particles were made primary particles. The length of the first electrode 61 and the second electrode 62 in the flow direction is set to 50 mm, the width is set to 10 mm, and the velocity of the aerosol passing between the first electrode 61 and the second electrode 62 is 100 m / s. did.

The aerosol thus obtained was sprayed from the spray nozzle toward the glass substrate for 20 minutes to form a BaTiO ₃ film having a thickness of 20 μm.

  During the film formation, the aerosol concentration was 5% by volume, and the variation in the aerosol concentration was 1%. Further, the pressure in the film formation chamber during film formation was 200 Pa, and the film formation rate was 1 μm / min ± 0.5 μm / min.

[Comparative example]
In the comparative example not according to the present invention, the primary particle formation mechanism was not provided in Example 1, but film formation was performed in the same manner as in Example 1 using an AD film formation apparatus having the same configuration.

  During the film formation, the aerosol concentration was 10% by volume, and the variation in the aerosol concentration was 4%. Further, the pressure in the film formation chamber during film formation was 200 Pa, and the film formation rate was 1 μm / min ± 0.5 μm / min.

FIG. 8 is a characteristic diagram of BaTiO ₃ films of Examples and Comparative Examples. Referring to FIG. 8, the water absorption rate indicating the denseness of the film was better for the BaTiO ₃ films of Example 1 and Example 2 than for the comparative example. In the relative dielectric constant showing more microscopic denseness, both Example 1 and Example 2 were higher than Comparative Example 200. From these facts, it can be seen that the BaTiO ₃ films of Example 1 and Example 2 are formed more densely than the comparative example.

Further, it can be seen that the dielectric loss tan δ is reduced in the BaTiO ₃ film of Example 2 as compared with the comparative example. Therefore, if the BaTiO ₃ film is not sufficiently densified, it becomes conductive due to moisture adhering to the particle surface, and as a result, the dielectric loss increases. However, since the dielectric loss of the BaTiO ₃ film of Example 2 is reduced, it can be seen that the BaTiO ₃ film is densified.

Further, the adhesion strength between the BaTiO ₃ film and the glass substrate (film-substrate adhesion strength) is 3 kg / mm ² or more of the comparative example, whereas the BaTiO ₃ films of Example 1 and Example 2 are 5 kg / mm. ^2. It can be seen that the adhesion hardness between the film and the substrate is improved.

The surface roughness reflects the denseness of the BaTiO ₃ film and the generation of vacancies in the surface or film, and the smaller the surface roughness, the better. As shown in FIG. 8, the surface roughness of Example 1 and Example 2 is reduced compared to the comparative example. Further, the maximum pore diameter on the surface of the BaTiO ₃ film is reduced in Example 1 and Example 2, and particularly in Example 2 as compared with the comparative example. From these facts, it can be seen that the BaTiO ₃ films of Examples 1 and 2 have improved film density and suppressed generation of vacancies.

As described above, according to Example 1, Example 2, and the comparative example, it can be seen that the BaTiO ₃ film having finer and less voids can be formed in Example 1 and Example 2 than in the comparative example. In particular, it can be seen that a better quality BaTiO ₃ film was formed in Example 2 than in Example 1.

The water absorption was determined by immersing the substrate on which the BaTiO ₃ film was formed in water for 1 hour, and dividing the difference in mass before and after that by the mass of the film.

The relative dielectric constant and tan δ (dielectric loss) are as follows: a lower electrode is provided on a glass substrate, a BaTiO ₃ film and an upper electrode are formed thereon, and a high frequency of 100 MHz is applied to the BaTiO ₃ film via the lower electrode and the upper electrode. A voltage was applied and measured. Tanδ was measured using a network analyzer using the perturbation method.

Further, the film-substrate adhesion strength of the BaTiO ₃ film to the glass substrate was measured using the Sebastian method. In the Sebastian method, a glass substrate on which a BaTiO ₃ film is formed is fixed, and an adhesion tester is fixed to the surface of the BaTiO ₃ film with an adhesive. The adhesion tester is pulled up, and the strength of the adhesion tester (kg / mm ² ) per unit area when the BaTiO ₃ film is peeled from the glass substrate is used as an index of adhesion. It shows that adhesiveness is so large that is large.

The surface roughness of the BaTiO ₃ film was measured by a stylus method, and the maximum surface pore diameter was measured by surface observation with a scanning electron microscope (SEM).

  The preferred embodiments of the present invention have been described in detail above, but the present invention is not limited to the specific embodiments, and various modifications and changes can be made within the scope of the present invention described in the claims. It can be changed.

In addition, the following additional notes are disclosed regarding the above description.
(Additional remark 1) The aerosol formation means which forms the aerosol which consists of microparticles | fine-particles which consist of inorganic materials, and carrier gas,
A film forming means for forming an inorganic material film on a substrate by spraying the aerosol through a spray nozzle;
An aerosol deposition film forming apparatus comprising primary particle forming means for dispersing fine particles contained in the aerosol between the aerosol forming means and the film forming means.
(Additional remark 2) The said primary particle-izing means consists of a barrier part arrange | positioned in the flow path of aerosol,
2. The aerosol deposition film forming apparatus according to appendix 1, wherein fine particles contained in the aerosol collide with the barrier portion and are dispersed.
(Additional remark 3) The said primary particle-izing means consists of the 1st barrier member arrange | positioned in the flow path of aerosol, and the 2nd barrier member arrange | positioned in the downstream,
3. The aerosol deposition film forming apparatus according to appendix 2, wherein openings for allowing aerosol to pass are respectively provided in a part of the first barrier member and the second barrier member.
(Supplementary Note 4) The first barrier member and the second barrier member are provided to face each other,
4. The aerosol deposition film forming apparatus according to claim 3, wherein the opening of the first barrier plate and the opening of the second barrier plate are provided at positions that do not face each other.
(Additional remark 5) The said primary particle-izing means consists of the 1st barrier member arrange | positioned in the flow path of aerosol, and the 2nd barrier member arrange | positioned in the downstream,
The first barrier member is fixed to one side of the inner wall that defines the flow path and opens to the other side, and the second barrier member is fixed to the other side and opens to the one side. The aerosol deposition film-forming apparatus according to appendix 2, characterized in that:
(Supplementary note 6) The aerosol deposition according to supplementary note 5, wherein the first barrier member and the second barrier member are formed such that respective upstream surfaces are inclined from upstream to downstream. Deposition device.
(Additional remark 7) The said primary particle-izing means consists of a nozzle part and the 3rd barrier member arrange | positioned in the downstream,
The nozzle part has a tapered nozzle flow path whose opening area decreases toward the downstream,
The third barrier member is disposed in the vicinity of the opening on the downstream side of the nozzle flow path, has another opening at a position not facing the opening, and prevents the aerosol flowing out from the nozzle flow path. The aerosol deposition film-forming apparatus according to appendix 2, wherein the contained fine particles collide with the third barrier member.
(Supplementary Note 8) The primary particle forming means includes a first small flow path and a second small flow path formed by branching an aerosol flow, and a first small flow path and a second small flow path on the downstream side thereof. The flow path intersects each other, and the fine particles contained in the aerosol flowing through the first small flow path and the fine particles contained in the aerosol flowing through the second small flow path collide with each other. 2. The aerosol deposition film forming apparatus according to appendix 1, wherein the aerosol deposition film forming apparatus is dispersed.
(Supplementary Note 9) The primary particle forming means includes a pair of electrodes provided in an aerosol flow path, and an AC power source that applies an AC voltage between the pair of electrodes.
2. The aerosol deposition film forming apparatus according to claim 1, wherein the fine particles contained in the aerosol are charged, and the fine particles are dispersed by colliding with the electrode by an electric attractive force.
(Additional remark 10) The said electrode is arrange | positioned along the flow direction of aerosol, and a voltage is applied to the direction orthogonal to this flow direction, The aerosol deposition film-forming apparatus of Additional remark 9 characterized by the above-mentioned.
(Supplementary note 11) The aerosol deposition film forming apparatus according to supplementary note 10, wherein each of the pair of electrodes has a flat plate shape and is arranged in parallel to each other.
(Supplementary note 12) The aerosol deposition film forming apparatus according to supplementary note 11, wherein the primary particle forming means includes a plurality of pairs of electrodes arranged in a direction substantially orthogonal to the flow direction.
(Supplementary note 13) The aerosol deposition film forming apparatus according to supplementary note 12, wherein the primary particle forming means is provided in a flow path having a larger cross-sectional area than the flow path from the aerosol forming means.

1 is a schematic configuration diagram of an aerosol deposition film forming apparatus according to a first embodiment of the present invention. It is a block diagram of the primary particle formation mechanism which comprises the aerosol deposition film-forming apparatus which concerns on 1st Embodiment. It is a block diagram of the 1st modification of the primary particle formation mechanism which comprises the aerosol deposition film-forming apparatus which concerns on 1st Embodiment. It is a block diagram of the 2nd modification of the primary particle formation mechanism which comprises the aerosol deposition film-forming apparatus which concerns on 1st Embodiment. It is a block diagram of the 3rd modification of the primary particle formation mechanism which comprises the aerosol deposition film-forming apparatus which concerns on 1st Embodiment. It is a block diagram of the primary particle formation mechanism which comprises the aerosol deposition film-forming apparatus which concerns on the 2nd Embodiment of this invention. It is a block diagram of the modification of the primary particle formation mechanism which comprises the aerosol deposition film-forming apparatus which concerns on 2nd Embodiment. It is a characteristic diagram of BaTiO ₃ films of Examples and Comparative Examples.

Explanation of symbols

10 Aerosol deposition film forming equipment (AD film forming equipment)
20 Aerosol formation part 21 Aerosol generator 27 Fine particles 27a Fine particle aggregate 27b Fine particles formed into primary particles 29 Aerosol 30, 30A, 30B, 30C, 60, 60A Primary particle formation mechanism 31 First barrier plate 31a, 32a, 38a Opening 31b, 32b Upstream surface 31c Downstream surface 32 Second barrier plate 34-1 to 34-4 Barrier member 36 Nozzle portion 36a Tapered flow channel 36b Flow channel 36c Downstream surface 38, 39 Barrier plate 38b Upstream surface 39a First Flow path 39b Second flow path 39c Merge section 39d Third flow path 40 Film formation section 41 Film formation chamber 42 Injection nozzle 43 Substrate 44 Substrate holder 45 XYZ stage 46 Aero deposition film (AD film)
61, 61-1 to 61-3 1st electrode 62, 62-1 to 62-3 2nd electrode 63 AC power supply 64 Grounding 65-1 to 65-5 Flow path

Claims (5)

Aerosol forming means for forming an aerosol made of fine particles made of an inorganic material and a carrier gas;
A film forming means for forming an inorganic material film on a substrate by spraying the aerosol through a spray nozzle;
A primary particle forming means for dispersing fine particles contained in the aerosol between the aerosol forming means and the film forming means ,
The primary particle forming means comprises a barrier portion disposed in the aerosol flow path, and collides and disperses the fine particles contained in the aerosol against the barrier portion,
The primary particle forming means includes a first barrier member disposed in the aerosol flow path and a second barrier member disposed downstream thereof,
The first part of the barrier member and the second barrier members, aerosol deposition film forming device you wherein an opening for passing the aerosol is respectively provided. The primary particle forming means includes a nozzle portion and a third barrier member disposed on the downstream side thereof,
The nozzle part has a tapered nozzle flow path whose opening area decreases toward the downstream,
The third barrier member is disposed in the vicinity of the opening on the downstream side of the nozzle flow path, has another opening at a position not facing the opening, and prevents the aerosol flowing out from the nozzle flow path. aerosol deposition film forming apparatus of particles contained claim 1, wherein the impinging on the third barrier member. The first barrier member and the second barrier member are provided to face each other;
2. The aerosol deposition film forming apparatus according to claim 1, wherein the opening of the first barrier plate and the opening of the second barrier plate are provided at positions that do not face each other. The first barrier member is fixed to one side of the inner wall that defines the flow path and opens to the other side, and the second barrier member is fixed to the other side and opens to the one side. And
2. The aerosol deposition film forming apparatus according to claim 1, wherein each of the first barrier member and the second barrier member is formed such that an upstream surface of each of the first barrier member and the second barrier member is inclined from upstream to downstream. . Aerosol forming means for forming an aerosol made of fine particles made of an inorganic material and a carrier gas;
A film forming means for forming an inorganic material film on a substrate by spraying the aerosol through a spray nozzle;
A primary particle forming means for dispersing fine particles contained in the aerosol between the aerosol forming means and the film forming means,
The primary particle forming means comprises a pair of electrodes provided in the aerosol flow path, and an AC power source for applying an AC voltage between the pair of electrodes,
The aerosol particles charges the included, the electrode characteristics and to Rue allo sol a deposition film forming device to disperse particles by colliding with electrical attraction.

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