KR20190141027A - Device manufacturing method - Google Patents

Abstract

Provided are a substrate processing apparatus and a device manufacturing method capable of forming a fine pattern on a substrate with high accuracy. A functional layer (coupling agent) having a difference in hydrophilicity due to light energy is applied onto the substrate, and light patterning is performed to impart contrast to the functional layer in hydrophilicity, and then includes a raw material material for an electronic device or the like. By misting the solution with ultrasonic waves or the like and spraying the surface of the substrate, mist is adhered to the lyophilic portion having a high surface energy in the substrate surface to selectively deposit the raw material material.

Description

Device manufacturing method {DEVICE MANUFACTURING METHOD}

The present invention relates to a device manufacturing method, a substrate processing method and a film forming apparatus by mist.

In a large screen display element (display panel) such as a liquid crystal display element, a transparent electrode layer such as ITO, a semiconductor material layer such as Si, an insulating film layer, or a metal film layer for wiring is deposited on a flat glass substrate. The resist is coated to transfer the circuit pattern, and after the transfer, the photoresist is developed and then etched to form a circuit pattern. By the way, since a glass substrate enlarges with the big screen of a display element, the conveyance apparatus and processing apparatus of a board | substrate also enlarged, and there existed a problem that a manufacturing line (factory) enlarges. Accordingly, a roll-to-roll method of directly forming a display element on a flexible substrate (for example, a film member such as polyimide, PET, metal foil, or a very thin glass sheet material) (hereinafter, The technique called simply "roll system" is proposed (for example, refer patent document 1).

When processing a flexible film member by a roll system, compared with the conventional production method, the amount of use of various materials related to manufacture, the amount of use of various powers (electric power, pneumatic, refrigerant, etc.) are reduced, and the environment is reduced. There is a desire for an additive manufacturing method with less load. The manufacturing method disclosed in Patent Document 1 also uses a lithography method using a conventional photoresist, and a manufacturing method by an inkjet method in which a necessary material is deposited only on a necessary part when fine patterning such as TFT (thin film transistor) or wiring is performed. Main subject is.

Patent Literature 2 discloses a self-organizing monomolecular film (SAM layer) uniformly when a conductive ink material is selectively coated on a film material by such an inkjet method to form an electrode layer or a wiring layer. A method of coating an ink material after irradiating patterned ultraviolet rays corresponding to the shape of an electrode or a wiring to modify the wettability (hydrophilic liquid property) of the surface of the SAM layer is disclosed. have.

In addition, Patent Document 3 discloses a method of applying and patterning a mist of a material solution to be formed on a substrate via a shadow mask as a method that can expect high productivity. have. In this patent document 3, similar to the inkjet method, the surface of the substrate is previously given a contrast by lyophilic and liquid-repellent, and then a shadow mask is superimposed on the substrate to form a pattern. It is also disclosed, and in the experimental example, the opening pattern of 0.5 mm x 12 mm on the shadow mask is formed in the same dimension on the board | substrate.

Patent Document 1: International Publication No. WO 2008/129819 pamphlet Patent Document 2: International Publication No. WO 2010/001537 Pamphlet Patent Document 3: Japanese Patent No. 4387775

However, in the inkjet method, functional materials such as nano-ink conductive materials are selectively applied to designated areas on the substrate as small droplets from the ink discharge head, so that the pattern size (line width) is used. Or dot) is small, for example, 20 µm or less, due to the poor accuracy of the impact of the ink droplets from the head, resulting in contrast due to lyophilic and liquid repellency on the substrate. There is a problem that it is difficult to make clean patterning even when the ink concentrates on the hydrophilic part. Of course, considering the ink ejecting head or the ink material, it is also possible to consider reducing the amount of ink droplets ejected at once from the nozzle of the head, but there is a problem that the productivity is significantly lowered.

On the other hand, in the method disclosed in Patent Document 3, since the shadow masks are arranged at intervals with respect to the substrate, there is a problem that the pattern size formed on the substrate is generally larger than the opening pattern on the shadow mask. In patent document 3, since the large pattern of 500 micrometers x 1200 micrometers is transferred, even if a pattern edge is about 5 micrometers or about 10 micrometers thick, there is little influence. However, in the case of a fine pattern of 20 μm or less, it is a big problem that the pattern edge is also thick about 5 μm or 10 μm, and when a plurality of such fine patterns are adjacent to each other, the patterns of neighbors are connected. Problems arise.

Furthermore, even when a lipophilic and liquid-repellent contrast is given to the surface of the substrate and a shadow mask is used in combination, a relative alignment error between the shadow mask and the hydrophilic liquid-treated substrate is generated. Limited by In addition, preparation was required to uniformly form a liquid repellent layer made of a liquid repellent material on the surface of the lyophilic substrate in advance, and selectively remove and pattern the liquid repellent layer using a photolithography technique. In addition to this, there is a problem that it is difficult to produce a line pattern or a contact hole (via hole) pattern having a fine line width of 20 μm or less as a shadow mask itself.

This invention is made | formed in view of the above, and provides the device manufacturing method, board | substrate processing method, and film-forming apparatus by mist which can refine | miniaturize and form the electronic device material substance on board | substrates, such as a film, with high precision. It aims to do it.

In the first aspect of the present invention, as a device manufacturing method for forming an electronic device on the surface of a substrate, while having a fluorine group having a liquid repellency in nitro benzyl, the irradiation of light energy of ultraviolet rays having a wavelength of 400 nm or less A functional layer forming step of forming a functional layer on the surface of the substrate by a photosensitive hydrophilic liquid coupling agent wherein the bond of the fluorine group is broken by the hydrophilic liquid and the hydrophilic liquid is modified. And the ultraviolet rays patterned on the functional layer on the substrate by any one of an exposure machine, a maskless exposure machine, and a beam scanning type drawing machine which project the pattern of the mask by the projection optical system. By irradiating light energy of the functional layer to form a region in which the fluorine group is separated and a region in which the fluorine group is left, resulting in contrast due to hydrophilic liquidity in the functional layer. The optical patterning process which produces | generates the pattern which attached | subjected) and the said board | substrate processed by the said optical patterning process are conveyed continuously along a predetermined conveyance direction by a conveyance mechanism, and the said board | substrate has a predetermined length with respect to the said conveyance direction A surface in which the functional layer of the substrate is formed in the chamber mechanism with a gas mixed with a predetermined carrier gas as a mist as a functional solution containing molecules or particles of material material for the electronic device while passing through the chamber mechanism. A device including a mist deposition step of spraying so as to be followed, and an adjusting step of measuring the state of the layer by the deposited material material by a measuring device, and adjusting the conditions of the mist deposition step based on the measurement result. It is provided to a manufacturing method.

According to the second aspect of the present invention, as a substrate processing method for forming an electronic device on the surface of a substrate, hydrophilic liquid property is modified by irradiation of light energy of ultraviolet rays having a wavelength of 400 nm or less. The functional layer forming process which forms the functional layer by the photosensitive hydrophilic fluid coupling agent which becomes into the surface of the said board | substrate, and was patterned corresponding to the said electronic device by the exposure machine or the drawing machine. An optical patterning step of irradiating the optical energy of the ultraviolet light to the functional layer on the substrate to impart contrast to the functional layer by the hydrophilicity according to the pattern, and the contrast provided by the hydrophilicity The said board | substrate is continuously conveyed along a predetermined conveyance direction by a conveyance mechanism, and the said board | substrate is made to pass through the chamber provided with a predetermined length with respect to a conveyance direction. And a mist deposition process of spraying a gas, which mists a functional solution containing molecules or particles of a material material for the device, to flow along the surface in which the functional layer of the substrate is formed in the chamber. Is provided.

According to a third aspect of the present invention, there is provided a film forming apparatus by mist, which sprays a gas containing mist onto the surface of a substrate, deposits particles contained in the mist on the surface of the substrate, and forms the film on the surface as the substrate. And a conveying mechanism for continuously moving the substrate on which the lyophilic portion is formed at a predetermined conveying speed, the substrate passing through a predetermined length along the conveying direction, and a material material for the electronic device. There is provided a film forming apparatus by a mist including a chamber for spraying a gas misting a functional solution containing molecules or particles along a surface of the substrate at a flow rate adjusted according to the conveying speed.

In the present invention, it is possible to form a fine pattern on a substrate with higher precision than a printing method or an inkjet method, and to easily form a thin film layer made of a material to be selectively patterned with a uniform thickness. do.

1 is a diagram illustrating a schematic configuration of a substrate processing apparatus according to a first embodiment.
FIG. 2 is a diagram showing the chemical structure of a photosensitive silane coupling agent deposited on a substrate.
3 is a diagram illustrating an example of a pixel circuit of an active matrix display.
4A is a plan view illustrating a transistor structure of the pixel circuit of FIG. 3.
FIG. 4B is a sectional view seen from the arrow 4B-4B in FIG. 4A.
FIG. 5: is a figure which shows the whole structure of the substrate processing apparatus which concerns on 2nd Embodiment.
FIG. 6: is a figure which shows the structure of a part of unit of the substrate processing apparatus by 3rd Embodiment.
It is a figure which shows the various patterns formed on the sheet | seat as a to-be-processed substrate.
8 is a diagram illustrating a configuration of a part of units of the substrate processing apparatus according to the fourth embodiment.

(1st embodiment)

EMBODIMENT OF THE INVENTION Hereinafter, 1st Embodiment of the substrate processing apparatus of this invention is described with reference to FIGS. 1 shows a schematic overall configuration of a substrate processing apparatus, and in the present embodiment, the flexible substrate P supplied from the supply roll FR1 is typically provided to four processing units U1, U2, U3, and U4. After sending in order, it is set as the structure wound up by collection | recovery roll FR2, and while the board | substrate P is sent from supply roll RF1 to collection | recovery roll RF2, the fine pattern by a functional material is carried out on the board | substrate P. Precisely formed.

The processing unit (functional layer forming unit) U1 includes, for example, a transfer drum Gpa for printing and the like, and a silane couple having a fluorine group having a liquid repellency in a photosensitive hydrophilic coupling agent, for example, nitrobenzyl. The ring agent is uniformly applied to at least the entire pattern formation region of the surface of the substrate P. FIG. In addition, since a pattern is not usually formed on the back surface of the substrate P, the transfer drum Gpb is formed on the back surface of the substrate P so that unnecessary deposition does not occur in the mist deposition in the later step. A water repellent film may be coated.

The photosensitive silane coupling agent (photosensitive SAM) used by this embodiment is comprised by the chemical formula as shown in FIG. 2 as an example, The detail is, for example, an independent administrative corporation and a science on June 19, 2009. Article 1: Presented at the "New Technology Briefing" held by the Technology Promotion Organization: "Cell Patterning Technology by Near-Ultraviolet Light Using Surface Modifier", or Japanese Patent Application Publication No. 2003-321479, Japanese Patent Publication 2008- 050321 is disclosed.

In FIG. 2, when the silane coupling agent which has a fluorine group apply | coated to the surface of the board | substrate P dries a solvent after application | coating, the surface becomes the liquid-repellent area | region HPB which has a fluorine group. When the surface is irradiated with UV light for patterning for a predetermined time at a predetermined illuminance, the bonding of the fluorine group is decreased, and the portion thereof becomes relatively liquid-repellent and becomes a lyophilic region (HPR). In the experimental example shown in Japanese Patent Laid-Open No. 2008-050321, the contact angle in the unirradiated region of ultraviolet rays on the surface of the substrate was 110 ° (water repellent), and the substrate was washed with an aqueous solution of tetramethyl ammonium hydroxide (TMAH) after ultraviolet irradiation. Thereby, it is disclosed that the contact angle of the area | region which received the ultraviolet irradiation was reduced (change to lyophilic) about 20 degrees.

By the way, the board | substrate P with which the coupling agent was apply | coated is sent to processing unit U3 (patterning part) after fully drying (heat-processing to 200 degrees or less) in next processing unit U2, and here, a pattern The predetermined amount of light energy of the ultraviolet-ray is irradiated to the layer (functional layer) by the coupling agent of the surface of the board | substrate P. The processing unit U3 includes a drum mask DM in which a mask for fine patterns is formed, a light source in an ultraviolet region (wavelength of 400 nm or less), an illumination system IU for irradiating the drum mask DM with illumination light of ultraviolet rays, The projection optical system PL etc. which image the ultraviolet-ray patterned by the drum mask DM on the board | substrate P are provided. The processing unit U3 is a stepper type or a scanning type exposure apparatus, but may be a maskless exposure machine using a beam scan type drawing machine, a DMD, or the like.

As shown in FIG. 2, immediately after apply | coating the photosensitive silane coupling agent to the surface of the board | substrate P, and drying, the fluorine group which has liquid repellency couple | bonds with nitro benzyl, and the part becomes liquid repellency area | region (HPB). However, when ultraviolet UV light is irradiated with a predetermined amount of energy, the nitrobenzyl group in the irradiated portion reacts, and the bond of the fluorine group is reduced, and the liquid repellency of the portion is lowered to become the lyophilic region (HPR). In other words, the light pattern generated by the drum mask DM is transferred as a pattern forming contrast on the substrate P with a difference in hydrophilicity.

In addition, in order to remove the fluorine group in which bonds were separated from the surface of the substrate P, the substrate P exposed by the processing unit U3 was washed with TMAH as disclosed in Japanese Patent Laid-Open No. 2008-050321. It is preferable to dry. For this purpose, between the processing unit U3 and the processing unit U4, the washing tank by TMAH, the washing tank by pure water, a drying part, etc. are provided.

The board | substrate P which received the exposure process (or the washing | cleaning and drying process) is then sent to the processing unit (mist deposition part) U4. In the processing unit U4, a so-called film deposition method called mist deposition is applied, but the principle device configuration for this is disclosed in, for example, Japanese Patent Laid-Open No. 2005-307238, and the mist deposition method is described. Experimental example in which a thin film of zinc oxide (ZnO) was deposited is described in Paper 2: Kyoto University Publication, "A Study on the Mist CVD Method and Its Application to Zinc Oxide Thin Film Growth" (March 24, 2008 issuance) [URI: http://hdl.handle.net/2433/57270].

In the processing unit U4, the atomizer which mist-forms the liquid (functional solution) containing the molecule | numerator and particle | grains of the raw material material which should be deposited on the lyophilic region HPR of the board | substrate P with an ultrasonic vibrator. GS1, a gas supply unit GS2 for supplying a carrier gas such as nitrogen, argon, or air at a predetermined flow rate, a mixer (ULW) for mixing mist of the functional solution with the carrier gas at a predetermined concentration; The reaction chamber TC which makes the mixed gas contact the surface of the board | substrate P at a predetermined | prescribed flow rate, and the recovery port part De which collect | recovers the gas in the chamber TC are provided.

As the raw material material, a solution containing a molecule or carbon nanotube, which is an oxide semiconductor or an organic semiconductor, an electrode or wiring solution containing metal nanoparticles, or a solution having a molecular structure that is an insulating film is selected. When zinc oxide (ZnO) is selected as the raw material, as disclosed in the preceding article 2, ZnAc ₂ , 98% H ₂ O solution is supplied to the atomizer GS1, and the internal 2.4 MHz ultrasonic vibrator By this, the ZnAc ₂ solution is misted. The mist is introduced into the reaction chamber TC together with the carrier gas, and selectively into the lyophilic region HPR on the surface of the substrate P traveling at a constant speed in the chamber TC. Mist) is captured.

The substrate P subjected to the mist deposition treatment in the processing unit U4 is sent to a drying (heating) unit or the like not shown, and the raw material substance deposited on the lyophilic region HPR on the surface of the substrate P. The solvent component and the like are removed from the mixture, and then sent to a downstream treatment step, and then wound around the recovery roll FR2 after a suitable treatment step. Thus, on the board | substrate P which passed the processing unit U4, the thin film layer by a raw material material is deposited as a pattern of the shape along the lyophilic region HPR.

By the way, in the active matrix display panel AMOLED which uses an organic EL as a light emitter, a pixel circuit by a thin film transistor TFT as shown in FIG. 3 is provided for each pixel (sub pixel). In Fig. 3, the light emitting diode OLED as the organic EL element is driven by two of the pixel switching transistor TR1 and the current driving transistor TR2. The luminance signal Yc corresponding to the pixel is applied to the drain electrode D1 of the transistor TR1, and a synchronous clock pulse applied to the gate electrode G1 of the transistor TR1 ( In response to Hcc, the transistor TR1 is turned on / off.

When the transistor TR1 is turned on, the voltage level of the luminance signal Yc is maintained at the capacitor Cg and is applied to the gate electrode G2 of the transistor TR2. The transistor TR2 performs voltage / current conversion that causes a drive current corresponding to the voltage applied to the gate electrode G2 to flow from the drain electrode D2 to the source electrode S2. As a result, the current corresponding to the luminance signal Yc is supplied to the light emitting diode OLED from the power supply bus line Vdd, and the light emitting diode OLED emits light with the luminance corresponding to the magnitude of the current.

Such a pixel circuit is configured as shown in Figs. 4A and 4B, for example. FIG. 4A shows a planar arrangement of only the transistors TR1 and TR2 in one pixel circuit, and FIG. 4B is a cross section seen from the arrow 4B-4B in FIG. 4A. 4A and 4B are bottom-gate-type transistors. First, a printing method using conductive ink or the like is formed in a recess formed on the upper surface of the substrate P by an imprint method or the like. Gate electrodes G1 and G2 are formed by an electroless plating method or the like. Next, as shown in FIG. 4B, the gate insulating film Is is laminated, but here, instead of the entire surface of the substrate P, the source electrode S1 and the transistor TR2 of the transistor TR1 are formed. An opening HA for electrically connecting the gate electrode G2 is formed by a selective deposition method such as a printing method or an inkjet method so as to be formed between the transistor TR1 and the transistor TR2. In addition, the layer of the gate electrode may be formed by a mist deposition method.

On the insulating film Is, the semiconductor layer MS made of an organic type, an oxide type, or a carbon nanotube or the like provided as a solution is selectively deposited in correspondence with the formation region of each transistor by a printing method, an inkjet method, or the like. After the low temperature annealing or the like (200 ° C. or less) for crystallization (orientation) of the semiconductor layer MS is completed, a conductive ink or the like is used to correspond to the drain electrodes D1 and D2 and the source electrodes S1 and S2. The pattern is coated. At this time, in the opening HA of the insulating film Is, the gate electrode G2 of the transistor TR2 is exposed, and a pattern corresponding to the source electrode S1 of the transistor TR1 is coated with conductive ink or the like. At this time, the source electrode S1 and the gate electrode G2 are connected in the opening HA.

In the pixel circuit constituted as described above, the process according to the present embodiment is, for example, a process of forming the gate electrodes G1 and G2, a process of forming the semiconductor layer MS, or the drain electrodes D1 and D2. ) And the source electrodes S1, S2. However, in the thin film formation by the mist deposition method, the mist size at the time of misting the solution containing a raw material substance, the density | concentration of the raw material substance contained in mist, and the density | concentration of the mist in a carrier gas (henceforth generically, "mist concentration" ), The flow rate of the carrier gas, the temperature in the reaction chamber TC, and the like are preferably optimized for the size of the pattern to be formed.

In this embodiment, in order to form efficiently the fine pattern similar to the conventional photolithography method by the mist deposition method, the material (silane coupling agent) which changes lyophilic and liquid repellent by photosensitive on the board | substrate P Is applied and fine patterned light is irradiated onto the substrate P to form a high precision pattern having hydrophilic contrast. Therefore, since the surface energy becomes high in the surface of the board | substrate P with the high lyophilic region HPR compared with the area | region HPB with high liquid repellency, it is easy for a mist to adhere and the selective of a raw material material Deposition becomes possible.

Here, the surface energy of the high liquid-repellent region (HPB) is Epb, the surface energy of the high lyophilic region (HPR) is Epr, the surface energy of the solvent of the mist is Eem, the mist diameter is Φm, and the dimension of the pattern to be formed. When (minimum line width, etc.) is ΔDp, it is set to a relationship that satisfies any one or both of the following relations I and II.

Relationship I: Surface energy Epb <Eem <Epr

Relationship II: Mist size (diameter) 0.2 · ΔDp <Φm <ΔDp

When the mist diameter Φm is larger than the minimum line width ΔDp to be patterned, the mist is protruded and adhered to the high lyophilic region HPR (line width ΔDp), but the mist is large due to its surface energy. It grows in mist and may protrude from the area | region HPR with high lipophilicity, and may flow. Therefore, a mist diameter too large than the pattern dimension (DELTA) Dp which should be formed is not preferable. If too small, the deposition time for pattern formation is too long, resulting in a decrease in productivity.

As an example, in the pixel circuit shown in FIGS. 4A and 4B, the pattern line width of the drain and source electrodes constituting the transistors TR1 and TR2 is about 20 μm, the pattern line width of the gate electrode is about 6 μm, and the semiconductor layer MS ), When the gate electrode is formed by the mist deposition method, the mist size Φ m is 1.2 µm <φm <6 µm, and the semiconductor layer MS is subjected to the mist deposition method. The mist size phi m at the time of forming is set to 6 탆 <phi m <30 탆. In addition, the electrode (wiring) layer, semiconductor layer, insulating film, etc. for forming a TFT have different optimum thicknesses in terms of electrical performance, so that the mist concentration in the reaction chamber TC is changed depending on the thickness of the pattern to be deposited. The adjustment of the conveyance speed of the board | substrate P, the flow rate of mist gas, the temperature in reaction chamber TC, etc. is necessary.

The process shown in FIG. 1 is for forming one layer by the mist deposition method, and in order to form some layers of the device which has many layer structures by the mist deposition method, the processing unit (U1) in FIG. The set of ˜U4) may be serially connected by the number of layers, and the substrate P may be conveyed in sequence.

(2nd embodiment)

Next, the device manufacturing system which embodied the said substrate processing apparatus is demonstrated with reference to FIG. FIG. 5: is a figure which shows the structure of a part of device manufacturing system (flexible device manufacturing line). The flexible substrate P (sheet, film, etc.) withdrawn from the supply roll FR1, in turn, passes through n processing apparatuses U1, U2, U3, U4, U5, ..., Un, and the recovery roll FR2. The example until it is wound up is shown. The upper control device 5 collectively controls the respective processing devices U1 to Un that constitute the production line.

In FIG. 5, the rectangular coordinate system XYZ is set so that the surface (or back surface) of the board | substrate P may become perpendicular to an XZ plane, and the width direction orthogonal to the conveyance direction (long direction) of the board | substrate P is carried out. It is assumed that it is set in the Y direction. In addition, the substrate P is subjected to a predetermined pretreatment in advance and subjected to surface modification for strengthening the deposition of the photosensitive silane coupling agent, or a fine partition structure (concave-convex structure) for precision patterning on the surface. It may be formed.

Although the board | substrate P wound around the feed roll FR1 is pulled out by the nip drive roller DR1 and conveyed to the processing apparatus U1, the center of the Y direction (width direction) of the board | substrate P is carried out. Is controlled by the edge position controller EPC1 so as to fall within a range of about ± several tens of micrometers to several tens of micrometers with respect to the target position.

Processing apparatus U1 is a coating apparatus which apply | coats a photosensitive functional liquid (photosensitive silane coupling agent) to the surface of the board | substrate P continuously or selectively about the conveyance direction (long direction) of the board | substrate P by a printing system. . In the processing apparatus U1, the cylinder roller DR2 by which the board | substrate P is wound, the coating roller for uniformly apply | coating the photosensitive functional liquid on the surface of the board | substrate P on this cylinder roller DR2, or An application mechanism Gp1 including a printing plate body roller for patterning and applying the photosensitive functional liquid, and a drier for rapidly removing a solvent or water contained in the photosensitive functional liquid applied to the substrate P. Gp2) etc. are provided.

The processing apparatus U2 heats the board | substrate P conveyed from the processing apparatus U1 to predetermined temperature (for example, about several 10-120 degreeC), and makes the photosensitive functional layer apply | coated to the surface stable. It is a heating device. In the processing apparatus U2, a plurality of rollers and air turn bars for returning and conveying the substrate P, a heating chamber portion HA1 for heating the substrate P brought in, and heated The cooling chamber part HA2, the nip drive roller DR3, etc. for reducing the temperature of the board | substrate P so that it may match with the environmental temperature of a post process (processing apparatus U3) are provided.

The processing apparatus U3 which performs patterning is an exposure apparatus which irradiates the patterning light of the ultraviolet-ray corresponding to the display circuit pattern and wiring pattern with respect to the photosensitive functional layer of the board | substrate P conveyed from the processing apparatus U2. . In the processing apparatus U3, the edge position controller EPC, the nip drive roller DR4, and the board | substrate P which control the center of the Y direction (width direction) of the board | substrate P to a fixed position are predetermined tension. Partially wound and given to the rotating drum DR5 (cylindrical body) which supports the pattern-exposed part on the board | substrate P in a uniform cylindrical surface shape, and the predetermined | prescribed hang (DL) DL to the board | substrate P Two sets of drive rollers DR6 and DR7 are provided.

Moreover, in the processing apparatus U3, the illumination apparatus IU which is provided in the transmissive cylindrical mask DM (mask unit) and the cylindrical mask DM, and illuminates the mask pattern formed in the outer peripheral surface of the cylindrical mask DM with an ultraviolet-ray. (Image 10) of the mask pattern of the cylindrical mask DM and the substrate P on a part of the substrate P supported by the lighting unit 10 and the cylindrical surface shape by the rotating drum DR5. In order to relatively position (align) the alignment microscopes AM1 and AM2 which detect an alignment mark or the like previously formed on the substrate P, are provided.

The processing apparatus U4 is a processing apparatus which performs mist deposition with respect to the photosensitive functional layer of the board | substrate P conveyed from the processing apparatus U3, The atomizer GS1 shown in FIG. 1, carrier gas In addition to the supply section GS2, the mixer ULW, the reaction chamber TC, and the recovery port section De, the differential exhaust chambers provided at the front and rear ends of the reaction chamber TC ( DE1, DE2, a temperature control mechanism HP for adjusting the temperature of the gas of the misted raw material material passing through the reaction chamber TC and the temperature of the substrate P to be conveyed, Dust collector (RT) for trapping molecules and particles of the raw material contained in the gas recovered through the recovery port (De) and unit controller (CUC) for collectively controlling the operation of the processing device (U4). Equipped with.

In mist deposition, a solution of various raw materials can be atomized. Among such materials, in particular, carbon nanotubes (hereinafter referred to as 'CNT') may be harmful to the human body when scattered in the air. . Therefore, the reaction chamber TC has a high airtight structure, and at the front and rear ends thereof, the substrate P can be transported and sealed to prevent the misted gas containing the raw material from leaking out of the apparatus. Differential exhaust chambers DE1 and DE2 are provided. In addition, about the structure of atomizer GS1, the carrier gas supply part GS2, etc., the thing as disclosed in the previous paper 2 can be used, and the ultrasonic vibrator is provided in atomizer GS1, and According to the mist size, the oscillation frequency and the oscillation intensity are adjusted.

The processing apparatus U5 warms the board | substrate P conveyed from the processing apparatus U4, and deposits the raw material substance deposited on the lyophilic region HPR of the board | substrate P by the mist deposition method. Although it is a heating and drying apparatus which dries and adjusts moisture content to a predetermined value, the detail is abbreviate | omitted. Then, the board | substrate P which passed through the last processing apparatus Un of a series of processes through several processing apparatuses is wound up to the collection roll FR2 via the nip drive roller DR1. Even when the coil is wound up, the edge position controller EPC2 and the driving roller DR1 are used so that the center of the substrate in the Y direction (width direction) or the substrate end in the Y direction is not shifted in the Y direction. The relative position of the recovery roll FR2 in the Y direction is controlled in order.

The host controller 5 controls each of the processing apparatuses U1 to Un in FIG. 5 collectively, but various measurement sensors and substrates P for measuring the state of the pattern formed on the substrate P. FIG. In response to signals from various sensors or the like for monitoring the conveyance state of the feeder, the feed back control on the process and the feed forward control are also performed in the element. In the device manufacturing system described above, since the exposure apparatus capable of precisely patterning a fine pattern is used as the processing apparatus U3, the boundary between the hydrophilic liquid portion formed on the substrate P becomes very clear and the substrate P Since the misted raw material substance is deposited on the lyophilic region (HPR) on the C), a fine pattern can be formed with high accuracy.

According to the manufacturing method using the above manufacturing system, since patterning applies the exposure method similar to the photolithography method with respect to the photosensitive functional material, compared with the printing method, the inkjet method, or the metal mask (shadow mask) method, it is highly precise. Even fine patterning is possible. In addition, since the expensive apparatus used in the conventional photolithography process such as a vacuum film forming apparatus or an etching apparatus is not used, and raw materials can be deposited only on a portion to be deposited, there is no need to remove unnecessary portions by etching, The advantage that the environmental load is small can be obtained.

(Third embodiment)

In the mist deposition processing apparatus U4 shown in FIG. 5, the above-mentioned relationship I or relationship II is satisfied, and the mist concentration, gas flow rate, temperature, and substrate P of the reaction chamber TC are satisfied. It is preferable to set a conveyance speed | rate etc. as an adjustment parameter. This is to control the film thickness and the compactness of the raw material material deposited in the high lyophilic region HPR on the substrate P. In addition, it is also possible to provide a function of measuring the film thickness of the raw material material deposited in the high lyophilic region (HPR), and to dynamically change the processing time and conditions (adjustment parameters) of the mist deposition according to the measured value. useful.

FIG. 6: shows the example which provided the function which measures the thickness of the pattern to be deposited in the mist deposition processing apparatus U4 shown in FIG. 5, and attaches | subjects the same code | symbol about the structure of the same function as the member in FIG. Doing. In FIG. 6, the substrate P has a predetermined tension in the reaction chamber TC by the driving roller DR8 provided in the differential exhaust chamber DE1 and the driving roller DR9 provided in the differential exhaust chamber DE2. Is sent in the X direction.

In the present embodiment, at a position close to the differential exhaust chamber DE1 in the reaction chamber TC, the first nozzle NZ1 for ejecting the mist of gas containing the solution containing the raw material material on the surface of the substrate P is provided. The second nozzle NZ2 which is connected from the mixer ULW1 and blows off the mist of gas of the solution containing a raw material substance is connected from the mixer ULW2. The two mixers ULW1 and ULW2 are appropriately controlled by the unit control unit CUC so as to make the mist concentration contained in the gas blown out from the nozzles NZ1 and NZ2 the same or different. Mist density | concentration is by changing the mixing ratio of the carrier gas supplied from supply part GS2 (refer FIG. 5) to each of mixer ULW1, ULW2, and the mist gas supplied from atomizer GS1 (refer FIG. 5). It can be realized.

Downstream in the reaction chamber TC, a nozzle VT for sucking and recovering the gas ejected from the nozzles NZ1 and NZ2 is provided at a position close to the differential exhaust chamber DE2 and the gas in the chamber TC. Is sent to the recovery port part De at a flow rate controlled by the exhaust unit Exo. By adjusting the total flow rate of the gas ejected from the nozzles NZ1 and NZ2 and the gas flow rate sucked by the nozzle VT, the gas along the conveyance direction (X direction) of the substrate P in the chamber TC is adjusted. You can create a flow. The flow can be made slower, faster or the same with respect to the conveyance speed of the board | substrate P. FIG.

In the structure of FIG. 6, mist deposition is performed between the flow path from nozzle NZ1 or nozzle NZ2 to nozzle VT in chamber TC, but the mist concentration adjustment range is large and gas Since the flow velocity can be adjusted according to the conveyance speed of the substrate P, pattern formation (deposition) to achieve a desired film thickness is possible.

By the way, in this embodiment, in the reaction chamber TC, the solution containing the raw material substance which became the mist and deposited on the board | substrate P in the downstream position as the downstream side of the gas recovery nozzle VT. The measurement sensor TMS which measures the layer thickness of this is provided, and the measured value is sent to the unit control part CUC. The unit control unit CUC determines whether or not to adjust processing conditions (mist concentration, gas flow rate, temperature, etc.) in the chamber TC based on the measured value. When adjusting the conveyance speed of the board | substrate P as adjustment of a process condition, the unit control part CUC outputs signal Ds1 to the drive motor for drive roller DR9 (or DR8), and rotation speed is adjusted. do.

As the measurement sensor TMS, an optical interference film thickness meter, a spectroscopic ellipsometer, or the like is used, but the mist deposited on the substrate P at a position downstream of the reaction chamber TC is a solvent ( Moisture), the thickness of the pattern formed densely from the raw material can not be accurately determined. Therefore, as shown in FIG. 6, after the processing apparatus U4 for mist deposition (after the differential exhaust chamber DE2), and after the processing apparatus U5 which heat-drys the board | substrate P, a pair of nips The retention part of the board | substrate P comprised by the drive rollers NR1 and NR2 and dancer roller DSR may be provided, and the measurement sensor TMS of a film thickness may be provided immediately after that.

In this way, immediately after the retention part of the board | substrate P, the pattern to be measured on the board | substrate P is located just under the measurement sensor TMS, and the board | substrate P for a predetermined time (for example, several seconds). ) Can be stopped, and the measurement time of the measurement sensor TMS can be secured. The time which can stop the board | substrate P is determined by the speed Vo of the board | substrate P carried out from the processing apparatus U5, and the rocking stroke Ld of the dancer roller DSR in the Z direction. For example, if the speed Vo of the substrate P is 5 cm / s and the stroke Ld is 50 cm, the substrate P can be stopped for up to 20 seconds at the position of the measurement sensor TMS immediately after the retention portion.

In the measurement sensor TMS after the processing apparatus U5, since the liquid component is missing from the pattern layer of the raw material material deposited by mist deposition, the thickness can be measured correctly. It is preferable that both the measurement sensor TMS in the reaction chamber TC and the measurement sensor TMS behind the processing apparatus U5 can measure the film thickness of a fine pattern (for example, 20 micrometers or less in line width). Do. For example, the product names ST2000-DLXn and ST4000-DLX of optical coherence film thickness meters sold by K-MAC of Korea are microscope type, so they are easy to assemble, and the diameter of the optical spot for measurement is small to several micrometers. The measurement time is also within a few seconds. In addition, product name RE-8000 equipped with product name lambda ace VM-1020 / 1030, the spectroscopic ellipsometer of the optical interference type film thickness measuring apparatus of Dainippon Screen Manufacturing Co., Ltd. is a measurement sensor after processing apparatus U5 ( TMS) can also be used.

When measuring the thickness of the pattern by the raw material substance deposited on the board | substrate P by the measurement sensor TMS as mentioned above, the part of TFT and wiring of the device (display panel) formed on the board | substrate P are measured. Although the negative specific layer may be measured directly, the formation area of the thickness measurement test pattern (mark) may be provided outside the device formation area on the board | substrate P, and you may make it measure the thickness of the raw material material deposited there. An example in the case of providing such a test pattern is demonstrated with reference to FIG.

FIG. 7: is a top view which shows arrangement | positioning of the some device (display panel) area | region 100 formed on the board | substrate P, and the some marker area | regions MK1-MK5 in which a test pattern is formed. Here, a display panel for televisions with a screen size of 32 inches is produced at an aspect ratio of 16: 9, and the longitudinal direction of the display panel region 100 is arranged in the long direction (X direction) of the substrate P. Each panel region 100 is disposed with a predetermined margin in the long direction of the substrate P, and a margin of a predetermined width is set on both sides of the width direction (Y direction) of the substrate P. Three marker regions MK1, MK2, and MK3 are provided in the margins between the panel regions 100 in the Y direction, and two markers are provided on both sides of the panel region 100 in the Y direction. Regions MK4 and MK5 are provided.

6 measurement sensors TMS shown in FIG. 6 are provided here and spaced apart in the width direction of the board | substrate P corresponding to arrangement | positioning of marker area | regions MK1-MK5. The marker regions MK1 to MK5 can be observed by any of the measurement visual fields St1, St2, and St3 of each measurement sensor TMS. Among the marker regions MK1 to MK5, the same test pattern is formed in all three marker regions MK1 to MK3 arranged in the Y direction.

An example of the test pattern is shown representatively of the marker region MK1, and is shown in the broken line circle in FIG. 7 below. In the marker region MK1, a plurality of test patterns may be formed, but line and space test patterns MPa, MPd, MPe, MPg, and MPh having different line widths, circular test patterns MPb, and rectangles. The large test pattern MPc of a shape, the test pattern MPf of a two-dimensional dot shape, etc. can be arrange | positioned. As for the test pattern of a line & space shape, the thing of a pitch direction in the X direction and the thing of the Y direction is set. The test pattern MPe is formed by plural L-shaped lines in the inclined 45 ° direction, and the test pattern MPh is formed as a 45 ° inclined lattice pattern.

The line width of the line & space can be determined corresponding to the size of the pattern formed by the mist deposition. For example, in the case of generating an electrode pattern or a wiring pattern having a line width of 20 μm by mist deposition in the panel region 100 of the substrate P, for example, 40 μm, as a line & space of the test pattern, 4 sets of 30 micrometers, 20 micrometers, 15 micrometers, and the line width were exposed with the mask pattern for the panel area 100 in the exposure process of processing apparatus U3. Also for other test patterns MPb, MPc, and MPf, what is necessary for measurement is exposed together in the exposure process of processing apparatus U3.

In the marker regions MK4 and MK5 disposed on both sides of the panel region 100 in the Y direction, only one line-shaped test pattern having a width in the Y direction of several mm and a length in the X direction of several tens of mm is formed. It's okay to do it. Thus, when it is set as the elongate test pattern in the elongate direction of the board | substrate P, conveyance of the board | substrate P will not be stopped, for example by the measurement sensor TMS in reaction chamber TC shown in FIG. It becomes easy to measure the film thickness of the test pattern formed in the marker regions MK4 and MK5.

By the way, marker area | region MK1 and marker area | region MK4 can be observed by measurement sensor TMS which has measurement visual field St1, and marker area | region MK2 is a measurement sensor (measuring measurement field St2) ( TMS) and the marker region MK3 and the marker region MK5 are observable by the measurement sensor TMS having the measurement visual field St3, but the marker region MK3 and the marker region MK5 can be observed by the test patterns of the marker regions MK1 to MK3. The film thickness measurement is performed by the measurement sensor TMS behind the processing apparatus U5 in FIG. 6, and the film thickness measurement of the test patterns of the marker regions MK4 and MK5 is performed by the measurement sensor TMS in the reaction chamber TC. You may share to perform by. In addition, in each marker region MK1 to MK5, a test pattern is formed by one mist deposition. Therefore, when patterning mist deposition over a plurality of layers, the marker regions MK1 to MK5 are patterned for each layer. It is better to shift the position of MK5).

Since there are no other basic pattern layers in the marker regions MK1 to MK5 as described above, the thicknesses of the various test patterns formed by the processing apparatus U4 (mist deposition) can be accurately measured. In addition, since the size (line width, etc.) of the test pattern used for measurement can be selected (changed) according to the size of the device pattern (pattern in the display panel region 100), the film thickness condition can be precisely controlled. Become. In addition, in each of the three marker regions MK1 to MK3 between the panel regions 100, the difference in film formation conditions in the width direction of the substrate P (mist concentration) is compared by comparing the film thicknesses of the same test patterns. Non-uniformity, etc.) can be confirmed and corrected. In addition, the measurement sensor TMS may add not only the thickness of the pattern formed into a film but the sensor which measures the line width etc. together.

(4th embodiment)

FIG. 8: Mist D while integrating the processing apparatus U4 for mist deposition shown in FIG. 5 and the processing apparatus U5 which performs a heat drying process, and winding the board | substrate P around a rotating drum, and conveying it. An example of the apparatus which performs a position is shown.

In FIG. 8, the flexible board | substrate P carried in is half to the rotating drum RD which rotates around the axis AX1 via the nip drive roller NDR and the tension roller DR10. Wound over the circumference and folded at the air turn bar ATB in the heat drying unit 20 as the processing apparatus U5, and the roller DR11, the tension roller DR12, and the nip drive roller NDR are It is carried out by mediation. In the circumferential range in which the substrate P is wound around the rotating drum RD, cylindrical partitions constituting the reaction chamber TC are provided, and both ends of the partition wall in the circumferential direction are provided in the chamber TC. An air seal bearing Pd is provided to prevent mist gas from leaking into the environment. Of course, the air seal bearing for preventing the clearance with the rotating drum RD is also provided in the edge part of the axis AX1 direction (Y direction) of the cylindrical partition which comprises the chamber TC.

As shown in FIG. 1, FIG. 5, and FIG. 6, the mist from the atomizer GS1 and the gas from the carrier gas supply part GS2 are mixed by the mixer ULW, and become a mist containing gas, and are cylindrical It is supplied to one end side (part in which the board | substrate P contacted the rotating drum RD) of the reaction chamber TC of the shape. The mist-containing gas travels along a narrow cylindrical space along the surface of the substrate P wound on the rotary drum RD, and the substrate (from the rotary drum RD at the other end side (rotary drum RD). At the portion away from P), it is exhausted from the recovery port part De.

In this embodiment, since the back surface of the board | substrate P is brought into close contact with the outer peripheral surface of the rotating drum RD, since unnecessary mist does not return to the back surface of the board | substrate P, a back surface can be kept clean. Moreover, when the temperature control mechanism is provided in the rotating drum RD along the outer periphery, temperature control with high responsiveness of the board | substrate P can be performed.

In accordance with the rotation of the rotary drum RD, the board | substrate P by which the mist was deposited in the lyophilic part HPR of the surface is sent linearly to the 1st space AT1 of the heat drying unit 20, and an electric heater and The pattern by the liquid deposited by mist deposition is dried by the temperature control mechanism HP, such as a warm air heater. The board | substrate P which passed the drying space AT1 is folded by about 180 degrees by the air turn bar ATB arrange | positioned in 2nd space AT2, and linearly advances in 3rd space AT3, and a roller (DR11). The spaces AT1, AT2, and AT3 are divided into partitions, and the partitions are provided with slit-shaped openings through which the substrate P can pass. The recovery port portion De is connected to each of the spaces AT2 and AT3, and the remaining mist-containing gas is recovered. In addition, when the raw material material deposited in the mist deposition is a semiconductor material, the space AT1 functions as an annealing for crystallizing or oriented the semiconductor material.

The air turn bar ATB has an outer circumferential surface of a substantially half circumference of the cylinder, and numerous gas ejection holes and suction holes are provided on the outer circumferential surface. Thereby, the board | substrate P is folded so that the surface (surface on which the raw material material was deposited) does not contact the surface of the air turn bar ATB. The gas blown out from the air turn bar ATB also has a function of further drying the pattern of the raw material material deposited on the surface of the substrate P.

The board | substrate P folded by the air turn bar ATB is controlled by predetermined temperature by the warm gas which blows out from the nozzle ANZ in space AT3, reaches roller DR11, and divides it by the partition. It passes through the roller DR12 in the true space, the nip drive roller NDR, and passes through the air seal bearing Pd arranged so that the board | substrate P may be interposed, and of the next processing apparatus or film thickness or line width, It is sent to the measurement sensor part.

When conveying the board | substrate P using the rotating drum RD as shown in FIG. 8, the diameter of the rotating drum RD shall be about 50 cm, and the board | substrate P may be in close contact with the outer peripheral surface of the rotating drum RD. When the range is set at about 240 °, the substantial length of the reaction chamber TC is about 100 cm (50 × π × 240/360), rather than making the reaction chamber TC a straight line as shown in FIGS. 5 and 6. The footprint of the device can be made small. Moreover, since the board | substrate P is sent in close contact with the outer periphery of the rotating drum RD, stable mist deposition can be implement | achieved without the board | substrate P oscillating up and down during conveyance.

As mentioned above, although preferred embodiment which concerns on this invention was described referring an accompanying drawing, it cannot be overemphasized that this invention is not limited to the example concerned. All shapes, combinations, and the like of the respective constituent members shown in the above-described examples are examples, and various modifications can be made based on design requirements and the like without departing from the spirit of the present invention. For example, the board | substrate P is not limited to the thin film and sheet | seat with flexibility, In addition to a glass substrate, a silicon wafer, etc., a plastic substrate and a resin substrate may be sufficient. Moreover, the board | substrate P does not need to process the elongate thing wound by the roll by the roll-to-roll system, and the system which processes the sheet | leaf cut to predetermined size (A4, B5 etc.) may be sufficient.

In addition, although the mist deposition method was used as a method of selectively forming a semiconductor layer, an electrode layer, or a wiring layer in the desired area | region on the board | substrate P in the above-mentioned each embodiment, it is not limited to that, but a spray method and a dip It can use instead of the film-forming methods, such as a deep coat method. The spray method is to apply the spray-like material solution sprayed from the nozzle onto the substrate P, similarly to the mist deposition method, and the dip coating method uniformly fixes the substrate P in the bath of the material solution. It is to immerse it in time.

In any case, for example, as described in the third embodiment (Fig. 7), light patterning is performed so that the marker regions MK1 to MK5 are formed at appropriate positions on the substrate P, and the spray method, After the deposition treatment of the material solution by the dip coating method, the deposition method (deposition state) in various test patterns in the marker regions MK1 to MK5 is confirmed by the measurement sensor TMS as shown in FIG. Various conditions of the dip coat method can feed back correct. The various conditions of the spray method are the fine pore diameter of the spraying nozzle, the spray pressure, the distance between the substrate P and the nozzle, the relative movement speed between the nozzle and the substrate P, and the like. The temperature of the material solution, the immersion time of the substrate P, the pulling speed, and the like.

In addition, in the case of using a conventional photolithography process in which the photoresist layer is subjected to photopatterning (exposure treatment) and then developed, and the resist layer is etched according to the pattern, the surface of the substrate P (base layer is If present, the surface) is brought into a high lyophilic state, and then a photoresist material having high liquid repellency is applied to the surface of the substrate P with a uniform thickness. After that, the development process is performed so that the portion (the surface of the substrate P or the surface of the base layer) from which the register layer has been removed is exposed as a surface having high lyophilic property, so that the mist deposition method (or the spray method) is performed. By a dip coating method, a precise pattern by the material solution is formed.

FR1-Feed Roll FR2-Recovery Roll
P-Board
U1, U2, U3, U4, U5, Un-Processing Units (Processing Units)
Gpa-rotary drum for application of photosensitive silane coupling agents
Gp1-applicator IU-ultraviolet illuminator
DM-Drum Mask PL-Projection Optics
DE1, DE2-differential exhaust chamber TC-reaction chamber
GS1-atomizer of material material GS2-carrier gas supply
ULW-Mixer HPB-Liquid Repellent
HPR-Hydrophilic RD-Rotary Drums
MK1 to MK5-marker zone 20-heat drying unit
100-display panel area

Claims (9)

A device manufacturing method comprising the step of depositing a material material for an electronic device on a surface of a substrate to a predetermined thickness.
Moving the substrate at a predetermined conveyance speed continuously by a conveying mechanism in a conveying direction along the surface of the substrate;
Blowing the mist containing gas provided in the said chamber containing the mist which atomized the functional solution containing the particle | grains of the said material substance, passing the said board | substrate in the chamber provided over the predetermined length along the said conveyance direction. The mist-containing gas is discharged from the nozzle for the injection into the chamber, and the mist-containing gas in the chamber is recovered by a recovery nozzle provided in the chamber, so that the mist-containing gas is at the same flow rate as the conveying speed of the substrate or faster than the conveying speed. And spraying along the surface of the substrate in the chamber to attach the mist to the substrate. The method according to claim 1,
Wherein the mist is generated by an atomizer for vibrating the functional solution with an ultrasonic vibrator, and the mist-containing gas is sprayed into the chamber in a state in which the mist generated in the atomizer is mixed with a carrier gas at a predetermined concentration. . The method according to claim 2,
The functional solution is a device manufacturing method of H ₂ O solution containing any one of particles, carbon nanotubes, or metal nanoparticles to be a semiconductor. The method according to claim 3,
The carrier gas is a device manufacturing method comprising any one of nitrogen, argon, air. The method according to claim 4,
The said ejection nozzle is arrange | positioned at the upstream of the said conveyance direction of the said board | substrate, The said recovery nozzle is arrange | positioned at the downstream side of the said conveyance direction of the said board | substrate. The method according to claim 5,
After drying the substrate passing through the chamber, measuring the thickness of the material material deposited on the surface of the substrate,
Based on the measured value of the thickness of the material material deposited on the substrate, the concentration of the mist contained in the mist-containing gas, the concentration of particles of the material material contained in the mist, the temperature in the chamber, and the substrate The device manufacturing method which adjusts any one of the said conveyance speeds. The method according to any one of claims 1 to 6,
Before the step of attaching the mist, the surface of the substrate is formed such that contrast due to a region having high lyophilic and high liquid repellency to the mist is formed on the surface of the substrate. The device manufacturing method further comprises the step of modifying. The method according to claim 7,
The modifying step may be performed by applying a silane coupling agent having a fluorine group on the surface of the substrate, and then irradiating and irradiating ultraviolet rays having a wavelength of 400 nm or less, and the region having high lyophilic properties. A device manufacturing method for forming a region having high liquid repellency. A device manufacturing method for forming a thin film by deposition of nanoparticles by attaching a mist including nanoparticles of a material material constituting the electronic device to a surface of the substrate, in order to form an electronic device on the surface of the substrate,
Moving the substrate at a predetermined conveyance speed continuously by a conveying mechanism in a conveying direction along the surface of the substrate;
Modifying the surface of the substrate such that a region having high affinity for the mist is formed on the surface of the substrate;
The mist-containing gas containing mist generated by atomization of the solution containing the nanoparticles while passing the substrate in the chamber provided over the predetermined length along the conveyance direction is provided from the ejecting nozzle provided in the chamber. The mist-containing gas is recovered in the chamber at a flow rate equal to the conveying speed of the substrate or at a flow rate faster than the conveying speed by recovering the mist-containing gas in the chamber from the recovery nozzle provided in the chamber. Spraying along the surface of the substrate to attach the mist to the substrate;
Drying the substrate passing through the chamber and measuring the thickness of the material material by the nanoparticles deposited on the surface of the substrate;
Based on the measured value of the thickness of the material substance, among the concentration of the mist contained in the mist-containing gas, the concentration of the particles of the material substance contained in the mist, the temperature in the chamber, and the conveying speed of the substrate Adjusting any one.

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