JPH02163379A - Formation of thin film and device therefor - Google Patents

Abstract

PURPOSE:To form an oxide thin film having a low content of dust on the surface of a substrate at a high rate by allowing an organometallic compd. to chemically react with the oxygen active species formed by high-temp. nonequilibrium or equilibrium plasma. CONSTITUTION:A substrate 11 controlled to a specified temp. by a temp. control mechanism 10 is arranged in a airtight treating chamber 21 capable of being evacuated. A raw gas is uniformly blown against the substrate 11 from a gas blowing plate 22 opposed to the substrate. The raw gas consists of an organometallic compd. and the oxygen active species. Tetraethoxysilane, tantalum alcoholates, etc., are used as the organometallic compd. The compds. of P, B, etc., are further added to the compd., and the mixture is supplied through an organometallic compd. inlet mechanism 40 using a bubbler 42. Meanwhile, the oxygen active species is generated by high-temp. nonequilibrium plasma or high-temp. equilibrium plasma in a generator 50 provided with a discharge tube 54, and supplied to an inlet mechanism 60. The raw gas is subjected to a chemical reaction, and a high-quality oxide thin film of silicon oxide, tantalum oxide, etc., contg. P, B, etc., is formed on the surface of the substrate 11.

Description

DETAILED DESCRIPTION OF THE INVENTION (Field of Industrial Application) The present invention relates to a method and apparatus for producing insulating films, dielectric films, and protective films for semiconductor electronic devices, superconducting devices, various electronic components, and various sensors.

(Conventional technology) Semiconductor electronic devices, superconducting devices, various electronic components,
Various methods have been attempted to fabricate insulating films, dielectric films, and protective films for various sensors, including thermal oxidation of the substrate material, thermal CVD on the substrate surface, sputtering, plasma-assisted CD, and spin code. ing.

In recent years, as devices have become more integrated or stacked, there is a need for a film forming method that provides good coverage of stepped portions or good flatness.

Now, one of the methods that is attracting attention is the use of tetraethoxysilane (also called tetraethyl orthosilicate, hereinafter abbreviated as "TEO8'") or diacetoxyditertiary-butoxysilane (hereinafter abbreviated as "DADBS"). There is a CVD technology. (Please note that these TE01.
DADBS and the like are organic compounds of silicon, which is a semiconductor, and in this specification, such semiconductor organic compounds will also be collectively referred to as "organometallic compounds."

For example, Rano Ikeda "Electrochemistry j Vo1.56. No.
, 7 (1988) P, 527-P, 532, and the cited references therein include articles regarding this method.

Ikeda et al. used atmospheric pressure CVD using TE01 and ozone to produce a silicon oxide film (hereinafter referred to as "NSCSC film") with good flatness and a phosphorus-containing silicon oxide film (hereinafter referred to as "PSA film") with good coverage of stepped portions. A boron-containing silicon oxide film (hereinafter abbreviated as "BSG film") was fabricated. In this case, ozone is used as the oxidation source, thereby making it possible to fabricate the NSC film at a low temperature of 400°C.
In addition, the OH groups in the film are reduced to obtain a high quality NSG film. However, there is a drawback: the deposition rate is approximately 1400A/m
i n, and it takes about 7 to make a 1 μm NSG film.
1μm, which is required for single-wafer type equipment.
/ min is far below.

Also, R.A., Levy et al., J. Electroch.
em, Soc, Vat, 134. No. 7 (1987
) P, 1744-P, 1749 and its cited references,
N S G using oxygen and DADBS or TE01
It is introduced that a film, a PSG film, a BSG film, and a boron/phosphorous containing silicon oxide film (hereinafter abbreviated as "BPSG film") were fabricated. In this case, although the film-forming temperature is 550°C, which is considerably higher than the method using ozone mentioned above, the film-forming rate is slow at 300 A/min.
This has also not reached a level that can be used industrially.

In addition, in the patent publication, “Unexamined Japanese Patent Publication No. 61-7
No. 7895 [Vapor Phase Growth Method]” and “U.S. Patent No. 3,93
4,060", but similarly to the above, these methods cannot be said to have reached a satisfactory level in terms of film formation speed and film quality.

In addition, Noguchi et al.
In Lecture No. 29P-G-5 (Spring 1988), by using oxygen atoms created by microwave discharge and tetramethoxysilane (hereinafter abbreviated as "TMO8"), tetramethylsilane (hereinafter referred to as "T This shows that the carbon content in the produced film is lower than that when using the film (abbreviated as “S”). However, the film made using this TM01 also contains a large amount of OH from its infrared absorption spectrum.
The presence of groups was observed, and it is clear that the film was not necessarily good. This is considered to be due to insufficient supply of oxygen active species.

Another example using oxygen atoms is described in JP-A-63-83275 rCVD Apparatus, in which NSG films,
To produce PSG films and BSG films, oxygen atoms and silane are reacted. This reaction usually proceeds rapidly at room temperature and under reduced pressure, producing silicon oxide powder dust. Furthermore, since the reaction occurs rapidly, it is difficult to introduce and mix the two gas components into the reaction chamber, making it difficult to produce a film with good uniformity.

In order to solve this problem, the invention disclosed in Japanese Patent Application Laid-open No. 63-83275 suppresses the reaction between oxygen atoms and silane by cooling the gas outlet, and introduces the gas onto the heated surface of the substrate to be treated, where it reacts. It shows a device designed to cause However, in this method, it is necessary to cool the gas outlet, which makes the device complicated, and it is impossible to completely suppress the reaction in a space far from the substrate surface, so some dust is inevitably generated. There is a drawback that this occurs.

(Problems to be solved by the invention) As mentioned above, in the conventional method, ozone + TEO8 system,
In each of the oxygen + DADBS system and oxygen + TEO8 system, 1 μm / m is industrially required for single wafer equipment.
There was a drawback that it was not possible to obtain a film formation rate on the order of in.

In addition, in the oxygen atom + silane system, which allows this fast film formation rate to be obtained, the reaction occurs rapidly in the mixing part of both gases, so a method is required to suppress the reaction by cooling the mixing part and the gas outlet part. This method has the disadvantage that the device becomes complicated and it is not possible to suppress the generation of dust due to reactions in the space.

In addition, oxygen atoms created by microwave discharge and TMA
Alternatively, in the method of using TMOS in combination, the amount of oxygen active species is insufficient, so if TMA is used, the film will contain carbon-based impurities, and if TMOS is used, the film will contain ○H groups. The drawback was that a high-quality film could not be obtained.

(Objective of the Invention) The present invention solves this problem by using a large amount of oxygen active species obtained from a high-temperature non-equilibrium plasma or a high-temperature equilibrium plasma in place of ozone, and in place of silane with less reactive T.
E01. Provides a method and apparatus for producing an insulating film, dielectric film, or protective film quickly and with little dust on a substrate surface set at a predetermined temperature by using an organometallic compound such as DADBS, TMoS, or tantalum alcoholade. The purpose is to

(Means for Solving the Problems) In order to achieve the above object, the present invention uses an organometallic compound and oxygen active species produced by high-temperature non-equilibrium plasma or high-temperature equilibrium plasma as raw material gases. A thin film production method that uses a chemical reaction to create an oxide film on the surface of a substrate, and an apparatus for realizing this method include a processing chamber that can be kept airtight, a substrate installed in the processing chamber, and a A substrate temperature adjustment mechanism that adjusts the temperature of the substrate, an organometallic compound introduction mechanism that introduces an organometallic compound into the front space of the substrate in the processing chamber, a high temperature nonequilibrium plasma or high temperature equilibrium plasma generation mechanism, and a and an oxygen active species introduction mechanism for introducing oxygen active species into the front space of the substrate.

High temperature nonequilibrium or high temperature equilibrium plasmas create much higher amounts of oxygen active species than glow plasmas or microwave plasmas used in device fabrication processes. This oxygen active species and T, which is less reactive than silane,
E01. By using organometallic compounds such as DADBS, TMOS, or tantalum alcoholade, a chemical reaction is induced only on the surface of the substrate set at a predetermined temperature, and the film thickness,
An oxide film with uniform film quality distribution can be produced.

(Example) This invention belongs to the applicant of this application.
By using No. 9646, ``Surface Treatment Method and Apparatus,'' as a basic technology, a useful invention could be obtained by applying it to a low-temperature oxide film production process that was not generally known at the time of filing. ``LTE plasma'' in the specification of the above patent application corresponds to ``high-temperature non-equilibrium plasma or high-temperature equilibrium plasma'' in the specification of the present application.

(Function) As a first embodiment of the present invention, the production of an NSC film will be described.

FIG. 1 shows a front sectional view of an apparatus for implementing the method of the present invention. Reference numeral 21 denotes a processing chamber made of stainless steel, and has a structure that allows it to be evacuated or kept airtight as required.

It also has a structure that allows it to be pressurized. 11 is
This is the substrate on which a thin film is to be fabricated.

Describing the substrate temperature adjustment mechanism 10 (12, 13, 14, etc.), 12 is a substrate holder that holds the substrate 11 and controls the temperature of the substrate. 13 is a heater, 14 is a thermocouple, and the substrate holder 12 has a diameter of 15 cm and can be heated to about 450°C. The temperature of the substrate holder 12 is measured by the thermocouple 14, and P, PI, PID are measured by using a temperature controller and a thyristor unit (not shown).
The temperature of the substrate holder 12 is adjusted by adjusting the power applied to the heater 13 by ON/OFF control using a control or a relay called Arashi. When necessary, use a cooling mechanism such as water cooling for this part.

The processing chamber 21 has a cylindrical shape with a diameter of about 25 cm and a height of about 30 cm, and can be evacuated through a valve 31 using a mechanical booster pump 32 and an oil rotary pump 33. A vacuum gauge 34 measures the pressure inside the processing chamber 21. In this embodiment, the pressure in the processing chamber 21 was kept constant by adjusting the opening and closing of the valve 31.

Reference numeral 22 denotes a gas blowing plate, which corresponds to the ``distribution plate'' in the specification of Japanese Patent Application No. 82-254268 "Film Forming Apparatus 3 and Method" filed by the applicant of the present application, and its structure is as follows. It is the same as that described in detail in the previous S self-clarification, and 24 is a heater for setting the gas blowing plate 22 to a predetermined temperature, and 23 is a diffusion plate, which is 1 mm in diameter on a 2 mm thick plate. A type with multiple holes in the front and back is used.

This gas blowing plate 22 distributes and blows out TEOS, which is easily liquefied, in a gaseous state to the space in front of the substrate 11 with good uniformity. If it is not heated here, dew condensation will occur on the TEOS, and the process gas will be supplied. becomes unstable, causing problems in the stability and reproducibility of film formation.

Another effect of the heating by the gas blowing plate 22 is that intermediate products are generated due to thermal denaturation of the process gas.
It is also possible that it contributes to film formation (Tokusan Sho 62-
No. 254268 "Film forming apparatus and method"). however,
At present, the mechanism has not been clarified.

Next, the organometallic derivative introduction mechanism 40 will be described.
43 is TEOS, which is a liquid at normal temperature and normal pressure. The carrier gas nitrogen is supplied from a cylinder (not shown) through a pressure reducing valve and a flow controller (arrow 45).
. Reference numeral 42 designates a bubbler, in which TEO 343 in a liquid state is bubbled with nitrogen introduced through a valve 44 and vaporized, and then guided to the front space of the substrate 11 through the valve 41 and the gas blowing plate 22 described above.

46 indicates a constant temperature bath. The valve 41 and piping are kept warm in order to adjust the bubbling temperature and to keep the liquefied TEOS in a gaseous state.

In this example, the capacity of the bubbler 42 was approximately 11, and each bubbler 42 was filled with 300 g of TEOS.

Next, the oxygen active species of another process gas produced by the high temperature equilibrium plasma generation mechanism 50 and the oxygen active species introduction mechanism 60 that introduces them will be described. 54 is a discharge tube, a double tube made of quartz glass. It has a structure that allows water to flow between the double pipes for cooling. In this example, the inner tube of the quartz glass tube has a diameter of 3 cm and a length of 53 cm. 56.56' indicates the flow of cooling water.

53 is a coil made of a copper vibrator, and although not shown, this vibrator is also water-cooled from the inside.

One end of the coil 53 is grounded, and the other end is connected to the high frequency power source 51 through the matching circuit 52. In this embodiment, the high frequency power source 51 has a frequency of 13.56 MHz and an output of 10
A kW high frequency separately excited power source was used. Oxygen (arrow 57) is introduced from a high-pressure cylinder (not shown) via a pressure reducing valve and a flow controller.

The oxygen active species introducing mechanism 60 for introducing oxygen active species into the processing chamber 21 is made of stainless steel piping 63, a stainless steel flange 61 welded to the piping 63 and having an O-ring groove cut therein, and welded to the discharge tube 54. It is composed of a quartz glass flange 58, a rubber o ring 59 that acts as a seal between both flanges, a normal screw (not shown) for joining both flanges, and a valve 62.

As described in Japanese Patent Application No. 61-069646, when high frequency power is injected into the coil 53 from the high frequency power supply 51, a high frequency glow discharge is initially generated within the discharge tube 54. When the injected power is further increased, the coil 5
A locally pinched high-temperature non-equilibrium plasma or high-temperature equilibrium plasma 55 is generated inside the plasma. (About this high-temperature non-equilibrium plasma or high-temperature equilibrium plasma, see Mito et al., "Vacuum" Vol. 31, No. 4 (1988) P, 271-P.
, 27B and its cited references) This high-temperature non-equilibrium plasma or high-temperature equilibrium plasma has an extremely high emission intensity compared to a high-frequency glow discharge, and a large amount of active species are generated, especially atomic It is characterized by a large number of active species, and electrically, the discharge impedance is extremely low.

FIG. 2a shows an example commonly observed in the emission spectroscopic analysis of high-frequency or microwave glow discharge, and FIG. 2b shows an example commonly observed in the emission spectroscopic analysis of high-temperature non-equilibrium plasma. The vertical axis of FIG. 2a is magnified 4500 times compared to the vertical axis of FIG. 2b. (Accordingly, the emission intensity of b is about 4500 times stronger than that of a). It is also clear that the light emission b strongly depends on the light emission from oxygen atoms, and that oxygen dissociation progresses in the high-temperature non-equilibrium plasma, producing a large amount of active species.

Examples of utilizing the active species of this high-temperature non-equilibrium plasma or high-temperature equilibrium plasma include Japanese Patent Application No. 163350/1983 filed by the originator of Honrin, ``Method for Improving Oxide Superconductors,'' and 46th Application No. Physics Society Academic Conference (Autumn 1986) Lecture No. 6P-No B-16, Lecture Proceedings Volume 1, P
, 131, etc., and their usefulness is clear. However, there is no literature that mentions a method for producing an oxide thin film using a combination of oxygen active species of this high-temperature non-equilibrium plasma or high-temperature equilibrium plasma and an organometallic compound.

Now, the oxygen active species generated in the high temperature nonequilibrium plasma or the high temperature equilibrium plasma 55 of this embodiment are introduced into the front space of the base 11 through the oxygen active species introduction mechanism 60 and the gas blowing plate 22.

In this embodiment, the internal pressure of the processing chamber 21 is 200 Torr.
, oxygen flow ffi 1011/min, bubbling nitrogen eM TL 21/min, constant temperature bath 46 temperature 30°C, waste blowing plate 22 temperature 80°C1, substrate holder 12 temperature 400°C1, high frequency power 8.5kW. , N at a deposition rate of approximately 1.2 μm/min.
An SC film could be obtained. This NSC film was found to be of good quality with no contamination observed by infrared absorption spectroscopy and with few ○H groups.

The fact that a high-quality film was obtained at a film formation rate of approximately 1.2 μrn/rn i * is an industrial necessity, and it is a film forming rate of 1 μm/min, which is required for single-wafer processing equipment. It satisfies the speed.

When oxygen active species are created by ordinary microwave glow discharge, it is clear from the emission spectroscopic analysis pattern on the second surface that atomic oxygen is generated in the discharge plasma, but this is caused by high-temperature non-equilibrium plasma. Or, compared to high-temperature equilibrium plasma, it is much less. Moreover, since microwaves are absorbed by water, the power loss of microwaves is large and discharge 7
The disadvantage is that it is difficult to perform water cooling.

A second embodiment of the method of the invention involves introducing the nitrogen carrier trimethyl phosphate through valve 71 of the apparatus of FIG. Trimethyl phosphate is transported by being bubbled with nitrogen in a bubbler (not shown) whose flow rate is controlled. Pubbling temperature: 60'C, nitrogen flow rate 1.5 s/m i
It is n. In the same manner as in the embodiment shown in FIG.
Phosphorus was selected as the element to be added, and a phosphorus-containing dinocone film, ie, a PSG film, was fabricated at a speed of 1.3 μm/min.

Further, as a third embodiment of the method of the present invention, triethoxyboron is used instead of trimethyl phosphate in the second embodiment.

In this case, boron can be selected as the element to be added to the oxide film, and boron can be included. The bubbling temperature of triethoxyboron was set to 15°C, 1 nitrogen flow, 10.2Q/
By keeping the other conditions the same as in the first example, the BSG film could be formed on the surface of the substrate 11 at a rate of 1.3 μm/min.

Further, as a fourth embodiment of the present invention, by using the second and third embodiments together, that is, by introducing both phosphoric acid trimethyl ester and triethoxyboron, the substrate 11
One example is one in which a BPSG film can be formed on the surface at a speed of 1.3 μm/min.

Further, even when DADBS was used instead of TE03O, an NSC film could be similarly produced. Further, as in the case of TE01, when trimethyl phosphate and triethoxyboron were used in combination, PSG films, BSG films, and BPSG films could be produced at high speed and with good quality. Furthermore, in the case of arsenic as the element to be added, arsine or triethoxyarsine may be used.

Further, in a fifth embodiment of the present invention, tantalum alcoholade such as tantalum methylate or tantalum ethylate is used as the organic gold 7χ compound in place of TE01 in the first embodiment, and the bubbling temperature is 60 to 160°C. When the temperature of the substrate holder 12 is 4500C, a film of tantalum oxide can be formed on the surface of the substrate 11 at a rate of 30C)4/min. This tantalum oxide film is mainly used as a dielectric film in some device capacitors.
The required film thickness is about 250A. Therefore, film formation is completed in about 1 minute and is considered to be industrially useful.

Although the above embodiments all show examples of film formation under reduced pressure, the process pressure may be normal pressure or higher pressure. NSG film, PSG film with particular emphasis on flatness
When forming a film, a BSG film, or a BPSG film, the higher the pressure, the better the flatness will be.

However, in this case, a high-temperature non-equilibrium plasma or a high-temperature equilibrium plasma with a large discharge power is required. For low power, it is necessary to reduce the inner diameter of the discharge tube.

In the case of pressurization at normal pressure or higher, the mechanical booster pump 32 and oil rotary pump 33 are removed as necessary in each of the above figures.

Further, as the gas introduced by arrow 57, in addition to oxygen, nitrous oxide or ozone-containing oxygen can be used.

Further, regarding the amount of oxygen active species, details can be found in "January Sem 1 Conductor World, July 1988 issue, p. 131, p. 138" by Katozai et al., and the literature cited therein.

As seen in these documents, in this example as well, the addition of nitrogen or a trace amount of fluorine gas (trifluorine nitrogen, freon, etc.) leads to a decrease in the OH groups in the film, resulting in good results. I am getting .

However, regarding the stability of the electrical characteristics of the oxide film caused by the mixing of this additive gas into the target oxide film,
It's not clear at this point.

Another example of equipment used to carry out the method of the invention is shown in FIG. The same members as in FIG. 1 are numbered the same.

This embodiment mainly has a structure in which the gas blowing plate 22 of the embodiment shown in FIG. 1 is removed. In these devices,
The disadvantage is that the thickness and quality distribution of the produced film is poor. However, since organometallic compounds and oxygen active species can be directly introduced, faster film formation (approximately 2 μm/min) is possible.
was possible. It has been found that rotating the substrate is effective in improving the film thickness and film quality distribution.

FIG. 4 shows another embodiment of the present invention. The same members as in FIG. 1 are numbered the same.

Reference numeral 28 denotes a processing chamber made of a quartz glass tube (inner diameter 30 cm, length 80 am), in which the substrate 11 can be heated from the outside with an electric furnace (or emitted light from a halogen lamp) 81. 82 is a substrate holder made of quartz glass. Reference numeral 101 denotes a hatch, which has a structure that allows the base 11 to be taken in and out along with the base holder 82 in the direction of an arrow 102.

Reference numeral 92 denotes a check valve, which has a structure that allows gas to be exhausted only in the direction of arrow 91. The quartz glass discharge tube 54 and the processing chamber 28 may be configured integrally without providing the bulb 62. In this case, the oxygen active species introduction mechanism 40 is simple, consisting only of a welded portion or a connecting portion between the processing chamber 28 and the discharge tube 54.

This embodiment has the advantage that a large number of wafers can be processed at once. The processing chamber 22 may have a vertical structure,
In that case, the temperature distribution of the substrate may be modified and a film with better uniformity may be produced.

Furthermore, in the embodiments shown in FIGS. 1, 3, and 4, the bubbler 42 of the organometallic compound introduction mechanism 40 was used.
Instead of bubbling, the structure may be such that the organometallic compound is simply vaporized using the vapor pressure and introduced into the processing chamber while controlling the flow rate, or a vaporizer that forcibly vaporizes the compound may be installed. good. When forming a film under pressure, the combined use of a vaporizer is particularly effective.

Furthermore, although nitrogen has been described as an example of the carrier gas for the organometallic compound, any inert gas such as argon or helium or any other gas with low reactivity may be used.

(Effect of the invention) By using organometallic compounds and oxygen active species produced by high-temperature non-equilibrium plasma or high-temperature equilibrium plasma, it is possible to produce high-quality oxide films at high speed, which can be used for semiconductor electronic devices, superconducting devices, and various other materials. It can be used to create insulating films, dielectric films, and protective films for electronic components and various sensors.

[Brief explanation of the drawing]

FIG. 1 is a front sectional view of an embodiment of the present invention, FIG. 2 a is an emission spectroscopic analysis pattern of a normal high frequency or microwave glow discharge of oxygen, and b is an emission spectroscopic analysis pattern from a high-temperature non-equilibrium plasma or a high-temperature equilibrium plasma. Analysis pattern, Figure 3, Figure 4
The figure is a front sectional view of another embodiment of the present invention. 10... Base temperature adjustment mechanism, 11... Base, 12.
... Base holder, 21... Processing chamber, 22... Gas blowing plate, 33... Oil rotary pump, 40... Organometallic compound introduction mechanism, 42... Bubbler, 50...
Generation mechanism, 54...Discharge tube, 55...High temperature nonequilibrium plasma or high temperature equilibrium plasma, 60...Oxygen active species introduction mechanism, 81...Electric furnace, 101...Hatch. Patent Department Representative B Den Anelva Co., Ltd. Patent Attorney Kenji Murakami in re n 5 / ty (Orb, unl't5) #7 re r7s ”'9 Carb, unt'ts) Figure 2

Claims (7)

[Claims] (1) The method is characterized in that an organic metal compound and oxygen active species produced by high-temperature nonequilibrium plasma or high-temperature equilibrium plasma are used as raw material gases, and a chemical reaction between them is used to produce an oxide film on the surface of the substrate. A thin film fabrication method. (2) Claim 1, wherein the organometallic compound is tetraethoxysilane and the oxide film is a silicon oxide film.
The method for producing a thin film described in Section 1. (3) Claim 1, wherein the organometallic compound is tantalum alcoholade, and the oxide film is a tantalum oxide film.
The method for producing a thin film described in Section 1. (4) Using an organometallic compound, a hydride or an organic compound of the element to be added, and an oxygen active species created by high-temperature non-equilibrium plasma or high-temperature equilibrium plasma as raw material gases, the chemical reaction between them is used to form a surface of the substrate. A method for producing a thin film, comprising: producing an oxide film containing the element to be added. (5) The organometallic compound is tetraethoxysilane, the element to be added is phosphorus and/or boron, and the organic compound of the element to be added is trimethyl phosphate, triethoxyboron, or both. 5. The thin film manufacturing method according to claim 4, wherein the oxide film to be manufactured is a silicon oxide film containing phosphorus and boron, or either one of them. (6) A processing chamber that can be kept airtight, a substrate installed in the processing chamber, a substrate temperature adjustment mechanism that adjusts the temperature of the substrate, and a space in front of the substrate in the processing chamber that controls the organometallic compound. A mechanism for introducing an organometallic compound into the substrate, a mechanism for generating high-temperature nonequilibrium plasma or high-temperature equilibrium plasma, and an active oxygen species introduction mechanism for introducing oxygen active species produced thereby into the front space of the substrate. Features of thin film production equipment. (7) A temperature-controlled gas blowing plate that uniformly supplies the organometallic compound to the front space of the substrate is installed as a member for introducing the organometallic compound into the processing chamber. The thin film production apparatus according to scope 6.