JPS59213603A - Manufacture of thin film of composite material - Google Patents

Abstract

PURPOSE:To obtain a thin film used for an electronic material with a low-temp. heat treatment by coating a composite metallic soln. of metallic akoxides and a metallic chelate on a substrate, and submitting to heat decomposition. CONSTITUTION:The >=1 kind among metallic chelates such as ketones is dissolved in >=1 kind among metallic alkoxides or its polymers. The composite metallic soln. is coated on a substrate, heated and decomposed by using a muffle furnace etc., and annealed to form a uniform transparent thin film. The thickness of the thin film to be formed is regulated in accordance with the content of metallic constituents, viscosity, and the amt. of coating etc. of the metallic soln. The thin film of the composite material obtained with this method is provided with the excellent electromagnetic, optical, and mechanical functions.

Description

DETAILED DESCRIPTION OF THE INVENTION This invention relates to a method for producing a thin film of a composite agglomerate, which is dissolved in a co-trapping solvent and then thermally decomposed.

Metal compound thin films, especially uniform IIIIj:2 ft ribs of two or more metals present in the form of oxides, nitrides, etc., are excellent materials for pore magnetic, optical, etc. The company is actively researching and developing these membranes, especially for use as electronic forestry materials.

In addition, thin film technology is a key technology that is the basis of the electronic industry, and various thin films are manufactured mainly using l1 nitride technology.

Composite oxide thin films are also expected to have a wide range of applications, including optical-related devices, memory materials, piezoelectric materials, and sensors, and some have even been put into practical use. The thin film method using the Shikaji Otsuchi technology has the following problems:
Application fields have disadvantages such as internal pressure is required to increase the area, it is difficult to form films with high melting point oxides, it is difficult to change films with good crystallinity and chemistries, and productivity is low. Currently, there are restrictions on.

On the other hand, using metal alkoxide, oxide thin jl)
17. The method of forming i has been attracting attention.

This method takes advantage of the hydrolyzability of metal alkoxides, and involves first hydrolyzing a solution of metal alkoxides with water in the air after washing, and then treating the metal alkoxide solution with water to form an amorphous oxide. An abrasive film can be easily obtained.This method requires simple and inexpensive equipment (iN: is sufficient, it is easy to scale up a large area, productivity is low and cost is low, and it is homogeneous and has chemical properties. It has an advantage over deoxidation methods that use vacuum technology, such as the ability to obtain a high-quality R-container.
)k IIs”, alkaline penetration prevention film, anti-reflection 11Q
Tetraisopropyl titanate and its polymers have been applied to heat ray reflective films, optical filters, base films for promoting adhesion with organic substances, etc.

However, composite metal oxide thin films have not yet been put into practical use due to problems.

In order to obtain a complex oxide nJJ containing two or more metals, If<r, one must prepare a system in which two or more metal alkoxides are combined, or synthesize a composite metal alkoxide and decompose it to obtain the desired composite. Efforts are underway to directly obtain the oxide thermal form).

However, these methods have some drawbacks. In other words, the hydrolyzability of metal alkoxides differs markedly depending on the element and type 8 of the alkoxy group89. Therefore, a mixed system of metal alkoxides with a ratio of 2 and 1 or more is unstable and does not have a uniform composition. There is love. Furthermore, composite metal alkoxides have poor yields during synthesis, are difficult to isolate, and often contain a large amount of impurities such as alkalis and halogens that have adverse effects. Especially when the metal is a transition metal such as nickel, copper, cobalt, or zinc, many of these alkoxides are insoluble in organic solvents, so hydrolysis is difficult in systems using common solvents. However, it is not possible to change the uniform thin film. In this way, in the method of using a metal alkoxide, there is a [18 degree] in the rrJ combination that creates the code oxide, and there is little freedom. However, these drawbacks can be overcome by various NeV composite oxides using gold E (alkoxide): jj
It is clear that new uses for complex oxides will be found once cavities can be fabricated.

This invention is presented (Sai!, @ p!y, Monster F, I II
However, as a result of repeated efforts, it was found that using a solution system in which a metal alkoxide and a chemical compound were dissolved, He discovered that it has an excellent formation effect not found in other metals, and reached the conclusion of his research.

Ketones having two or more carbonyl groups, such as β-dikene, are known to form stable complexes with most metals. Made by
Industrially, it is used for various extraction and separation operations of metals in analytical chemistry.

The present invention was made in recognition of the fact that there are many common solvents in metal chelate compounds and alkoxides. Even for metal chelate compounds that are soluble in Ff1, their solubility tends to be Ff1 in the coexistence of metal alkoxides.
Furthermore, in general (many of these metal chelate compounds are used in sublimation IM equipment, the yield of the target oxide often decreases when subjected to firing treatment, but in the coexistence of metal alkoxides, sublimation This is based on the surprising fact that A? film of composite oxide can be easily obtained by heat treatment at a lower temperature than before.

Although a detailed explanation of this phenomenon has not been made, metal alkoxides and metal chelate compounds both have reactivity and form complex compounds, so if they are allowed to coexist in a dissolution medium, each separately dissolved TI'
(Instead, some 11-position or complex formation reaction occurs, resulting in a different compound than the initial one, which improves the solubility of the gold 1 bar 1 ketone complex and also improves the solubility of the gold 1 bar 1 ketone complex during heat treatment.) 1. It is thought that the sublimation property of the compound is reduced.

The metal alkoxide used in the present invention is not particularly limited as long as it can form a solution together with the total ketone polyisomer, for example, gold L- of the general formula %): Examples include alkoxides, metal alkoxides, partial gold 17+; alkoxides, metal oxides thereof, and poly-h-: alkoxides.

In addition, in the general formula (where Ml and M2 are the same or +, i, )l,'! r; Gold JrE atoms, such as lithium, sodium, potassium, rubidium, cesium, beryllium, magnesium, calcium, strontium, barium, titanium, silconium r'
11b, hafnium, vanadium, niobium, tantalum,
Chromium, molybdenum, tungsten, manganese, iron, nickel, cobalt, copper, zinc, cadmium, mercury, boron, aluminum, gallium, indium, thallium, silicon, germanium, s, lead, arsenic, antimony, bismuth, selenium, tellurium, Examples include lanthanoid metals.

B1, R2 and R are the same or different organic functional groups, preferably 1 to 20 carbon atoms, particularly preferably 1
~8 alkyl groups, aryl groups, alkenyl groups, aralkyl groups, or hydroxyl-substituted or halogen-substituted products thereof. n is the valence of metal M, m is a positive integer that is the sum of the valences of gold kP, which includes n x m, a
represents a positive integer less than n.

X is a halogen atom, an oxygen atom, a nitrogen atom, a carbon atom having 1 to 20 carbon atoms (-9, a residue of an organic functional group such as a diketone);

Among the metals M1, alkoxides that are easy to synthesize and are stable include, for example, aluminum, gallium, yttrium, indium, silicon, titanium, germanium, zirconium, tin, vanadium, niobium, antimony, tantalum, bismuth, chromium, and molybdenum. , tungsten, manganese, 4., 1: among them, iron, titanium, zirconium, silicon, and aluminum are useful.

The compound that forms an alkoxide with gold 11. As an example (:I, Takie is methyl alcohol, ethyl alcohol, n-7' propyl alcohol, isopropyl alcohol, n-butyl alcohol, isobutyl alcohol, pentyl alcohol, hexyl alcohol, 2-ethylhexyl alcohol, octyl alcohol , t-butyl alcohol, lauryl alcohol, 1,4-phthanediol, glycerin, ethylene glycol, octyl alcohol, monoargylconyl of ethylene glycol. Specific examples of metal alkoxides that can be used in the present invention include D.C. Bradley (D.O.
BracL]-eyno et al., Metal Arco Beef Size (
Metal Alkoxides, 1978, Academic Press, Inc. 1'9 may also be used.

It is preferable that the gold used in the present invention be an alkoxide (one with appropriate hydrolyzability and stability). It is determined by 6.
If the speeds are close, and when alkali gold Kl or alkaline earth gold 9i is used as the metal, the hydrolysis FN speed should be increased to 11f or faster. Therefore, it is important to appropriately determine the gold IE and alcohol to be used depending on the desired hydrolysis rate and stability.

The metal chelate compound used in the present invention is gold1. There are no particular limitations as long as it forms a solution together with the zeta alkoxide. Examples of metals forming gold chelate compounds include aluminum, barium, beryllium, calcium, cadmium, cobalt, chromium, copper, iron, gallium, mercury, indium, iridium, potassium, lithium, magnesium, and manganese. , molybdenum, sodium, nickel, lead, platinum, palladium, rhodium, ruthenium, scandium, silicon, tin, strontium, thorium, titanium, thallium, tungsten, uranium, vanadium, yttrium, zinc, zirconium, rank-made gold flat etc. or partially oxidized r1'4Jrj thereof.

Gold 1. >1; As a compound forming a chelate compound, a metal chelate compound or a metal compound formed among oxygen-containing compounds, nitrogen-containing compounds, sulfur-containing compounds, etc. that are conventionally known as chelating agents. If it forms a solution together with the alkoxide, it is not particularly controlled.

As a chelating agent, for example, EDTA (ena1/diaminetetraacetic acid), NTA and trilo 3%, 'i: acid)
, UDA (uramyl diacetic acid), dimethylglyoxime, dithizone, oxine, ketone, glycine, methyl acetoacetate, ethyl acetoacetate-1-g and monovalent carboxylic acids such as lylunic acid, oleic acid, octylic acid, oxalic acid, One or more types of polycarboxylic acids such as citraconic acid, maleic acid, phthalic acid, naphthenic acid, etc., among which ketones, methyl acetoacetate, ethylacetoacetate, monovalent carboxylic acids and polycarboxylic acids Acids are preferred, and ketones are particularly preferred.

When a ketone is used as a chelating agent, the metal chelate compound produced is, for example, -n', y Formula 11 (A)
bf: or M2 (Nori. (B) 6) is a monomer metal ketone complex or a koji compound of a metal ketone complex. It is a partial oxide, b, C and d are all positive integers, and the sum of C and d and b participate in the bonding of metal M2 with the ketone (tll Wr<).

A is a ketone having two or more carbonyl groups, and gold 7
There is no particular restriction as long as it forms a complex with M2,
For example, the general formula R0OOHR500R6 (R4 and R
are the same or different and are an alkyl group, an aryl group, an aralkyl group, an alkenyl group, or a halogen-substituted product or a sulfur-substituted product thereof, especially those having 1 to 2 carbon atoms.
β-diketones, triketones, polyketones, etc., in which 0 is indicated by a clever symbol, can be used.

B is water, a halogen atom, a phosphorus spore, a sulfur atom (ocalphonyl), and a convenient person that combines carboxyl and S.

Examples of the β-diketone include acetyl 7'cetone, benzoylacetone, dibenzoylacetone, dipivaloylmethane, dipivaloylmethane, 3-methylpentane-2-dione, 2,2-dimethylpentane-3 ,5
-Diones or their fluorides; (-mides, etc.) are preferred, with acetylacetone being particularly preferred. Triketones include (po-acetoacetylacetone, etc.).

As the metal ketone complex used in the present invention, 1j11
In addition to this, R.O.M.
metal beta diketones and allied derivatives (Mθtalβ-Dike)
-tones and Allied Derivat
j. veF3)'', published by Academic Press in 1978.

The preparation of the composite gold molten resin used in the present invention includes gold 1~.

Alkoxide and gold (E-chelate compounds or other soluble compounds require γ6, especially fS, or if they are not compatible, Idori Sougei or Must Hair 7).

Commonly used dissolving agents include, for example, monovalent alcohols; carboxylic acid esters: ketones; aliphatic hydrocarbon bath media; aromatic hydrocarbons such as benzene, toluene, and xylene; dioxane, tetrahydrofuran, etc. For example, a mixed melt containing 1 or 2 tons of organic solvents such as ether, it-methyl-2-pyrrolidone, dimethylpolamide, dimethylacetamide, and pyridine may be mentioned.

Among them, monohydric or polyhydric lower alcohols; lower carboxylic acid esters; ethers such as dioxane and tetrahydrofuran; and nitrogen-containing organic solvents such as N-methyl-2-pyrrolidone, dimethylformamide, and dimethylacetamide. Although it can be widely used in various combinations of A alkoxide and metal ketone complex, specific solvents (J) may be selected as appropriate for the combination of metal alkoxide and metal chelate compound.

The order in which the metal alkoxide and metal chelate compound are dissolved in the solvent is not particularly limited.

Gold 1 again? (? Even in combinations where one or both of the alkoxide and the metal chelate compound are not soluble in the solvent,
When adding aldehyde and heat-treating if necessary,
A homogeneous solution can be obtained. It is preferable that the heat treatment is carried out below the reflux temperature of the ordinary solvent (11).

In addition to the above-mentioned solubilizing effect, the addition of aldehyde also has the effect of further suppressing the sublimation of the kinpei ketone lead body.

Preferred aldehydes include aldehydes having 1 to 8 carbon atoms, particularly formaldehyde, paraformaldehyde, acetaldehyde, benzaldehyde, and the like.

The solubilizing effect of the addition of aldehyde is particularly excellent when the metal M2 of the metal chelate compound is a metal of Group I or Group II of Period 9, and the effect of suppressing sublimation is particularly excellent when the metal M2 is a stable metal chelate compound. ing. The amount of aldehyde used is that the total number of moles of metal M and metal M2 is 1
In this case, the above-mentioned effects are usually achieved at an amount of 0.001 mol or more, preferably 0.1 mol or more.

Although the solubilizing effect and sublimation suppressing effect of the addition of aldehyde has not yet been elucidated, some kind of reaction occurs between the aldehyde, the metal chelate compound, and the metal alkoxide, and the organic solvent of the metal ketone complex and/or metal alkoxide It is thought that this improves the solubility in the water and reduces sublimation during heat treatment.

Is it possible to arbitrarily adjust the ratio of metal alkoxide and gold compound in the composite metal solution depending on their mutual solubility and the composition of the target i′i phase mixture?
3I', 'I' alloy 1.<y''/metal M (molar ratio) is 0.0 or more, preferably gold rl'; A solution with a molar number of is easy to use.

In addition, when adding a slight lubricant component for doping, Ii (gold 1 iris alkoxide containing ζ component or gold rr1
．． The amount of the compound to be used may be extremely small.

In water valve 1, gold 17M alkoxide and total chelation 1 must each have a single composition.
It may also contain a metal alkoxide and a gold 7E chelate compound. 5
Above gold + alkoxide or all 1 chelate compound
i.1 may be used once a month as a solution of threads containing three or more components.

1ii JRLl both 1jjf (I・guka:・; in addition to the heat; 1γ; IXi'
;You may add a thin IF.
, 1 is also used to control the thickness of 1i1', :i. You can also add gold 17.
With lit] 7・'Fri! 11 compounds may be added.

However, these additives are dissolved in a common solvent and heat content;
9'r Goods ``N, 轡N・, (It is important that it does not have a negative effect on the production.

In the present invention, the FV rib-like collar joint J is 'J'::
1.7 Same as the bath solution of alkoxide alone] τ′ is hydrolyzed with γi′ (/F: 0; jλ1′−alloy 1,...'+ i' ffi+
After applying the liquid to the substrate, it is thermally decomposed and then transferred to the manufacturer.
It can be built on 6/11 with the metal included.

According to the invention, melt I! IYf gold 5t-: The alkoxide and the gold layer chelate compound were carefully determined, and 1 liter
1 (if desired, [1, 13! 2 n:;; (ii) can be replaced with H, but in particular mixed metals that cannot be obtained by using metal alkoxide alone or alkali gold with poor stability), When the purpose is to create a composite material containing alkaline earth metals or metals that cannot form metal/alkoxides, it is possible to obtain an excellent effect by uniformly mixing the components. It is played.

Furthermore, by selecting various atmospheres during heating, the instant formation of the composite material can be changed.

For example, when heating in the air, a thin layer of composite oxide is used, and when heat-treated in a reducing atmosphere containing hydrogen, carbon monoxide, etc., composite metals such as alloys i';', g I
! It is packed. Nitrogen atmosphere II containing NH3 and N2
If heat-treated under atmospheric pressure, it can be converted to densities containing titanium.

As the coating method and thermal decomposition method in the present invention, any number of methods can be adopted. For example, composite metal f(rm) is deposited on a substrate by spraying, depping, spin coating, etc., and then heated to dissipate heat. How to do it, minute IJ'l'
Methods include spraying a solution onto a heated substrate and thermally decomposing it on the substrate, gasifying the solution and then heating it to thermally decompose it, or decomposing it with ζ-oplasma or laser light and decomposing the decomposed product on the substrate. When a metal alkoxide is used alone, a method similar to a deposition method or a printing method can be adopted. In particular, methods for producing thin films using organic and spray pyrolysis are highly productive and practical using inexpensive equipment.

When producing a thin film using the coating method, the content of metal components in the melt is 0.01 to 20 h1%, preferably 0.1 to 10 tonnage%, and when the heating humidity is 200°C or higher, the depth is generally If the content Ut'l is less than the above range, the coating components may burst on the substrate and cause uneven coating. As a result, cracks may occur due to thermal strain during heat treatment and the II+i gas, or cracks may occur due to thermal decomposition and particle formation without adhesion to the substrate. However, these conditions may vary greatly depending on the combination of the metal alkoxide and gold 7 chelate compound used, the common 118 class 11, cloth means, and cloth atmosphere, and depending on each combination. It is important to determine the conditions suitable for P.

In addition, when using the dipping method, the pulling speed is 0.5~
When the time is 100 am for 7 minutes, preferably 2 to 20 am for 7 minutes, a thin film with excellent uniformity can be obtained.

When producing a film using the spray pyrolysis method, the metal in the solution is Ingredients contained) 0.01 to 20 box base%, preferably 0
．． A stable metal chelate obtained by blowing air, or an inert gas such as nitrogen, argon, or helium, or a gas containing Mizunari 4 as a carrier gas onto a substrate at a concentration of 05 to 5 fffyH%. When using a compound, especially by including water vapor in the carrier gas, decomposition is improved, film quality and stoichiometry are improved! +-, nidigureta-n:, j7i”i
It can be grown. Also, in order to improve the film quality, 1 (11μ ~
It is important to make the mist particles uniform and fine, and it is preferable to spray particles of 20 μm or less. To achieve this, it is necessary to vibrate the nozzle and the space where the mist is scattered using high frequency or ultrasonic waves to make the mist uniformly fine, or to apply an electric field between the nozzle and the substrate to quickly deposit the mist on the substrate. preferable. Note that the processing speed of the solution and the flow rate of the carrier gas vary greatly depending on the equipment, and can be adjusted to suit your needs. There is a need to.

The thickness of the thin film to be formed depends on the gold content, viscosity, coating amount, etc. of the gold IIi solution used! Although it can be
In the dipping method, a film thickness of 10% can be achieved with one application in consecutive chambers.
0 to 3000 X, preferably L-< is preferably adjusted to 100 to 1500 If it exceeds 100 lbs., it is recommended to reapply after treatment to remove the carbide.

Alternatively, the same or different instant molten ridges may be repeatedly spread to form the same or different instant ridges.

As the substrate material, it is recommended to use any material that can withstand the heat applied when forming a thin film, such as ceramic plates such as glass, alumina, and silica, metal plates such as stainless steel, and metal plates. 171, a heat-resistant film made of polyimide or the like, and a film with excellent surface flatness is particularly preferred.

Ice obtained by this invention! 1. Thin film of repellent is extremely promising as a new coconut retardant.
, J frH', Hj sensor ablation material, μλ bi1 ablation material 1, optical interface device 114; l material, magnetic recording material, pressure@
It has excellent performance as a child kidnapping test, a cosmic body shrine 1, etc.

Tsuki'ni tree-! jF', 'J', and i are explained based on Examples and Comparative Examples [! 11 However, the term ``but not occurring'' is not limited to such embodiments.

Examples 1-4 Iron triisopropoxide 10. Dy] submerged in ethyl alcohol 100yl 7<;fn' L-1 (this spinel ferrite thread j) (Fe: other metals = 2:
1) When acetylacetonates of each metal shown in Table 1 were added, all of them were quickly dissolved to form a homogeneous solution containing two types of gold (11i'+IiV). Among Kanemaro 1 acetylacetonates, nickel, Kobal 1- and zinc acetylacetonates were hardly soluble in ethyl alcohol when used alone, so they were dissolved by heating.

Corning #7913 (trade name, Vycor Glass (96%) manufactured by Corning Glass Works) was added to this solution.
After dip coating on 10 cm of SiO2]) at a pulling rate of 7 minutes, the material was heated to 800°C at a heating rate of approximately 5°C/min using a Matsufuru furnace, kept for 1 hour, and then slowly cooled. A homogeneous, reddish-brown, highly transparent thin film with a diameter of approximately 800× was deposited on a glass plate.

The composition of the obtained thin film was determined by the elemental ratio of iron to other metals by optical X-ray analysis. The results are shown in Table 1.

I was born again, 11. Since the diffraction pattern of nZ by X-ray diffraction was unclear due to its large film thickness, the composite metal solution was dried and then heat-treated in the same manner as above to produce a powder. , the crystal structure was investigated by X-ray diffraction method. The results are shown in Table 1.

AA in Table 1 11 stone% I fl indicates acetylarethonetonone (C5H702).

Example 10 g of triethoxide was added to a solution of 10 g of triethoxide (water ethyl alcohol = 2:0.5:0.5, 71/5.46 acetylacetonate). Furthermore, 0.5 g of formaldehyde was added, ethyl alcohol was removed after centrifugal flow for 30 minutes, and then 10 g of tetrahydrofuran was added.
0g was added to make a homogeneous solution. This solution was stable for over a month.

This solution was dip coated onto Corning #7059 (trade name, alkali-free glass manufactured by Corning Glass Works) in the same manner as in Examples 1 to 4, and heated at 5°C/min using a Matsufuru Furnace Trowel. When the mixture was heated to 600°C at a temperature rate, kept for 1 hour, and then allowed to cool, a yellow-brown transparent homogeneous Hj;II4,q was obtained. Elemental analysis of this grant using fluorescent X-ray analysis revealed that Fs
:Ni:Zn=2: 0.4'9: 0.47, and the objective is (Nio.5'Zr, 5)Fθ20
It was found that 4 spinel ferrite thin 111'-2 was changed.

Example 6 Iron triethoxide 15 was dissolved in 11 water ethyl alcohol IDO, 'F'e: Ba = 12'
2.2y of barium acetylacetonate was added so that the ratio was 1:1. B a (AA) 2 did not dissolve even when heated, so when paraformaldehyde 1y was further added to the depth of the solution and counterflowed for 15 minutes, the swamped barium acetylacetonate 1. dissolved and became a homogeneous solution. . This solution was stable for more than 1 month when kept tightly capped.

This solution was dip-coated onto a Vycor glass plate at a pulling rate of 10 am/min and an electric current of +r Iw, and after baking at 800°0 for 1 hour at a heating rate of 5°C/min in a Matsufuru furnace. When left to cool, the ferromagnetic N of l3a0.6 Fe 203 with a thickness of about 1oooX and excellent transparency was obtained.
(, ibj was changed.

Comparison example 1 (Fa against ioog):
25 g of iron acetylacetonate and 9.1 g of nickel acetylacetonate in an elemental ratio of N1 = 2:1.
．． When the mixture was mixed, the two types of gold were dissolved and a homogeneous melt was obtained.Using this melt Y, the same method as in Example 1 When dip-coating was performed on Vycor glass, many island-like unevenness occurred and the coating state was non-uniform.Even when this material was fired, a uniform nickel ferrite thin film could not be obtained.

Soft ratio example 2: 25g of iron triimpropoxide and 2.2g of barium diimpropoxide so that Fe:Sr=12:1
Example 5 Dissolved in 9 ml of water and 100 ml of ethyl alcohol.
When the coating was dip-coated on Vycor glass using the same method as above and then fired, a cloudy, non-uniform coating was formed on the surface of the glass. As a result, it was found that the particles did not adhere to the glass surface and had become particles.

Even if this solution was stored in a closed container, a large amount of precipitate was generated after it was left for 2 days, and it was unstable.

Example 7 16.79p of barium acetylacetonate was suspended in 100g of absolute ethyl alcohol, and barium and 41J
:Titanium tetrane propoxide i4 containing titanium in the ratio
．． When 1 g of paraformaldehyde was added to the solution for 1'.hFj, a red and uniform bath solution was obtained after 5 minutes. The solvent of this solution was replaced from ethyl alcohol to tetrahydrofuran of 11;
When stored at r+"l, it was stable for more than 1 month.

this#)'! After applying dip coating on Vycor glass using a method of Example 1 and 1,
00°C (When 13" was made with a trowel, the thickness was 12DD.
The yellow color of X was changed to transparent N'Xlj month φ.

When I checked the elemental composition of this 7:'j IE:q by ESOA (1:g spectrochemical analysis)1゛1), I found that 10
Ba;Ti:O=,,1:'l: to a depth of 00X
3, and it turned out to be ;"jj II'X': of B a T i O3.

Comparison meeting: j3 Barium diimpropoxide 12. Elg and titanium tetraisopropoxide '14.2. anhydrous ethyl alcohol H]O
When dip-coating was applied to a Vycor glass board using the same method as in Example 7 (a) using f/nf, the resultant surface was uneven and extremely white.

Note that this solution had a large amount of brown precipitate after 2 days, and it was found that the solution was poor in stability.

Claims (1)

[Scope of Claims] 1. A composite metal solution in which one or more of gold-17 pair alkoxide or its polymer and one or more metal chelate compounds is dissolved in a plate (・; Characterized by thermal decomposition. 1. Method for producing a film-like platform material. 2. Is the gold snake chelate compound a metal diketone complex? ;?Tit'l desired range The manufacturing method according to claim 1. 3. The manufacturing method according to claim 1, wherein the composite metal solution is prepared in the presence of a common solvent. 4: ij: II ff: medium carbon number 1 ~20 monohydric or polyhydric alcohols, carboxylic acid esters, alcoholic acid esters, ketones, aliphatic or aromatic hydrocarbons 7 H11', I2, ethers or nitrogen-containing solubles 11 5. The method for producing 1ieJ according to claim 1, wherein the composite metal solution is prepared in the presence of an aldehyde.