JP2003012967A - Solution material for forming dielectric thin film and method for forming dielectric thin film using the material - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a solution material for forming a dielectric thin film which can form a dielectric thin film with an improved reproducibility and a stabilized surface morphology. SOLUTION: This solution material is prepared by adding 1,500-5,000 ppm Hdpm to a mixture comprising at least one organometallic compound material and at least one organic solvent selected from among tetrahydrofuran, methyltetrahydrofuran, n-octane, isooctane, hexane, cyclohexane, pyridine, lutidine, butyl acetate, and amyl acetate.

Description

Detailed Description of the Invention

[0001]

The present invention relates to a DRAM (Dynami
c Random Access Memory) and other complex oxide dielectric thin films used for dielectric filters, etc.
osition, hereinafter referred to as MOCVD method. The present invention relates to a solution raw material for forming a dielectric thin film, which is formed by More specifically, the present invention relates to a solution raw material for forming a dielectric thin film, which improves the reproducibility of the formed film and stabilizes the surface morphology.

[0002]

2. Description of the Related Art In recent years, high integration of semiconductor memory devices such as DRAMs has been rapidly advanced for the purpose of high speed, low power consumption and low cost. However, no matter how the degree of integration is improved, the capacitor, which is a component of DRAM or the like, must have a certain capacitance. As the integration density of memory devices increases rapidly,
It is necessary to reduce the thickness of the dielectric thin film used as a capacitor, and it is becoming difficult to reduce the thickness of the conventional SiO ₂ and secure a certain capacity at the same time. Therefore, if the material can be changed to increase the dielectric constant, the capacity can be secured as in the case of thinning. Therefore, research on using a dielectric material with a high dielectric constant as the dielectric film of a capacitor for memory devices. Have been attracting attention recently. As the performance required for such a memory capacitor material, it is most important that it is a thin film having a high dielectric constant as described above and a small leak current. That is,
As long as a high dielectric constant material is used, it is necessary to make the film as thin as possible and to minimize the leakage current.

From this point of view, 2 having a higher dielectric constant is used.
The use of complex oxide-based dielectric materials consisting of oxides containing one or more metals has been investigated. Examples of such a dielectric material include lead titanate (PT), lead zirconate titanate (PZT), and lead lanthanum zirconate titanate (PL).
ZT), strontium titanate (ST), barium titanate (BT), barium strontium titanate (B
ST) and the like. Examples of the organic metal compound used as a raw material for the dielectric thin film include dipivaloylmethane ((CH ₃ ) ₃ CC
OCH ₂ COC (CH ₃ ) ₃ , hereinafter referred to as dpm. ) Etc. β-
An organometallic complex having a diketone compound as a ligand or [Zr
Metal alkoxides such as (Ot-Bu) ₄ ] are commonly used. Both metal alkoxides and β-diketonato complexes are used as raw materials for metals such as Ti, Zr and Ta.
A β-diketonato complex is mainly used as a metal raw material of or.

The β-diketonato complex is generally susceptible to deterioration under the influence of moisture and carbon dioxide in the air. In addition, during storage, an oligomer is formed to increase the molecular weight and increase the evaporation temperature, which easily causes alteration. For example, dpm is a typical β-diketone compound, but its metal complex, [Ba (dpm) ₂ ] and [Sr (dpm) ₂ ], should be stored in a desiccator when storing them. Even if the value is paid, the TG (Thermogravimetry) is changed, and it is extremely unstable. Therefore, β-
The diketonato complex requires meticulous care in order to prevent deterioration during storage and during handling, and has poor operability as a raw material. Therefore, as a means for suppressing the deterioration of the organometallic compound as the raw material, the purity of the organometallic compound has been increased to achieve long-term storage stability.

As a method of forming a complex oxide-based dielectric thin film, a sol-gel method in which a metal alkoxide raw material is spin-coated to form a film on a substrate has been extensively studied so far. Since the sol-gel method does not vaporize the metal component, the composition control of the film is easy. However, the capacitor electrode of the DRAM has a step, and the higher the degree of integration, the larger the step becomes and becomes complicated. Therefore, it is difficult to uniformly form the dielectric thin film on the electrode serving as the substrate by the spin coating method.
Therefore, in recent years, in view of high integration of devices, a dielectric thin film is formed by MOCVD method which is excellent in step coverage (= step coverage, throwing power to the surface of a complicated shape with steps). Research has been activated.

In the MOCVD method, a metal oxide produced by heating an organic metal compound, which is a raw material of various metals, under reduced pressure to vaporize the vapor, transporting the vapor to a film forming chamber and thermally decomposing it on the substrate. Is a method of adhering to the substrate. M
The OCVD method is generally performed because it has better step coverage than other film manufacturing methods. In the formation of the dielectric thin film by this MOCVD method, initially, the raw material organometallic compound was directly heated and vaporized, and the generated vapor was sent to the film forming chamber for film formation. However, organic metal compound raw materials, especially compounds such as the dpm complex recommended for MOCVD, have poor long-term storage stability and vaporization characteristics, and must be stably transported to the CVD reaction part by heating at low temperatures. Was impossible. Further, when heating at a high temperature in order to increase the vaporization efficiency of the raw material, the raw material is transported while being thermally decomposed before reaching the film forming chamber, resulting in poor crystallinity of the film and compositional deviation. Therefore, it is difficult to stably transport the raw material of the organometallic compound to the film forming chamber, the expensive raw material becomes disposable after each film formation, and it is difficult to control the composition of the film. There is also a problem that it is not possible to form a dielectric film having Further, in this method, when the vaporization rate is suppressed and the synthesis (reaction) time is lengthened, the stability of the raw material deteriorates over time and the vaporization property gradually decreases, so that the formed film is It is unavoidable that the composition in the thickness direction becomes inhomogeneous and the leak current increases.

As a method for solving the above-mentioned problems, a solution vaporization CVD method capable of stably supplying a raw material organometallic compound to a film forming chamber is widely used at present. This solution vaporization CVD method is an improvement of the MOCVD method, and is a solid C
This is a method of dissolving a VD raw material in various organic solvents and supplying it as a liquid to a CVD apparatus.

[0008]

However, although the effect of improving the long-term storage stability of the solution raw material was obtained by highly purifying the organometallic compound as the raw material, the highly purified raw material was used by the MOCVD method. When a dielectric thin film is formed on a substrate by using
As shown in FIG. 5, the so-called abnormal growth of the film has been observed, in which the thin film 2 is formed only on the bottom of the trench or the hole of the substrate 1, and the remarkable grain growth occurs on the film surface. 3 is a diagram in which a thin film is not formed at the bottom of the trench and the thin film formed outside the trench is abnormally grown, FIG. 4 is a diagram in which the thin film formed at the bottom of the trench is abnormally grown, and FIG. 5 is shown at the top of the trench. It is the figure which the thin film grew abnormally so that a trench might be covered.

An object of the present invention is to provide a solution material for forming a dielectric thin film, which can improve the reproducibility of the formed dielectric thin film and stabilize the surface morphology.

[0010]

The invention according to claim 1 is
Selected from the group consisting of one or more organic metal compound raw materials and tetrahydrofuran (hereinafter referred to as THF), methyltetrahydrofuran, n-octane, isooctane, hexane, cyclohexane, pyridine, lutidine, butyl acetate and amyl acetate. 2,2,6,6-as an additive to a raw material liquid prepared by mixing one or more organic solvents
It is a solution raw material for forming a dielectric thin film, which contains 1500 to 5000 ppm of tetramethyl-3,5-heptanedione (hereinafter referred to as Hdpm). In the invention according to claim 1, Hdpm is 1500 to 5000 pp as an additive in a raw material liquid in which an organic metal compound raw material is dissolved in an organic solvent.
By including m, Hdpm suppresses intramolecular and intermolecular interactions of the organometallic compound, so that the dielectric thin film formed by using this solution raw material has good film reproducibility and stabilized surface morphology. It The amount of Hdpm added is 1
It is 500 to 5000 ppm. Preferably 3000 to
It is 4000 ppm. If the added amount is less than the lower limit value,
Intramolecular and intermolecular interactions of the organometallic compound cannot be suppressed, and effects such as improvement in film reproducibility and stabilization of surface morphology do not appear. If the amount added exceeds the upper limit, the thin film to be formed causes abnormal growth.

The invention according to claim 2 is the invention according to claim 1, which is a solution raw material in which the organometallic compound is a compound in which a metal atom is bonded to an organic group through an oxygen atom. The invention according to claim 3 is the invention according to claim 2, wherein the organometallic compound is a compound selected from the group consisting of a metal alkoxide, a metal β-diketonato complex, and a mixture of a metal alkoxide and a β-diketonato complex. It is a solution raw material. The invention according to claim 4 is the invention according to claim 3, wherein the alkoxide is isopropoxide or tert-butoxide, and the β-diketonato complex is a dipivaloylmethanato complex. The invention according to claim 5 is the invention according to claim 4, wherein the organometallic compound is B
a and Sr dipivaloylmethanato complex and isopropoxide, tert-butoxide, dipivaloylmethanato complex, a mixture of isopropoxide and dipivaloylmethanato complex, and tert-butoxide and dipivaloylmethanato complex A solution raw material which is a Ti compound selected from the group consisting of a mixture with a complex and whose dielectric thin film is a barium strontium titanate complex oxide thin film. The invention according to claim 6 is the invention according to claim 4, wherein the organometallic compound is P
b with the dipivaloylmethanato complex and tert-butoxide,
A Zr compound selected from the group consisting of dimethylheptadionate complex and isopropoxide, and isopropoxide,
tert-butoxide, dipivaloylmethanato complex, a mixture of isopropoxide and dipivaloylmethanato complex, and
The solution raw material is a Ti compound selected from the group consisting of a mixture of tert-butoxide and a dipivaloylmethanato complex, and the dielectric thin film is a lead zirconate titanate complex oxide thin film.

The invention according to claim 7 is, as shown in FIG. 2, a complex oxide type dielectric thin film formed on a substrate 13 by a metal organic chemical vapor deposition method using the solution raw material according to any one of claims 1 to 6. 15 is a method of forming 15. The invention according to claim 8 is the invention according to claim 7, which is a method of forming a dielectric thin film by a metal organic chemical vapor deposition method by supplying a solution raw material in a liquid state to a vaporization chamber. The invention according to claim 9 is the invention according to claim 8, which is a method for supplying separate solution raw materials for each metal to the vaporization chamber. In the invention according to any one of claims 7 to 9, claims 1 to 6
By forming a complex oxide-type dielectric thin film on a substrate by MOCVD using any of the solution raw materials described above, it is possible to obtain a dielectric thin film with good film-forming reproducibility and stabilized surface morphology.

The invention according to claim 10 is a complex oxide type dielectric thin film formed on a substrate by the method according to any one of claims 7 to 9. The invention according to claim 11 is a dielectric thin film made of barium strontium titanate formed on a substrate by the method according to any one of claims 7 to 9. The invention according to claim 12 is a dielectric thin film made of lead zirconate titanate formed on a substrate by the method according to any one of claims 7 to 9.

[0014]

BEST MODE FOR CARRYING OUT THE INVENTION Next, embodiments of the present invention will be described. Examples of the complex oxide-based dielectric thin film that can be formed from the solution raw material according to the present invention include lead titanate (PT), lead zirconate titanate (PZT), lead lanthanum zirconate titanate (PLZT), and titanium. Examples thereof include thin films of strontium acid salt (ST), barium titanate (BT), barium strontium titanate (BST), and the like, but other thin films are also applicable.

As the organic metal compound raw material, an organic compound containing a metal selected from Pb, Ti, Zr and alkaline earth metals (Ca, Ba, Sr, etc.), which are the constituent metals of the thin film, is used. In addition, alkali metal (C
s), various transition metals such as Mn, Nb and V, and rare earth metals such as La may also be used. In the case of a BST thin film, organometallic compounds of Ti, Ba and Sr are used as raw materials.

The organometallic compound raw material is vaporizable,
A substance that is thermally decomposed by heating and easily transformed into an oxide by introducing an oxidizing agent (oxygen) is used. Such an organometallic compound is generally a compound having a structure in which a metal atom is bonded to an organic group through an oxygen atom. Examples of preferred compounds of this type include metal alkoxides, metal β-diketonato complexes, and mixtures of metal alkoxides and β-diketonato complexes. Examples of β-diketonato complexes include:
Acetylacetone, hexafluoroacetylacetone,
There are metal complexes having β-diketones such as dpm and pentafluoropropanoylpivaloylmethane as ligands. Of these, preferred is a complex with dpm. The metal alkoxide preferably has an alkoxy group having 1 to 6 carbon atoms, and particularly preferably has a branched alkoxy group (isopropoxide, tert-butoxide, etc.). Particularly preferred organometallic compounds are metal dipivaloylmethanato complexes, metal isopropoxides, metal tert-butoxides, mixtures of metal isopropoxides and dipivaloylmethanato complexes, metal tert-butoxides and dipivaloylmethanato complexes. It is a mixture of complexes. For alkaline earth metals, alkali metals and Pb, it is preferable to use β-diketonato complexes (for example, dipivaloylmethanato complex), and Ti, Z
Regarding the transition metals such as r, V, and Nb, generally, both β-diketonato complex and metal alkoxide can be used, and a mixture of metal alkoxide and β-diketonato complex can also be used.

Materials for forming a BST thin film include dipivaloylmethanato complexes of Ba and Sr, isopropoxide, tert-butoxide, dipivaloylmethanato complex, and isopropoxide and dipivaloylmethanato complex. Preference is given to using Ti compounds selected from mixtures and mixtures of tert-butoxide and dipivaloylmethanato complexes.
In addition, as a raw material for forming the PZT thin film, a Pb dipivaloylmethanato complex, a Zr compound selected from the group consisting of tert-butoxide, a dimethylheptadionate complex, and isopropoxide, isopropoxide, and tert-butoxide. It is possible to use a Ti compound selected from the group consisting of butoxide, dipivaloylmethanato complex, mixture of isopropoxide and dipivaloylmethanato complex and mixture of tert-butoxide and dipivaloylmethanato complex. preferable.

The organic solvent may be one or more selected from the group consisting of THF, methyltetrahydrofuran, n-octane, isooctane, hexane, cyclohexane, pyridine, lutidine, butyl acetate and amyl acetate. Preferred is THF.

The solution raw material for forming a dielectric thin film of the present invention is 1
Hdpm 1500 as an additive to a raw material liquid obtained by mixing one or more kinds of organometallic compound raw materials and an organic solvent.
It is characterized by containing ˜5000 ppm.

For example, as an organometallic compound [Ba (d
pm) ₂ ] and THF as an organic solvent and the organic metal compound is dissolved in the organic solvent, the raw material liquid is [Ba (dp
[alpha] orbital is empty in the metal element Ba in m) ₂ ], the bond cleavage between the metal Ba and the ligand dpm occurs in the molecule of the organometallic compound (intramolecular cleavage). ), Further, intermolecular polymerization between the metal Ba and the ligand dpm occurs,
It is massified. Since the oligomer that has been polymerized becomes thermally unstable, when it is vaporized in the vaporization chamber of the CVD apparatus, it is heated and divided into indeterminate small molecules and organic compounds, and small molecules are formed in the film formation chamber. Molecules that are partially oligomers will be supplied at the same time. Therefore, the dielectric thin film formed on the substrate does not have reproducibility of film formation on the surface covered with the step of the submicron unit, and the surface is roughened to cause abnormal morphology.

Hdpm was added to this raw material liquid as an additive in an amount of 15
By including 0.005 to 5000 ppm, Hdpm stabilizes the compound by bidentate chelate coordination, which causes a trap effect on the empty α orbital of the metal element and suppresses intermolecular polymer formation. Stable vaporization during formation is maintained, the film reproducibility of the formed dielectric thin film is improved, and the morphology of the thin film surface is stabilized.
Although an organometallic compound containing Ba has been described as an example, T
A similar coordination stabilizing effect can be obtained for an organometallic compound containing i or Sr.

As a method for preparing the solution raw material of the present invention, two or more kinds of organic metal compounds containing each metal element constituting the dielectric thin film are dissolved together or separately in an organic solvent, and further an additive is added. Hdpm as 1500-5000
A solution raw material used for forming a dielectric thin film by the MOCVD method is prepared by including the same in the amount of ppm. M using this solution raw material
A dielectric thin film is formed on a substrate or another substrate by the OCVD method. In this embodiment mode, the MOCVD method is a solution vaporization CVD method in which each solution is supplied to a heated vaporization chamber, each solution raw material is instantly vaporized, and the vaporized material is sent to the film formation chamber.

As shown in FIG. 2, the MOCVD apparatus comprises a chamber 10 and a steam generator 11. Chamber 10
A heater 12 is provided inside the substrate, and a substrate 13 is held on the heater 12. The inside of the chamber 10 is evacuated by a pipe 17 including a pressure gauge 14 and a needle valve 16. The steam generator 11 includes a raw material container 18, and the raw material container 18 stores a solution raw material in which an organic metal compound is dissolved in an organic solvent and further an additive is added. A carrier gas introduction pipe 21 is connected to the raw material container 18 via a gas flow rate control device 19, and a supply pipe 22 is connected to the raw material container 18. Needle valve 23 on supply pipe 22
Also, a solution flow rate controller 24 is provided, and the supply pipe 22 is connected to the vaporization chamber 26. A carrier gas introduction pipe 29 is connected to the vaporization chamber 26 via a needle valve 31 and a gas flow rate adjusting device 28. The vaporization chamber 26 is further connected to the chamber 10 by a pipe 27. In this device, N ₂ , H
A carrier gas composed of an inert gas such as e or Ar is introduced into the raw material container 18 from the carrier gas introduction pipe 21, and the solution raw material stored in the raw material container 18 is conveyed to the vaporization chamber 26 by the supply pipe 22. The organometallic compound that has been vaporized in the vaporization chamber 26 to become vapor is further injected into the carrier gas introduction pipe 28.
2 by the carrier gas introduced into the vaporization chamber 26 from
It is supplied into the chamber 10 via 7. In the chamber 10, the vapor of the raw material organometallic compound is thermally decomposed, and the metal oxide generated thereby is deposited on the heated substrate 13 to form a dielectric thin film.

The solution raw material of the present invention has stable vaporization of each raw material compound in a solution state, and the metal atomic ratio of the formed thin film is almost the same as the metal atomic ratio in the solution. A complex oxide-based dielectric thin film having a predetermined composition can be formed, and the quality of the film is stable.

The dielectric thin film formed by the MOCVD method using the solution raw material of the present invention is useful as a DRAM capacitor. The MOCVD method is generally excellent in step coverage, but when the solution raw material of the present invention is used, the film-forming reproducibility is improved and the surface morphology is stabilized as compared with the thin film formed using the conventional solution raw material. Further, the solution raw material of the present invention has excellent composition controllability of the film because the vapor of each raw material compound can be stably supplied to the film forming chamber as described above, and a dielectric material having a desired composition and dielectric properties can be obtained. The body thin film can be stably formed on the substrate. The dielectric thin film formed by using the solution raw material of the present invention can also be used as a dielectric filter in a piezoelectric resonator, an infrared sensor, or the like.

[0026]

EXAMPLES Next, examples of the present invention will be described together with comparative examples. Example 1 First, as an organic barium compound, a bis (dipivaloylmethanato) barium complex [Ba (dp
m) ₂ ], a bis (dipivaloylmethanato) strontium complex [Sr (dp
m) ₂ ] and bisisopropoxybisdibivaloylmethanato titanium complex [Ti (O-i-
Pr) ₂ (dpm) ₂ ] was prepared. Further, THF was prepared as an organic solvent and Hdpm was prepared as an additive.
Next, each organic metal compound raw material and THF are mixed to form THF.
A raw material liquid is prepared by dissolving each organometallic compound raw material in
Furthermore, 1500 ppm of Hdpm was added to this raw material liquid to prepare a BST dielectric thin film solution raw material.

<Example 2> The addition amount of Hdpm was 5,000.
A solution raw material for a BST dielectric thin film was prepared in the same manner as in Example 1 except that ppm was used.

Comparative Example 1 A solution raw material for a BST dielectric thin film was prepared in the same manner as in Example 1 except that no additive was added. <Comparative Example 2> A solution raw material for BST dielectric thin film was prepared in the same manner as in Example 1 except that the addition amount of Hdpm was 1000 ppm. <Comparative Example 3> A solution raw material for a BST dielectric thin film was prepared in the same manner as in Example 1 except that the added amount of Hdpm was 5100 ppm.

<Comparison Evaluation> Examples 1-2 and Comparative Examples 1--2
The solution raw materials for BST dielectric thin film prepared in
It is divided into two parts and introduced into a MOCVD apparatus as shown in FIG.
Two types of BST dielectric thin films were formed on each substrate. Atomic force microscope (Atomic Force Microscop)
e: AFM) and Scanning Tunnel Microscope
ing Microscope, hereinafter referred to as STM. ) Etc. were used to measure the film quality of the thin film formed on the substrate surface. The surface of each of the formed dielectric thin films was observed to examine the surface morphology. BST of Examples 1-2 and Comparative Examples 1-3
Table 1 shows the long-term storage stability of the solution raw material for the dielectric thin film, the film-forming reproducibility of the formed dielectric thin film, and the surface morphology.

[0030]

[Table 1]

As is clear from Table 1, in Comparative Example 1 in which the solution raw material containing no additive is used, the film reproducibility is poor and the surface morphology is not stable. Further, in Comparative Examples 2 and 3 in which the added amount of Hdpm as an additive is out of the range of the present invention, as shown in FIGS. 3 to 5, there are variations in film quality, and a film is formed only on the trench bottom. In addition, the surface morphology was not stable due to abnormal growth of the thin film outside the trench. On the other hand, in Examples 1 and 2, as shown in FIG. 1, the dielectric thin film formed by using the solution raw material of the present invention had good film-forming reproducibility and stabilized surface morphology. I understand.

[0032]

As described above, the solution raw material for forming a dielectric thin film of the present invention includes one or more organic metal compound raw materials, tetrahydrofuran, methyltetrahydrofuran, n-octane, isooctane, hexane and cyclohexane. Hdpm as an additive to a raw material liquid prepared by mixing one or more organic solvents selected from the group consisting of pyridine, lutidine, butyl acetate and amyl acetate.
Since Hdpm suppresses the intramolecular and intermolecular interactions of the organometallic compound by containing 0 to 5000 ppm, the film reproducibility of the dielectric thin film formed by using this solution raw material is improved and the surface morphology is improved. Stabilized.

[Brief description of drawings]

FIG. 1 is a diagram showing a surface morphology around a trench of a dielectric thin film formed on a substrate by using a solution raw material for forming a dielectric thin film of the present invention.

FIG. 2 is a schematic diagram of a MOCVD apparatus.

FIG. 3 is a diagram showing a surface morphology around a trench of a dielectric thin film formed on a substrate by using a conventional solution raw material for forming a dielectric thin film.

FIG. 4 is a view showing a surface morphology around a trench of a dielectric thin film formed on a substrate by using another conventional solution raw material for forming a dielectric thin film.

FIG. 5 is a view showing a surface morphology around a trench of a dielectric thin film formed on a substrate using another conventional solution raw material for forming a dielectric thin film.

[Explanation of symbols]

13 board 15 Dielectric thin film

─────────────────────────────────────────────────── ─── Continuation of front page (51) Int.Cl. ⁷ Identification code FI theme code (reference) H01L 27/105 C07F 3/00 F 5F058 27/108 7/00 A 5F083 // C07F 3/00 7/24 7/28 F 7/00 H01L 27/10 444C 7/24 651 7/28 (72) Inventor Hiroto Uchida 1-297 Kitabukurocho, Saitama City, Saitama Prefecture Mitsubishi Materials Corporation Research Institute (72) Inventor Katsumi Ogi 1-297 Kitabukuro-cho, Saitama-shi, Saitama Prefecture F-term in the Research Institute of Mitsubishi Materials Corporation (reference) 4H006 AA03 AB82 4H048 AA01 AA03 AB78 VA60 VB10 VB30 4H049 VN04 VN05 VN06 VP01 VQ21 VQ24 V21 VQ21 VQA VJ02 VV22 VV09 V038 V038 JC38 KA03 NA17 4K030 AA11 BA01 BA18 BA42 LA19 5F058 BA11 BC03 BC04 BC20 BF06 BF27 BJ01 5F083 AD00 FR01 GA06 JA13 JA14 JA15 JA17 PR2 1

Claims (12)

[Claims] 1. A raw material of one or more organic metal compounds, tetrahydrofuran, methyltetrahydrofuran,
2,2 as an additive to a raw material liquid prepared by mixing one or more organic solvents selected from the group consisting of n-octane, isooctane, hexane, cyclohexane, pyridine, lutidine, butyl acetate and amyl acetate A solution raw material for forming a dielectric thin film, which comprises 1,500 to 5,000 ppm of 6,6,6-tetramethyl-3,5-heptanedione. 2. The solution raw material according to claim 1, wherein the organometallic compound is a compound in which a metal atom is bonded to an organic group through an oxygen atom. 3. The solution raw material according to claim 2, wherein the organometallic compound is a compound selected from the group consisting of a metal alkoxide, a metal β-diketonato complex and a mixture of a metal alkoxide and a β-diketonato complex. 4. The alkoxide is isopropoxide or te.
The solution raw material according to claim 3, which is rt-butoxide and the β-diketonato complex is a dipivaloylmethanato complex. 5. A dipivaloylmethanato complex in which the organometallic compound is Ba and Sr, isopropoxide, tert-butoxide, dipivaloylmethanato complex, a mixture of isopropoxide and dipivaloylmethanato complex, and The solution raw material according to claim 4, comprising a Ti compound selected from the group consisting of a mixture of tert-butoxide and a dipivaloylmethanato complex, wherein the dielectric thin film is a barium strontium titanate complex oxide thin film. 6. A dipivaloylmethanato complex whose organometallic compound is Pb, a Zr compound selected from the group consisting of tert-butoxide, a dimethylheptadionate complex and isopropoxide, and isopropoxide and tert-butoxide. ,
Dipivaloylmethanato complex, composed of a Ti compound selected from the group consisting of a mixture of isopropoxide and dipivaloylmethanato complex and a mixture of tert-butoxide and dipivaloylmethanato complex, the dielectric thin film The solution raw material according to claim 4, which is a lead zirconate titanate composite oxide thin film. 7. A method of forming a complex oxide type dielectric thin film (15) on a substrate (13) by a metal organic chemical vapor deposition method using the solution raw material according to any one of claims 1 to 6. 8. The method according to claim 7, wherein the dielectric thin film is formed by a metal organic chemical vapor deposition method by supplying a solution raw material in a liquid state to a vaporization chamber. 9. The method according to claim 8, wherein separate solution raw materials for each metal are supplied to the vaporization chamber. 10. A complex oxide type dielectric thin film formed on a substrate by the method according to claim 7. 11. A dielectric thin film made of barium strontium titanate formed on a substrate by the method according to claim 7. 12. A dielectric thin film made of lead zirconate titanate formed on a substrate by the method according to claim 7.