JP2014218691A - Method for producing layered structure - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a method for producing a layered structure, which makes it possible to produce the layered structure having a characteristic equivalent to that obtained by a conventional ALD method and which is excellent in productivity as compared with the conventional ALD method.SOLUTION: The method comprises: a lamination step of successively supplying a first gas phase material containing a first coordination compound having a first ligand and a second gas phase material containing a second coordination compound having a second ligand to form, on a substrate, a laminate composed of layers based on the respective gas phase materials laminated thereon; and a chemical conversion step of forming a layered structure from the laminate, the chemical conversion step including application of a chemical reaction to the laminate. The laminate can maintain a form of a layered body on the substrate by means of at least one of a chemical bond and a chemical interaction between the first coordination compound and the second coordination compound within a temperature range which is equal to or lower than an upper limit temperature of an ALD window of the first coordination compound and which is equal to or lower than an upper limit temperature of an ALD window of the second coordination compound. The chemical reaction, which is performed in the chemical conversion step, is not performed in the lamination step.

Description

  The present invention relates to a method for manufacturing a layered structure such as a thin film. Specifically, a multi-component thin film using an atomic layer deposition method (also referred to as “ALD method” in this specification) can be manufactured. The present invention relates to a method for manufacturing a layered structure.

  The ALD method is a technique for forming a single-layer film based on a reaction gas on a substrate and forming a thin film (such as an oxide film) based on the single-layer film. It is characterized by high coverage, and is used as a method for manufacturing an insulating film (dielectric film) such as Sr—Ti—O or Al—Ti—O.

If this insulating film made of strontium titanate is taken as a specific example, its production requires eight steps as shown in Patent Document 1 and the like.
First step: A precursor containing strontium is supplied, and the precursor is adsorbed on the substrate.
Second step: A purge gas is supplied to perform a primary purge of the reaction chamber, thereby forming a precursor monolayer (Sr-based monolayer) containing strontium on the substrate.
Third step: A reactive gas containing oxygen is supplied to oxidize the Sr-based single layer formed in the first step, thereby forming a layered body (Sr-O layer) containing a strontium oxide.
Fourth step: Purging gas is supplied to perform secondary purging of the reaction chamber to remove oxygen-containing reaction gas.
5th process: The precursor containing titanium is supplied and the said precursor is made to adsorb | suck on the Sr-O layer formed on the board | substrate.
Sixth step: A purge gas is supplied to perform a third purge of the reaction chamber to form a precursor monolayer (Ti-based monolayer) containing titanium on the Sr—O layer.
Seventh step: A layer containing titanium oxide is formed on the Sr—O layer by oxidizing the Ti-based single layer formed in the fifth step by supplying a reaction gas containing oxygen.
Eighth step: A purge gas is supplied to perform a fourth purge of the reaction chamber to remove the reaction gas containing oxygen.

Japanese Patent No. 4153236

  As described above, the conventional ALD method requires 8 steps to form a single Si—Ti—O-based thin film, and cannot be said to be a method with excellent productivity. For this reason, there is a strong demand for a method for producing a thin film that can produce a multi-component film equivalent to the conventional ALD method but is more excellent in productivity.

  The present invention is a layered structure that can produce a multi-component thin film by a method that is more productive while being equivalent to the conventional ALD method in terms of film thickness uniformity and step coverage height. An object is to provide a manufacturing method.

The present invention provided to solve the above problems includes the following contents.
(1) Sequentially a first gas phase material containing a first coordination compound having a first ligand and a second gas phase material containing a second coordination compound having a second ligand Forming a layered structure from the laminate including a laminating step of forming a laminate on the substrate by laminating layers based on respective vapor phase materials and supplying a chemical reaction to the laminate A chemical conversion step, wherein the first coordination compound and the first coordination compound in a temperature range below the upper limit temperature of the ALD window of the first coordination compound and below the upper limit temperature of the ALD window of the second coordination compound Due to at least one of a chemical interaction and a chemical bond with the second coordination compound, the layered body can be maintained in the form of a layered body on the substrate. In the layering step, the chemical conversion step is performed. Layered structure characterized by no chemical reaction The method of production.

(2) The manufacturing method according to (1), wherein the chemical reaction performed in the chemical conversion step includes an oxidation reaction.

(3) The chemical reaction in the chemical conversion step includes, as an elementary process, a reaction in which at least one of the first ligand and the second ligand is desorbed from the laminate. The layered structure containing an element based on a central substance of the first coordination compound and an oxide of an element based on the central substance of the second coordination compound is formed on the substrate as described in (2) above. Manufacturing method.

(4) The ALD window of the first vapor phase material and the ALD window of the second vapor phase material have overlapping temperature regions, and the stacking step and the chemical conversion are performed within the overlapping temperature region. The method according to any one of (1) to (3), wherein the step is performed.

(5) At least one of the first gas phase material and the second gas phase material contains an additional substance that is a substance other than the first coordination compound and the second coordination compound, (1) The manufacturing method as described in any one of (4).

  The present invention provides a method for producing a layered structure with higher productivity than the conventional ALD method.

Hereinafter, embodiments of the present invention will be described in detail.
1. Manufacturing Process A manufacturing method according to an embodiment of the present invention includes a first gas phase material including a first coordination compound having a first ligand and a second coordination having a second ligand. A laminating step for sequentially supplying a second gas phase material containing a compound to form a laminate on which a layer based on each gas phase material is laminated, and a chemical forming step for subjecting the laminate to a chemical reaction; Is provided. The laminate formed by the laminating step has a chemical interaction between the first coordination compound and the second coordination compound within the temperature range of at least a part of the ALD window of the second vapor phase material, and Due to at least one of the chemical bonds, the laminate can maintain the form of the layered body on the substrate. In the lamination process, the chemical reaction performed in the chemical conversion process is not performed. In the present specification, the chemical bond means a generic name of a covalent bond and an ionic bond, and the chemical interaction is an interaction other than a chemical bond, specifically, a van der Waals interaction, It means generic terms such as Coulomb interaction, hydrogen bond, and π-π interaction. In the present specification, these chemical bonds and chemical interactions may be collectively referred to as “chemical interactions and the like”.

(1) Lamination process The lamination process according to the present embodiment includes the following four sub-processes.
(1-1) First laminating step In the first laminating step, a first gas phase material containing a first coordination compound having a first ligand is placed in a reaction chamber in which a substrate is arranged. The first coordination compound is saturatedly adsorbed on the substrate. In the stage of the first lamination step, the first coordination compound may be further adsorbed on the first coordination compound adsorbed on the substrate. In addition, the kind of board | substrate is not specifically limited. Examples include a silicon substrate and a glass substrate. In the case of a silicon substrate or the like, an oxide film may be formed on the surface thereof.

  The temperature in the vicinity of the substrate in the first stacking step and the substrate in the reaction chamber (also referred to as “first stacking temperature” in this specification) is a temperature at which the first coordination compound can be saturated and adsorbed on the substrate. There is no particular limitation.

  The first gas phase material may be composed of the first coordination compound, or may contain a carrier gas or the like as a substance other than the first coordination compound. The type of carrier gas in this case is not particularly limited, and examples include hydrogen gas and the like in addition to rare gases such as argon. The first gas phase material is a substance that does not chemically interact with the second coordination compound as a substance other than the first coordination compound, and is similar to the first coordination compound. The substance which can adsorb | suck to a board | substrate may be included. Such a substance is also referred to as a first additional substance. Details of the first addition substance will be described later together with details of the first coordination compound.

  Note that the first coordination compound adsorbed on the substrate is different from the first coordination compound as a result of the interaction with the deposition target such as the substrate (for example, one or more ligands are in the first coordination. Or a state in which the coordination form of the ligand is changed.). In this specification, the material in such a state is also referred to as a first coordination compound for convenience.

  In addition, the first lamination step includes the first coordination on the layered structure formed by passing through the primary purge step to the chemical conversion step (which may further include a tertiary purge step) described below. This includes the case where a compound is adsorbed. Thus, you may adjust the whole thickness of a layered structure by repeating the manufacturing process of the layered structure which concerns on this embodiment.

(1-2) Primary Purge Step In the primary purge step, instead of supplying the first vapor phase material, a purge gas is supplied to the reaction chamber to purge the reaction chamber. By this step, basically, the first gas phase material other than the first coordination compound adsorbed on the substrate is discharged out of the reaction chamber. As a result, a single layer of the first coordination compound (also referred to as “first single layer” in this specification) is formed on the substrate. In the primary purge step, at least one of before and after supplying the purge gas may include an evacuation operation of the reaction chamber, or instead of supplying the purge gas, the reaction chamber is evacuated to the outside of the reaction chamber of the first gas phase material. May be discharged. In this specification, the exhausting operation of the reaction chamber included in such a purging step is also referred to as “vacuum purging”.

  The temperature in the primary purge step and in the vicinity of the substrate in the reaction chamber (also referred to herein as “first purge temperature”) is such that the first coordination compound is formed so that a first monolayer is formed. The temperature is within the ALD window. The kind of purge gas is not particularly limited, and a known material such as argon or nitrogen molecule can be used as appropriate.

  Note that in this specification, an “ALD window” refers to a material based on a substance that is adsorbed (physical adsorption or chemical adsorption) on a deposition target. This means a temperature region in which the single layer film can be maintained. When the temperature is lower than the ALD window, the substance is condensed on the surface of the deposition target, and it is difficult to stably form the single layer film. On the other hand, when the temperature is higher than the ALD window, the substance cannot be stably adsorbed on the deposition target, or the substance is decomposed on the surface of the deposition target. It becomes difficult to form a layer film stably. The ALD window is determined by the substance to be adsorbed and the deposition target, and is relatively highly dependent on the substance to be adsorbed.

  When the first vapor phase material includes the first additive substance, a layer of the first additive substance may be formed on the substrate. If the first purge temperature is within the ALD window of the first additive material, the first additive material layer can coexist on the substrate with the first monolayer.

(1-3) Second laminating step In the second laminating step, a second gas phase material containing a second coordination compound having a second ligand is supplied into the reaction chamber. The second coordination compound is saturatedly adsorbed on the monolayer by chemical interaction or the like. In the second lamination step, the second coordination compound may be further adsorbed on the second coordination compound adsorbed on the first monolayer.

  The temperature in the vicinity of the substrate in the second lamination step and the substrate in the reaction chamber (also referred to as “second lamination temperature” in this specification) is the second coordination compound in a state where the first monolayer is maintained. So that the second coordination compound is saturated on the first monolayer by chemical interaction or the like, at a temperature below the upper limit of the ALD window of the first coordination compound. The temperature can be absorbed.

  In the case where the first gas phase material contains the first additive substance, the first additive substance is used if the second lamination temperature is not higher than the upper limit temperature of the ALD window of the first additive substance. The second coordination compound can be adsorbed onto the first additional material layer while the first layer coexists with the first monolayer on the substrate.

  The second gas phase material may be composed of the second coordination compound, or may contain a carrier gas or the like as a substance other than the second coordination compound. The kind of carrier gas is not particularly limited, and examples include hydrogen and the like in addition to a rare gas such as argon. The second gas phase material may contain a substance that can be adsorbed on the first additional substance layer as a substance other than the second coordination compound. Such a substance is also referred to as a second additional substance. When the second addition substance does not cause chemical interaction or the like with the first coordination compound, the second coordination compound can be preferentially formed on the first monolayer. On the other hand, when the second addition substance can cause chemical interaction with the first coordination compound, the adsorption of the second addition substance to the first monolayer is Adsorption and competition. Details of the second addition substance will be described later together with details of the second coordination compound.

  In addition, the second coordination compound adsorbed on the first monolayer is the second coordination compound as a result of chemical interaction with the material (first coordination compound) constituting the first monolayer. The state is different from that of the compound (for example, one or more ligands are in a state of being detached from the second coordination compound, or the ligand is in a changed state of coordination. It may be. In this specification, the material in such a state is also referred to as a second coordination compound for convenience.

(1-4) Secondary Purge Step In the secondary purge step, instead of supplying the second gas phase material, a purge gas is supplied to the reaction chamber to purge the reaction chamber. By this step, basically, the second gas phase material other than the second coordination compound adsorbed on the first monolayer is discharged out of the reaction chamber. As a result, a single layer of a second coordination compound (also referred to as “second single layer” in this specification) is formed on the first single layer. The secondary purge process may include a vacuum purge process.

  In the secondary purge step, the temperature in the vicinity of the substrate and the substrate in the reaction chamber (also referred to as “second purge temperature” in this specification) is set so that the second monolayer is formed on the first monolayer. The temperature is equal to or lower than the upper limit temperature of the ALD window of the first coordination compound and the temperature within the ALD window of the second coordination compound.

  In the case where the ALD window of the first vapor phase material and the ALD window of the second vapor phase material have an overlapping temperature region, the overlapping temperature region from the first lamination step to the secondary purge step If it is performed within the range, it is preferable that the set temperatures of these steps can be unified and the temperature control becomes easy.

  When the second gas phase material includes the second additive material, the second additive material layer is also present when the second purge temperature is below the upper temperature limit of the second additive material ALD window. It is formed.

  The kind of purge gas is not particularly limited, and a known material such as argon or nitrogen molecule can be used as appropriate.

  Thus, by performing the stacking step, a stacked body in which the second single layer is stacked on the first single layer (also referred to as “precursor stacked body” in this specification) is formed. The precursor laminate according to the present embodiment can maintain the form of the layered body on the substrate by chemical interaction between the first coordination compound and the second coordination compound. This point will be described later.

(2) Chemical conversion step In the chemical conversion step, a chemical reaction is performed on the precursor laminate formed by the above-described lamination step, and the element contained in the first coordination compound (specifically, the center of the first coordination compound) And a layered structure including an element contained in the second coordination compound (specifically, an element based on the central substance of the second coordination compound). Form.

  The specific content of this chemical reaction is not particularly limited as long as the chemical reaction is not performed in the lamination step. In order to advance this chemical reaction, a reaction gas is usually supplied.

  In the case of supplying the reaction gas, a process of supplying a reaction gas to advance a chemical reaction (also referred to as a “reaction gas formation process” in this specification) and a purge gas are supplied instead of the supply of the reaction gas. The chemical conversion step is completed (also referred to as “tertiary purge step” in this specification). That is, in the case of supplying the reaction gas, the multi-component thin film is obtained by the convenient six steps of the first lamination step, the primary purge step, the second lamination step, the secondary purge step, the reaction gas chemical conversion step, and the tertiary purge step. Forming a layered structure that can be realized is realized. Thus, the manufacturing method of the layered structure according to the present embodiment can reduce the number of steps by 25% as compared with the ALD process according to the prior art. The details of the tertiary purge process are the same as those of the primary purge process and the secondary purge process, and thus the description thereof is omitted.

  When the chemical reaction of the chemical conversion step includes heating the substrate and the vicinity of the substrate, the heating temperature is equal to or lower than the upper limit temperature of the ALD window of the first coordination compound and the ALD of the second coordination compound. The temperature is equal to or lower than the upper limit temperature of the window. In this case, when the heating temperature is within a temperature region where the ALD window of the first coordination compound and the ALD window of the second coordination compound overlap, the process proceeds from the first lamination process to the chemical conversion process. Until then, the temperature setting of the substrate and the vicinity of the substrate can be unified, and the temperature control becomes easy.

2. Coordination Compound Here, the first coordination compound and the second coordination compound will be described. As described above, in the stacking process, particularly in the secondary purge process, the precursor stack is maintained in the form of a layered body on the substrate due to the chemical interaction between the first coordination compound and the second coordination compound. It is possible.

  The type of this chemical interaction is such that the chemical interaction is not more than the upper limit temperature of the ALD window of the first coordination compound and lower than the upper limit temperature of the ALD window of the second coordination compound. As long as it occurs appropriately, there is no particular limitation. Examples of such chemical interaction include chemical interaction between at least one ligand constituting the first ligand and at least one kind of ligand constituting the second ligand. Etc.

  The chemical interaction or the like generated between the first coordination compound and the second coordination compound may be one kind or plural kinds. Further, the quantitative relationship that causes such chemical interaction is not limited. For example, 1 mol of the second coordination compound may have a chemical interaction or the like with respect to 1 mol of the first coordination compound, or the second coordination compound may have a relationship of 2 mol with respect to 2 mol of the first coordination compound. A relationship in which 1 mol of the coordination compound of the above causes a chemical interaction or the like may be employed. Further, one first coordination compound may cause a chemical interaction or the like with one second coordination compound, and one first coordination compound may include a plurality of second coordination compounds. A chemical interaction or the like may occur, or a plurality of first coordination compounds may cause a chemical interaction or the like with one second coordination compound.

  The first coordination compound and the second coordination compound are not particularly limited as long as they can cause such chemical interaction and the like and can form a layered structure by a chemical reaction in the chemical conversion step. A coordination compound having a ligand capable of causing the chemical interaction as described above may be used. The first coordination compound and the second coordination compound may be different types of substances or the same type of substances. As an example of different types, there is a case where one coordination compound is an electron donating substance and the other coordination compound is an electron withdrawing substance.

  The first ligand contained in the first coordination compound and the second ligand contained in the second coordination compound may each be composed of one type of ligand or a plurality of types of ligands. You may be comprised from the ligand. Different types may be sufficient as a 1st ligand and a 2nd ligand, and the same type may be sufficient as them. At least one of the ligands constituting the first ligand and at least one of the ligands constituting the second ligand are the same species, and the ligands of that kind are chemically interacting with each other. It is also possible to provide a field that produces the like (eg, π-π interaction).

  Alternatively, the first ligand may cause a chemical interaction or the like directly with respect to the central substance of the second coordination compound, or the second ligand may be Chemical interaction or the like may occur directly on the central substance. As a result, in the former case, at least one of the ligands constituting the second ligand is eliminated from the second coordination compound, and in the latter case, the coordination constituting the first ligand is eliminated. At least one of the ligands may be detached from the first coordination compound.

Specific examples of the first ligand and the second ligand include the following combinations of ligands. “Active hydrogen” in the following examples means hydrogen capable of causing an interaction based on hydrogen bonding with another substance.
A combination of any primary to tertiary amino compounds or functional groups based thereon with organic compounds having at least one active hydrogen or functional groups based thereon; and compounds containing or based on oxygen or sulfur A combination of a functional group and an organic compound having at least one active hydrogen or a functional group based thereon.

3. Chemical reaction in the chemical conversion process The type of chemical reaction in the chemical conversion process is not limited as described above. When the layered structure is an oxide-based thin film such as a strontium titanate thin film or an aluminum titanate thin film, this chemical reaction includes an oxidation reaction.

  The chemical reaction in the chemical conversion step includes, as an elementary process, a reaction in which at least one of the first ligand and the second ligand is released from the precursor laminate, and by this chemical conversion step, the chemical reaction of the first coordination compound is performed. A layered body containing an element based on the central substance and an element based on the central substance of the second coordination compound may be formed.

  As a specific example, the element based on the central substance of the first coordination compound is titanium, the element based on the central substance of the second coordination compound is aluminum, and the chemical reaction in the chemical conversion step is an oxidation reaction Is mentioned. In this case, it includes a reaction in which the ligand of each coordination compound is desorbed from the precursor laminate, and an oxidation reaction of titanium and an oxidation reaction of aluminum. As a result, the Ai-Ti-O-based thin film is layered. Obtained as a structure. Compared with the case where an aluminum titanate thin film is formed by the ALD method according to the prior art, as described above, in addition to the simplification of the manufacturing process, the oxidation reaction of titanium and aluminum in the precursor laminate including titanium and aluminum Since the oxidation reaction proceeds, a composite oxide of titanium and aluminum is easily obtained, and as a result, it is expected that an aluminum titanate thin film excellent in stoichiometry is easily obtained. That is, according to the manufacturing method which concerns on one Embodiment of this invention, the manufacturing method of the layered structure excellent in stoichiometry is provided.

When a reaction gas is supplied to advance the chemical reaction in the chemical conversion step, the type of the reaction gas is appropriately set according to the chemical reaction to be advanced. For example, when the chemical reaction is an oxidation reaction, the specific type of reaction gas preferably includes a substance containing oxygen. As such a gas species, ozone (O ₃ ) is typical. Even if the gas for the oxidation reaction is oxygen molecules, a plasma containing oxygen is generated by applying external energy (heating, voltage application, etc.), and the oxidation reaction proceeds by the chemical species contained in the plasma. Good. When the chemical reaction is a nitriding reaction, a reaction gas containing ammonia is exemplified. In addition, the specific kind of external energy application | coating method performed in order to advance a chemical reaction is not limited, Irradiation of electromagnetic waves, such as an ultraviolet-ray and an X-ray (laser irradiation is included) other than said methods, such as a heating. ), Electron beam or ion irradiation, magnetic field application, and the like.

4). Additive Substances The specific types of the first addition substance and the second addition substance are appropriately determined in consideration of the composition of the first coordination compound, the second coordination compound, and the layered structure that is the production target. Is set.

  By using at least one of the first additional substance and the second additional substance, the layered structure can be doped and the composition of the layered structure can be adjusted. In the present specification, a substance contained in at least one of the first gas phase material and the second gas phase material, such as the first addition substance and the second addition substance, Substances other than the compound, the second coordination compound, and the carrier gas may be collectively referred to as “additional substances”.

  When an additive substance is included in the precursor laminate and a component derived from the additive substance is contained in a layered structure formed by a chemical reaction in the chemical conversion step, the component may be used as a dopant for the layered structure. it can.

  Specifically, when the first additive substance is contained in the precursor laminate, a part of the element based on the first coordination compound is replaced with an element based on the first additive substance in the layered structure. It becomes possible. When the second additive substance is contained in the precursor laminate, in the layered structure, a part of the element based on the second coordination compound can be replaced with the element based on the second additive substance. .

  The embodiment described above is described for facilitating understanding of the present invention, and is not described for limiting the present invention. Therefore, each element disclosed in the above embodiment is intended to include all design changes and equivalents belonging to the technical scope of the present invention.

  EXAMPLES Next, although an Example demonstrates this invention further in detail, this invention is not limited only to these specific examples.

1. Production of layered structure comprising Al-Ti-O-based thin film (Example 1)
A silicon substrate was placed in the reaction chamber, the substrate temperature was 150 ° C., and the pressure in the chamber was 200 Pa. In this state, a first gas phase material made of tetrakis (dimethylamino) titanium (IV) as a first coordination compound was supplied into the reaction chamber. Next, supply of the first vapor phase material was stopped, and argon as a primary purge gas was supplied into the reaction chamber to form a first single layer on the silicon substrate. Subsequently, a second gas phase material composed of trimethylaluminum as the second coordination compound was supplied. Thereafter, the supply of the second gas phase material is stopped, and argon as a secondary purge gas is supplied into the reaction chamber, and a precursor stack made of tetrakis (dimethylamino) titanium (IV) and trimethylaluminum is formed on the silicon substrate. Formed body. The supply of secondary purge gas was stopped, ozone was supplied into the reaction chamber, and the substrate temperature was set to 150 ° C., thereby obtaining a layered structure made of an Al—Ti—O-based thin film from the precursor laminate. .
A layered structure composed of an Al—Ti—O-based thin film was obtained on a silicon substrate by carrying out the above process as one cycle for 150 cycles.

(Comparative example)
ALD method according to the prior art using tetrakis (dimethylamino) titanium (IV) and trimethylaluminum, that is, a method of performing 8 steps to form a single Sr—Ti—O-based film, as in the examples A layered structure made of an Al—Ti—O-based thin film was obtained on a silicon substrate by performing a 150 cycle lamination process.

2. Evaluation Method and Evaluation Results The obtained layered body was measured using an X-ray photoelectron spectrometer (XPS) to obtain a spectrum of oxygen 1s.
As a result, in both the examples and the comparative examples, a spectrum having a peak at about 530 eV indicating stoichiometrically appropriate TiAl ₂ O ₅ was obtained.
As a result of calculating the ratio R of the average value of the peak intensity at 531 to 531.5 eV derived from Al ₂ O ₃ with respect to the peak intensity at 530 eV, the ratio was 0.45 in the example, whereas it was 0. 5 in the comparative example. Thus, it was suggested that the layered structure according to the example may have a stoichiometrically superior composition.

  The present invention can be suitably used for the production of layered structures such as Sr—Ti—O-based thin films and Al—Ti—O-based thin films.

Claims (5)

Sequentially supplying a first gas phase material comprising a first coordination compound having a first ligand and a second gas phase material comprising a second coordination compound having a second ligand And a laminating process for forming a laminate on the substrate, in which layers based on each vapor phase material are laminated,
A chemical conversion step of forming a layered structure from the laminate including performing a chemical reaction on the laminate,
Within the temperature range below the upper limit temperature of the ALD window of the first coordination compound and below the upper limit temperature of the ALD window of the second coordination compound, the first coordination compound and the second coordination compound are The laminated body can maintain the form of a layered body on the substrate by at least one of chemical interaction and chemical bonding of:
In the laminating step, the chemical reaction performed in the chemical conversion step is not performed.   The manufacturing method according to claim 1, wherein the chemical reaction performed in the chemical conversion step includes an oxidation reaction.   The chemical reaction of the chemical conversion step includes, as an elementary process, a reaction in which at least one of the first ligand and the second ligand is detached from the laminate, The manufacturing method according to claim 2, wherein a layered structure containing an element based on a central substance of a coordination compound and an oxide of an element based on the central substance of the second coordination compound is formed on the substrate.   The ALD window of the first vapor phase material and the ALD window of the second vapor phase material have overlapping temperature regions, and the stacking step and the chemical conversion step are performed within the overlapping temperature region. The production method according to any one of claims 1 to 3, wherein:   The at least one of the first gas phase material and the second gas phase material contains an additional substance that is a substance other than the first coordination compound and the second coordination compound. 5. The production method according to any one of 4 above.