JP3986674B2 - Semiconductor device, method for manufacturing the same, and method for forming interlayer insulating film - Google Patents

Description

[0001]
BACKGROUND OF THE INVENTION
The present invention relates to a semiconductor device having an interlayer insulating film excellent in relative dielectric constant and adhesiveness, a manufacturing method thereof, and a method of forming an interlayer insulating film excellent in relative dielectric constant and adhesiveness.
[0002]
[Prior art]
With the progress of higher integration of semiconductor integrated circuits, an increase in wiring delay time due to an increase in inter-wire capacitance, which is a parasitic capacitance between metal wirings, has hindered performance enhancement of semiconductor integrated circuits. The wiring delay time is a so-called RC delay that is proportional to the product of the resistance of the metal wiring and the capacitance between the wirings.
[0003]
Therefore, in order to reduce the wiring delay time, it is necessary to reduce the resistance of the metal wiring or to reduce the capacitance between the wirings.
[0004]
As a method of reducing the capacitance between wirings, it is conceivable to reduce the relative dielectric constant of an interlayer insulating film formed between metal wirings, and a material different from that of a conventional silicon oxide film is used as an interlayer insulating film. Is being considered.
[0005]
In a semiconductor integrated circuit having a minimum processing dimension of 0.25 μm, a fluorine-added silicon oxide film obtained by adding fluorine to a silicon oxide film is being used as an interlayer insulating film. The relative dielectric constant of the fluorine-added silicon oxide film is about 3.3 to 3.9, which is smaller than 4.2 to 4.5 of the conventional silicon oxide film. It has been reported to be effective in reducing time.
[0006]
However, it is clear that further miniaturization of semiconductor integrated circuits will progress further. For semiconductor integrated circuits having a minimum processing dimension of 0.13 μm or less, it is practical to use an interlayer insulating film having a relative dielectric constant of 2.50 or less. It is considered indispensable to realize a typical processing speed.
[0007]
Therefore, studies have been made on a low dielectric constant SOG (spin-on-glass) film, an organic film, and a porous film as an interlayer insulating film having a relative dielectric constant smaller than that of a fluorine-added silicon oxide film.
[0008]
Examining the currently known interlayer insulating film from the viewpoint of material properties, the organic film has a small relative dielectric constant, and perfluorocarbon polymer is the material having the smallest relative dielectric constant. Perfluorocarbon polymer has a minimum dielectric constant of about 1.9.
[0009]
However, since the perfluorocarbon polymer has a carbon-carbon skeleton and is terminated with fluorine except for the bonds involved in the skeleton formation, the perfluorocarbon polymer has very poor adhesion. The reason for this is that, in the perfluorocarbon polymer, since the polarization of the carbon-fluorine bond is small, the carbon-fluorine bond has low chemical reactivity and has little interaction with other materials. This is because it is difficult to occur.
[0010]
As a typical method for forming a perfluorocarbon polymer film, a plasma CVD method has been reported, and the perfluorocarbon polymer film formed by the plasma CVD method is generally called an amorphous fluorocarbon (a-CF) film. Many.
[0011]
However, since the a-CF film has very poor adhesion to the insulating film or metal film, it is indispensable to form an adhesion layer between the a-CF film and the insulating film or metal film. As a layer, a laminated structure of a silicon rich oxide film and a diamond like carbon (DLC) film has been proposed. The silicon-rich oxide film has adhesion with the base oxide film and the metal film and also has adhesion with the DLC film, and the DLC film has adhesion with the a-CF film. Yes.
[0012]
Hereinafter, a conventional wiring structure and a method for forming the same will be described with reference to FIG. First, after the metal wiring pattern 11 is formed on the semiconductor substrate 10, the first adhesion layer having a thickness of 30 nm is formed as a first adhesion layer over the entire surface of the semiconductor substrate 10 including the metal wiring pattern 11. The silicon-rich oxide film 12 and the first DLC film 13 having a thickness of 30 nm are sequentially deposited.
[0013]
Next, an a-CF film 14 having a thickness of 200 nm is deposited on the first DLC film 13 so as to be filled between the metal wiring patterns 11, and then the entire surface is formed on the a-CF film 14. Then, as the second adhesion layer, a second silicon-rich oxide film 15 having a thickness of 30 nm and a second DLC film 16 having a thickness of 30 nm are sequentially deposited.
[0014]
[Problems to be solved by the invention]
However, the relative permittivity of the first and second silicon-rich oxide films 12 and 15 is 3.9 or more, and the relative permittivity of the first and second DLC films 13 and 16 is 2.8 or more. These dielectric constants are considerably higher than those of the a-CF film 14. For this reason, since the 1st adhesion layer which consists of the 1st silicon rich oxide film 12 and the 1st DLC film 13 with a high relative dielectric constant intervenes between metal wiring patterns 11, between metal wiring patterns 11 There is a problem that the effective relative dielectric constant of the insulating film increases. For example, when the interval between the metal wiring patterns 11 is 250 nm, the first silicon-rich oxide film 12 having a thickness of 30 nm and the first DLC film 13 having a thickness of 30 nm are interposed between the metal wiring patterns 11. When the first adhesion layer made of is interposed, an adhesion layer having a high relative dielectric constant of 120 nm thickness is interposed between the metal wiring patterns 11, and therefore, between the metal wiring patterns 11. An increase in the effective relative dielectric constant of the insulating film becomes a big problem.
[0015]
Further, the first and second silicon-rich oxide films 12 and 15, the first and second DLC films 13 and 16, and the a-CF film 14 having greatly different reaction systems are formed in the same processing chamber of the CVD apparatus. In this case, since the atmosphere in the processing chamber changes drastically, the film forming process is not stable. For this reason, each film quality of the first and second silicon-rich oxide films 12 and 15, the first and second DLC films 13 and 16, and the a-CF film 14 changes, so that the adhesion is not stable. is there.
[0016]
When the first and second silicon-rich oxide films 12 and 15, the first and second DLC films 13 and 16, and the a-CF film 14 are formed in the same processing chamber, This mixture is deposited on the inner wall of the processing chamber, and the deposited mixture is peeled off from the inner wall of the processing chamber by oxygen used when depositing the silicon-rich oxide film, so that there is a problem that particles are generated.
[0017]
In addition, there is a problem that it is difficult to control the process because films having greatly different properties such as an oxide film and an organic film need to be stacked with a thin film thickness.
[0018]
The present invention solves the above problems all at once, reduces the effective relative dielectric constant of the insulating film between the metal wirings, and improves the adhesion between the metal wiring and the organic insulating film. A first object is to reduce particles generated in the processing chamber and to facilitate process control.
[0019]
[Means for Solving the Problems]
In order to achieve the first object, a first semiconductor device according to the present invention is formed on a semiconductor substrate including a metal wiring pattern formed on the semiconductor substrate and the metal wiring pattern. A first adhesion layer made of a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a carbon bond and an organic silane derivative, and an organic containing a fluorine-carbon bond formed on the first adhesion layer An organic insulating film composed of a fluorinated organic film containing a compound as a main material, and a siloxane-containing fluorinated organic film formed on the organic insulating film and containing as a main material an organic compound containing a fluorine-carbon bond and an organic silane derivative And an inorganic insulating film made of an inorganic compound formed on the first adhesion layer.
[0020]
In order to achieve the first object, a second semiconductor device according to the present invention is a siloxane-containing fluorine which is formed on a semiconductor substrate and mainly comprises an organic compound containing a fluorine-carbon bond and an organic silane derivative. A first adhesion layer made of a fluorinated organic film, an organic insulating film formed on the first adhesion layer and made of an organic compound containing a fluorine-carbon bond as a main material, and an organic insulation A wiring groove formed in the film, a second adhesion layer formed on a sidewall of the wiring groove, and comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative; And a metal wiring embedded in a portion surrounded by the first adhesion layer and the second adhesion layer inside the wiring groove.
[0021]
In order to achieve the first object, a third semiconductor device according to the present invention is a siloxane-containing fluorine which is formed on a semiconductor substrate and mainly contains an organic compound containing a fluorine-carbon bond and an organic silane derivative. A first adhesion layer made of a fluorinated organic film, an organic insulating film formed on the first adhesion layer and made of an organic compound containing a fluorine-carbon bond as a main material, and a first The main raw material is an organic compound and an organic silane derivative containing a fluorine-carbon bond, formed in a contact hole and a wiring groove which are formed in the adhesion layer and the organic insulating film, and are formed on the side walls of the connection hole and the wiring groove. A second adhesion layer made of a siloxane-containing fluorinated organic film, and a contact and metal wiring made of a metal film embedded in a portion surrounded by the second adhesion layer inside the connection hole and the wiring groove. Eteiru.
[0022]
In order to achieve the first object, a fourth semiconductor device according to the present invention is a siloxane-containing fluorine which is formed on a semiconductor substrate and mainly comprises an organic compound containing a fluorine-carbon bond and an organic silane derivative. A first adhesion layer made of a fluorinated organic film; a first inorganic insulation film made of an inorganic compound formed on the first adhesion layer; and a fluorine-carbon film formed on the first inorganic insulation film. A second adhesion layer comprising a siloxane-containing fluorinated organic film comprising a bond-containing organic compound and an organic silane derivative as a main raw material, and an organic compound containing a fluorine-carbon bond formed on the second adhesion layer A first organic insulating film made of a fluorinated organic film mainly composed of silane, and a siloxane formed on the first organic insulating film and mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative Contains A third adhesion layer made of a fluorinated organic film; a second inorganic insulation film made of an inorganic compound formed on the third adhesion layer; and a second inorganic insulation film formed on the second inorganic insulation film, A fourth adhesion layer composed of a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a carbon bond and an organic silane derivative, and a fluorine-carbon bond formed on the fourth adhesion layer; A second organic insulating film made of a fluorinated organic film containing an organic compound as a main raw material; an organic compound containing a fluorine-carbon bond and an organic silane derivative formed on the second organic insulating film as a main raw material; A fifth adhesion layer made of a siloxane-containing fluorinated organic film, a third inorganic insulating film made of an inorganic compound formed on the fifth adhesion layer, a first adhesion layer, and a first inorganic insulation Film, second adhesion layer, first organic insulating film, third Connection formed in an interlayer insulating film composed of an adhesion layer, a second inorganic insulating film, a fourth adhesion layer, a second organic insulating film, a fifth adhesion layer, and a third inorganic insulating film, and communicating with each other A sixth adhesion layer made of a siloxane-containing fluorinated organic film mainly formed of an organic compound containing a fluorine-carbon bond and an organic silane derivative, formed on the sidewalls of the hole and the wiring groove, and the connection hole and the wiring groove; A contact and a metal wiring made of a metal film embedded in a portion surrounded by a sixth adhesion layer inside the connection hole and the wiring groove are provided.
[0023]
According to the first to fourth semiconductor devices, the relative dielectric constant of the adhesion layer made of the siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative was 2.5 or less. Therefore, it is smaller than the relative dielectric constant (3.9 or higher) of the conventional silicon-rich oxide film or the relative dielectric constant (2.8 or higher) of the DLC film.
[0024]
An organic compound containing a fluorine-carbon bond and an organic silane derivative are copolymerized by plasma in an arbitrary mixing ratio and in the absence of an oxidizing agent to form a siloxane-containing fluorinated organic film (organic / inorganic composite film). In this siloxane-containing fluorinated organic film, siloxane is formed from the alkoxy group of the organosilane derivative, and the formed siloxane oxygen and metal wiring pattern (or contact embedded in the connection hole or metal wiring embedded in the wiring trench) ) Are strongly bonded to each other, and the adhesion between the adhesion layer and the metal wiring pattern (or contact or metal wiring) is increased. Further, since the oxygen of the formed siloxane is strongly bonded to the inorganic compound of the inorganic insulating film, the adhesion between the adhesive layer and the inorganic insulating film is also improved.
[0025]
The organic group of the organic silane derivative composing the adhesion layer and the organic group of the organic compound containing a fluorine-carbon bond composing the organic insulating film undergo a copolymerization reaction, and the organic group of the organic silane derivative becomes the carbon skeleton of the organic compound. Since it is covalently bonded, the adhesion between the adhesion layer and the organic insulating film is increased.
[0026]
In order to achieve the first and second objects, a first method of manufacturing a semiconductor device according to the present invention includes a step of forming a metal wiring pattern on a semiconductor substrate, and a semiconductor substrate including the metal wiring pattern. A step of forming a first adhesion layer comprising a siloxane-containing fluorinated organic film comprising, as a main raw material, an organic compound containing a fluorine-carbon bond and an organic silane derivative by a plasma CVD method; A step of forming an organic insulating film made of a fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond by plasma CVD, and on the organic insulating film by plasma CVD, A step of forming a second adhesion layer comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative, and the first adhesion layer And a step of forming an inorganic insulating film made of an inorganic compound above.
[0027]
In the first method for manufacturing a semiconductor device, an organic compound as a raw material for the siloxane-containing fluorinated organic film constituting the first adhesion layer, an organic compound as a raw material for the fluorinated organic film constituting the organic insulating film, It is preferable that the organic compound which is a raw material of the siloxane-containing fluorinated organic film constituting the two adhesion layers is the same kind of organic compound.
[0028]
In the first method for manufacturing a semiconductor device, the organosilane derivative used as a raw material for the siloxane-containing fluorinated organic film constituting the first adhesion layer and the second adhesion layer is R¹ _nSi (OR²)_4-n(However, n is an integer of 1 to 3, and R¹Is an alkyl group or an aryl group, R²Is an alkyl group or an aryl group. It is preferable that it is an organosilane derivative represented by the general formula.
[0029]
In order to achieve the first and second objects described above, a second method of manufacturing a semiconductor device according to the present invention includes an organic compound containing a fluorine-carbon bond and an organic silane derivative as a main raw material on a semiconductor substrate. Forming a first adhesion layer made of a siloxane-containing fluorinated organic film, forming a first inorganic insulation film made of an inorganic compound on the first adhesion layer, and a first inorganic insulation film A step of forming a second adhesion layer composed of a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative, and on the second adhesion layer, A step of forming a first organic insulating film made of a fluorinated organic film mainly containing an organic compound containing a fluorine-carbon bond, and an organic containing a fluorine-carbon bond on the first organic insulating film Compounds and organosilane derivatives Forming a third adhesion layer made of a siloxane-containing fluorinated organic film mainly composed of a body, forming a second inorganic insulating film made of an inorganic compound on the third adhesion layer, Forming a fourth adhesion layer comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative on the inorganic insulating film, and a fourth adhesion Forming a second organic insulating film made of a fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond on the layer, and a fluorine-carbon bond on the second organic insulating film Forming a fifth adhesion layer made of a siloxane-containing fluorinated organic film mainly containing an organic compound containing silane and an organic silane derivative, and a third inorganic insulation made of an inorganic compound on the fifth adhesion layer Forming a film and 1st adhesion layer, 1st inorganic insulating film, 2nd adhesion layer, 1st organic insulation film, 3rd adhesion layer, 2nd inorganic insulation film, 4th adhesion layer, 2nd organic insulation Forming a connection hole and a wiring groove communicating with each other in an interlayer insulating film composed of the film, the fifth adhesion layer, and the third inorganic insulating film, and containing a fluorine-carbon bond on the side wall of the connection hole and the wiring groove Forming a sixth adhesion layer made of a siloxane-containing fluorinated organic film mainly composed of an organic compound and an organic silane derivative, and a portion surrounded by the sixth adhesion layer inside the connection hole and the wiring groove A step of embedding a metal film to form a contact and metal wiring made of the metal film.
[0030]
According to the first and second methods for manufacturing a semiconductor device, the relative dielectric constant of the adhesion layer made of a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative is 2. 5 or less, which is smaller than the relative dielectric constant (3.9 or more) of the conventional silicon-rich oxide film or the relative dielectric constant (2.8 or more) of the DLC film.
[0031]
An organic compound containing a fluorine-carbon bond and an organic silane derivative are copolymerized by plasma in an arbitrary mixing ratio and in the absence of an oxidizing agent to form a siloxane-containing fluorinated organic film (organic / inorganic composite film). In this siloxane-containing fluorinated organic film, siloxane is formed from the alkoxy group of the organosilane derivative, and the formed siloxane oxygen and metal wiring pattern (or contact embedded in the connection hole or metal wiring embedded in the wiring trench) ) Are strongly bonded to each other, and the adhesion between the adhesion layer and the metal wiring pattern (or contact or metal wiring) is increased. Further, since the oxygen of the formed siloxane is strongly bonded to the inorganic compound of the inorganic insulating film, the adhesion between the adhesive layer and the inorganic insulating film is also improved.
[0032]
The organic group of the organic silane derivative composing the adhesion layer and the organic group of the organic compound containing a fluorine-carbon bond composing the organic insulating film undergo a copolymerization reaction, and the organic group of the organic silane derivative becomes the carbon skeleton of the organic compound. Since it is covalently bonded, the adhesion between the adhesion layer and the organic insulating film is increased.
[0033]
In addition, the step of forming an organic insulating film composed of a fluorinated organic film mainly containing an organic compound containing a fluorine-carbon bond is a siloxane mainly containing an organic compound containing a fluorine-carbon bond and an organic silane derivative. The organic insulating film forming step is performed between the steps of forming the adhesive layer made of the fluorinated organic film, and the organic insulating film forming step and the adhesive layer forming step are the same reaction process. And the process of forming the adhesion layer before and after that can be performed continuously, the process of the reaction system can be easily controlled, and the atmosphere in the processing chamber can be kept constant.
[0034]
The method for forming a first interlayer insulating film according to the present invention is directed to a method for forming an interlayer insulating film comprising a first adhesion layer, an organic insulating film, and a second adhesion layer sequentially deposited on a semiconductor substrate. After introducing the first source gas containing an organic compound containing a fluorine-carbon bond and the second source gas containing an organosilane derivative into the processing chamber in which the semiconductor substrate is held, While the introduction amount is kept substantially constant, the siloxane-containing fluorinated organic film is formed on the semiconductor substrate by the plasma comprising the first source gas and the second source gas while reducing the introduction amount of the second source gas. The step of forming the first adhesion layer and the first raw material gas are introduced into the processing chamber while maintaining the introduction amount thereof substantially constant, while the introduction of the second raw material gas is stopped and the first raw material gas is introduced. The plasma comprising A step of forming an organic insulating film made of an organic compound containing a fluorine-carbon bond on the adhesion layer; a first source gas is introduced into the processing chamber while keeping the introduction amount substantially constant; The siloxane-containing fluorinated organic film is formed on the organic insulating film by plasma composed of the first source gas and the second source gas while introducing the source gas again and increasing the introduction amount of the second source gas. Forming a second adhesion layer.
[0035]
According to the method for forming the first interlayer insulating film, the introduction amount of the first source gas introduced into the processing chamber is kept substantially constant, while the introduction amount of the second source gas is reduced, and the first source gas is introduced onto the semiconductor substrate. After forming the first adhesion layer, the introduction amount of the first source gas introduced into the processing chamber is kept substantially constant, while the introduction of the second source gas is stopped to An organic insulating film is then formed, and then the amount of the first source gas introduced into the processing chamber is kept substantially constant, while the amount of the second source gas introduced again is increased while the organic insulating film is increased. In order to form the second adhesion layer on the film, that is, with the introduction amount of the first source gas kept substantially constant, the introduction amount of the second source gas is reduced, stopped, and increased. The first adhesion layer, the organic insulating film and the second adhesion layer can be continuously formed. .
[0036]
The second interlayer insulating film forming method according to the present invention is directed to an interlayer insulating film forming method comprising a first adhesion layer, an organic insulating film, and a second adhesion layer, which are sequentially deposited on a semiconductor substrate. The first source gas containing an organic compound containing a fluorine-carbon bond and the second source gas containing an organosilane derivative are kept substantially constant in the processing chamber in which the semiconductor substrate is held. And introducing a first adhesion layer made of a siloxane-containing fluorinated organic film on the semiconductor substrate with plasma made of the first source gas and the second source gas, and a first in the processing chamber. While introducing the source gas while keeping the introduction amount substantially constant, the introduction of the second source gas is stopped, and the fluorine-carbon bond is formed on the first adhesion layer by the plasma made of the first source gas. Containing A step of forming an organic insulating film made of a compound, and a first source gas is introduced into the processing chamber while maintaining the introduction amount thereof substantially constant, and the second source gas is introduced again and the second source gas is introduced. Forming a second adhesion layer composed of a siloxane-containing fluorinated organic film on the organic insulating film by plasma composed of the first source gas and the second source gas while keeping the introduction amount of the gas substantially constant; It has.
[0037]
According to the method for forming the second interlayer insulating film, after forming the first adhesive layer in the processing chamber while maintaining the introduction amounts of the first source gas and the second source gas substantially constant, While maintaining the introduction amount of the first source gas introduced into the room substantially constant, the introduction of the second source gas is stopped to form an organic insulating film on the first adhesion layer, and then While maintaining the introduction amount of the first source gas introduced into the processing chamber substantially constant, introducing the second source gas again and keeping the introduction amount of the second source gas substantially constant, the organic insulating film In order to form the second adhesion layer thereon, that is, by introducing, stopping and introducing the second source gas while maintaining the introduction amount of the first source gas substantially constant, The adhesion layer, the organic insulating film, and the second adhesion layer can be formed continuously.
[0038]
DETAILED DESCRIPTION OF THE INVENTION
(First embodiment)
Hereinafter, a semiconductor device and a manufacturing method thereof according to a first embodiment of the present invention will be described with reference to FIGS. 1 (a) to (c) and FIGS. 2 (a) to (c).
[0039]
First, as shown in FIG. 1A, after a metal wiring pattern 101 having a height of, for example, 800 nm and a wiring space of 250 nm is formed on a semiconductor substrate 100, the semiconductor substrate 100 including the metal wiring pattern 101 is included. A first adhesion layer 102 made of a siloxane-containing fluorinated organic film having a thickness of 20 nm, for example, is deposited on the entire surface. As a method for depositing a siloxane-containing fluorinated organic film, a first raw material gas mainly composed of an organic compound having a fluorine-carbon bond and an organic silane derivative, for example, C_FourF₈/ CH_Four/ Plasma CVD method using a mixed gas of vinyltrimethoxysilane (vinyltrimethoxysilane) can be mentioned. As deposition conditions, for example, RF power is 200 W, process pressure is 200 mmTorr, and deposition time is 4 seconds.
[0040]
Next, as shown in FIG. 1B, an organic insulating film 103 made of a fluorinated amorphous carbon film having a film thickness of, for example, 200 nm is formed on the first adhesion layer 102 over the entire surface. It deposits so that the space part between them may be filled completely. As a method for depositing a fluorinated amorphous carbon film, a second source gas containing an organic compound having a fluorine-carbon bond as a main source, for example, C_FourF₈/ CH_FourAs a deposition condition, for example, the RF power is 200 W, the process pressure is 200 mmTorr, and the deposition time is 60 seconds.
[0041]
Next, as shown in FIG. 1C, a second adhesion layer 104 made of a siloxane-containing fluorinated organic film having a thickness of, for example, 20 nm is deposited on the entire surface of the organic insulating film 103. As a method for depositing the siloxane-containing fluorinated organic film, as in the case of the first adhesion layer 102, a first source gas containing an organic compound having a fluorine-carbon bond and an organic silane derivative as a main source, for example, C_FourF₈/ CH_FourA plasma CVD method using a mixed gas of / vinyltrimethoxysilane may be mentioned. As deposition conditions, for example, RF power is 200 W, process pressure is 200 mmTorr, and deposition time is 4 seconds.
[0042]
Next, as shown in FIG. 2A, after depositing an inorganic insulating film 105 made of a silicon oxide film having a film thickness of, for example, 50 nm over the entire surface of the second adhesion layer 104, the inorganic insulating film is deposited. The surface of the film 105 is planarized by, eg, CMP. As a method of depositing a silicon oxide film, SiH_FourAnd N₂A plasma CVD method using a mixed gas of O 2 may be mentioned.
[0043]
Next, as illustrated in FIG. 2B, the first adhesion layer 102, the organic insulating film 103, the second adhesion layer 104, and the inorganic insulating film 105 are selectively etched to form the connection hole 106. After the formation, a metal plug 107 is formed by filling the connection hole 106 with a metal film made of, for example, tungsten. The silicon oxide film 105 as the inorganic insulating film 105 serves as an etching stopper when the connection hole 106 is formed by dry etching.
[0044]
According to the first embodiment, the relative dielectric constant of the first and second adhesion layers 102 and 104 made of the siloxane-containing fluorinated organic film was very low and 2.5 or less.
[0045]
Further, the adhesion between the first and second adhesion layers 102 and 104 made of a siloxane-containing fluorinated organic film and the organic insulating film 103 made of a fluorinated amorphous carbon film is extremely excellent. No peeling of the film 103 was observed.
[0046]
Hereinafter, a first process sequence when the first adhesion layer 102, the organic insulating film 103, and the second adhesion layer 104 are successively deposited will be described.
[0047]
The first process sequence is the introduction of a first source gas mainly containing an organic compound having a fluorine-carbon bond and an organosilane derivative while keeping the deposition conditions such as RF power at 200 W and process pressure at 200 mm Torr. This is a method of changing the introduction amount of the second source gas using an organic compound having a fluorine-carbon bond as a main source in a pulsed manner while keeping the amount constant.
[0048]
The first process sequence will be specifically described with reference to FIG. First, C in the plasma CVD processing chamber_FourF₈Gas, CH_FourImmediately after introducing the gas and vinyltrimethoxysilane gas, a high frequency power for plasma generation is applied, and C_FourF₈Gas, CH_FourThe first adhesion layer 102 is deposited by introducing a gas and vinyltrimethoxysilane gas at a constant introduction amount for 4 seconds. Next, while stopping the introduction of vinyltrimethoxysilane gas, C_FourF₈Gas and CH_FourThe organic insulating film 103 is deposited by introducing the gas at a constant introduction amount for 60 seconds. Next, C_FourF₈Gas and CH_FourThe second adhesion layer 104 is deposited by introducing the vinyltrimethoxysilane gas again for a predetermined amount of 4 seconds while keeping the respective introduction amounts of the gas constant. As a method of applying high-frequency power for generating plasma, No. 1 in FIG. 1 may be stopped for a short time immediately before and immediately after the introduction and stop of the vinyltrimethoxysilane gas. As shown in Fig. 2, it is continued regardless of the introduction and stop of vinyltrimethoxysilane gas, and C_FourF₈Gas, CH_FourYou may stop just before the introduction stop of gas and vinyltrimethoxysilane gas.
[0049]
According to the first process sequence, in the step of depositing the first adhesion layer 102 and the second adhesion layer 104, since the vinyltrimethoxysilane gas is introduced in a certain amount, the first and second adhesion layers 102, 104 are used. The content of siloxane in is substantially constant in the film thickness direction of the adhesion layer.
[0050]
Also, according to the first process sequence, C_FourF₈Gas, CH_FourSince the introduction and stop of the vinyltrimethoxysilane gas can be performed by a simple operation of opening and closing the valve without changing the introduction amount of the gas and the vinyltrimethoxysilane gas with time, the first and second adhesion layers 102 104 can be easily reduced. For this reason, since the effective relative dielectric constant between the metal wiring patterns 101 can be reduced, an increase in capacitance can be suppressed.
[0051]
However, the first process sequence has a disadvantage that the adhesiveness is slightly lowered because the composition changes sharply at the interface between the first or second adhesion layers 102 and 104 and the organic insulating film 103. .
[0052]
Hereinafter, a second process sequence when the first adhesion layer 102, the organic insulating film 103, and the second adhesion layer 104 are successively deposited will be described.
[0053]
The second process sequence is the introduction of a first source gas mainly containing an organic compound having a fluorine-carbon bond and an organosilane derivative while keeping the deposition conditions, for example, RF power at 200 W and process pressure at 200 mm Torr. In this method, the amount of the second raw material gas introduced using an organic compound having a fluorine-carbon bond as a main raw material is continuously changed while the amount is kept constant.
[0054]
The second process sequence will be specifically described with reference to FIG. First, C in the plasma CVD processing chamber_FourF₈Gas, CH_FourImmediately after the gas and vinyltrimethoxysilane gas are introduced, a high frequency power for plasma generation is applied, and C_FourF₈Gas and CH_FourWhile maintaining the gas introduction amount constant, the introduction amount of the vinyltrimethoxysilane gas is continuously decreased, and the introduction of the vinyltrimethoxysilane gas is stopped after 4 seconds from the start of the introduction, whereby the first adhesion layer 102. To deposit. Next, while stopping the introduction of vinyltrimethoxysilane gas, C_FourF₈Gas and CH_FourThe organic insulating film 103 is deposited by introducing the gas into the respective introduction amounts for 60 seconds. Next, C_FourF₈Gas and CH_FourThe second adhesion layer 104 is deposited by continuously introducing the vinyltrimethoxysilane gas again and continuously increasing the amount of introduction for 4 seconds while keeping the amount of introduction of each gas constant. As a method of applying high frequency power for generating plasma, as shown in FIG._FourF₈Gas, CH_FourStarting immediately after the introduction of the gas and vinyltrimethoxysilane gas,_FourF₈Gas, CH_FourThe process is terminated immediately before the introduction of the gas and vinyltrimethoxysilane gas is stopped.
[0055]
According to the second process sequence, it is necessary to change the introduction amount of the vinyltrimethoxysilane gas with time, so it is somewhat difficult to shorten the deposition time of the first and second adhesion layers 102 and 104. For this reason, since the film thickness of the first and second adhesion layers 102 and 104 is thicker than that in the first process sequence, the effective relative dielectric constant between the metal wiring patterns 101 is slightly increased. Since the composition change between the first and second adhesion layers 102 and 104 and the organic insulating film 103 is continuous, the adhesion is very high.
[0056]
In the first embodiment, an organic compound as a main raw material for the siloxane-containing fluorinated organic film constituting the first adhesion layer 102 and a main raw material for the fluorinated amorphous carbon film constituting the organic insulating film 103 are used. As an organic compound and an organic compound which is a main raw material of the siloxane-containing fluorinated organic film constituting the second adhesion layer 104, C_FourF₈Instead of this, instead of C_TenF₁₈The general formula: C_xF_yAn organic compound having a fluorine-carbon bond represented by (x is an integer of 1 to 15 and y is an integer of 4 to 32) can be widely used.
[0057]
In the first embodiment, vinyltrimethoxysilane is used as the organic silane derivative that is the main raw material of the fluorinated amorphous carbon film constituting the organic insulating film 103.¹ _nSi (OR²)_4-n(However, n is an integer of 1 to 3, and R¹Is an alkyl group or an aryl group, R²Is an alkyl group or an aryl group. ) Can be widely used.
[0058]
(Second Embodiment)
4A, 4B, 5A, 5B, 6A, and 6B are described below with respect to a wiring structure and a method for forming the same according to the second embodiment of the present invention. The description will be given with reference.
[0059]
First, as shown in FIG. 4A, the entire surface of the first organic insulating film 201 made of a fluorinated amorphous carbon film formed on the semiconductor substrate 200 and having the wiring trench 201a is 20 nm, for example. After depositing a first adhesion layer 202 made of a siloxane-containing fluorinated organic film having a thickness of 5 nm, a metal film 203 is formed by embedding a metal film inside the wiring groove 201a, and then, for example, 50 nm over the entire surface. A first inorganic insulating film 204 made of a silicon oxide film having a thickness of 1 is deposited.
[0060]
Next, as shown in FIG. 4B, a second adhesion layer 205 made of a siloxane-containing fluorinated organic film having a thickness of 20 nm, for example, a film of 800 nm, for example, is formed on the first inorganic insulating film 204. Second organic insulating film 206 made of a fluorinated amorphous carbon film having a thickness, for example, a third adhesion layer 207 made of a siloxane-containing fluorinated organic film having a thickness of 20 nm, for example, a silicon oxide film having a thickness of 50 nm A second inorganic insulating film 208 made of, for example, a fourth adhesion layer 209 made of a siloxane-containing fluorinated organic film having a thickness of 20 nm, for example, a third organic film made of a fluorinated amorphous carbon film having a thickness of 300 nm. Insulating film 210, for example, a fifth adhesion layer 211 made of a siloxane-containing fluorinated organic film having a thickness of 20 nm, and, for example, 5 Sequentially depositing a third inorganic insulating film 212 made of a silicon oxide film having a thickness of nm.
[0061]
Next, as shown in FIG. 5A, the first inorganic insulating film 204, the second adhesion layer 205, the second organic insulation film 206, the third adhesion layer 207, and the second inorganic insulation film 208. In addition to forming the connection hole 213, and forming the wiring groove 214 in the fourth adhesion layer 209, the third organic insulating film 210, the fifth adhesion layer 211, and the third inorganic insulating film 212, the connection hole 213 is formed. A sixth adhesion layer 215 made of a siloxane-containing fluorinated organic film having a thickness of 20 nm, for example, isotropically deposited over the entire surface including the inside of the wiring trench 214.
[0062]
Next, as shown in FIG. 5B, the sixth adhesion layer 215 is etched back to remove portions of the sixth adhesion layer 215 located at the bottoms of the connection holes 213 and the wiring grooves 214. In addition, from the sixth adhesion layer 215 to each side surface (each side wall of the connection hole 213 and the wiring groove 214) exposed in the connection hole 213 and the wiring groove 214 in the second and third organic insulating films 206 and 210. A side wall 216 is formed.
[0063]
Next, as shown in FIG. 6A, a titanium nitride film having a film thickness of, for example, 5 nm is formed over the entire surface of the third inorganic insulating film 212 including the insides of the connection holes 213 and the wiring grooves 214. A barrier layer 217 is deposited.
[0064]
Next, as shown in FIG. 6B, after depositing a metal film 218 made of, for example, copper over the entire surface of the barrier layer 217 including the insides of the connection holes 213 and the wiring grooves 214, A portion exposed on the third inorganic insulating film 212 is removed by, for example, a CMP method to form a dual damascene structure made of the metal film 218.
[0065]
As a method for depositing the siloxane-containing fluorinated organic film to be the first, second, third, fourth, fifth, and sixth adhesion layers 202, 205, 207, 209, 211, and 215, the first embodiment is used. In the same manner as in Example 1, a first raw material gas mainly containing an organic compound having a fluorine-carbon bond and an organic silane derivative, such as C_FourF₈/ CH_FourA plasma CVD method using a mixed gas of / vinyltrimethoxysilane can be mentioned. As deposition conditions, for example, RF power is 200 W, process pressure is 200 mmTorr, and deposition time is 4 seconds.
[0066]
As a method of depositing the fluorinated amorphous carbon film to be the first, second and third organic insulating films 201, 206, 210, a second source gas containing an organic compound having a fluorine-carbon bond as a main source, for example, C_FourF₈/ CH_FourAs a deposition condition, for example, the RF power is 200 W, and the process pressure is 200 mmTorr.
[0067]
According to the second embodiment, the side wall 216 including the sixth adhesion layer 215 is formed on the side surface exposed to the connection hole 213 and the wiring groove 214 in the second organic insulating film 206 and the third organic insulating film 210. After the formation, the barrier layer 217 made of a titanium nitride film is deposited, so that the adhesion between the second and third organic insulating films 206 and 210 and the barrier layer 217 is improved.
[0068]
【The invention's effect】
According to the first to fourth semiconductor devices, the dielectric constant of the adhesion layer composed of a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative is the same as that of a conventional silicon-rich oxide. It is smaller than the relative dielectric constant of the adhesion layer composed of the laminated film of the film and the DLC film.
[0069]
Since the adhesion between the adhesion layer and the metal wiring pattern (or contact or metal wiring), the adhesion between the adhesion layer and the inorganic insulating film, and the adhesion between the adhesion layer and the organic insulating film are all high, the metal wiring pattern ( Alternatively, the adhesion between the inorganic insulating film and the organic insulating film can be improved by a single adhesive layer.
[0070]
Therefore, according to the first to fourth semiconductor devices, the effective relative dielectric constant of the insulating film between the metal wirings can be reduced, and the adhesion between the metal wiring and the organic insulating film can be improved. it can.
[0071]
According to the first and second semiconductor device manufacturing methods, the relative dielectric constant of the adhesion layer can be reduced as compared with the conventional laminated film of the silicon-rich oxide film and the DLC film, and the metal wiring pattern (or contact or metal wiring). ), An improvement in adhesion between the inorganic insulating film and the organic insulating film can be realized by a single layer and a single type of adhesion layer.
[0072]
In addition, the process of forming the organic insulating film and the process of forming the adhesion layer before and after that can be performed continuously, the process of the reaction system is easily controlled, and the atmosphere in the processing chamber is kept constant. Can do.
[0073]
Therefore, according to the first and second semiconductor device manufacturing methods, the effective relative dielectric constant of the insulating film between the metal wirings can be reduced and the adhesion between the metal wiring and the organic insulating film can be improved. The process controllability can be easily realized without generating particles in the processing chamber.
[0074]
In the first method for manufacturing a semiconductor device, the organic compound that is a raw material of the first adhesion layer, the organic compound that is a raw material of the organic insulating film, and the organic compound that is a raw material of the second adhesion layer are the same kind of organic compound. And process controllability is further improved.
[0075]
In the first method for manufacturing a semiconductor device, the raw material for the first adhesion layer and the second adhesion layer is R¹ _nSi (OR²)_4-n(However, n is an integer of 1 to 3, and R¹Is an alkyl group or an aryl group, R²Is an alkyl group or an aryl group. ), The relative dielectric constant of the adhesion layer can be reliably reduced and the adhesion can be improved with certainty.
[0076]
According to the first interlayer insulating film forming method, the first source gas introduction amount is decreased, stopped, and increased while the first source gas introduction amount is kept substantially constant. Since the adhesion layer, the organic insulating film, and the second adhesion layer can be continuously formed, the composition of the first adhesion layer, the organic insulating film, and the second adhesion layer is continuously changed. Get higher.
[0077]
According to the method for forming the second interlayer insulating film, the first adhesion layer is formed by introducing, stopping, and introducing the second source gas while keeping the introduction amount of the first source gas substantially constant. Since the organic insulating film and the second adhesion layer can be formed continuously, the thickness of the first and second adhesion layers can be reduced, so that the effective relative dielectric constant of the interlayer insulation film can be made extremely small. it can.
[Brief description of the drawings]
FIGS. 1A to 1C are cross-sectional views showing respective steps of a semiconductor device manufacturing method and an interlayer insulating film forming method according to a first embodiment of the present invention;
FIGS. 2A to 2C are cross-sectional views showing respective steps of a semiconductor device manufacturing method and an interlayer insulating film forming method according to the first embodiment of the present invention;
FIGS. 3A and 3B are diagrams showing a sequence of a source gas introduction method in the method for manufacturing a semiconductor device and the method for forming an interlayer insulating film according to the first embodiment of the present invention. FIGS.
FIGS. 4A and 4B are cross-sectional views showing respective steps of a semiconductor device manufacturing method and an interlayer insulating film forming method according to a second embodiment of the present invention. FIGS.
FIGS. 5A and 5B are cross-sectional views showing respective steps of a semiconductor device manufacturing method and an interlayer insulating film forming method according to a second embodiment of the present invention. FIGS.
FIGS. 6A and 6B are cross-sectional views showing respective steps of a semiconductor device manufacturing method and an interlayer insulating film forming method according to a second embodiment of the present invention. FIGS.
FIG. 7 is a cross-sectional view of a conventional semiconductor device.
[Explanation of symbols]
100 Semiconductor substrate
101 Metal wiring pattern
102 1st adhesion layer
103 Organic insulation film
104 Second adhesion layer
105 Inorganic insulating film
106 Connection hole
107 Metal plug
200 Semiconductor substrate
201 first organic insulating film
201a Wiring groove
202 First adhesion layer
203 metal wiring
204 First inorganic insulating film
205 Second adhesion layer
206 Second organic insulating film
207 Third adhesion layer
208 Second inorganic insulating film
209 Fourth adhesion layer
210 Third organic insulating film
211 Fifth adhesion layer
212 Third inorganic insulating film
213 Connection hole
214 Wiring groove
215 Sixth adhesion layer
216 sidewall
217 Barrier layer
218 Metal film

Claims (8)

A metal wiring pattern formed on a semiconductor substrate;
A first adhesion layer comprising a siloxane-containing fluorinated organic film formed on the semiconductor substrate including the metal wiring pattern and made mainly of an organic compound containing a fluorine-carbon bond and an organic silane derivative;
An organic insulating film formed on the first adhesion layer and made of a fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond;
A second adhesion layer formed on the organic insulating film and comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative;
A semiconductor device comprising: an inorganic insulating film made of an inorganic compound formed on the second adhesion layer. A first adhesion layer formed on a semiconductor substrate and comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative;
A first inorganic insulating film made of an inorganic compound formed on the first adhesion layer;
A second adhesion layer formed on the first inorganic insulating film and comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative;
A first organic insulating film formed on the second adhesion layer and made of a fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond;
A third adhesion layer formed on the first organic insulating film and comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative;
A second inorganic insulating film made of an inorganic compound formed on the third adhesion layer;
A fourth adhesion layer formed on the second inorganic insulating film and comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative;
A second organic insulating film formed on the fourth adhesion layer and made of a fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond;
A fifth adhesion layer formed on the second organic insulating film and comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative;
A third inorganic insulating film made of an inorganic compound formed on the fifth adhesion layer;
The first inorganic insulating film, the second adhesive layer, the first organic insulating film, the third adhesive layer, the second inorganic insulating film, the fourth adhesive layer, and the second organic A connection hole formed in communication with an interlayer insulating film composed of an insulating film, the fifth adhesion layer, and the third inorganic insulating film, and formed in at least the first organic insulating film of the interlayer insulating film And a wiring groove formed in at least the second organic insulating film of the interlayer insulating film,
A sidewall formed of a sixth adhesion layer formed of a siloxane-containing fluorinated organic film mainly formed of an organic compound containing a fluorine-carbon bond and an organic silane derivative, formed on the side wall of the connection hole and the wiring groove;
A semiconductor device comprising a contact and a metal wiring made of a metal film embedded in a portion surrounded by the sidewall in the connection hole and the wiring groove. Forming a metal wiring pattern on a semiconductor substrate;
A first adhesion layer comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative by plasma CVD on the semiconductor substrate including the metal wiring pattern. Forming a step;
Forming an organic insulating film made of a fluorinated organic film mainly containing an organic compound containing a fluorine-carbon bond on the first adhesion layer by a plasma CVD method;
Forming a second adhesion layer made of a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative on the organic insulating film by a plasma CVD method;
And a step of forming an inorganic insulating film made of an inorganic compound on the second adhesion layer.   An organic compound that is a raw material for the siloxane-containing fluorinated organic film that constitutes the first adhesion layer, an organic compound that is a raw material for the fluorinated organic film that constitutes the organic insulating film, and the second adhesion layer 4. The method of manufacturing a semiconductor device according to claim 3, wherein the organic compound that is a raw material of the siloxane-containing fluorinated organic film is the same kind of organic compound. The organosilane derivative used as a raw material for the siloxane-containing fluorinated organic film constituting the first adhesion layer and the second adhesion layer is R ¹ _n Si (OR ² ) _4-n (where n is 1 to 3). It is an integer, R ¹ is an alkyl group or an aryl group, and R ² is an alkyl group or an aryl group.) A method for manufacturing a semiconductor device. Forming a first adhesion layer composed of a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative on a semiconductor substrate;
Forming a first inorganic insulating film made of an inorganic compound on the first adhesion layer;
Forming a second adhesion layer comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative on the first inorganic insulating film;
Forming a first organic insulating film made of a fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond on the second adhesion layer; and
Forming a third adhesion layer comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative on the first organic insulating film;
Forming a second inorganic insulating film made of an inorganic compound on the third adhesion layer;
Forming a fourth adhesion layer made of a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative on the second inorganic insulating film;
Forming a second organic insulating film composed of a fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond on the fourth adhesion layer;
Forming a fifth adhesion layer comprising a siloxane-containing fluorinated organic film mainly composed of an organic compound containing a fluorine-carbon bond and an organic silane derivative on the second organic insulating film;
Forming a third inorganic insulating film made of an inorganic compound on the fifth adhesion layer;
The first inorganic insulating film, the second adhesive layer, the first organic insulating film, the third adhesive layer, the second inorganic insulating film, the fourth adhesive layer, and the second organic An insulating film, an interlayer insulating film composed of the fifth adhesion layer and the third inorganic insulating film, a connection hole formed in at least the first organic insulating film of the interlayer insulating film, and the interlayer insulating film Forming at least the second organic insulating film so that the wiring grooves communicate with each other;
Forming a sidewall comprising a sixth adhesion layer comprising a siloxane-containing fluorinated organic film mainly comprising an organic compound containing a fluorine-carbon bond and an organic silane derivative on the sidewalls of the connection hole and the wiring groove; ,
And a step of burying a metal film in a portion surrounded by the sidewall in the connection hole and the wiring groove to form a contact and a metal wiring made of the metal film. Method. A method for forming an interlayer insulating film comprising a first adhesion layer, an organic insulating film, and a second adhesion layer, which is sequentially deposited on a semiconductor substrate,
After introducing a first source gas containing an organic compound containing a fluorine-carbon bond and a second source gas containing an organosilane derivative into a processing chamber in which a semiconductor substrate is held, the first source gas While maintaining the introduction amount substantially constant, while reducing the introduction amount of the second source gas, the siloxane-containing fluorinated organic material is formed on the semiconductor substrate by the plasma comprising the first source gas and the second source gas. Forming the first adhesion layer comprising a film;
The first source gas is introduced into the processing chamber while maintaining the introduction amount thereof substantially constant, while the introduction of the second source gas is stopped, and the first source gas is caused to be plasma by the plasma made of the first source gas. Forming an organic insulating film made of an organic compound containing a fluorine-carbon bond on one adhesive layer;
While introducing the first source gas into the processing chamber while maintaining the introduction amount thereof substantially constant, while introducing the second source gas again and increasing the introduction amount of the second source gas, Forming the second adhesion layer made of a siloxane-containing fluorinated organic film on the organic insulating film by plasma made of the first source gas and the second source gas. A method for forming an interlayer insulating film. A method for forming an interlayer insulating film comprising a first adhesion layer, an organic insulating film, and a second adhesion layer, which is sequentially deposited on a semiconductor substrate,
A first source gas containing an organic compound containing a fluorine-carbon bond and a second source gas containing an organosilane derivative are kept in a processing chamber in which a semiconductor substrate is held, while the respective introduction amounts are kept substantially constant. Forming the first adhesion layer made of a siloxane-containing fluorinated organic film on the semiconductor substrate with the plasma made of the first source gas and the second source gas while introducing,
The first source gas is introduced into the processing chamber while maintaining the introduction amount thereof substantially constant, while the introduction of the second source gas is stopped, and the first source gas is caused to be plasma by the plasma made of the first source gas. Forming an organic insulating film made of an organic compound containing a fluorine-carbon bond on one adhesive layer;
The first raw material gas is introduced into the processing chamber while keeping the introduction amount thereof substantially constant, the second raw material gas is introduced again, and the introduction amount of the second raw material gas is kept substantially constant. However, the method includes the step of forming the second adhesion layer made of the siloxane-containing fluorinated organic film on the organic insulating film by the plasma made of the first source gas and the second source gas. A method of forming an interlayer insulating film characterized by the above.

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