KR20070093303A - Organosilane composition, hardmask composition coated under photoresist and process of producing integrated circuit devices using thereof - Google Patents

Abstract

An organosilane-based composition is provided to form an anti-reflection composition which has high etching selectivity and sufficient multi-etching resistance and minimizes reflectivity between a resist and a lower layer. An organosilane-based composition comprises an organosilane polymer and a hydrolysate produced by reacting at least any one selected from compounds represented by the formula 1: [RO]3Si-(CH2)n-R' and formula 2: [RO]3Si-R' with a compound represented by the following formula 3: R1-Si-(OR2)a(OR3)b(OR4)c. In the formula 1, R is a methyl group or ethyl group, n is 1 to 5, and R' is an aromatic group or substituted aromatic group. In the formula 2, R is a methyl group or ethyl group and R' is an aromatic group or substituted aromatic group. In the formula 3, R1 is a methyl group or ethyl group, each of R2-R4 is a C1-4 alkyl group or phenyl group and is identical to or different from one another, a, b, and c satisfy the relations of 0<a<=3, 0<b<=3, and 0<c<=3, wherein a+b+c=3.

Description

Organosilane compound, hardmask composition for resist underlayer film comprising same, and method for manufacturing semiconductor integrated circuit device using same

The present invention relates to an organosilane compound, a hard mask composition for a resist underlayer film, and a method for manufacturing a semiconductor integrated circuit device using the same. The present invention provides excellent pattern reproducibility, good adhesion to a resist, and exposes a resist. After that, it is possible to provide a composition for underlayer film of a resist which is excellent in resistance to a developing film to be used and has a small film reduction during plasma etching.

Most lithographic processes increase the resolution by using an antireflective coating material (ARC) to minimize the reflectivity between the imaging layer, such as a layer of resist material and the substrate. However, these ARC materials impose poor etch selectivity on the imaging layer due to the similar basic composition of the layers. Therefore, many imaging layers are also consumed during the etching of ARC after patterning, requiring further patterning during subsequent etching steps.

In addition, for some lithographic techniques, the resist material used does not provide sufficient resistance to subsequent etching steps to effectively transfer the desired pattern to the layer underlying the resist material. In many cases, for example when extremely thin resist materials are used, when the substrate to be etched is thick, when substantial etch depth is required, it is desired to use a specific etchant for a given substrate layer, or In any combination of the above cases, a hard mask for resist underlayer film is used. The hard mask for the resist underlayer film serves as an intermediate layer between the patterned resist and the substrate to be patterned. The hard mask for resist underlayer film receives a pattern from the patterned resist layer and transfers the pattern to the substrate. The hard mask layer for the resist underlayer film must be able to withstand the etching process required to transfer the pattern.

For example, when processing a substrate such as a silicon oxide film, a resist pattern is used as a mask, but since the thickness of the resist is also thinned along with miniaturization, it is difficult to process the oxide film without damaging the mask property of the resist. Therefore, the process of first transferring a resist pattern to the underlayer film for oxide film processing, and performing a dry etching process to an oxide film as a mask is taken. The underlayer film for oxide film processing means a film formed under the antireflection film while also serving as a lower reflection film. In this step, since the etching rate of the resist and the underlayer film for oxide film processing is similar, it is necessary to form a mask capable of processing the underlayer film between the resist and the underlayer film. That is, a multilayer film made of an oxide film processing underlayer film-underlayer film processing mask-resist is formed on the oxide film. In Japanese Patent No. 2000-0077018 (Publication No.), a condensation product of a silane compound such as Ra _a Si (OR) _4-a is used as a material for resist underlayer film to obtain the same effect as described above. However, the condensation product of the patent has a problem that the Si-OH group is present in a high concentration is poor in film properties and difficult to form patterns during photoresist processing.

The present invention is to solve the problems of the prior art as described above, to provide an antireflective composition that has high etching selectivity, sufficient resistance to multiple etching, and minimizes the reflectivity between the resist and the underlying layer to be useful in lithographic processes It aims to use. Another object of the present invention is to provide a method of patterning a backing material layer on a substrate using the hardmask composition of the present invention.

In addition, the inventor of the present invention utilizes the fact that the aromatic group or the substituted aromatic group in Formula 1 or Formula 2 exhibits an absorption spectrum at 193 nm, while providing a material having high absorption at 193 nm, and at the same time, aromatic. It is a technical object of the present invention to provide a hard mask composition for a resist underlayer film having a desired absorbance and a refractive index in a specific frequency band by adjusting the concentration ratio of a) group or a substituted aromatic group.

In order to solve the above technical problem, the inventors of the present invention have a very low concentration of Si-OH groups when the hydrolysis or condensation reaction of the present invention proceeds to form a very linear polymer under synthetic conditions, resulting in a stable material and at the same time an excellent membrane. The present invention has been accomplished by knowing that it produces excellent patterns in processing properties and photoresist.

Therefore, according to the present invention, an organosilane-based compound comprising a hydrolyzate and an organosilane-based polymer produced by reacting at least one of the compounds represented by Formula 1 and Formula 2 with the compound represented by Formula 3 Is provided.

[Formula 1]

[RO] ₃ Si- (CH ₂ ) _n -R '

(R: methyl group or ethyl group, n: 1-5, R ': aromatic group or substituted aromatic group.)

[Formula 2]

[RO] ₃ Si-R '

(R: methyl group or ethyl group, R ': aromatic group or substituted aromatic group.)

[Formula 3]

R1-Si- (OR ₂ ) _a (OR ₃ ) _b (OR ₄ ) _c

(R1: methyl or ethyl group, R2 to R4 are each 1-4 alkyl groups or phenyl groups, the main chain may be the same or different from each other, a, b, c are each 0 <a ≤ 3, 0 <b ≤ 3, 0 <c≤3 and a + b + c = 3.)

The organosilane compound is characterized in that it comprises a hydrolyzate and an organosilane polymer produced by further reacting the compound represented by the following formula (4).

[Formula 4]

[RO] ₃ Si-H

(R: methyl group or ethyl group.)

The organosilane-based compound is characterized in that it further comprises an acid catalyst.

The acid catalyst is nitric acid, sulfuric acid, p-toluenesulfonic acid mono hydrate, diethylsulfate, 2,4,4,6-tetrabromocyclo Hexadienone, benzoin tosylate, 2-nitrobenzyl tosylate and an alkyl ester of organic sulfonic acid, characterized in that any one selected from the group consisting of.

The organosilane-based compound is characterized in that it is produced by reacting a mixture of 5 to 90 parts by weight of any one or more of the compounds represented by Formula 1 and Formula 2 and 5 to 90 parts by weight of the compound represented by Formula 3.

The organosilane-based mixture of the present invention is characterized by reacting by adding 5 to 90 parts by weight of the compound represented by Formula 4 to 100 parts by weight of the mixture.

[Formula 4]

[RO] ₃ Si-H

(R: methyl group or ethyl group.)

The hydrolyzate is characterized in that any one or more of the structures of the formulas (5) to (8).

[Formula 5]

Ph [CH ₂ ] _n Si [OH] ₃

[Formula 6]

HSi [OH] ₃

[Formula 7]

CH ₃ Si [OH] ₃

[Formula 8]

R1-Si [OH] ₃

(R1: methyl group or ethyl group)

The organosilane polymer is characterized in that it has a structure of formula (9).

 [Formula 9]

The organosilane polymer is characterized in that it has a structure of formula (10).

[Formula 10]

In addition, the present invention provides a hard mask composition for a resist underlayer film comprising the organosilane compound and a solvent.

In addition, there is provided a hard mask composition for a resist underlayer film comprising any one or a mixture of organosilane polymers of the formulas (9) and (10) and a solvent.

[Formula 9]

[Formula 10]

The solvent is propylene glycol monomethyl ether acetate (GMEA; propyleneglycolmonomethyletheracetate), ethyl lactate (EL), cyclohexanone, 1-methoxypropan-2-ol (PGME; 1-Methoxypropan-2-ol) ol), characterized in that it comprises any one or more.

The hard mask composition for a resist underlayer film of the present invention may further include any one or more of a crosslinking agent, a radical stabilizer, and a surfactant.

The hard mask composition for the resist underlayer film of the present invention is pyridine p-toluenesulfonic acid, 2,4,4,6-tetrabromocyclohexadienone, benzoin tosylate, 2-nitrobenzyl tosylate And any one or more compounds selected from the group consisting of other alkyl esters of organic sulfonic acids.

According to the present invention, there is also provided a method comprising the steps of: (a) providing a layer of material on a substrate; (b) forming a hardmask layer of organic material over the material layer; (c) forming an antireflective hardmask layer using the hardmask composition for resist underlayer film over the material layer; (d) forming a radiation-sensitive imaging layer over the antireflective hardmask layer; (e) generating a pattern of radiation-exposed regions within the imaging layer by exposing the radiation-sensitive imaging layer to radiation in a patterned manner; (f) selectively removing portions of the radiation-sensitive imaging layer and the antireflective hardmask layer to expose portions of the organic-containing hardmask material layer; (g) selectively removing portions of the patterned antireflective hardmask layer and the organic-containing hardmask material layer to expose portions of the material layer; And (h) forming a patterned material shape by etching the exposed portion of the material layer.

Further, according to the present invention, there is provided a semiconductor integrated circuit device which is formed by the above manufacturing method.

Hereinafter, the present invention will be described in more detail.

In the present invention, an organosilane-based compound including a hydrolyzate and an organosilane-based polymer produced by reacting any one or more of the compounds represented by Formula 1 and Formula 2 with the compound represented by Formula 3 is provided.

[Formula 1]

[RO] ₃ Si- (CH ₂ ) _n -R '

(R: methyl group or ethyl group, n: 1-5, R ': aromatic group or substituted aromatic group.)

[Formula 2]

[RO] ₃ Si-R '

(R: methyl group or ethyl group, R ': aromatic group or substituted aromatic group.)

[Formula 3]

R1-Si- (OR ₂ ) _a (OR ₃ ) _b (OR ₄ ) _c

(R1: methyl or ethyl group, R2 to R4 are each 1-4 alkyl groups or phenyl groups, the main chain may be the same or different from each other, a, b, c are each 0 <a ≤ 3, 0 <b ≤ 3, 0 <c≤3 and a + b + c = 3.)

In the present invention, an organosilane-based compound produced by reacting a mixture of 5 to 90 parts by weight of at least one of the compounds represented by Formula 1 and Formula 2 with 5 to 90 parts by weight of the compound represented by Formula 3 is provided. The organosilane compound may be provided in the form of a hydrolyzate and an organosilane polymer.

In addition, the composition may include an acid catalyst, and in some cases, 5 to 90 parts by weight of the compound represented by Formula 4 may be added to 100 parts by weight of the mixture.

[Formula 4]

[RO] ₃ Si-H

(R: methyl group or ethyl group.)

In the present invention, the acid catalyst is nitric acid, sulfuric acid, p-toluenesulfonic acid mono hydrate, diethylsulfate, 2,4,4,6-tetra Any one selected from the group consisting of bromocyclohexadienone, benzoin tosylate, 2-nitrobenzyl tosylate and alkyl esters of organic sulfonic acid can be used.

The acid catalyst can appropriately control the hydrolysis or condensation reaction during the synthesis of the resin by adjusting the type, the amount and the method of addition.

The aromatic group or substituted aromatic group included in the compound of Formula 1 or Formula 2 provides a material having a high anti-reflective property by utilizing the point of absorption spectrum in the DUV region and at the same time an aromatic group Alternatively, by adjusting the concentration ratio of the substituted aromatic group, it is possible to provide a hard mask composition having a desired absorbance and refractive index at a specific wavelength.

Increasing the relative input amount of the compound of Formula 3 may increase the Si content, by adjusting the Si content can be given an etching selectivity between the upper photoresist layer and the hard mask layer consisting of the lower organic material.

The weight ratio in the reaction of any one or more of Formulas 1 and 2 with the compounds represented by Formula 3 may be 5 to 90 in each case when the sum of the total compounds is 100 parts by weight. In particular, in the case of Formula 1 or Formula 2, the k (absorbance) value is obtained at about 0.2 by 193 nm. Therefore, in order to have appropriate antireflection properties, the relative amount of the formula (1) or (2) may be adjusted.

The structure of the hydrolyzate obtained in the present invention is preferably the same as any one of the following formulas (5) to (8).

[Formula 5]

Ph [CH ₂ ] _n Si [OH] ₃

[Formula 6]

HSi [OH] ₃

[Formula 7]

CH ₃ Si [OH] ₃

[Formula 8]

R1-Si [OH] ₃

(R1: methyl group or ethyl group)

In addition, the structure of the organosilane-based polymer is preferably the same as any one of the following formula (9) or formula (10), the molecular weight (Mw) is 1,000 to 300,000, preferably 3,000 to 100,000.

[Formula 9]

[Formula 10]

In addition, another aspect of the present invention relates to a hard mask composition for a resist underlayer film, wherein the hard mask composition of the present invention includes an organosilane compound and a solvent comprising the hydrolyzate and the organosilane-based polymer.

In the hard mask composition of the present invention, the composition including the hydrolyzate and the organosilane-based polymer is preferably 1 to 50 parts by weight based on the total composition, and more preferably 1 to 30 parts by weight.

In the present invention, the solvent may be used alone or in combination of two or more solvents, at least one of which uses a high boiling solvent. High boiling solvent prevents voids and improves flatness by drying the film at low speed. Here, "high boiling solvent" means a solvent that volatilizes near a temperature lower than the temperature at the time of coating, drying and curing the invention.

As the high boiling solvent, propylene glycol monomethyl ether acetate (GMEA; propyleneglycolmonomethyletheracetate), ethyl lactate (EL;

One or more of cyclohexanone and 1-methoxypropan-2-ol (PGME; 1 -Methoxypropan-2-ol) may be used, but is not limited thereto.

In addition, the hard mask composition may optionally include only an organosilane polymer obtained by separating the hydrolyzate from the composition including the hydrolyzate and the organosilane-based polymer.

In addition, the present invention may further include any one or more of a crosslinking agent, a radical stabilizer, and a surfactant in the composition as necessary.

In the present invention, the hard mask composition in the pyridine p-toluenesulfonic acid (Pyridine p-toluenesulfonic acid), 2,4,4,6-tetrabromocyclohexadienone, benzoin tosylate, 2-nitrobenzyl tosylate And it may further comprise any one or more compounds selected from the group consisting of other alkyl esters of organic sulfonic acid. The compound serves to promote crosslinking of the resin to improve the etching resistance and solvent resistance.

(A) providing a layer of material on a substrate; (b) forming a hardmask layer of organic material over the material layer; (c) forming an antireflective hardmask layer using the hardmask composition for resist underlayer film over the material layer; (d) forming a radiation-sensitive imaging layer over the antireflective hardmask layer; (e) generating a pattern of radiation-exposed regions within the imaging layer by exposing the radiation-sensitive imaging layer to radiation in a patterned manner; (f) selectively removing portions of the radiation-sensitive imaging layer and the antireflective hardmask layer to expose portions of the organic-containing hardmask material layer; (g) selectively removing portions of the patterned antireflective hardmask layer and the organic-containing hardmask material layer to expose portions of the material layer; And (h) forming a patterned material shape by etching the exposed portion of the material layer.

The invention may be used to form patterned material layer structures, such as metal wiring lines, contact holes or vias, insulation sections such as cell trench isolation, trenches for capacitor structures, and those that may be used in the design of integrated circuit devices. The invention is particularly useful with regard to forming patterned layers of oxides, nitrides, polysilicones and chromium.

In addition, the present invention provides a semiconductor integrated circuit device, which is formed by the above manufacturing method.

Hereinafter, the present invention will be described in more detail with reference to examples, but these examples are for illustrative purposes only and should not be construed as limiting the present invention.

Example 1

In a 10 liter four-necked flask equipped with a mechanical stirrer, a cooling tube, a dropping funnel, and a nitrogen gas introduction tube, 2100 g of methyltrimethoxysilane and 340 g of phenyltrimethoxysilane were dissolved in 5600 g of PGMEA, and then 1000 ppm. 925 g of nitric acid aqueous solution was added to the solution. Thereafter, the reaction was carried out at 60 ° C. for 1 hour, and then negative pressure was applied to remove the generated methanol. The reaction was run for 1 week while maintaining the reaction temperature at 50 ° C. After the reaction, hexanes were added to separate the produced solid, thereby obtaining the polymer having Mw = 15K and polydispersity = 4. 10 g of this solid was dissolved in 100 g of PGMEA and 100 g of ethyl lactate to make a solution.

The sample was coated on a silicon wafer by spin-coating to bake at 200 ° C. for 60 seconds to form a film having a thickness of 600 μs.

Example 2

The compound was synthesized in the same manner as in Example 1 except that 1750 g of methyltrimethoxysilane, 340 g of phenyltrimethoxysilane, and 313 g of trimethoxysilane were used to synthesize the compound and form a film. I was.

[Comparative Example]

1,4-Bis (methoxymethyl) benzene with nitrogen gas flowing into a 1 liter four-necked flask equipped with a mechanical stirrer, a cooling tube, a 300 ml dropping funnel, and a nitrogen gas introduction tube. Stir well with 8.31 g (0.05 mole), 0.154 g (0.001 mole) diethyl sulfate and 200 g of γ-butyrolactone. After 10 minutes, a solution of 28.02 g (0.08 mol) of 4,4 '-(9-fluorenylidene) diphenol in 200 g of γ-butyrolactone was slowly added dropwise for 30 minutes, followed by reaction for 12 hours. . After completion of the reaction, the acid was removed using water, and then concentrated by an evaporator. It was then diluted with MAK and methanol and adjusted to a solution of 15 wt% MAK / methanol = 4/1 (weight ratio). The solution was placed in a 3 L separatory funnel, and n-heptane was added thereto to remove the low molecular weight containing the monomer to obtain the desired resin (Mw = 12,000, polydispersity = 2.0, n = 23).

0.8 g of the phenolic resin prepared and 0.2 g of an oligomeric crosslinking agent (Powderlink 1174) consisting of repetition of the following structural units and 2 mg of pyridinium P-toluene sulfonate were dissolved in 9 g of PGMEA, followed by filtration. A solution was made.

Powderlink 1174 structure

The sample was coated on a silicon wafer by spin-coating to bake at 200 ° C. for 60 seconds to form a film having a thickness of 1500 Å.

The refractive index n and extinction coefficient k of Comparative Examples 1 and the films prepared in Examples 1 and 2 were obtained. The instrument used was Ellipsometer (J. A. Woollam) and the measurement results are shown in Table 1.

Film Preparation Samples Used Optical properties (193nm) Optical properties (248nm) n (refractive index) k (absorption coefficient) n (refractive index) k (absorption coefficient) Comparative Example 1 1.44 0.70 2.02 0.27 Example 1 1.70 0.23 1.53 0.00 Example 2 1.71 0.23 1.54 0.00

Example 3

The photoresist for ArF was coated on the wafer made in Example 1, baked at 110 ° C. for 60 seconds, and exposed to light using an ArF exposure equipment, ASML1250 (FN70 5.0 active, NA 0.82), followed by development with TMAH (2.38 wt% aqueous solution). And using a FE-SEM to examine the line and space (line and space) pattern of 80nm as shown in Table 4 below. The exposure latitude (EL) margin according to the change of the exposure dose and the depth of focus (DoF) margin according to the distance change with the light source are considered and recorded in Table 2.

Example 4

    The same procedure as in Example 3 was carried out except that the wafer made in Example 2 was used.

Comparative Example 2

    The same process as in Example 3 was carried out except that the wafer made in Comparative Example 1 was used.

Sample used to make film Pattern EL margin (△ mJ / exposure energy mJ) DoF margin (μm) Comparative Example 2 0.2 0.2 Example 3 0.2 0.2 Example 4 0.2 0.1

The patterned specimens of Table 2 CHF ₃ / CF ₄ with a mixed gas proceeds to dry etching, and then proceeds to dry etching again using a CHF ₃ / CF ₄ gas mixture containing oxygen, and then, CHF ₃ / Dry etching was again performed using a CF ₄ mixed gas. Finally, after removing all remaining organics using O ₂ gas, the cross section was examined by FE SEM and the results are listed in Table 3.

Sample used to make film Pattern shape after etching Comparative Example 2 Tapered shape, rough surface Example 3 Vertical shape Example 4 Vertical shape

 According to the present invention, it is possible to provide an antireflective composition having high etching selectivity, sufficient resistance to multiple etching, and minimizing reflectivity between the resist and the underlying layer, which can be usefully used in lithographic processes.

In addition, it is possible to provide a hard mask composition for a resist underlayer film having a desired absorption and refractive index in a specific frequency band by providing a material having a high absorbance at 193 nm and simultaneously adjusting the concentration ratio of the aromatic group or the substituted aromatic group.

Claims (16)

      An organosilane compound comprising a hydrolyzate and an organosilane polymer produced by reacting any one or more of the compounds represented by Formula 1 and Formula 2 with the compound represented by Formula 3. [Formula 1] [RO] ₃ Si- (CH ₂ ) _n -R ' (R: methyl group or ethyl group, n: 1-5, R ': aromatic group or substituted aromatic group.) [Formula 2] [RO] ₃ Si-R ' (R: methyl group or ethyl group, R ': aromatic group or substituted aromatic group.) [Formula 3] R1-Si- (OR ₂ ) _a (OR ₃ ) _b (OR ₄ ) _c (R1: methyl or ethyl group, R2 to R4 are each 1-4 alkyl groups or phenyl groups, the main chain may be the same or different from each other, a, b, c are each 0 <a ≤ 3, 0 <b ≤ 3, 0 <c≤3 and a + b + c = 3.) The organosilane-based compound according to claim 1, wherein the organosilane-based compound comprises a hydrolyzate and an organosilane-based polymer produced by further reacting a compound represented by the following formula (4). [Formula 4] [RO] ₃ Si-H (R: methyl group or ethyl group.)    The organosilane compound according to claim 1, wherein the organosilane compound further comprises an acid catalyst. The acid catalyst of claim 3, wherein the acid catalyst is nitric acid, sulfuric acid, p-toluenesulfonic acid mono hydrate, diethylsulfate, 2,4,4, An organosilane-based compound, wherein the compound is any one selected from the group consisting of 6-tetrabromocyclohexadienone, benzoin tosylate, 2-nitrobenzyl tosylate, and alkyl esters of organic sulfonic acid. According to claim 1, wherein the organosilane compound is produced by reacting a mixture of 5 to 90 parts by weight of any one or more of the compounds represented by Formula 1 and Formula 2 and 5 to 90 parts by weight of the compound represented by Formula 3 An organosilane compound characterized by the above-mentioned. The organosilane compound according to claim 5, wherein the compound is reacted by adding 5 to 90 parts by weight of the compound represented by Formula 4 to 100 parts by weight of the mixture. [Formula 4] [RO] ₃ Si-H (R: methyl group or ethyl group.) According to claim 1, wherein the hydrolyzate is an organosilane-based compound, characterized in that any one or more of the structures of the formula (5-8). [Formula 5] Ph [CH ₂ ] _n Si [OH] ₃ [Formula 6] HSi [OH] ₃ [Formula 7] CH ₃ Si [OH] ₃ [Formula 8] R1-Si [OH] ₃ (R1: methyl group or ethyl group) The organosilane compound according to claim 1, wherein the organosilane polymer has a structure represented by the following Chemical Formula 9.  [Formula 9]

The organosilane compound of claim 2, wherein the organosilane polymer has a structure represented by Formula 10 below. [Formula 10]

A hard mask composition for a resist underlayer film comprising the organosilane compound according to claim 1 and a solvent. A hardmask composition for a resist underlayer film comprising any one or a mixture of organosilane polymers of formulas (9) and (10) and a solvent. [Formula 9]

[Formula 10]

The method of claim 10, wherein the solvent is propylene glycol monomethyl ether acetate (GMEA; propyleneglycolmonomethyletheracetate), ethyl lactate (EL; ethyl lactate), cyclohexanone (Cyclohexanone), 1-methoxypropan-2-ol (PGME; 1-Methoxypropan-2-ol) hard mask composition for a resist underlayer film, characterized in that it comprises any one or more. The hard mask composition of claim 10, wherein the hard mask composition further comprises any one or more of a crosslinking agent, a radical stabilizer, and a surfactant. The method of claim 10, wherein the hard mask composition is pyridine p-toluenesulfonic acid, 2,4,4,6-tetrabromocyclohexadienone, benzoin tosylate, 2-nitrobenzyl tosyl A hard mask composition for a resist underlayer film, further comprising any one or more compounds selected from the group consisting of a rate and other alkyl esters of organic sulfonic acids. (a) providing a layer of material on the substrate; (b) forming a hardmask layer of organic material over the material layer; (c) forming an antireflective hardmask layer over the material layer using the hardmask composition for resist underlayer films according to any one of claims 10-14; (d) forming a radiation-sensitive imaging layer over the antireflective hardmask layer; (e) generating a pattern of radiation-exposed regions within the imaging layer by exposing the radiation-sensitive imaging layer to radiation in a patterned manner; (f) selectively removing portions of the radiation-sensitive imaging layer and the antireflective hardmask layer to expose portions of the organic-containing hardmask material layer; (g) selectively removing portions of the patterned antireflective hardmask layer and the organic-containing hardmask material layer to expose portions of the material layer; And (h) forming a patterned material shape by etching the exposed portion of the material layer. A semiconductor integrated circuit device formed by the manufacturing method of claim 15.