JP2001083658A - Photo-image recording material and photo-image recording method - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain a photo-image recording material having high sensitivity without using silver halide and having satisfactory image preservability as a photo-image recording material which forms a latent image under light and performs image recording, and to provide a photo-image recording method. SOLUTION: The photo-image recording material 1 has a recording layer 3 on the substrate 1. The recording layer 3 contains at least a photo-acid generating agent, a precursor of a developer and an electron donative leuco dye. The precursor is a material which forms an electron accepting compound having a phenolic hydroxyl group under a generated acid. The recording layer 3 is positive-imagewise irradiated with light of a specified wavelength to form an acid latent image and then the layer 3 is heated to form the objective positive image.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

[0001] 1. Field of the Invention [0002] The present invention relates to an optical image recording material for forming a latent image with light to record an image, and an optical image recording method using the optical image recording material.

[0002]

2. Description of the Related Art As an optical image recording material for forming an image by forming a latent image with light, a silver halide photograph using silver halide is used as an optical image recording method, and a thermally developed silver halide photograph ( For example, dry silver developed by 3M Company and a heat-development diffusion transfer type silver halide photograph (for example, pictography developed by Fuji Photo Film Co., Ltd.) have been conventionally known. In a recording method that does not use silver halide,
Electrophotography, free radical photography using a photo-free radical generator, photosensitive pressure-sensitive recording using photopolymerizable microcapsules (for example, Cycolor developed by Mead) and the like are available.

However, an image recording material using silver halide has problems that the material unit price is expensive and a processing solution is required, which is not preferable from the viewpoint of environmental conservation.

Further, in the electrophotographic system, since toner is used as an image recording material, there is a limit in increasing the image resolution. Further, in a free-radical photograph or a photosensitive pressure-sensitive recording method using photopolymerizable microcapsules, high sensitivity comparable to an image recording method using silver halide can be obtained, but image storability is insufficient.

On the other hand, as a method for forming a latent image with light without using silver halide, several methods using a photoacid generator have been proposed. For example, an optical recording material using a substance that changes to an acid under the action of ultraviolet rays and a leuco dye that forms a color upon contact with the acid (Japanese Patent Laid-Open No. 54-1239)
No. 44), a photosensitive recording material carrying microcapsules enclosing a photoacid generator and an electron-donating colorless dye as a core substance (JP-A-63-95436), a photodecomposable compound and its decomposition product ( A light- and heat-sensitive recording material (JP-A-9-156215) comprising an element which forms a color by reacting with a free radical having a strong oxidizing power (for example, an oxidative coloring type leuco dye, a coupler and an aromatic primary amine compound, etc.); It has been disclosed.

However, in these methods, there is a problem that a high color density cannot be obtained because there is no sufficient affinity between the acid which is the main component of the reaction and the leuco dye (electron donating property). In addition, a large amount of a photoacid generator or a large amount of light irradiation energy is required to generate a leuco dye (electron-donating colorless dye) or an acid necessary to sufficiently develop a coloring element. However, none of them have achieved sufficient performance.

On the other hand, an image recording material utilizing an acid multiplication reaction has been proposed as a method of minimizing the amount of a photoacid generator and the energy of light irradiation while generating a necessary acid. . For example, an energy-sensitive acid generator that is an onium borate complex composed of an onium cation and a borate anion, and an acid proliferating agent that newly generates an acid by an acid generated from the energy-sensitive acid generator. An image recording composition comprising an actinic ray acid generator composition and a dye precursor (oxidative color-forming leuco dye) having a property of forming a color by reaction with an acid generated from the composition (Japanese Patent Laid-Open No. 10-1508) ) Is disclosed.

[0008] However, this method has a problem that the type of acid which acts on the leuco dye to generate color is limited to the acid generated from the acid multiplying agent, so that sufficient color-forming properties cannot be obtained. .

[0009]

SUMMARY OF THE INVENTION In order to solve the above-mentioned problems, the present invention makes it possible to form a latent image with light without using silver halide and to record a high-sensitivity image.
Another object of the present invention is to provide an optical image recording material having sufficient image storability and an optical image recording method.

[0010]

In order to increase the image recording sensitivity, it is necessary to improve the sensitivity in forming a latent image by light. For this purpose, a catalytic reaction or the like is efficiently introduced into image formation. It is important to. Further, in order to further increase the sensitivity, image amplification by a chain reaction, an autocatalytic reaction, or the like is indispensable. Therefore, the present inventor focused on an acid-catalyzed deprotection group reaction and an acid multiplication reaction (a reaction in which an acid is used as a catalyst to generate an acid) showing an autocatalytic reaction without using silver halide. Was completed.

That is, the optical image recording material of the present invention comprises a recording layer containing at least a photoacid generator, a developer precursor and an electron-donating leuco dye on a support, and the developer precursor is The composition was such that the substance produced an electron-accepting compound having a phenolic hydroxyl group by an acid.

Further, the optical image recording material of the present invention is configured such that the developer is a substance having a phenolic hydroxyl group substituted with a protecting group removed by the acid.
The structure was such that the protecting group was either an alkoxycarbonyl group or a silyl group, and the developer precursor had a chemical structure site represented by the following structural formula 1.

[0013]

Embedded image (Wherein, R _{1 to} R ₃ are an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group,
Represents an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, a hydrogen atom, or a halogen atom. )

In the optical image recording material of the present invention, the photoacid generator can generate at least one of the acids represented by the following structural formulas 2, 3 and 4 by light irradiation. It was configured to be a suitable photoacid generator.

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Embedded image (Wherein, R _{1 to} R ₁₀ represent an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group, an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, hydrogen, Atom, halogen atom.)

Further, in the optical image recording material of the present invention, the recording layer contains an acid multiplying agent, and the acid multiplying agent is a substance that generates an acid by using an acid as a catalyst. Using an acid as a catalyst, the following structural formulas 2, 3, and 4
The acid proliferating agent is capable of generating at least one of the acids represented by

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[0020]

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[0021]

Embedded image (Wherein, R _{1 to} R ₁₀ represent an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group, an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, hydrogen, Atom, halogen atom.)

Further, in the optical image recording material of the present invention, the recording layer has a structure in which a plurality of microcapsules are dispersed and supported, and the photoacid generator, the color former precursor and the electron donating leuco dye are used. A configuration in which at least one kind is encapsulated in the microcapsules, the recording layer has a structure in which a plurality of microcapsules are dispersed and supported in a binder resin, and the photoacid generator, the acid multiplying agent, The structure was such that at least one of the developer precursor and the electron-donating leuco dye was encapsulated in the microcapsules.

The microcapsules are heat-responsive microcapsules in which the substance permeability changes due to a physical change or a chemical change due to heat, or the material permeability changes due to a physical change or a chemical change due to light. The configuration was such that it was a photoresponsive microcapsule that changed.

The optical image recording material of the present invention is configured such that the recording layer contains a spectral sensitizing dye which sensitizes the photoacid generator by electron transfer or excitation energy transfer. .

Further, the optical image recording material of the present invention is configured such that the recording layer contains a heat-fusible substance and / or a high boiling point solvent.

Further, the optical image recording material of the present invention has a constitution in which the recording layer is formed in a plurality of fine patterns, and the electron-donating leuco dye contained in each fine pattern has the same hue. The layers had a multilayer structure, and the electron-donating leuco dye contained in each layer had the same hue.

The optical image recording method of the present invention comprises a first step of irradiating a recording layer of any of the above optical image recording materials with light of a specific wavelength like a positive image to form an acid latent image; A second step of forming a positive image by heating at least a part including the light irradiation part.

In the optical image recording method of the present invention, a first step of forming an acid latent image by irradiating a recording layer of any of the above optical image recording materials with light of a specific wavelength like a positive image. A second step of irradiating the entire surface with light having a wavelength different from the light irradiated in the first step, and a third step of heating at least a part including the light irradiation part in the first step to form a positive image; .

Further, according to the optical image recording method of the present invention, the recording layer of the optical image recording material having a multi-layered recording layer is irradiated with light containing a plurality of specific wavelength lights like a positive image. The configuration includes a first step of forming an acid latent image, and a second step of heating at least a portion including the light irradiation portion to form a positive image.

Further, in the optical image recording method of the present invention, after a step of forming a positive image by heating at least a portion including the light-irradiated portion, the dye in the recording layer is thermally diffused and transferred to an object to be transferred. Or, or a configuration having a step of peeling the recording layer from the support and thermally transferring the recording layer to the transfer-receiving member, or in the step of heating at least a portion including the light-irradiated portion to form a positive image, The dye in the recording layer is thermally diffused and transferred to the transfer member, or the recording layer is peeled off from the support and transferred to the transfer member.

In the present invention, an acid latent image is formed like a positive image by the photoacid generator by irradiation with light, and an electron-accepting compound having a phenolic hydroxyl group is generated from the developer by the acid. The electron-accepting compound causes a color-forming reaction with the electron-donating leuco dye to form an image. In addition, the acid latent image can be amplified by including an acid proliferating agent in the recording layer.

[0032]

Embodiments of the present invention will be described below.

Optical Image Recording Material FIG. 1 is a schematic sectional view showing one embodiment of the optical image recording material of the present invention. In FIG. 1, an optical image recording medium 1 is
The recording medium includes a support 2 and a recording layer 3 provided on the support 2. The recording layer 3 includes at least a photoacid generator,
It contains a developer precursor and an electron-donating leuco dye, and the developer precursor is a substance that generates an electron-accepting compound having a phenolic hydroxyl group by an acid generated from a photoacid generator.

The optical image recording material 1 of the present invention has the following features:
The following optical image recording mechanism is provided. That is, an acid is generated from the photoacid generator by the light applied to the recording layer 3 to form a positive image-like acid latent image (acid latent image forming process). Next, an electron-accepting compound having a phenolic hydroxyl group from the developer precursor by the generated acid (a developer)
Is generated (a color developer generation process). Next, an image is obtained by contacting the electron-accepting compound (color developer) with the electron-donating leuco dye to cause a color-forming reaction (development process).

In a conventional heat-sensitive recording material containing an electron-accepting compound (developing agent) and an electron-donating leuco dye, the developing site of the electron-accepting compound (for example, a phenolic hydroxyl group of a phenolic compound) is reduced. In the bare state, the presence of the electron-accepting compound (developing agent) and the electron-donating leuco dye in amounts necessary to obtain a sufficient color density may cause an unprinted state due to the effect of the storage environment. It will develop color. However, as described above, the optical image recording material of the present invention is provided with a “developer developing process” and an electron-accepting compound (developer) is generated only at a light irradiation site. As well as being excellent in storage stability.

The optical image recording material of the present invention utilizes a color development reaction between an electron accepting compound (a color developer) generated by an acid generated from a photoacid generator and an electron donating leuco dye. Since there is sufficient affinity between the electron-accepting compound (developing agent), which is the main component of the reaction, and the electron-donating leuco dye, a high coloring density can be obtained.

As another embodiment of the optical image recording material of the present invention, the recording layer 3 may further contain an acid breeding agent. By using the acid multiplying agent in this way, the acid multiplying process in which the acid is used as a catalyst to generate and multiply the acid between the above-described "optical latent image forming process" and "the color developer generating process" of the optical image recording. ] Will be added. Thereby, the sensitivity in the “acid latent image forming process” is improved.

As a support constituting the optical image recording material of the present invention, synthetic paper (polyolefin, polystyrene, etc.), high quality paper, art paper, coated paper, cast coated paper, wallpaper, backing paper, synthetic resin or synthetic resin Various papers such as emulsion-impregnated paper, synthetic rubber latex-impregnated paper, synthetic resin internal paper, paperboard, cellulose fiber paper, and various plastic films such as polyolefin, polyvinyl chloride, polyethylene terephthalate, polyethylene naphthalate, polystyrene, polymethacrylate, and polycarbonate. Alternatively, a sheet can be used, and a white opaque sheet or a sheet having microvoids formed by adding a white pigment or a filler to these synthetic resins can also be used, and there is no particular limitation. Further, a laminate made of any combination of the above materials can also be used.
The thickness of such a support is preferably about 2 to 300 μm.

A release layer may be provided between the support and the recording layer so that the recording layer can be released from the support by heating or the like. Examples of the resin for forming the release layer include polyurethane resins, polyester resins, melamine resins, urea resins, silicone resins, polyamide resins, acrylic resins, vinyl resins such as vinyl chloride resins, and mixtures or copolymers thereof. No. In order to adjust the release property of the release layer, waxes, Teflon (trade name) powder, silicone oil, micro silica,
An additive such as a fluorine-based surfactant can be contained. The thickness of such a release layer is preferably about 0.01 to 10 μm.

In the transfer-type image recording method described below, a protective layer may be provided between the recording layer and the above-mentioned peeling layer in order to improve the image storability of the transferred optically recorded image. As a resin for forming this protective layer,
Polyurethane resin, polyester resin, polycarbonate resin, polyurea resin, acrylic resin, polystyrene resin, styrene-acrylonitrile copolymer, styrene-ethylene-acrylonitrile copolymer, styrene-butadiene-acrylonitrile copolymer, polysulfone resin, Polyvinyl chloride resin, vinyl acetate resin, vinyl chloride-vinyl acetate copolymer, polyvinyl acetal resin, polyvinyl butyral resin, polyvinyl alcohol resin, epoxy resin, cellulose resin, ethylene-vinyl acetate copolymer, ethylene -Vinyl chloride copolymers, polyethylene resins, polypropylene resins and the like. The thickness of such a protective layer is 0.01 to 1
About 0 μm is preferable.

Next, the recording layer constituting the optical image recording material of the present invention will be described in detail. [Photoacid Generator] The photoacid generator used in the recording layer in the present invention is a compound that is decomposed by light irradiation to generate an acid, and the generated acid acts on the developer precursor to form a phenolic acid. When a compound capable of producing an electron-accepting compound having a hydroxyl group or an acid multiplying agent is used, it is required that the acid multiplying agent can efficiently perform an acid multiplying reaction. Examples of such a photoacid generator include aryldiazonium salts, diaryliodonium salts, triarylsulfonium salts, triarylsulfoxonium salts, pyridinium salts, quinolinium salts, isoquinolinium salts, sulfonic acid esters, iron arene complexes and the like. These are suitable as light triggers for the deprotection reaction of the developer precursor and the acid growth reaction.

In order to further increase the efficiency of the acid growth reaction, at least one of the acids represented by the following structural formulas 2, 3 and 4 must be used among the above photoacid generators. The generated photoacid generator is particularly effective. These acids have an appropriate acid strength and an affinity for a color developer precursor described below, and also have an affinity for an acid multiplying agent when an acid multiplying agent is used.

[0043]

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[0045]

Embedded image (Wherein, R _{1 to} R ₁₀ represent an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group, an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, hydrogen, Atom, halogen atom.)

Hereinafter, examples of the photoacid generator that can be used in the present invention are shown in Structural Formulas 5 to 28, but the present invention is not limited to these photoacid generators. In the following structural formulas 5 to 28, R _{1 to} R ₉ are an alkyl group,
Alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group, an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, a hydrogen atom, a halogen atom, X ^- is the structural formula 2, represents a sulfonium ion obtained by removing a hydrogen atom from the acids represented by Structural Formulas 3 and 4.

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[0070]

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[Acid multiplying agent] The acid multiplying agent used in the recording layer in the present invention is a substance which generates an acid by using the acid generated by the above-described photoacid generator upon irradiation with light as a catalyst. Those which can generate at least one of the acids represented by Formula 2, Structural Formula 3 and Structural Formula 4 have been found to be effective. These acids have appropriate acid strength and affinity for the developer precursor described below.

[0072]

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[0073]

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[0074]

Embedded image (Wherein, R _{1 to} R ₁₀ represent an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group, an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, hydrogen, Atom, halogen atom.)

In the following, examples of the acid proliferating agent which can be used in the present invention are shown in Structural Formulas 29 to 46, but are not limited to these acid proliferating agents. Various acid multiplying agents capable of generating an acid having an affinity for the developer precursor can be used.
In the following structural formulas 29 to 46, R _{1 to} R ₁₄ represent an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group, an alkoxycarbonyl group. , An aryloxycarbonyl group, a hydroxyl group, a hydrogen atom, and a halogen atom.

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[0090]

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[Developer Precursor] The developer precursor used for the recording layer in the present invention is a substance which generates an electron accepting compound having a phenolic hydroxyl group (a developer) by the action of an acid, and is preferably used. Is a substance having a phenolic hydroxyl group substituted with a protecting group which is removed by the action of an acid.

Examples of the above protecting group include an alkoxycarbonyl group (for example, t-butoxycarbonyl group, isopropyloxycarbonyl group, 1-phenylethoxycarbonyl group, 1,1-diphenylethoxycarbonyl group,
-Cyclohexeneoxycarbonyl group, 2-chloroethoxycarbonyl group, etc.), silyl group (for example, trimethylsilyl group, triethylsilyl group, t-butyldimethylsilyl group, t-butyldiphenylsilyl group, phenyldimethylsilyl group, etc.), alkoxymethyl Groups (for example, methoxymethyl group, ethoxymethyl group, 1-methoxyethyl group, 1-phenoxyethyl group, tetrahydropyranyl group, tetrahydrofuranyl group, 4,5-dihydro-2-
A methylfuran-5-yl group and the like, and a secondary or tertiary alkyl group having a hydrogen atom at the β-position (for example, t-
Preferred examples include a butyl group, a cyclohexyl group, and a 2-cyclohexenyl group. In the present invention, an alkoxycarbonyl group and a silyl group are particularly preferred as the protecting group, and an alkoxycarbonyl group is more preferred.

Further, focusing on the chemical structure of the color developing portion (phenolic hydroxyl group substituted with a protecting group) of the color developing agent precursor used in the present invention, it has a chemical structural portion represented by the following structural formula 1. Compounds are preferred as developer precursors.

[0097]

Embedded image (Wherein, R _{1 to} R ₃ are an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group,
Represents an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, a hydrogen atom, or a halogen atom. )

Examples of such a developer precursor include 4-t-butylphenol, 4-octylphenol, 4-phenylphenol, 1-naphthol, 2-naphthol, hydroquinone, resorcinol, and 4-t-butylphenol.
Octyl catechol, 2,2'-dihydroxybiphenyl, 4,4'-dihydroxydiphenyl ether, 2,
2-bis (4-hydroxyphenyl) propane [generic name bisphenol A], tetrabromobisphenol A,
1,1-bis (4-hydroxyphenyl) cyclohexane, 2,2-bis (4-hydroxy-3-methylphenyl) propane, 2,2-bis (4-hydroxyphenyl) -4-methylpentane, 1,4 -Bis (4-hydroxycumyl) benzene, 1,3,5-tris (4-hydroxycumyl) benzene, 4,4- (m-phenylenediisopropylidene) bisphenol, 4,4- (p-phenylenediene) Isopropylidene) bisphenol, bis (4-hydroxyphenyl) acetic acid ethyl ester, 4,
4-bis (4-hydroxyphenyl) valeric acid-n
-Butyl ester, benzyl 4-hydroxybenzoate, phenethyl 4-hydroxybenzoate,
2,4-hydroxybenzoic acid-2-phenoxyethyl ester, 4-hydroxyphthalic acid dimethyl ester, gallic acid-n-propyl ester, gallic acid-n-octyl ester, gallic acid-n-dodecyl ester, gallic acid-n -Octadecyl ester, hydroquinone monobenzyl ether, bis (3-methyl-4-hydroxyphenyl) sulfide, bis (2-methyl-4-hydroxyphenyl) sulfide, bis (3-phenyl-4-hydroxyphenyl) sulfide, bis ( 3-cyclohexyl-4-hydroxyphenyl) sulfide, bis (4
-Hydroxyphenyl) sulfoxide, bis (4-hydroxyphenyl) sulfone [generic name bisphenol S], tetrabromobisphenol S, bis (3-allyl-4-hydroxyphenyl) sulfone, 2,4'-
Bishydroxydiphenylsulfone, 4-hydroxy-4'-methyldiphenylsulfone, 4-hydroxy-4'-chlorodiphenylsulfone, 4-hydroxy-4'-n-propoxydiphenylsulfone, 4-hydroxy-4'-isopropoxydiphenyl Sulfone, 4-hydroxy-4'-n-butoxydiphenylsulfone, 3,4-dihydroxy-4'-methyldiphenylsulfone, 2,4-dihydroxydiphenylsulfone, 2-methoxy-4'-hydroxydiphenylsulfone, 2-ethoxy -4'-hydroxydiphenylsulfone, bis (2-hydroxy-5-t-butylphenyl) sulfone, bis (2-hydroxy-5-chlorophenyl) sulfone, 4-hydroxybenzophenone, 2,4-dihydrido The phenolic hydroxyl groups of phenol derivatives such as xylbenzophenone, 1,7-bis (4-hydroxyphenylthio) -3,5-dioxaheptane, and 1,5-bis (4-hydroxyphenylthio) -3-oxapentane t-butoxycarbonyl group, isopropyloxycarbonyl group, 1-phenylethoxycarbonyl group, 1,1-diphenylethoxycarbonyl group, 2
And compounds substituted with an alkoxycarbonyl group such as -cyclohexeneoxycarbonyl group, 2-chloroethoxycarbonyl group.

[Electron-donating Leuco Dye] As the electron-donating leuco dye used in the recording layer in the present invention, the above-described electron-accepting compound ( Compounds that change from a colorless or pale color to a desired color by reaction with a color developer can be appropriately selected. For example, fluoran compounds, diaryl phthalide compounds, indolyl phthalide compounds, vinylog phthalide compounds, azaphthalide compounds, diarylmethane compounds, rhodamine lactam compounds, spiropyran compounds, fluorene compounds, etc. It is suitably used as a donor leuco dye.

More specifically, the fluoran compounds include 3,6-dimethoxyfluoran and 2-chloro-6.
-Cyclohexylaminofluoran, 3-chloro-6-
Cyclohexylaminofluorane, 2-methyl-6-cyclohexylaminofluoran, 3-methyl-6-cyclohexylaminofluoran, 1,3-dimethyl-6
Diethylaminofluoran, 2-t-butyl-6-diethylaminofluoran, 2-chloro-6-diethylaminofluoran, 2-chloro-3-methyl-6-diethylaminofluoran, 2-methyl-6- (N-ethyl -4
-Methylanilino) fluoran, 8-diethylaminobenzo [a] fluoran, 2-benzylamino-6-diethylaminofluoran, 2-benzylamino-4-methyl-6-diethylaminofluoran, 2-n-octylamino-6-diethylamino Fluoran, 2-anilino-6- (N-ethyl-NN-hexylamino) fluoran, 2- (N-methylanilino) -6- (N-ethyl-4-methylanilino) fluoran, 2-chloro-3-
Methyl-6- [4- (4-anilino) anilino] fluoran, 2-anilino-3-methyl-6-diethylaminofluoran, 2-anilino-3-methyl-6-diethylaminofluoran, 2-anilino-3- Methyl-6-di-n-propylaminofluoran, 2-anilino-3-
Methyl-6-di-n-butylaminofluoran, 2-anilino-3-methyl-6-di-n-pentylaminofluoran, 2-anilino-3-methyl-6- (N-methyl-N-ethyl Amino) fluorane, 2-anilino-3-
Methyl-6- (N-methyl-NN-propylamino)
Fluoran, 2-anilino-3-methyl-6- (N-methyl-NN-butylamino) fluoran, 2-anilino-3-methyl-6- (N-methyl-N-isobutylamino) fluoran, 2- Anilino-3-methyl-6
(N-methyl-Nn-pentylamino) fluoran,
2-anilino-3-methyl-6- (N-methyl-N-cyclohexylamino) fluoran, 2-anilino-3-
Methyl-6- (N-methyl-NN-propylamino)
Fluoran, 2-anilino-3-methyl-6- (N-methyl-N-ethylamino) fluoran, 2-anilino-
3-methyl-6- (N-ethyl-NN-butylamino) fluoran, 2-anilino-3-methyl-6- (N
-Ethyl-N-isobutylamino) fluoran, 2-anilino-3-methyl-6- (N-ethyl-Nn-pentylamino) fluoran, 2-anilino-3-methyl-
6- (N-ethyl-N-isopentylamino) fluoran, 2-anilino-3-methyl-6- (N-ethyl-N
-N-octylamino) fluoran, 2-anilino-3
-Methyl-6- [N-ethyl-N- (3-ethoxypropyl) amino] fluoran, 2-anilino-3-methyl-6- (N-ethyl-Np-triamino) fluoran, 2-anilino-3 -Chloro-6-diethylaminofluoran, 2-anilino-3-chloro-6-di-n-butylaminofluoran, 2- (2-chloroanilino)-
6-diethylaminofluoran, 2- (2-chloroanilino) -6-di-n-butylaminofluoran, 2-
(2-fluoroanilino) -6-diethylaminofluoran, 2- (2-fluoroanilino) -6-di-n-butylaminofluoran, 2- (3-trifluoromethylanilino) -6-dimethyl Aminofluoran, 2- (3
-Trifluoromethylanilino) -6-diethylaminofluoran, 2- (3-trifluoromethylanilino)
-6-di-n-butylaminofluoran, 2- (3-methylanilino) -3-methyl-6-diethylaminofluoran, 2- (3-methylanilino) -3-methyl-6
-Di-n-butylaminofluoran, 2- (4-methylanilino) -3-methyl-6-diethylaminofluoran, 2- (4-t-amylanilino) -3-methyl-6
-Diethylaminofluoran, 2- (3-chloro-4-
Methylanilino) -3-methyl-6-diethylaminofluoran, 2- (2,4-dimethylanilino) -3-methyl-6-diethylaminofluoran, 2- (2,4-
Dimethylanilino) -3-methyl-6-di-n-butylaminofluoran, 2- (2,6-dimethylanilino)
-3-methyl-6-diethylaminofluoran, 2-
(2,6-dimethylanilino) -3-methyl-6-di-
n-butylaminofluoran, 2- (2,6-diethylanilino) -3-methyl-6-diethylaminofluoran, 2- (2,6-diethylanilino) -3-methyl-
6-di-n-butylaminofluoran, 2-anilino-
3-methoxy-6-diethylaminofluoran, 2,2
-Bis {4- [6 '-(N-cyclohexyl-N-methylamino) -3'-methylspiro (phthalide-3,9'
-Xanthen) -2'-ylamino] phenyl} propane and the like.

Further, as a diarylphthalide compound, 3,3-bis (4-dimethylaminophenyl) -6
-Dimethylaminophthalide (generic name CVL), 3,3-
Bis (4-dimethylaminophenyl) phthalide, 3-
(4-dimethylaminophenyl) -3- (4-diethylamino-2-methylphenyl) -6-dimethylaminophthalide, 3,3-bis (9-ethylcarbazole-3-
Yl) -6-dimethylaminophthalide, 3- (4-dimethylaminophenyl) -3- (1-methylpyrrole-3
-Yl) -6-dimethylaminophthalide and the like.

The indolylphthalide compounds include 3- (4-dimethylaminophenyl) -3- (1,1
2-dimethylindol-3-yl) phthalide, 3,3
-Bis (1,2-dimethylindol-3-yl) -6
-Dimethylaminophthalide, 3,3-bis (1-ethyl-2-methylindol-3-yl) phthalide, 3,3
-Bis (1-n-butyl-2-methylindole-3-
Yl) phthalide, 3,3-bis (1-n-octyl-2)
-Methylindol-3-yl) phthalide, 3- (2-
Ethoxy-4-diethylaminophenyl) -3- (1-
Ethyl-2-methylindol-3-yl) phthalide,
3- (2-ethoxy-4-dibutylaminophenyl)-
3- (1-ethyl-2-methylindol-3-yl)
Phthalide, 3- (2-ethoxy-4-diethylaminophenyl) -3- (1-octyl-2-methylindol-3-yl) phthalide and the like.

The vinylogphthalide compounds include 3- (4-diethylaminophenyl) -3- [2,
2-bis (1-ethyl-2-methylindol-3-yl) ethenyl] phthalide, 3,3-bis [2- (4-diethylaminophenyl) -2- (4-methoxyphenyl) ethenyl] -4,5 , 6,7-Tetrachlorophthalide, 3,3-bis [2- (4-pyrrolidinophenyl)-
2- (4-methoxyphenyl) ethenyl] -4,5
6,7-tetrachlorophthalide, 3,3-bis [2,2
-Bis (4-dimethylaminophenyl) ethenyl]-
4,5,6,7-tetrachlorophthalide, 3,3-bis [2,2-bis (4-pyrrolidinophenyl) ethenyl]
-4,5,6,7-tetrabromophthalide and the like.

The azaphthalide compounds include
3,3-bis (4-diethylamino-2-ethoxyphenyl) -4-azaphthalide, 3- (4-diethylamino-2-ethoxyphenyl) -3- [4- (N-ethyl-
N-phenylamino) -2-ethoxyphenyl] -4-
Azaphthalide, 3- (4-diethylamino-2-ethoxyphenyl) -3- (1-ethyl-2-methylindol-3-yl) -4-azaphthalide, 3- (4-diethylamino-2-ethoxyphenyl) -3 -(1-n-octyl-2-methylindol-3-yl) -4-azaphthalide and the like.

Examples of the diarylmethane compound include 4,4'-bis (dimethylamino) benzhydryl benzyl ether, N-halophenylleuco auramine and the like.

The rhodamine lactam compounds include rhodamine B anilinolactam and rhodamine B (4
-Nitroanilino) lactam, rhodamine B (4-chloroanilino) lactam and the like.

The thiazine compounds include benzoyl leucomethylene blue, p-nitrobenzoyl leucomethylene blue and the like.

The spiropyran compounds include 3
-Methylspirodinaphthopyran, 3-ethylspirodinaphthopyran, 3-phenylspirodinaphthopyran, 3-
Benzylspirodinaphthopyran, 3-propylspirodibenzopyran and the like.

Further, as the fluorene-based compound,
3,6-bis (dimethylamino) fluorenespiro [9,3 ']-6'-dimethylaminophthalide, 3-diethylamino-6- (N-allyl-N-methylamino)
Fluorenspiro [9,3 ']-6'-dimethylaminophthalide, 3,6-bis (dimethylamino) -spiro [fluorene-9,6'-6'H-chromeno (4,3-
b) Indole], 3,6-bis (dimethylamino)-
3'-Methyl-spiro [fluorene-9,6'-6'H
-Chromeno (4,3-b) indole], 3,6-bis (diethylamino) -3'-methyl-spiro [fluorene-9,6'-6'H-chromeno (4,3-b) indole], etc. Is mentioned.

The recording layer constituting the optical image recording material of the present invention comprises the above-mentioned photoacid generator, color developer precursor and electron-donating leuco dye as essential components, and if necessary, an acid multiplying agent. However, it is preferable to further use a binder. As the binder to be used, polyurethane resin, polyester resin, polycarbonate resin, polyurea resin, acrylic resin, polystyrene resin, styrene-acrylonitrile copolymer, styrene-ethylene-acrylonitrile copolymer, styrene-butadiene-acrylonitrile copolymer , Polysulfone resin, polyvinyl chloride resin, vinyl acetate resin, vinyl chloride-vinyl acetate copolymer, polyvinyl acetal resin, polyvinyl butyral resin, polyvinyl alcohol resin, epoxy resin, cellulose resin, ethylene-acetic acid Examples thereof include a vinyl copolymer, an ethylene-vinyl chloride copolymer, a polyethylene resin, and a polypropylene resin.

For forming the recording layer of the optical image recording material of the present invention, a sensitizer, a surfactant, an antistatic agent, a leveling agent, a defoaming agent, a high boiling point solvent, Additives such as a fusible substance, a release agent, and a plasticizer can be used. The recording layer, the photo-acid generator described above, a developer precursor, an electron-donating leuco dye, an acid multiplying agent added as needed,
Further, a binder and at least one of the above-mentioned additives are dissolved or dispersed in a suitable solvent, coated on a support by a known coating method such as a gravure printing method, a screen printing method, and a gravure reverse printing method, and dried. Can be formed. The thickness of the recording layer is preferably set in a range of about 0.1 to 50 μm.

The above-described optical image recording material 1 of the present invention includes a recording layer 3 having a single-layer structure, and the recording layer 3 is provided with an electron-donating leuco dye having a single hue or two or more hues together with other constituent materials. Although it can be contained, the present invention is not limited to this.

In the optical image recording material of the present invention, a plurality of microcapsules are dispersed and supported in a recording layer, and the above-mentioned photoacid generator, color former precursor and electron-donating leuco dye are used if necessary. At least one of the acid proliferating agents may be encapsulated in microcapsules.

In the case of an image recording material using microcapsules, there are a method of color separation by light and a method of color separation by heat. In the optical image recording material of the present invention, a method of color separation by light (irradiation light) The method of performing color separation by changing the wavelength for each color) is more effective.

When color separation is performed by light, microcapsules having a difference in thermal response are not particularly required, and microcapsules generally used for image recording materials can be used. Using at least two or more types of microcapsules, each of the capsules can be multicolored by containing a spectral sensitizing dye having a different photosensitive wavelength, and if at least three or more types of microcapsules are used, the same applies. To achieve full color.

As the microcapsule, a heat-responsive microcapsule in which the substance permeability changes due to a physical change due to heat or a chemical change, or a physical change due to light,
It is preferable to appropriately use photoresponsive microcapsules whose substance permeability changes with a chemical change depending on the image recording method and the like.

For example, before image recording, the electron-donating leuco dye may be separated from the developer precursor, or the developer precursor may be separated from the photoacid generator or the acid multiplying agent. In the case of an image recording method in which these components are mixed by heating at the time of image recording, heat-responsive microcapsules can be used effectively.

Further, an electron-donating leuco dye, a photoacid generator, an acid multiplying agent, and a color developer precursor are placed in a state where they can be easily contacted by heat, and the acid generated from the photoacid generator by light irradiation is used. Simultaneous with the formation of the acid latent image, an image recording method including a step of polymerizing the capsule wall material, or
After forming an acid latent image by light irradiation, in the case of an image recording method including a step of polymerizing the capsule wall material by irradiating light having a different wavelength from the light at the time of forming the acid latent image, a photopolymerizable compound is used. A photoresponsive microcapsule that is contained in a capsule or contains a photopolymerizable compound in a wall material can be used effectively.

Examples of spectral sensitizing dyes to be used include “sensitizers” (Katsumi Tokumaru / Shin Okawara / ed. / Kodansha / published), “Latest application development of functional dyes” (Masahiro Irie / supervised, CMC / published) ) Etc. can be selected as appropriate. Specifically, cyanine dye, rhodocyanine dye, merocyanine dye, phthalocyanine dye, naphthalocyanine dye, oxonol dye, styryl dye, indophenol dye, naphthoquinone dye, anthraquinone dye, azo dye And triphenylmethane dyes, porphyrin dyes, coumarin dyes, xanthene dyes, etc., and various spectral sensitizing dyes can be selected according to the wavelength and intensity of light used as a recording source.

The development efficiency can be increased by adding a sensitizer such as a heat-fusible substance or a high-boiling solvent as required. Such a sensitizer performs a color-forming reaction by contacting an electron-accepting compound having a phenolic hydroxyl group (a color developing agent) generated from a color-developer precursor by the action of an acid with an electron-donating leuco dye. Or a substance having a property of increasing the affinity between an electron-accepting compound (developing agent) and an electron-donating leuco dye upon heating can be used. Specifically, p
-Benzylbiphenyl, m-terphenyl, 2-benzyloxynaphthalene, 1,4-dibenzyloxynaphthalene, dibenzyl oxalate, di-p-methylbenzyl oxalate, 1,2-diphenoxyethane, 1,2-di -M
-Toluoxyethane, 1,2-di-p-toluoxyethane, 1,4-diphenoxybutane, benzyl p-benzyloxybenzoate, phenyl 2-naphthoate, phenyl 1-hydroxy-2-naphthoate, terephthal Dibenzyl acid and the like. Among these, p-benzylbiphenyl, m-terphenyl, 2-benzyloxynaphthalene, di-p-methylbenzyl oxalate, 1,2-
Di-m-toluoxyethane is preferably used.

FIG. 2 is a schematic sectional view showing an example of the optical image recording material of the present invention having a recording layer having a multilayer structure. FIG.
In the optical image recording material 11, a recording layer 13 is provided on a support 12, and the recording layer 13 is a laminate of three layers 13a, 13b, and 13c having different hues of the electron-donating leuco dye contained therein. . The thickness of the recording layer 13 is 0.3 to
It is preferable to set the thickness in a range of about 50 μm, and it is preferable that the thickness of each of the recording layers 13a, 13b, 13c is set in a range of about 0.1 to 20 μm. The support 12 is the same as the support 2 described above, and each of the layers 13a, 13b, and 13c constituting the recording layer 13 includes a photoacid generator, a developer precursor, an electron-donating leuco dye, It contains an acid multiplying agent that is added as necessary, and further contains a binder and additives.

As in the case of the optical image recording material 11, the recording layer has a multi-layered structure, so that the recording layer can be multicolored. As in the case of using the above-mentioned microcapsules, the method of color separation by light and the method of heat There is a method of performing color separation. In the optical image recording material of the present invention, a method of performing color separation by light (a method of performing color separation by changing the wavelength of irradiation light for each color).
Is more effective.

In the case of performing color separation by light, it is possible to provide a recording layer having at least two layers, and to include a spectral sensitizing dye having a different photosensitive wavelength in each layer to achieve multicoloring. Has a structure of at least three layers, thereby achieving full-color printing in the same manner.
For example, in each of the layers 13a, 13b, and 13c of the recording layer 13, spectral sensitization having a different photosensitive wavelength depending on the hue of the photoacid generator, the developer precursor, the electron-donating leuco dye, and the electron-donating leuco dye. If an agent is included, full colorization can be achieved according to the wavelength of the irradiation light.

As the spectral sensitizing dye, those mentioned as the spectral sensitizing dye used together with the above microcapsules can be used.

When the recording layer has a multilayer structure,
The development efficiency can be increased by adding a sensitizer such as a heat-fusible substance or a high-boiling solvent as needed. Such a sensitizer performs a color-forming reaction by contacting an electron-accepting compound having a phenolic hydroxyl group (a color developing agent) generated from a color-developer precursor by the action of an acid with an electron-donating leuco dye. Of a vehicle-like nature that serves to assist
Alternatively, a compound having a property of increasing the affinity between an electron-accepting compound (a color developer) and an electron-donating leuco dye upon heating can be used. Specifically, the same substances as those described above can be used.

Further, in the optical image recording material of the present invention, the recording layer formed on the support can have a plurality of fine pattern shapes. Each fine pattern contains a photoacid generator (and, if necessary, an acid multiplying agent), a developer precursor, and an electron-donating leuco dye. Furthermore, if the electron-donating leuco dye containing a single hue contains a spectral sensitizer having a different photosensitive wavelength according to the hue of the electron-donating leuco dye and is contained in one fine pattern, the irradiation light Can be multicolored according to the wavelength of the light. Also in this case, the development efficiency can be increased by adding a sensitizer such as the above-mentioned heat-fusible substance or high-boiling solvent as needed.

The shape of the fine pattern may be any of a circle, a square, an ellipse, and a triangle, and the size is preferably about 0.1 to 100 μm.

The optical image recording material of the present invention is used for protecting the thermal head from sticking when the recording layer is heated or the like and protecting the optical image recording material from a solvent or the like in handling the optical image recording material in the optical image recording method described later. In addition, a lubricating layer may be provided on the recording layer. This lubricating layer is mainly composed of a pigment and a binder resin.

The pigments used include mica, talc, calcium carbonate, zinc oxide, titanium oxide, aluminum hydroxide, kaolin, laurite, synthetic silicate, amorphous silica,
Examples of the powder include urea formalin resin and the like. Of these, mica, talc, calcium carbonate, aluminum hydroxide, kaolin, and silica are particularly preferably used.

Further, in order to carry the pigment in the lubricating layer and further improve the transparency, the binder resin used includes completely saponified polyvinyl alcohol, carboxy-modified polyvinyl alcohol, silica-modified polyvinyl alcohol and the like. Are preferred.

The coating liquid for forming the lubricating layer can be obtained by mixing a pigment with the above solution of the binder resin. Depending on the purpose, zinc stearate, calcium stearate, paraffin wax, polyethylene wax and the like can be used. And various auxiliaries such as a dispersant, a fluorescent brightener, a crosslinking agent, a sulfosuccinic acid-based alkali metal salt and a fluorine-containing surfactant, and a polyoxyethylene surfactant. The lubricating layer is prepared by applying such a coating liquid by a conventionally known coating means in an amount of 0.1 to 0.1% by weight of the solid content.
It is provided in a range of about 20 g / m ² .

Optical Image Recording Method Next, the optical image recording method of the present invention will be described.

The first aspect of the optical image recording method of the present invention is as follows.
A first step of irradiating the recording layer of the optical image recording material of the present invention with a specific wavelength light like a positive image to form an acid latent image;
And a second step of forming a positive image by heating at least the light irradiation site.

In the first step, an acid is generated from the photoacid generator by the irradiated light (if an acid multiplying agent is used, the acid is generated by using the acid generated from the photoacid generator as a catalyst). ) And an acid latent image forming process in which an acid latent image is formed, and a developer generating process in which an electron-accepting compound having a phenolic hydroxyl group (a color developer) is generated from the developer precursor by the generated acid. And are included.

When an acid latent image is formed by irradiating a specific wavelength light like a positive image as described above, the specific wavelength light is 150
Wavelength light appropriately selected within the range of ~ 900 nm can be used, and it is preferable to use laser light when high resolution of an image is required. The laser light source used is excimer laser, argon laser, helium neon laser, semiconductor laser, glass (YAG)
Lasers, carbon dioxide lasers, dye lasers, and the like are included.

The second step includes a development process in which an image is formed by causing a color-forming reaction between an electron-accepting compound (a color developer) and an electron-donating leuco dye by heating. Examples of the heating method include a method of heating the entire surface with a heat roller or a heat drum, a method of irradiating a halogen lamp or an infrared to far-infrared lamp heater, a method of contacting with a heated block or plate, and heating with a thermal head of a thermal transfer printer. Method and the like.

In another embodiment of the optical image recording method of the present invention, a first step of forming an acid latent image by irradiating a recording layer of the optical image recording material of the present invention with light of a specific wavelength like a positive image. And a second step of irradiating the entire surface with light having a different wavelength from the light irradiated in the first step, and a third step of heating at least the light-irradiated portion in the first step to form a positive image. It is.

The first step includes an acid latent image forming process and a color developer generating process, as in the first step of the above embodiment. Further, the third step includes a development process as in the second step of the above-described embodiment. In the second step of the present embodiment,
This is a process for preventing unnecessary coloring at a site where coloring has been performed once and improving the storability of an image. For example, when the optical image recording material of the present invention using the above-described photoresponsive microcapsules is used, the entire surface is irradiated with light having a wavelength different from the specific wavelength light irradiated like a positive image, so that the photoresponsive microcapsules are irradiated. To separate a photoacid generator (acid multiplying agent, if necessary) and a developer precursor inside or outside the capsule, or a developer precursor and an electron-donating leuco dye. be able to. Thereby, the image storability becomes higher.

Further, another embodiment of the optical image recording method of the present invention is directed to an optical image recording material of the present invention in which the recording layer contains a spectral sensitizing dye. A first step of forming an acid latent image by irradiating light containing a plurality of specific wavelengths like a positive image, and a second step of forming a positive image by heating at least a light-irradiated portion. is there.

The first step includes an acid latent image forming process and a developer generating process as in the first step of the first embodiment, and the second step includes the first step. The development process is included in the same manner as in the second step of the embodiment. However, in this embodiment, multicoloring can be performed by the spectral sensitizing dye contained in the recording layer.

Another embodiment of the optical image recording material of the present invention is a first step in which a recording layer of the optical image recording material of the present invention is irradiated with light having a specific wavelength like a positive image to form an acid latent image. A second image forming a positive image by heating at least a light-irradiated portion.
And a third step in which the dye in the recording layer is thermally diffusion-transferred to the transfer object, or the recording layer is separated from the support and thermally transferred to the transfer object.

The first step includes an acid latent image forming process and a developer generating process as in the first step of the first embodiment, and the second step includes the first step. The development process is included in the same manner as the second step of the embodiment. Then, in the third step, the image formation is completed by heat-transferring only the image to the transfer object, or the image formation is completed by thermally transferring the recording layer itself on which the image has been formed to the transfer object. is there.

Further, another embodiment of the optical image recording method of the present invention is a method of forming an acid latent image by irradiating a recording layer of the optical image recording material of the present invention with light having a specific wavelength like a positive image. In one step, at least the light-irradiated portion is heated to form a positive image, and at the same time, the dye in the recording layer is thermally diffusion-transferred to the transfer target, or the recording layer is separated from the support to form And a second step of performing thermal transfer.

The first step includes an acid latent image forming process and a developing agent generating process as in the first step of the first embodiment, and the second step includes the first step. The development process is included in the same manner as the second step of the embodiment, but only the image is thermally diffusion-transferred to the transfer object at the time of image formation, or the recording layer itself on which the image is formed is thermally transferred to the transfer object. To complete image formation.

[0145]

Next, the present invention will be described in more detail with reference to specific examples.

Example 1 (Preparation of Optical Image Recording Material) A composition A for forming a recording layer having the following composition was dissolved in a mixed solvent of methyl ethyl ketone / toluene, and bar-coated on a support made of a polyethylene terephthalate film having a thickness of 125 μm. This was applied by a method and dried to form a recording layer having a thickness of 5 μm to obtain the optical image recording material of the present invention.

(Composition A for forming recording layer) Photoacid generator (substance represented by the following structural formula 47): 10 parts by weight Color developer precursor (substance represented by the following structural formula 48): 15 parts by weight Electron-donating leuco dye: 15 parts by weight (substance represented by the following structural formula 49) ・ Sensitizer (substance represented by the following structural formula: 50): 5 parts by weight ・ Polystyrene resin: 100 parts by weight

[0148]

Embedded image ("Ts" in the above structural formula 47 represents the para-toluenesulfonic acid obtained by removing the hydroxyl group. The same applies to the following structural formula.)

[0149]

Embedded image

[0150]

Embedded image

[0151]

Embedded image

(Image formation) Next, an image was formed on the above optical image recording material by the following operation. 1) Cover half of the optical image recording material with a light-shielding mask. 2) Expose light having a wavelength of 313 nm to an exposure energy of 100 m.
Irradiate so as to be J / cm ² 3) After heating at 120 ° C. for 5 minutes, the light-shielding mask is removed.

Next, the transmission density between the unexposed area and the exposed area was measured with a cyan filter of a Macbeth densitometer TR-924, and the density difference (transmission density of the exposed area−transmission density of the unexposed area) was obtained. As a result, the density difference was 0.5 or more.

Incidentally, in the optical image recording material formed in the same manner except that the photoacid generator was removed from the recording layer forming composition A, an image was formed by the same operation and the density difference was measured. There was almost no difference in concentration.

Example 2 An optical image recording material was produced in the same manner as in Example 1 except that the electron-donating leuco dye used in the composition A for forming a recording layer was changed to that represented by the following structural formula 51. Was prepared.

[0156]

Embedded image An image was formed on this optical image recording material in the same manner as in Example 1. The transmission density between the unexposed portion and the exposed portion was measured with a black filter of a Macbeth densitometer TR-924, and the density difference (exposed portion) was measured. (Transmission density of the unexposed part) was found to be 0.5 or more.

Incidentally, in the optical image recording material formed in the same manner except that the photoacid generator was removed from the composition for forming a recording layer, an image was formed by the same operation and the density difference was measured. There was little difference.

Example 3 (Preparation of Optical Image Recording Material) A composition B for forming a recording layer having the following composition was dissolved in a mixed solvent of methyl ethyl ketone / toluene, and bar-coated on a support made of a polyethylene terephthalate film having a thickness of 125 μm. This was applied by a method and dried to form a recording layer having a thickness of 5 μm to obtain the optical image recording material of the present invention.

(Composition B for forming recording layer) Photoacid generator (substance represented by the following structural formula 52): 5 parts by weight Acid proliferating agent (substance represented by the following structural formula 53): 5 parts by weight Agent precursor (substance represented by the following structural formula 54): 15 parts by weight Electron-donating leuco dye: 15 parts by weight (substance represented by the following structural formula 55) Sensitizer: 5 parts by weight (the structure of Example 1 above) (A substance represented by the formula 50) ・ Polystyrene resin: 100 parts by weight

[0160]

Embedded image

[0161]

Embedded image

[0162]

Embedded image

[0163]

Embedded image

(Image formation) Next, an image was formed on the above optical image recording material by the following operation. 1) Cover half of the optical image recording material with a light-shielding mask. 2) Expose light having a wavelength of 313 nm to an exposure energy of 50 mJ.
/ Cm ² and 3 is irradiated so) was heated for 5 minutes at 120 ° C., to remove the light shielding mask

Next, the transmission density between the unexposed area and the exposed area was measured with a magenta filter of a Macbeth densitometer TR-924, and the density difference (transmission density of exposed area−transmission density of unexposed area) was determined. As a result, the density difference was 0.5 or more.

Incidentally, in the optical image recording material formed in the same manner except that the photoacid generator was removed from the above-mentioned composition B for forming a recording layer, an image was formed by the same operation and the density difference was measured. There was almost no difference in concentration.

Example 4 An optical image recording material was prepared in the same manner as in Example 3 except that the electron-donating leuco dye used in the composition B for forming a recording layer was changed to the one represented by the following structural formula 56. Was prepared.

[0168]

Embedded image An image was formed on this optical image recording material in the same manner as in Example 3, and the transmission density between the unexposed portion and the exposed portion was measured with a black filter of a Macbeth densitometer TR-924. (Transmission density of the unexposed part) was found to be 0.5 or more.

Incidentally, in the optical image recording material formed in the same manner except that the photoacid generator was removed from the above-mentioned composition for forming a recording layer, an image was formed by the same operation and the density difference was measured. There was little difference.

[Example 5] (Preparation of optical image recording material for yellow) First, a recording layer forming composition C having the following composition was dissolved in a mixed solvent of methyl ethyl ketone / toluene, and the thickness was 6 μm.
m, coated on a support made of polyethylene terephthalate film by a bar coating method and dried to a thickness of 2 μm.
Was formed to obtain an optical image recording material for yellow of the present invention.

(Composition C for Forming Recording Layer) Photoacid Generator 25 parts by weight (substance represented by Structural Formula 52 in Example 3) Color developer precursor (substance represented by Structural Formula 57 below) 50 parts by weight-Electron-donating leuco dye ... 50 parts by weight (substance represented by the following structural formula 58)-Sensitizer (substance represented by the following structural formula 59) ... 25 parts by weight-Polystyrene resin ... 100 parts by weight

[0172]

Embedded image

[0173]

Embedded image

[0174]

Embedded image

(Preparation of Optical Image Recording Material for Magenta) Next, except that the electron-donating leuco dye used in the composition C for forming a recording layer was changed to that represented by the following structural formula 60, the same as above. Thus, an optical image recording material for magenta was produced.

[0176]

Embedded image (Preparation of optical image recording material for cyan)

Further, a light image for cyan was produced in the same manner as described above, except that the electron-donating leuco dye used in the composition C for forming a recording layer was replaced with the one represented by the structural formula 49 in Example 1 above. A recording material was produced.

(Preparation of Transferred Material) A composition for forming a receptor layer having the following composition was dissolved in a mixed solvent of methyl ethyl ketone / toluene, coated on a polyethylene terephthalate film having a thickness of 125 μm by a bar coating method, and dried.
A transfer layer was obtained by forming a receiving layer having a thickness of 5 μm. (Composition for forming a receiving layer) ・ Styrene-acrylonitrile copolymer: 100 parts by weight ・ Fluorine surfactant: 1 part by weight

(Image formation) Next, an image was formed on the receptor layer of the transfer-receiving member by using the optical image recording materials of the above-mentioned respective colors by the following operation. 1) Cover the right two-thirds of the optical image recording material for yellow with a light-shielding mask. 2) Expose light having a wavelength of 313 nm to an exposure energy of 100 m.
Irradiated so that J / cm ² 3) was heated for 5 minutes at 120 ° C., a light shielding mask is removed, heated to receive the dye for 5 minutes at 4) again 120 ° C. overlaying a receiving layer of the transfer member After thermal diffusion transfer to the layer, the optical image recording material for yellow is removed from the transfer-receiving body. 5) A part other than the central third of the optical image recording material for magenta is covered with a light-shielding mask. 7) Cover the left two-thirds of the optical image recording material for cyan with a light-shielding mask. 8) Perform the same operations as in 2) to 4) above.

As a result, a full-color image having magenta in one-third of the center of the receiving layer, yellow on one side and cyan in one side on the other side was obtained.

Further, when the exposure amount of the optical image recording material of each color was reduced stepwise, the color density of the exposed portion decreased with the decrease in the exposure amount.

Example 6 (Preparation of Optical Image Recording Material for Yellow) First, a recording layer forming composition D having the following composition was dissolved in a mixed solvent of methyl ethyl ketone / toluene, and a support made of a polyethylene terephthalate film having a thickness of 6 μm was prepared. The resultant was coated by a bar coating method and dried to form a recording layer having a thickness of 2 μm to obtain an optical image recording material for yellow of the present invention.

(Composition D for forming recording layer) Photoacid generator (substance represented by the following structural formula 61): 10 parts by weight Acid proliferating agent (substance represented by the following structural formula 62): 15 parts by weight Agent precursor (substance represented by the following structural formula 63): 50 parts by weight Electron-donating leuco dye: 50 parts by weight (substance represented by the structural formula 58 of Example 5) Sensitizer: 25 parts by weight (A substance represented by the structural formula 50 of Example 1) ・ Polystyrene resin: 100 parts by weight

[0184]

Embedded image

[0185]

Embedded image

[0186]

Embedded image

(Preparation of Optical Image Recording Material for Magenta) Next, the electron-donating leuco dye used in the composition D for forming a recording layer was changed to the one represented by the structural formula 60 in Example 5 above. An optical image recording material for magenta was produced in the same manner as described above.

(Preparation of Optical Image Recording Material for Cyan) Further, except that the electron-donating leuco dye used in the composition D for forming a recording layer was changed to the one represented by the structural formula 49 in Example 1 above, An optical image recording material for cyan was produced in the same manner as described above.

(Preparation of Transferred Body) A transferred body provided with a receiving layer having a thickness of 5 μm was prepared in the same manner as in Example 5.

(Image formation) Next, an image was formed on the receiving layer of the transfer-receiving member by using the optical image recording materials of the above-mentioned respective colors by the following operation. 1) Cover the right two-thirds of the optical image recording material for yellow with a light-shielding mask. 2) Expose light having a wavelength of 313 nm to an exposure energy of 50 mJ.
/ Cm ² and 3 is irradiated so) was heated for 5 minutes at 120 ° C., a light shielding mask is removed, the receiving layer is heated to dye 5 minutes at 4) again 120 ° C. overlaying a receiving layer of the transfer member After the thermal diffusion transfer, the yellow optical image recording material is removed from the transfer receiving body. 5) A part other than the central part of the magenta optical image recording material is covered with a light shielding mask. 6) The above 2) to 4) 7) Cover the left two-thirds of the optical image recording material for cyan with a light-shielding mask. 8) Perform the same operations as in 2) to 4) above.

As a result, a full-color image consisting of magenta in the central third of the receiving layer, yellow on one side and cyan on the other side was obtained.

Further, when the exposure amount of the optical image recording material of each color was reduced stepwise, the color density of the exposed portion decreased with the decrease in the exposure amount.

Example 7 (Preparation of Optical Image Recording Material) A composition for forming a release layer obtained by dissolving polyvinyl alcohol in water was coated on a support made of a polyethylene terephthalate film having a thickness of 6 μm by a bar coating method and dried. Then, a release layer having a thickness of 2 μm was formed.

Next, a composition for forming a protective layer in which a polystyrene resin was dissolved in toluene was applied on the above-mentioned release layer by a bar coating method and dried to form a protective release layer having a thickness of 2 μm.

Next, the recording layer forming composition E having the following composition was dissolved in a mixed solvent of methyl ethyl ketone / toluene, coated on the protective layer by a bar coating method, and dried to obtain a layer having a thickness of 2 mm.
A transfer layer type optical image recording material of the present invention was obtained by forming a μm recording layer.

(Composition E for Recording Layer Formation) Photoacid generator (substance represented by the following structural formula 64): 10 parts by weight Color developer precursor (substance represented by the following structural formula 65): 15 parts by weight Electron-donating leuco dye: 15 parts by weight (substance represented by structural formula 51 in Example 2 above) Sensitizer: 5 parts by weight (substance represented by structural formula 59 in Example 5) Polystyrene resin: 100 parts by weight

[0197]

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[0198]

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(Preparation of Transferred Body) A polymethyl methacrylate resin was dissolved in a mixed solvent of methyl ethyl ketone / toluene, coated on a 125 μm-thick polyethylene terephthalate film by a bar coating method, and dried.
A transfer layer was obtained by forming a receiving layer having a thickness of 5 μm.

(Image formation) Next, an image was formed on the receiving layer of the transfer-receiving material using the above-mentioned optical image recording material by the following operation. 1) Cover half of the optical image recording material with a light-shielding mask. 2) Expose light having a wavelength of 313 nm to an exposure energy of 100 m.
Irradiated so that J / cm ² 3) removing the light-shielding mask, a recording layer and 4 overlapping the receiving layer of the transfer member) heated for 5 min at 120 ° C. of the optical image recording material (acceptor this time recording layer 5) Remove the support of the optical image recording material from the transfer-receiving member. In the step 5), the layer may be peeled between the peeling layer and the protective layer or between the protective layer and the recording layer. .

The transmission density of the unexposed portion and the exposed portion of the recording medium transferred from the optical image recording material was measured using a black filter of a Macbeth densitometer TR-924. When the transmission density of the exposed portion−the transmission density of the unexposed portion) was determined, the density difference was 0.5 or more.

An optical image recording material formed in the same manner except that the photoacid generator was removed from the above-described composition E for forming a recording layer was subjected to image formation by the same operation and the density difference was measured. There was almost no difference in concentration.

Example 8 (Preparation of Capsule Solution) First, a recording layer forming composition F having the following composition was added to 50 parts by weight of a 5% aqueous polyvinyl alcohol solution, and emulsified and dispersed at 20 ° C. using a homogenizer. Thus, an emulsion having an average particle size of 2 μm was obtained. 50 parts by weight of water was added to the obtained emulsion, and stirring was continued at 40 ° C. for 3 hours. Thereafter, the temperature was returned to room temperature to obtain a capsule liquid.

(Composition F for Recording Layer Formation) Photoacid Generator: 1 part by weight (substance represented by Structural Formula 52 in Example 3) Color developer precursor (substance represented by Structural Formula 66 below) 2 parts by weight Electron-donating leuco dye 2 parts by weight (substance represented by structural formula 49 in Example 1 above) Sensitizer 1 part by weight (substance represented by structural formula 50 in Example 1 above) Wall material ... 20 parts by weight (tolylene diisocyanate / trimethylolpropane adduct)-Solubilizer (ethyl acetate) ... 16 parts by weight-High boiling point solvent (diisopropyl naphthalene) ... 5 parts by weight

[0205]

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(Preparation of Optical Image Recording Material) The above-mentioned capsule solution was coated on a support made of a polyethylene terephthalate film having a thickness of 125 μm by a bar coating method and dried to form a recording layer containing microcapsules (thickness of 10 μm).
m) was formed to obtain an optical image recording material of the present invention.

(Image formation) Next, an image was formed on the above optical image recording material by the following operation. 1) Cover half of the optical image recording material with a light-shielding mask. 2) Expose light having a wavelength of 313 nm to an exposure energy of 100 m.
Irradiate so as to be J / cm ² 3) After heating at 120 ° C. for 10 minutes, the light-shielding mask is removed.

Next, the transmission density between the unexposed area and the exposed area is measured by a cyan filter of Macbeth densitometer TR-924, and the density difference (transmission density of exposed area−transmission density of unexposed area) is obtained. As a result, the density difference was 0.5 or more.

The optical image recording material formed in the same manner except that the photoacid generator was removed from the above-mentioned composition F for forming a recording layer, an image was formed by the same operation and the density difference was measured. There was almost no difference in concentration.

Example 9 (Preparation of Capsule Solution) First, a recording layer forming composition G having the following composition was added to 50 parts by weight of a 5% aqueous solution of polyvinyl alcohol, and emulsified and dispersed at 20 ° C. using a homogenizer. Thus, an emulsion having an average particle size of 2 μm was obtained. 50 parts by weight of water was added to the obtained emulsion, and stirring was continued at 40 ° C. for 3 hours. Thereafter, the temperature was returned to room temperature to obtain capsule liquid 1.

(Composition G for forming a recording layer) Photoacid generator: 1 part by weight (substance represented by the structural formula 47 in Example 1) Acid proliferating agent (substance represented by the structural formula 53 in Example 3) 1 part by weight-Developer precursor-2 parts by weight (substance represented by structural formula 54 in Example 3 above)-Electron-donating leuco dye-2 parts by weight (substance represented by structural formula 58 in Example 5 above)・ Wall agent: 20 parts by weight (tolylene diisocyanate / trimethylolpropane adduct) ・ Solubilizer (ethyl acetate): 16 parts by weight ・ High boiling point solvent (diisopropyl naphthalene): 5 parts by weight

The composition G for forming a recording layer was prepared by adding a spectral sensitizing dye (benzoflavin: λmax = 460 nm).
Capsule solution 2 was obtained in the same manner as in capsule solution 1 except that 2 parts by weight was added and the electron-donating leuco dye was replaced with the substance represented by the structural formula 49 in Example 1 above.

(Preparation of Optical Image Recording Material) The above-mentioned capsule liquid 1 was coated on a support made of a polyethylene terephthalate film having a thickness of 125 μm by a bar coating method and dried to form a recording layer containing microcapsules (thickness of 10 μm).
m) was formed. Next, the above-mentioned capsule liquid 2 was applied on this recording layer by a bar coating method and dried to form a recording layer (thickness: 10 μm) containing microcapsules, thereby obtaining an optical image recording material of the present invention.

(Image formation) Next, an image was formed on the above optical image recording material by the following operation. 1) Cover one third of the right side of the optical image recording material with a light shielding mask. 2) Expose light having a wavelength of 313 nm to an exposure energy of 100 m.
Irradiated so that J / cm ² 3) 4 by moving the light shielding mask for shielding a left 3 minutes) 460 nm light exposure energy 100m wavelength
Irradiate so as to have J / cm ² 5) After removing the light-shielding mask, heat at 120 ° C. for 10 minutes

As a result, a multicolor image of green was formed in one-third of the center of the optical image recording material, yellow on the left side, and blue vertical stripes on the right side.

Example 10 (Preparation of Capsule Solution) First, a recording layer forming composition H having the following composition was added to 50 parts by weight of a 5% aqueous solution of polyvinyl alcohol, and emulsified and dispersed at 20 ° C. using a homogenizer. Thus, an emulsion having an average particle size of 2 μm was obtained. 50 parts by weight of water was added to the obtained emulsion, and stirring was continued at 40 ° C. for 3 hours. Thereafter, the temperature was returned to room temperature to obtain a yellow capsule liquid.

(Composition H for forming recording layer) Photoacid generator: 1 part by weight (substance represented by structural formula 52 in Example 3) Color developer precursor: 2 parts by weight (Example 3) (A substance represented by the structural formula 54) ・ Electron-donating leuco dye: 2 parts by weight (a substance represented by the structural formula 58 in Example 5) ・ Wall agent: 20 parts by weight (tolylene diisocyanate / trimethylolpropane adduct) Auxiliary agent (ethyl acetate) 16 parts by weight High-boiling solvent (diisopropylnaphthalene) 5 parts by weight

Further, a spectral sensitizing dye (benzoflavin: λmax = 460 nm) was added to the above-mentioned composition H for forming a recording layer.
A magenta capsule liquid was obtained in the same manner as in the above yellow capsule liquid except that 2 parts by weight was added and the electron-donating leuco dye was replaced with the substance represented by the structural formula 60 of Example 5 above.

Further, a spectral sensitizing dye (acridine orange: λmax = 539n) was added to the above-mentioned composition H for forming a recording layer.
m) A cyan capsule liquid was prepared in the same manner as in the above yellow capsule liquid except that 0.2 parts by weight was added and the electron-donating leuco dye was replaced with the substance represented by the structural formula 49 in Example 1 above. Was.

(Preparation of Optical Image Recording Material) Next, the above-mentioned cyan capsule solution was coated on a support made of a polyethylene terephthalate film having a thickness of 125 μm by a bar coating method and dried to form a recording layer (thickness) containing microcapsules. 10 μm). Next, the magenta capsule liquid was applied onto this recording layer by a bar coating method and dried to form a recording layer containing microcapsules (thickness:
μm). Further, the above-mentioned yellow capsule liquid was applied on this recording layer by a bar coating method and dried to form a recording layer (thickness: 10 μm) containing microcapsules. Thus, a recording layer having a three-layer structure was formed to obtain the optical image recording material of the present invention.

(Image formation) Next, an image was formed on the above optical image recording material by the following operation. 1) Cover the right two-thirds of the optical image recording material with a light-shielding mask. 2) Expose light having a wavelength of 313 nm to an exposure energy of 100 m.
Irradiate so as to be J / cm ² 3) One-third on the right side and one-third on the left side of the optical image recording material
Is shielded by a light-shielding mask. 4) Light having a wavelength of 460 nm has an exposure energy of 100 m.
Irradiated so that J / cm ² 5) 6 covering the left two-thirds light shielding mask of the optical image recording material) exposure energy light having a wavelength of 539nm is 100m
Irradiate so as to be J / cm ² 7) After removing the light-shielding mask, heat at 120 ° C. for 10 minutes

As a result, a full-color image of vertical stripes of magenta was formed on one-third of the center of the optical image recording material, yellow on the left side, and cyan on the right side.

[0223]

As described in detail above, the optical image recording material of the present invention has a recording layer on a support, and this recording layer comprises at least a photoacid generator, a developer precursor and an electron donor. It contains a leuco dye, and the developer precursor used is a substance that generates an electron-accepting compound having a phenolic hydroxyl group by an acid. Therefore, a positive image is generated by a photoacid generator by irradiating the recording layer with light. An acid latent image is formed like this
By this acid, an electron-accepting compound having a phenolic hydroxyl group is generated from the developer precursor only at the light irradiation site,
The electron-accepting compound can form an image by causing a color-forming reaction with the electron-donating leuco dye, and can provide a high sensitivity and a sufficient color-forming density without using silver halide, and have a sufficient image storage. Property is obtained. Further, according to the optical image recording method of the present invention, a high-resolution image having excellent storage stability can be formed.

[Brief description of the drawings]

FIG. 1 is a schematic sectional view showing one embodiment of an optical image recording material of the present invention.

FIG. 2 is a schematic sectional view showing another embodiment of the optical image recording material of the present invention.

[Explanation of symbols]

 1,11: Optical image recording material 2.12: Support 3,13: Recording layer 13a, 13b, 13c: Recording layer

Claims (20)

[Claims] 1. A recording medium comprising at least a photoacid generator, a developer precursor and an electron-donating leuco dye on a support, wherein the developer precursor has an electron acceptor having a phenolic hydroxyl group by an acid. An optical image recording material, which is a substance that produces an acidic compound. 2. The optical image recording material according to claim 1, wherein the developer precursor is a substance having a phenolic hydroxyl group substituted with a protecting group removed by the acid. 3. The optical image recording material according to claim 2, wherein the protecting group is one of an alkoxycarbonyl group and a silyl group. 4. The developer according to claim 2, wherein the developer precursor has a chemical structure represented by the following structural formula 1.
3. The optical image recording material according to item 1. Embedded image (Wherein, R _{1 to} R ₃ are an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group,
Represents an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, a hydrogen atom, or a halogen atom. ) 5. The photoacid generator which is capable of generating at least one of the acids represented by the following structural formulas 2, 3 and 4 upon irradiation with light. The optical image recording material according to any one of claims 1 to 4, wherein: Embedded image Embedded image Embedded image (Wherein, R _{1 to} R ₁₀ represent an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group, an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, hydrogen, Atom, halogen atom.) 6. The recording medium according to claim 1, wherein the recording layer contains an acid multiplying agent, and the acid multiplying agent is a substance that generates an acid by using the acid as a catalyst. Optical image recording material. 7. The acid proliferating agent which is capable of generating at least one of the acids represented by the following structural formulas 2, 3 and 4 using an acid as a catalyst. The optical image recording material according to claim 6, characterized in that: Embedded image Embedded image Embedded image (Wherein, R _{1 to} R ₁₀ represent an alkyl group, an alkenyl group, a cycloalkyl group, an aryl group, an alkoxy group, an aryloxy group, an alkylcarbonyl group, an arylcarbonyl group, an alkoxycarbonyl group, an aryloxycarbonyl group, a hydroxyl group, hydrogen, Atom, halogen atom.) 8. The recording layer has a structure in which a plurality of microcapsules are dispersed and supported, and at least one of the photoacid generator, the developer precursor, and the electron-donating leuco dye is contained in the microcapsules. The optical image recording material according to any one of claims 1 to 5, wherein the optical image recording material is included in a recording medium. 9. The recording layer has a structure in which a plurality of microcapsules are dispersed and supported in a binder resin, and the photoacid generator, the acid multiplying agent, the developer precursor, and the electron-donating leuco. The optical image recording material according to claim 6, wherein at least one kind of dye is included in the microcapsules. 10. The microcapsule according to claim 8, wherein the microcapsule is a thermoresponsive microcapsule whose substance permeability changes with a physical change or a chemical change by heat.
Or the optical image recording material according to claim 9. 11. The microcapsule according to claim 8, wherein the microcapsule is a light-responsive microcapsule whose substance permeability changes with a physical change or a chemical change by light.
Or the optical image recording material according to claim 9. 12. The recording layer according to claim 1, wherein the recording layer contains a spectral sensitizing dye that sensitizes the photoacid generator by electron transfer or excitation energy transfer. The optical image recording material according to any one of the above. 13. The recording layer according to claim 11, wherein the recording layer comprises a heat-fusible substance and / or
Or containing a high boiling point solvent.
The optical image recording material according to claim 12. 14. The recording layer according to claim 1, wherein the recording layer is formed in a plurality of fine patterns, and the electron-donating leuco dye contained in each of the fine patterns has the same hue. 3. The optical image recording material according to item 1. 15. The optical image according to claim 1, wherein the recording layer has a multilayer structure, and the electron-donating leuco dye contained in each layer has the same hue. Recording material. 16. A first step of irradiating a recording layer of the optical image recording material according to claim 1 with light of a specific wavelength like a positive image to form an acid latent image. A second step of heating at least a part including the light irradiation part to form a positive image. 17. A first step of irradiating a recording layer of the optical image recording material according to claim 8 with light of a specific wavelength like a positive image to form an acid latent image. A second step of irradiating the entire surface with light having a wavelength different from the light irradiated in the first step, and a third step of forming a positive image by heating at least a part including the light irradiation part in the first step;
An optical image recording method comprising: 18. An acid latent image is formed by irradiating the recording layer of the optical image recording material according to any one of claims 12 to 15 with light containing a plurality of specific wavelength lights like a positive image. An optical image recording method, comprising: a first step of forming a positive image by heating at least a part including the light-irradiated part. 19. After the step of forming a positive image by heating at least a part including the light-irradiated part, the dye in the recording layer is thermally diffused and transferred to a transfer-receiving member, or the recording layer is supported on a support. 19. The optical image recording method according to claim 16, further comprising the step of peeling off from the substrate and thermally transferring it to a transfer-receiving body. 20. In the step of forming a positive image by heating at least a portion including the light-irradiated portion, the dye in the recording layer is simultaneously transferred by thermal diffusion to a transfer-receiving member, or the recording layer is The optical image recording method according to any one of claims 16 to 18, wherein the optical image recording method is performed by peeling off from the substrate and thermally transferring the same to a transfer target.