US3080230A - Photographic stratum transfer process and element therefor - Google Patents

Photographic stratum transfer process and element therefor Download PDF

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Publication number
US3080230A
US3080230A US636863A US63686357A US3080230A US 3080230 A US3080230 A US 3080230A US 636863 A US636863 A US 636863A US 63686357 A US63686357 A US 63686357A US 3080230 A US3080230 A US 3080230A
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United States
Prior art keywords
layer
emulsion
silver halide
negative
transfer
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Expired - Lifetime
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US636863A
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English (en)
Inventor
Haydn Hildegard
Konig Anita Von
Weyde Edith
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Agfa Gevaert NV
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Agfa AG
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    • GPHYSICS
    • G03PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03CPHOTOSENSITIVE MATERIALS FOR PHOTOGRAPHIC PURPOSES; PHOTOGRAPHIC PROCESSES, e.g. CINE, X-RAY, COLOUR, STEREO-PHOTOGRAPHIC PROCESSES; AUXILIARY PROCESSES IN PHOTOGRAPHY
    • G03C8/00Diffusion transfer processes or agents therefor; Photosensitive materials for such processes
    • G03C8/40Development by heat ; Photo-thermographic processes
    • G03C8/4006Development by heat ; Photo-thermographic processes using materials covered by the groups G03C8/04 - G03C8/06
    • GPHYSICS
    • G03PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03CPHOTOSENSITIVE MATERIALS FOR PHOTOGRAPHIC PURPOSES; PHOTOGRAPHIC PROCESSES, e.g. CINE, X-RAY, COLOUR, STEREO-PHOTOGRAPHIC PROCESSES; AUXILIARY PROCESSES IN PHOTOGRAPHY
    • G03C5/00Photographic processes or agents therefor; Regeneration of such processing agents
    • G03C5/26Processes using silver-salt-containing photosensitive materials or agents therefor
    • G03C5/29Development processes or agents therefor
    • G03C5/315Tanning development
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10STECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S430/00Radiation imagery chemistry: process, composition, or product thereof
    • Y10S430/166Toner containing

Definitions

  • PHOTOGRAPHIC STRATUM TRANSFER PROCESS AND ELEMENT THEREFOR Filed Jan. 29, 1957 SILZz/erhaZL'de negative emulsion Uuzl includes developer and can corzlaz'n mozlsture-evolvug irgredzenb.
  • Non: lcderalgreversed pas iiive is ikerebyprovided wz'ihoul the useof bodzes ofprooessing INVENTORS lzfildegard Haydn An z'lat Uon/ JCo'u iy F ATTORNEYS v. t L fi PHGTO GRAPHHC STRATUM TRANSFER PRGCESS H AND ELEMENT THEREFOR Hildegard Haydn, Anita von Kiinig, and Edith Weyde', Legregkusen, Germany, assignors to Agra Alitiengese'llso a t Filed .Fan, 29, 1-957, Sen.- No; 636,863 Claims priority, application Gerrnany Feb. 18, 1956 Claims. (Cl.-96--27)
  • the present invention relates to a process for the direct production of positives by means of silver halide emulsions which are developed by heat without applicatiorr of any processing baths.
  • the silver halide developing substances which are used are those which so change the binding agent of the silver halide layer with the reduction of the exposed silver halide that itbecomes" infusible and unswellable, while the unmodified silver halide emuls'ion at the unexposed areas is used for building up the positive image by transferring the said unmodified silver halide emulsion to the transfer layer and reducing it in the transfer layer to a silver image.
  • Such silver halide developing substances are referred to herein as tanning developers.
  • A- black coloring or the record eaii also be obtained by using an emulsion of appropriate composition or by adding suitable compounds to the positive layer.
  • Any silver halide emulsion can be used for the production of the negative layer, such as silver chloride, silver bromide, silver chlorobromide, and silver iodobrom'i'de emulsions.
  • binding agent it is possible to use those which are normally used in the photographic art and which are hardened by the action of heat by developer-oxidation products, such as for example, gelatin, polyvinyl alcohol, carboxymethyl cellulose and mixtures of these substances.
  • the pH value of the emulsion is preferably adjusted to about 3.5-6.5.
  • non-tanning silver halide developing substances such as p-methyla'rnino phenol, p-amino phenol or their substitution products, to the hardening developers in amounts up to about 20% by weight as calcul'ated' on the tanning developer.
  • the photographic layers substances which slowly split off sulphur dioxide or sulphurous acid and the cleavage products of which do not cause either a hardening of the gelatin or any other undesirable influencing of the silver halide emulsion during storage.
  • examples of such substances are bisu-lphite compounds of such aldehydes or ketones as do not harden gelatin.
  • Particularly suitable for this purpose are aldehydes and ketones which have a relatively high boiling point, particularly a boiling point higher than C.
  • aldehydes are aromatic, ar'alipha'tic aldehydes, and heterocyclic aldehydes, such as be'nzald'ehyde, terephthalaldehyde, cinn'amaldehyde, salieylaldehyde, furfural,
  • cycloaliphatic ketones such as cyclope'ntanone and cyclohexanone
  • ar'aliphat'ic ketones such as benzala'eetone
  • heterocyclic ketone's' such as isatin
  • the acetonebisulphite compound would be less suitable, since this substance only gives slight protection against oxidation of the developer because it has a comparatively strong tendency to decompose with volatilization of the acetone.
  • substances which are particularly suitable are: Terephthalaldehyde bisulphite, cinnam'aldehyde bis'ulph'ite, benzal'dehyde bisulph'it'e, salicylal'dehyde bisulphite, cyclohexa'none" bisulphite, cycl'opentanone bisulphite', and f-urfural bi'sulphite, these compounds being preferably used in the form of their alkali-metal salts, suefr as their sodium, potassium, and lithium salts.
  • the organic developing substances are preferably applied in quantities of about 0.5-3 g. per cc. of an ordinary silver halide emulsion, whereas the aforementioned stabil'izers are preferably used in quantities of- O.2-'2 parts per part by weight of organic developing substance.
  • Suitable additive compounds of this type are salts of inorganie or organic acids containing water of crystalliiatiorr, such as for example, sodium citrate (C H G Na 51-33 0) sodium acetate (CH COONa-3H O), e'alciuin aeeta'te (ICa-(CH C0O') 2 2H O) trisodium phosphate Na3P0 4-1'2H 0'), sodium sulphate mason, arid/or substances which ensure a high residual moisture content, such as, for example, glycol, glycerol, and sorbit-o'l.
  • salts of inorganie or organic acids containing water of crystalliiatiorr such as for example, sodium citrate (C H G Na 51-33 0) sodium acetate (CH COONa-3H O), e'alciuin aeeta'te (ICa-(CH C0O') 2 2H O) trisodium phosphat
  • thjiwat'er content of the negative material amounts to 8-42, preferably 8-10 percent by weight.
  • the negative layer can be arranged on any suitable layer support which is stable at the temperatures usually used for heat development, such as for example, paper,
  • an intermediate layer by which the holding strength of the emulsion layer is reduced so that the stripping of the unexposed gelatin is promoted.
  • Particularly suitable for this intermediate layer are alcohol-soluble heat-resistant substances, such as ethyl cellulose, polyvinyl pyrrolidone, zein, polyethyl acrylate and polyvinyl acetate.
  • Any suitable heat-resistant support can be used as transfer layer.
  • the transfer layer can be any suitably coated or uncoated paper, or a plastic, fabric, or metal foil.
  • the coating of the said paper can contain additives which split off water and also additives by which the transferred record is blackened, such as, for example, nitrogen-containing organic compounds as, for instance, N-diethyl aminoethanol, triethanolamine, tetrarnethyl am- -monium hydroxide, pyridine, piperazine, hydrazine, or compounds containing sulphur, such as thioacetarnide.
  • additives which split off water and also additives by which the transferred record is blackened, such as, for example, nitrogen-containing organic compounds as, for instance, N-diethyl aminoethanol, triethanolamine, tetrarnethyl am- -monium hydroxide, pyridine, piperazine, hydrazine, or compounds containing sulphur, such as thioacetarnide.
  • additives which split off water and also additives by which the transferred record is blackened, such as, for example, nitrogen-containing organic compounds as, for instance, N-diethyl amino
  • the production of the positive or the transfer process can either take place together with the developing process Furthermore, several copies can be made from the negative, this taking place immediately after the first transfer or at different later stages. However, care should be taken that the negative is not exposed to light in the intervening period.
  • EXAMPLE 1 Negative Zayer. g. of pyrocatechol, dissolved in a small amount of water, 10 g. of terephthalaldehyde bisulphite, 200 g. of sodium acetate containing water of crystallization (CH COONa-3H O) and 0.05 g. of benzotriazole are added to 1 liter of any desired silver halide emulsion. Other additives known in the emulsion art can also be used. The emulsion is cast on paper or another layer support and dried.
  • Transfer layer A 1% solution of acetyl cellulose acetobutyrate in acetone is cast on a layer support, such as, for example, paper, and then dried. It is advisable to add a plasticizer such as a phthalic acid ester, to the layer.
  • a plasticizer such as a phthalic acid ester
  • the negative is brought into contact with the transfer layer.
  • the negative and transfer layer are then subjected to a temperature of 90 to 150 C., preferably l10l20 C., for 5 to seconds in a hot press.
  • the transfer layer can be heated at a lower temperature. After separation, the gelatin of the unexposed areas adheres to the transfer layer. After subsequent exposure thereof with diffused light and after reheating, a deep black unreversed positive is obtained of the original image.
  • EXAMPLE 2 Negative layer.-20 g. of pyrocatechol and 2 g. of prnethylaminophenol sulfate in a small quantity of Water, are added to 1 liter of any desired silver halide emulsion. This emulsion has added thereto 6 g. of cyclohexanone bisulphite, 180 g. of sodium acetate containing Water of crystallization, and 0.05 g. of benztriazole or corresponding amounts of other stabilizers. This emulsion is cast on a support as in Example 1 and dried.
  • Transfer layer A 1% alcoholic solution of acetyl cellulose has 5 g. of piperazine per liter added thereto. The solution is cast on a support and dried.
  • Negative layer 25 g. of 4-cyclohexyl pyrocatechol, dissolved in 30 cc. of dimethyl formamide, are added to one liter of any desired silver halide emulsion. 10 g. of terephthalaldehyde bisulphite, 225 g. of sodium acetate containing Water of crystallization, 0.05 g. of benztrilazole, and 0.03 g. of phenyl mercaptotetrazole are then added to the emulsion, which is then cast on a support as in Example 1 and dried.
  • Transfer layer A 2% solution of a copolymer of 30% acrylic acid and 70% of methyl methacrylate in dimethyl formamide is cast on a layer support and dried.
  • Negative layer 22 g. of monotertiary butyl pyrocatechol are introduced into 1 liter of silver chloride emulsion and then to the emulsion is added 200 g. of sodium acetate containing water of crystallization and 5.5 g. of cyclopentanone bisulphite. Stabilizers and other known additives such as wetting agents can be added.
  • This emulsion is cast on a support :as in Example 1 and dried.
  • Transfer Iayer.3 cc. of N-diethyl aminoethanol are added to liter of a 3% alcoholic solution of a condensation product obtained from hexamethylene diamine adipate and caprolactam(epsilon-caprolactam).
  • EXAMPLE 6 Negative [cyan-The starting material is a silver halide emulsion in which 10 to 30% of the normal gelatin is replaced by one of lower constants, i.e. and a gelatin which has been partially degraded as, for instance, by heating an aqueous solution of gelatin at a temperature of 80 C. for several hours. Developer and additives can be those of Examples 2-5.
  • a fine mesh fabric such as silk gauze or plastic fabric is suitable as positive material.
  • the fabric can also be coated with one of the aforementioned plastic solutions.
  • EXAMPLE 7 Negative layer.
  • the starting material is a silver halide i emulsion in which 15% of the gelatin is replaced by polyvinyl alcohol.
  • the additives can be the same as in the preceding examples.
  • Transfer layer One of the layers described above is used as positive layer, and the processing then takes place accordingly.
  • EXAMPLE 8 scribed is used as positive and also an ordinary piece of Writing paper.
  • EXAMPLE 9 A silver chloride emulsion with the following additives per liter of emulsion is used for producing the negative layer:
  • nitrobenzimidazole 0.1 g. of nitrobenzimidazole, and also 0.05 g. of mercaptobenzthiazole.
  • Transfer layer The paper is impregnated with a 10% sodium acetate solution and is then used as the transfer paper. On being heated, this paper gives oif a certain amount of water which accelerates the reactions.
  • This solution is cast onto a paper which has been treated beforehand with a 1% alcoholic solution of ethyl cellulose.
  • Transfer layer Any desired writing paper can be used.
  • the negative is brought into contact with the transfer layer.
  • the negative and transfer layer are then passed between two heated rollers, in which they are subjected to a temperature of approximately 90 to 150 C.
  • the two layers are then quickly pulled apart, only some of the unexposed negative layer remaining adhering to the positive (transfer) paper.
  • the operation can be repeated 3 or 4 times in the same way.
  • the thickness of the negative layer is of importance, since it is possible to produce more copies with a thicker coating of negative layer.
  • a photographic material for preparing positive photographic images without the use of bodies of processing liquid said material including a support and a light-sensitive tannable silver halide emulsion layer on the support, the emulsion layer containing an effective amount of a tanning delevoper, a non-tanning developer in an amount effective to accelerate the initiation of the development, and for every part by weight of developer about 0.2 to 2 parts by weight of a bisulphite of a compound selected from the group consisting of aldehydes and ketones that have a boiling point above 80 C. and that do not harden the emulsion.
  • a photographic material for preparing positive photographic images without the use of bodies of processing liquid including a support and a lightsensitive tannable silver halide emulsion layer on the support, the emulsion layer containing an effective amount of a tanning developer, a compound that evolves moisture at a temperature between 80 and 150 C. and in a concentration such that the water content of the emulsion is from 8 to 12%, and a bisulphite of a compound selected from the group consisting of aldehydes and ketones that have a boiling point above 80 C., the bisulphite being present in a concentration between 0.2 and 2 parts by weight for each part by weight of the developer.
  • a process for the product-ion of non-laterally-reversed positive photographic images without the use of bodies of processing liquid comprises exposing to an original image a light-sensitive silver halide emulsion layer containing a tanning developer that causes the emulsion to be tanned in its photographically exposed areas when developing action takes place, and also containing, in an amount between 0.2 and 2 parts by weight per part by weight of the developer, a bisulphite of a compound of the group consisting of aldehydes and ketones that have a boiling point above C.
  • blackening agent is selected from the class consisting of N-diethylaminoethanol, triethanolamine, tetramethylammonium hydroxide, pyridine, piperazine, hydrazine, and thioacetamide.

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  • Physics & Mathematics (AREA)
  • General Physics & Mathematics (AREA)
  • Silver Salt Photography Or Processing Solution Therefor (AREA)
  • Photosensitive Polymer And Photoresist Processing (AREA)
US636863A 1956-02-18 1957-01-29 Photographic stratum transfer process and element therefor Expired - Lifetime US3080230A (en)

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DEA24337A DE1015313B (de) 1956-02-18 1956-02-18 Verfahren zur direkten Herstellung von Positiven mit Hilfe der gerbenden Entwicklung

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BE (1) BE555103A (el)
CH (1) CH361193A (el)
DE (1) DE1015313B (el)
FR (1) FR1172609A (el)
GB (1) GB821506A (el)

Cited By (18)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3155517A (en) * 1962-11-08 1964-11-03 Du Pont Photographic compositions and elements
US3155515A (en) * 1961-12-08 1964-11-03 Du Pont Photographic products
US3157500A (en) * 1962-09-11 1964-11-17 Eastman Kodak Co Photographic products containing magnetic particles and processes therefor
US3180731A (en) * 1962-03-14 1965-04-27 Eastman Kodak Co Photothermographic elements and method of using same
US3203797A (en) * 1962-10-16 1965-08-31 Andrews Paper & Chem Co Inc Thermal diazotype method and developer sheet for use therein
US3203800A (en) * 1962-01-05 1965-08-31 Gevaert Photo Prod Nv Photographic material comprising a silver halide emulsion containing an anti-bronzing agent
US3212895A (en) * 1960-12-20 1965-10-19 Eastman Kodak Co Stability of rapid-processed photographic materials
US3232756A (en) * 1962-08-20 1966-02-01 Eastman Kodak Co Colloid transfer process
US3248219A (en) * 1960-09-06 1966-04-26 Cons Electrodynamics Corp Photographic element for dry processing
US3278307A (en) * 1961-11-21 1966-10-11 Eastman Kodak Co Photographic process for producing prints stabilized against print-out
US3293035A (en) * 1962-04-26 1966-12-20 Gevaert Photo Prod Nv Tanning development
US3301677A (en) * 1963-09-30 1967-01-31 Agfa Ag Photographic images and printing forms prepared by heat development
US3379532A (en) * 1963-07-05 1968-04-23 Zindler Lumoprint Kg Image receiving sheet with a double pvahygroscopic salt layer coating
US3523795A (en) * 1964-12-25 1970-08-11 Fuji Photo Film Co Ltd Heat developable photographic copying materials
US4359397A (en) * 1980-12-31 1982-11-16 Polaroid Corporation Benzotriazole complexes and film units employing same
US4418139A (en) * 1980-12-31 1983-11-29 Polaroid Corporation Film units containing thermally induced water-releasing benzotriazole complex
US4822717A (en) * 1986-07-25 1989-04-18 Fuji Photo Film Co., Ltd. Image-forming method employing light-sensitive material containing silver halide, reducing agent and polymerizable compound
US5304454A (en) * 1991-05-07 1994-04-19 Fuji Photo Film Co., Ltd. Image forming method using silver halide, reducing agent and polymerizable compound

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1080854B (de) * 1957-12-10 1960-04-28 Zindler Lumoprint Kg Verfahren zur Herstellung seitenrichtiger positiver Abbildungen unter Waermeeinwirkung und Positivmaterial zur Durchfuehrung dieses Verfahrens
DE1298415B (de) * 1962-10-29 1969-06-26 Eastman Kodak Co Verfahren zur UEbertragung von Bildern
NL301026A (el) * 1962-11-28
US3306747A (en) * 1962-12-26 1967-02-28 Polaroid Corp Diffusion transfer product with microcapsules containing glycerin-water solutions

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US742405A (en) * 1901-12-17 1903-10-27 Farbenfabriken Elberfeld Co Photographic plate and process of making same.
GB392938A (en) * 1930-12-11 1933-05-26 Kodak Ltd Improvements in or relating to photo-sensitive materials and the production of photographic images thereby
GB399269A (en) * 1932-05-31 1933-10-05 Michele Martinez Improvements in or relating to the formation of relief images for photographic and other purposes
US1954325A (en) * 1930-11-17 1934-04-10 Martinez Michele Photographically produced gelatin relief
GB427962A (en) * 1933-10-27 1935-04-29 Werner Paul Leuch Improvements in or relating to the production of photographic diazotype prints
US2596756A (en) * 1947-11-04 1952-05-13 Eastman Kodak Co Photomechanical copy method
US2716059A (en) * 1952-01-21 1955-08-23 Eastman Kodak Co Photographic transfer process
US2747999A (en) * 1953-03-16 1956-05-29 Eastman Kodak Co Photographic reproduction process
US2835575A (en) * 1955-04-05 1958-05-20 Eastman Kodak Co Photographic reproduction process
US2865745A (en) * 1955-08-25 1958-12-23 Eastman Kodak Co Photographic reproduction process

Patent Citations (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US742405A (en) * 1901-12-17 1903-10-27 Farbenfabriken Elberfeld Co Photographic plate and process of making same.
US1954325A (en) * 1930-11-17 1934-04-10 Martinez Michele Photographically produced gelatin relief
GB392938A (en) * 1930-12-11 1933-05-26 Kodak Ltd Improvements in or relating to photo-sensitive materials and the production of photographic images thereby
GB399269A (en) * 1932-05-31 1933-10-05 Michele Martinez Improvements in or relating to the formation of relief images for photographic and other purposes
GB427962A (en) * 1933-10-27 1935-04-29 Werner Paul Leuch Improvements in or relating to the production of photographic diazotype prints
US2596756A (en) * 1947-11-04 1952-05-13 Eastman Kodak Co Photomechanical copy method
US2675313A (en) * 1947-11-04 1954-04-13 Eastman Kodak Co Photographic reproduction process
US2716059A (en) * 1952-01-21 1955-08-23 Eastman Kodak Co Photographic transfer process
US2747999A (en) * 1953-03-16 1956-05-29 Eastman Kodak Co Photographic reproduction process
US2835575A (en) * 1955-04-05 1958-05-20 Eastman Kodak Co Photographic reproduction process
US2865745A (en) * 1955-08-25 1958-12-23 Eastman Kodak Co Photographic reproduction process

Cited By (21)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3248219A (en) * 1960-09-06 1966-04-26 Cons Electrodynamics Corp Photographic element for dry processing
US3212895A (en) * 1960-12-20 1965-10-19 Eastman Kodak Co Stability of rapid-processed photographic materials
US3278307A (en) * 1961-11-21 1966-10-11 Eastman Kodak Co Photographic process for producing prints stabilized against print-out
US3155515A (en) * 1961-12-08 1964-11-03 Du Pont Photographic products
US3155516A (en) * 1961-12-08 1964-11-03 Du Pont Photographic products
US3155514A (en) * 1961-12-08 1964-11-03 Du Pont Photographic compositions and elements
US3155507A (en) * 1961-12-08 1964-11-03 Du Pont Photographic processes
US3203800A (en) * 1962-01-05 1965-08-31 Gevaert Photo Prod Nv Photographic material comprising a silver halide emulsion containing an anti-bronzing agent
US3180731A (en) * 1962-03-14 1965-04-27 Eastman Kodak Co Photothermographic elements and method of using same
US3293035A (en) * 1962-04-26 1966-12-20 Gevaert Photo Prod Nv Tanning development
US3232756A (en) * 1962-08-20 1966-02-01 Eastman Kodak Co Colloid transfer process
US3157500A (en) * 1962-09-11 1964-11-17 Eastman Kodak Co Photographic products containing magnetic particles and processes therefor
US3203797A (en) * 1962-10-16 1965-08-31 Andrews Paper & Chem Co Inc Thermal diazotype method and developer sheet for use therein
US3155517A (en) * 1962-11-08 1964-11-03 Du Pont Photographic compositions and elements
US3379532A (en) * 1963-07-05 1968-04-23 Zindler Lumoprint Kg Image receiving sheet with a double pvahygroscopic salt layer coating
US3301677A (en) * 1963-09-30 1967-01-31 Agfa Ag Photographic images and printing forms prepared by heat development
US3523795A (en) * 1964-12-25 1970-08-11 Fuji Photo Film Co Ltd Heat developable photographic copying materials
US4359397A (en) * 1980-12-31 1982-11-16 Polaroid Corporation Benzotriazole complexes and film units employing same
US4418139A (en) * 1980-12-31 1983-11-29 Polaroid Corporation Film units containing thermally induced water-releasing benzotriazole complex
US4822717A (en) * 1986-07-25 1989-04-18 Fuji Photo Film Co., Ltd. Image-forming method employing light-sensitive material containing silver halide, reducing agent and polymerizable compound
US5304454A (en) * 1991-05-07 1994-04-19 Fuji Photo Film Co., Ltd. Image forming method using silver halide, reducing agent and polymerizable compound

Also Published As

Publication number Publication date
FR1172609A (fr) 1959-02-12
DE1015313B (de) 1957-09-05
GB821506A (en) 1959-10-07
CH361193A (de) 1962-03-31
BE555103A (el)

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