DE2364850A1 - METHOD OF PHOTOGRAPHIC ETCHING AND PHOTOGRAPHIC PRINTING USING RADIATION TRACES OF TONED PHOTOGRAPHS CAUSED BY GAP FRACTIONS AND / OR ALPHA PARTICLES - Google Patents

Description

DIPL-ING. HELMUT KOEPSELL 5 COLOGNE 1 12/27/73 = h,

PATENT Attorney Mitteistrasse 7

Telephone (0221) 219423 __ _Λ Telegram address: Koepsellpatent Cologne

As / 109

Registration number. please specify

Patent application

of the company

AUSTRALIAN ATOMIC ENERGY COMMISSION, Cliffbrook, 45 Beach Street, Coogee, New South Wales 2023, Commonwealth of Australia

Method of photo-etching and photogravure printing using cracking fragments and / or alpha particles Ray etch marks from toned photographs

The invention relates to the reproduction of photographs Illustrations or the like · There is a large and lasting one Need for the ability to transfer photographic images or the like. To surfaces that normally have no ability to take photos, i.e. are not photoreceptive.

This need is evidenced by the multiple reproduction of Photographs in newspapers, magazines and books, through the transfer of decorative images, patterns or the like Packaging, glassware, stoneware, ceramic tiles, tiles and the like., Through the reproduction of permanent measuring scales scientific instruments and through the use of photographic

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graphic techniques in the manufacture of electrically conductive and semiconducting circuits or circuits for elec- ^ electronic equipments.

A realistic reproduction of photographic images from such surfaces does not present difficult problems if the photograph consists of parts or areas, which are either completely opaque (opaque, opaque, milky) or completely transparent. The usual method is in that the material to be imaged is coated with a thin layer of a material that is normally by polymerization - can be made insoluble when exposed to light. Such © materials are used in the generally as photopolymerizable etch covers or -Designed protective layers. If such a thin layer exposed below a two-tone (black and white) photograph parts of the layer exposed to light become insoluble. Si® adhere strongly to the underlying surface at * Those parts that are covered by the black areas of the photo have been shielded, remain unchanged and can later be washed off so as to remove the corresponding areas of the metallic To leave the surface unprotected. These unprotected areas can then be designated or treated by suitable printing inks or chemical etchants or the like so as to reproduce the original photograph.

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If the photography does not consist of two tones (black and white) consists of many shades of gray, as is usually the case is the case, this method cannot be applied directly because the etching or the like. Resistant Coverage on the surface is either present or absent. It is not possible to have this coverage partially is present to partially protect the surface against subsequent attack by any chemical.

To overcome this difficulty, one is usually required Grid screen used to divide the light passing through the negative into a large number of small black and watery areas to subdivide. As a result, it remains resistant to etching or the like Cover detachable at certain points so that it can later be washed off leaving a large number of indentations can be. The surface density of this depression is roughly proportional to the blackening density of that area of the photograph, who was arranged above; however, there is no direct positional relationship between the original silver grains on the original photograph and the etching depressions that later form in the corresponding area of the die or the like. Usually, screens having about 150 lines or rows are used in the conventional method. 200 Lines, or lines per inch, is the maximum for a skilled engraver. This maintains the resolution of fine details in limited to the transmitted image.

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Be _x i application of the invention, a photograph is toned with a chemical substance which reacts with the silver grains. After toning, the silver grains, spontaneously or indirectly by being irradiated, emit densely ionizing radiation such as crack fragments or alpha particles. This densely ionizing radiation can produce a "radiation damage image" on any surface with which the photograph has been brought into contact. On many surfaces, this radiation damage map ^{11 will have} electrical, magnetic, and chemical properties different from areas of the surface unaffected by radiation. These different properties of the radiation damage map ¹¹ can find many useful applications in engineering or the like The different electrical and magnetic properties of the painting can be used directly in the production of electrical circuits or circuits An extremely useful manufacture of the increased reactivity of "radiation damage imaging" is the use of etchants to produce a gravure image many types of surfaces against which the toned photograph has been pressed.

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In this way the invention makes a method of precision dating or precision etching in down to the smallest localized areas of a surface for all areas in question Technique etc. applicable.

The essential advantages that can be achieved by the invention exist in that - no diffuser or soft focus is necessary to prevent the loss of. small details caused and that the etched depressions or doped or retouched areas of the transferred image are direct with regard to their position Relate to the silver grains of the original photograph, whereby a reproduction that is much more faithful to the original can be achieved. In fact, it can be assumed that no any other method of reproducing gravure images ever developed or contemplated by the Establishing a direct relationship in terms of their position between the elements of the transferred image and the silver grains the original photography made possible.

When an etch-resistant pad covers a metal plate or cylinder and parts of it are washed off a number of small areas in connection with the application of the conventional method described above or to produce when using the method according to the invention, For example, the actual metal can be etched through these holes or the like to make a number of etching pits

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generate that can be used to print ink or the like. onto an absorbent surface, such as B. paper to transfer. This is the most commonly used method of making a gravure plate or cylinder for the rapid multiple redesign of photographic images as with the rotogravure printing process. The invention includes a Method by which the printing ink dots that are transferred to the paper have a direct position with regard to their position Relationship to the location of the silver grains in the original Exhibit photography.

In lithographic printing, the transfer of the printing ink is based on the fact that certain areas of the plate are preferentially moistened by the printing ink, the transfer of the printing inks not being controlled by the depth of etching pits or the like. The new method is applicable in an equally good way M also in lithographic printing because the changed or influenced chemical properties of the "Strahlenschädehabbildung ¹ * manifest itself in the form of an increased capacity for the printing ink (this phenomenon _is;. Akin to the well-known methods, in which foils or plates made of plastic, which are used for packaging purposes, are made more receptive to printing inks by bombarding their surface with electrons).

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On the other hand, there is a possibility that when using Metallic surfaces for lithographic printing an etch protection can be used, which is penetrated by holes an etching trail created by a toned photograph. A chemical reagent then becomes the option given to be effective through these holes of the etching track, to make the underlying plate wettable by printing ink, in specific localized areas in a manner which corresponds to the manner generally customary and used in the prior art (cf. Example III).

The invention depends on and includes three main principles. These are:

1. Photographs can be toned with other substances in such a way that that the silver grains of the photograph combine with or through some other material be replaced.

2. The material used for toning the photograph can of those isotopes are selected, the fissure fragments or Alpha particles emit due to their radioactivity. The invention: continues to extend to certain elements which, although they are neither fissure fragments nor alpha particles, spontaneously emit, are brought about by bombarding them with neutrons can.

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3. If dense ionizing radiation such as crack fragments or Alpha particles cover the surface of many types of solids hits, traces of damage are caused that have different properties compared to the undamaged material. On many surfaces, the damaged areas can be etched away to leave indentations that can be clearly seen below Microscope are recognizable. It has been found that fissure fragments cause such effects on glass, mica, ceramics and many minerals and plastics. With alpha particles it has been found that this effect only occurs with particularly absorbent plastics such as nitrocellulose.

Fissure fragments are spontaneously emitted from some radioisotopes, z. B. California-252j many alpha-active radionuclides » are known, e.g. B. ELoniüm-210. A higher particle density in terms of fissure fragments can be achieved if fissile Elements like uranium-233, uran-235 or plutonium-239 with neutrons be irradiated. A higher density of parts in relation to alpha particles can also be achieved by using the elements boron or Lithium can be irradiated with neutrons.

When applying the invention, a photograph made with a of these materials is toned, pressed against the surface of a suitable body. Over time (and sometimes, however not always by means of neutron bombardment) the image on the Surface in the form of split fragments or alpha partial

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to the traces of damage caused. At this stage, the image is not visible even under the microscope. They only become visible after they have been developed by immersing them in a suitable etching liquid. For some applications, such as transferring decorative images onto mirrors or potion glasses, no further treatment is required. In other cases, however, there is the possibility of making the image more visible or vivid by filling the etching depressions or etching pits with a suitable color or a coloring or otherwise drawing liquid. Furthermore, when using inks with low viscosity and high pressure, images can be transferred to absorbent surfaces such as paper in order to form the basis of a "high f idelity ¹¹ printing process".

However, those made using these direct methods Etching depressions have very small dimensions "(since they cannot exceed the penetration depth of the ionizing particles); In addition, the process cannot be applied directly to metals can be applied (only non-conductors are able to maintain traces of action that can later be etched). This includes the direct design of gravure metal printing plates the end. In addition, the pressure and the

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low mechanical strength of sheets made of plastic, glass, etc. can cause difficulties.

However, this difficulty is caused by the following method of preparing metal plate !! eliminated with deeper etch pits been. This method can also be used to create deeper pits, depressions or the like on non-metallic surfaces to achieve; however, metals are generally used for printing plates used.

In this process, the material in which the damage or impact traces are caused and etched is in the form of a thin barrier layer on an underlying die or the like. Tcrhanden. The barrier layer can be on the die, mater or Like. Be applied as a solution, which then dries or polymerized to form a protective coat. There is also the option of chemical or protection To form electrochemical treatments, for example by producing a protective oxide layer on aluminum or titanium or other metals by anodizing them.

The barrier layer can be etched away at the points where alpha particles or fissure debris have passed; However the underlying die or the like is protected in all other places. Thus, the etching liquid penetrates through the

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Protective layer only penetrates in places where it is ionizing Particle has been traversed. This creates an etching pit in the die below or the like. Inside a distance of a few micrometers from a toned silver grain in the original photograph overlaid manufactured. In some cases, another etching liquid intended to attack the die or the like can be used after the first etching process has made holes in the protective layer. Electro-etching techniques can also be used to attack either the protective layer or the die or the like. Both. In all cases, whether one caustic or two are used, and whether or not an electrofitting method is used, the depth of the etching pits in the die or the like may be used. can be varied and adjusted as desired by adjusting the contact time with the etching liquid. That way, a solid intaglio printing plates can be manufactured that allow rapid transfer of color to paper without the application of excessive Pressure causes.

The method according to the invention can also be used for production of relief images (high etching, relief engraving)., at .which the image lies above the surrounding surface and is not sunk into it, as is the case with gravure printing the case is. Such relief images can also can be used for printing. In addition, when preparing such relief images using precious metals or

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Corrosion-resistant metals very durable and decorative photographs can be obtained, which are of particular value in connection with the production of jewels, jewelry or the like. And the maintenance of archives, registers or the like. Are.

One method for dividing or preparing such relief images is that prints or replicas of intaglio images are produced using the methods described above. One such method of making decorative metal photographs is by making an intaglio image on a glass plate using the methods described above, and then applying silver to the intaglio image using any of the known mirror making techniques . Metals other than silver can also be used. The metal can be applied using vacuum evaporation techniques or from chemical solutions. The thin metal layer on the glass plate is then reinforced in terms of its thickness by electroplating or electroplating, it being possible for additional quantities of the same metal or a different metal to be applied. When the metal is thick enough to have sufficient strength, it will separate from the glass. Many such metal relief photographs can be made from the same etched glass plate.

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Materials other than glass can also be etched to obtain relief photographs. The relief photography can also in a manner other than using the method described above with the application of silver and galvanic metallization. For example, an imprint or a replica of the intaglio image can be achieved by pouring molten materials onto the image. Another possibility is to pour liquids that solidify in place.

A relief image can also be produced in that a modification of the protective coating technique is used, described above had been described.

In the manufacture of such a plate, holes are first made through the protective layer, as in the manufacture of the gravure plate etched; however, in the second step, instead of etching the die or the like through the holes, electroplating is used used to build up the material of the die or the like, where the holes in the protective layer allow this. Off-set printing plates can be produced in this way. Lithographic Printing plates can be prepared in the same way or made by electroplating small quantities of a hydrophobic metal such as copper is applied to a surface of a hydrophilic metal such as nickel (or vice versa).

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As a modification of the method using the protective layer a material can be used as a cover or protection, which at Warming decays in those areas that have been irradiated. The layer below can then be etched occur.

Special applications of the method according to the invention are described in the following examples:

Example I Decorative etching of a polycarbonate plastic sheet

A fine grain photographic negative of medium sensitivity or brightness is exposed and developed in the usual way before applying e ~ with the fissile isotope uranium-233 using the following procedure:

The toning solution is made from a 1% solution of ferric calcium (red blood liquor salt). On every. 100 ml (milliliters) of this solution are added to 10 ml of anhydrous acetic acid and 2.5 ml of a uranyl nitrate solution which contains 1 mg of U - γ ml. Sufficient solution is made to cover the negative when it is rolled up along the inner wall of a cylindrical container. The container is tightly closed and is shaken with the negative for about two hours. The negative is then demineralized with

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Water several kale and then an hour in running water washed. It is then washed for a few minutes in a 2 # solution of ammonium thiocyanate until all traces of yellow Color has disappeared from the clear areas of the gelatin. After another ten minutes of washing in running water, it becomes the negative dried.

It is then covered with a sheet or sheet of transparent polycarbonate clamped together so that the layer is in contact with this film or the like. Is to be embossed or provided with an order. The negative is then thermal Neutrons irradiated, with a flow or a particle density of 5 x 10 neutrons / (cm) / (sec) during the Duration of ten minutes, so that uranium atoms split in the toned image and bombard the polycarbonate surface.

After removing from the neutron flux, the polycarbonate sheet is separated from the negative and in a solution for fifteen minutes etched by 6.5 N sodium hydroxide at 50 ° C. In this way the original image appears on the surface of the plastic. The image can be made more visible or more decorative by adding a suitable color to the etched pits rubbed and the excess is removed.

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It should be noted that the irradiated negative can also be immersed in the etching solution with the result that the Layer containing silver and uranium is dissolved away. When the carrier is made of a material in which gap traces are etched can be, e.g. B. cellulose-based plastics, is a gravure image that is "identical" to that of the polycarbonate film is formed, which can be used for the same purposes.

If the photographic plate has a glass support, a sodium hydroxide solution will remove the layer from the glass; then however, the glass plates must be transferred to the hydrofluoric acid to thin for etching.

Example II Production of a permanent relief photograph from precious metals

A fine grain photographic negative of medium sensitivity or brightness is exposed and developed in the usual way before it is with the spontaneously cleavable isotope Californium-252 being toned.

The negative is first hardened with formaldehyde and then with a 5% solution of potassium ferricyanide or red blood liquor salt shaken to convert the image to silver ferrocyanide.

The negative is washed thoroughly in running water and then left to stand in a solution containing California chloride for about four hours. The pH of the California solution should be adjusted to 2.0 with fuming nitric acid and should ^{contain approximately 1 micro-curie Gf-252 per cm 2} of film to be treated. As the California precipitates out of the solution, the photographic image slowly turns blue; this is a useful indicator of the extent to which the reaction has occurred. The photograph is then rinsed with demineralized water and then washed in running water for about thirty minutes. Negatives with a high haze density or background blackening are considerably improved by treating them for a few minutes before the final water wash in a 0.1 $ solution of urea or thiocarbamide, which is adjusted to pH3 with oxalic acid. The photograph is then dried and pressed against a smooth glass surface in which crack fragments from the photograph can cause traces of radiation. It is important that the glass surface is free from scratches; it must "under no circumstances be cleaned with abrasive powder or the like.

After overnight exposure to radiation, the glass is separated from the photograph and placed in a dilute solution (5 * $) of Etched hydrofluoric acid. The etching time depends to a certain extent on the type of glass and the length of the irradiation; however, it is generally 30 minutes. When the intaglio illustration is clear

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is visible and shows good contrasts, the plate is de-, washed in mineralized water and dried. The glass plate is then placed in a vacuum room; Gold is applied to the image by known evaporation techniques.

Only a very thin layer of gold can be applied in this way will; however, the thickness of the gold can be increased to any desired level by a conventional electroplating process after the plate has been removed from the vacuum system is. When the gold has reached the desired thickness, it can be dated Glass can be separated; it shows a raised relief figure on its surface, which is permanently resistant to the effects of light and atmospheric contamination.

The intaglio printing in the glass can be used to produce many such Metal relief photographs are used; if necessary, these can also be made from non-precious metals other than gold.

Example III

Making a lithographic printing plate with high

Rendering quality

A tri-metal lithographic printing plate of the type such as it is commonly used in this field, with a thin Layer of chrome on top of a thicker layer of copper

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is plated and supported by a steel support plate, is coated with a thin layer of nitrocellulose approximately 4 micrometers thick. This can be achieved in that the plate is immersed in a solution of nitrocellulose in a solvent such as ethyl acetate, whereupon the plate slowly is pulled out and the solvent can evaporate.

When the plate is completely dry, it becomes against a photograph pressed with Californium-252 using the im. previous example described procedure is toned. After a suitable exposure (obtained by counting the alpha rays emission the photograph can be estimated with a suitable alpha radiation counter) the protective layer is made of NiJBtrocellulose with 5N sodium hydroxide for a duration of approx Minutes at 30 ° C or until the image can be seen on the plate etched. The plate is then washed thoroughly and afterwards with one of the common etching liquids used in technology for dissolving chromium. In the places where this caustic liquid penetrates into the holes traced back to the radiation trail, the chromium is removed; the picture will be in the one below located copper. If the etching process is complicated, the anti-etching layer is made of nitrocellulose with a suitable one Solvent removed, plate treated with water and then lithographic ink. The paint sticks

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only on that in very small areas of the exposed copper metal shown image; the printing ink can be transferred to paper in conventional printing presses.

The examples described above are not intended to be limiting or represent limitations on the broad applicability and spirit of this invention.

The extent of the radiation traces or damage is related to the energy inherent in the formed particles. Generally it can be said that the closer the photograph to or the harder it is pressed against the surface to be depicted, the better the result. However can an image with a lesser degree of proximity or close concern can also be achieved. The terms "adjoin", "Near" or the like are used here to refer to this fact describe.

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Claims (1)

- 21 - Claims l) A method for reproducing photographic images or the like. On an occasionally non-photoreceptive surface, characterized in that the photograph is toned with substances that combine with the silver grains or replace the silver grains, so that the photograph either spontaneously or indirectly split fragments or alpha particles are emitted in quantities related to the distribution of silver grains in the photograph, the toned photograph being brought into a position near or adjacent to the surface on which the image is to be reproduced for a time which sufficient for the emissions from the photograph, image or the like _{to be reproduced as radiation exposure or T-} trace on the surface, and the areas having the traces or effects are related in terms of their position to the position of the silver grains in the original photograph. 2. The method according to claim 1, characterized by a white · The second step, in which the impact on the disturbance or traces of receding image is etched to form a gravure image. 3. Process for reproducing or transferring photographic Images on mirrors, glassware, ornaments, decorations, Jewelery, jewelery, scientific instruments, elec- 409827/1104 - ■■ trical parts and assemblies or pressure plates including of the method according to claim 2. 4. The method according to claim 1 or 2, characterized in that as a toner or grader material, the isotope such as California-252 is used, which is a spontaneous delivery of cleft fractures brings forth. 5. The method according to claim 1 or 2, characterized in that that as a toner or grader material the isotope uranium-233, Uranium-235, plutonium-239 or americium-242 is used, whichever Fissure fragments emitted when using it. Neutron is bombarded. 6. The method according to claim 1 or 2, characterized in that that as a toner or grader material, the isotope such. B. Polonium-210 is used, which spontaneously alpha particle emitted. 7. The method according to claim 1 or 2, characterized in that as a toner or grader material, the isotope such. B. Boron-10 used, which alpha particles emit when bombarded with neutrons. 8. The method according to claim 2, characterized in that the to surface to be treated a cellulose ester when using alph, particles is and mica, glass, Keianik, plastic or the like. When using split fragments. 4 0 9 8 2 7/110 4 - 23 - 9. The method according to claim 2 or 8, characterized in that the gravure images with printing ink or coloring agents be coated. 10. The method according to claim 2 or 8, characterized in that that the intaglio images have an overlay of a reflective coating to have. 11. The method according to claim 2 or 8, characterized in that the gravure pictures have an electrically conductive layer. 12. Method for transmitting or reproducing a photographic Imaging on a surface which is normally not receptive to photos and which is normally not broadcast by Split fragments or alpha particles can be made etchable, characterized in that the photograph is toned with substances that combine with or replace the silver grains, so that the photograph is either spontaneous or indirect Fissure fragments or alpha particles are emitted in quantities that are related to or dependent on the distribution of the Silver grains in photography, the surface to be provided with the image covered with a protective layer of a material is coated, which can be made etchable by emitted crack fragments or alpha particles, furthermore the toned photograph close to the protective layer for a long period of time . is placed that is sufficient for the emission of the 409 8 27/11 OA Photography the picture through traces of radiation or exposure to radiation reproduce on the protective layer, with the areas that have received the impacts in terms of their location a close relationship to the location of theS over grains in the original Have photography, furthermore using etching material, which which penetrates into the areas of the protective layer provided with the image, around the protective layer provided with the image to remove and a picture on the one below Etch surface. 13. Process for reproducing or transferring photographic Images on a surface that normally do not is photoreceptive and normally cannot be made etchable by radiation crack fragments or alpha ponds characterized in that the photograph is toned with substances that form a compound with the silver grains or replace these, making the photography either spontaneous or indirect Fissure fragments or alpha particles are emitted in quantities related to or dependent on the distribution of the silver grains in the photograph, the one with the figure to be provided surface is coated with a protective layer made of a material, which by radiation gap fragments or alpha particles can be made etchable, and furthermore the toned photograph is placed adjacent or close to the protective layer for a period of time sufficient so that the emissions from the photograph the picture 409827/1104 reproduce by radiation traces or effects on the protective layer, furthermore the areas which the effects have received a close relationship in terms of their position to the position of the silver grains in the original photograph have, and etching material is applied, which penetrates into the areas of the protective layer corresponding to the image removing the imaged protective layer further comprising applying a second etch material to form an image to etch the underlying surface. 14. The method according to claim 12 or 13, characterized in that that the protective layer is an oxide layer formed on a metal surface to be treated, or a layer of Silicon dioxide or titanium dioxide or the like. Which is using applied by chemical reactions in a suitable liquid or vapor or by vacuum deposition. 15. The method according to claim 12 or 13, characterized in that galvanic etching is used to either the protective layer or to etch the underlying surface, or both. 16. The method of claim 12, 13 or 14, wherein the with the image surface to be provided is a printing plate comprising a layer of hydrophobic material such as e.g. B. has copper on a thin layer of a hydrophilic material such as. B. Chromium adheres, which is deposited by plating or electroplating AnQ ft7 7/1104 can be brought, the protective layer on the hydrophilic Material is applied, characterized in that the ^ tze removing the hydrophilic material to expose the hydrophobic material in the shape and shape of the image. 17. The method according to claim 16, characterized in that the hydrophobic and hydrophilic layers are arranged reversed. 18. The method of claim 2, wherein the surface is normally cannot be electroplated, characterized in that that by using z. B. "Vacuum Evaporation Techniques or from chemical solutions or by casting a thin metal layer is applied to the etched imaging area and additional metal is applied by electroplating or the like is to form eisssp raised relief image. 19. The method according to claim 2, characterized in that a raised relief image is produced in that a poured liquid material in contact with the intaglio image and the material solidifies. 20. The method according to claim 13 or 14, 4 in which the surface is electroplated, characterized in that before the final removal of the protective layer, the etched imaging area is electroplated to form a relief image. 21. The method according to claim 18, 19 or 20, characterized in that that in addition the relief image is removed from the etched surface so as to provide one with the image To receive imprint. 22. The method according to claim 20 or 21, characterized in that that the prints, replicas or similar printing plates, pieces of jewelry, Ornaments, accessories provided with decoration, fittings or the like. Are. 23. The method according to claim 12 or 13, characterized in that the surface is a commercially available lithographic plate and the etching material makes the plate usable only for printing ink, 24. The method according to claim 1, characterized in that the changed electrical properties of the radiation damage image or the radiation effect or radiation trace used will. 2 $ .Method according to claim 1, characterized in that the changed χ chemical properties of the radiation damage figure or the radiation exposure or radiation trace used will. 409827/1104 26. Method for transmitting or reproducing a photographic Image on a surface that normally does not is receptive to photos and is normally not made etchable by emitted cracks or alpha particles can be characterized in that the photography with Substances are toned that combine with the silver grains or replace them, so that the photograph either spontaneously or indirectly eFissure fragments or alpha particles in Quantities emitted which are related to or depend on the distribution of silver grains in the photograph, where the surface to be provided with the image with a protective layer is coated from a material, which by radiation crack fragments or alpha particles can be made etchable, further with the toned photograph adjacent or near is placed on the protective layer for a period of time which is sufficient to ensure that the emissions from the photograph reflect the image through traces of steel or damage to the protective layer reproduce, furthermore, the areas that received the impacts are narrow in terms of their position Relation to the position of the silver grains in the original photograph have, and the protective layer is heated to vaporize the radiation damage image located thereon, and an etching material is applied to etch the underlying surface will. 27. Surfaces and objects provided with images that are produced by the method according to claims 2, 9-13 or 21 or 26 are made. 40 9 827/1104