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United States Patent O?iice 1 3,042,516 Patented July 3, 1962 2 of New Jersey the dark or in light in which the ultraviolet portions have been eliminated. These and other objects of the invention will become apparent from the description which follows. In a copending application, Serial No. 787,112, ?led January 16, 1959, an invention was described comprsiing No Drawing. Filed Sept. 22, 1959, Ser. No. 841,460 12 Claims. (CI. 96-48) on exposure to light and are capable of being ?xed in 3,042,516 PRINT-OUT CONIPOSITIONS FOR PHOTOGRAPHIC PURPOSES AND PROCESS OF USING SAME Eugene Wainer, Cleveland Heights, Ohio, assignor to Horizons Incorporated, Cleveland, Ohio, a corporation light sensitive print-out compositions which develop color stable form by subsequent heating, which compositions This invention relates to compositions of matter which 10 are composed of arylamines and halogenated hydrocar are sensitive to light and suitable for photographic and bons dispersed in a plastic ?lm-forming base, and which photographic reproduction purposes and to processes for may also contain minor amounts of basic materials such using such compositions. More particularly, this inven as amines or zinc oxide for stabilization of the mixture tion relates to the production of stable colored print-out before exposure, and minor amounts of phenol deriva tives for stabilization of the mixture after developing and ?xing, and particularly in the presence of light, heat and air. The invention described also comprehended combi nations of these arylamines to produce speci?c color effects, and sensitization of the system to the visible by images produced by exposing dry ?lms formed from such compositions of matter to light, the compositions com prising: a base consisting of a plastic binder or ?1m— forming dispersing medium, originally dissolved in a suit able solvent; one or more aryl amines; one or more hal~ ogenatcd hydrocarbon compounds selected from the 20 the addition of a yellow to red type color former, ex group consisting of halogenated hydrocarbon compounds posure to ultraviolet if this visible range color sensitizer which are capable of generating free radicals on exposure is not present, and ?nally disposing such over-all system to ultraviolet or visible light; and one or more sulfur compounds which may be either organic or inorganic on a suitable base such as glass, paper, plastic ?lm, and the like. sul?des, and the compositions may also include one or 25 Further, in this copending application, it is pointed out more additional constituents which affect the stability that fogging of the unexposed portions develops slowly and/or sensitivity of the system. over a period of weeks on exposure to air in the presence 'In general. the compositions of the present invention of light or heat or both, and it appears that this reaction provide a photographic system from which a stable image requires the presence of air, in that the colors which may be obtained entirely by dry processing techniques, 30 develop as a result of fogging tend to be ditferent in hue namely, simply by exposure to ultraviolet light followed by exposure to air containing signi?cant amounts of mois~ ture. Oxygen may be used in place of the air, in which than those obtained by the primary halogenating reac tion. This defect was minimized or eliminated by the case the ?xing reaction is more rapid. and by heat ?xing as a further step. Other techniques Such a system has utility in the photocopy ?eld of blueprints and tech nical information, the reproduction of typed and printed pages, the reproduction of information as exposed through micro?lm, the recording of information of tran sient events as on the face of a cathode-ray tube, and the like. Principal objects of this invention are to effect a re action between suitable arylamines, halogenated hydro addition of minor percentages of certain reducing agents, ' such as overcoating and the like were also utilized. Further, as described in the same copending applica tion, some of the halogenated hydrocarbons are so active that they require stabilization through the addition of mild bases such as alkyl amines, zinc oxide, and the like 40 in the formation of the active mixture prior to formation on the ?lm. The compositions of the present invention constitute carbon compounds, and sulfur compounds as above de improvements over those described in the aforesaid ap scribed so that under the influence of ultraviolet light a plication. The present compositions eliminate the need colored derivative is produced as the result of the fore 45 not only for the relatively complicated stabilization sys going reaction; to develop this color-forming reaction rapidly enough so that the total time of exposure and development may be accomplished in a few seconds in tem for prevention of fogging on storage prior to expo sure or fogging in the unexposed areas after exposure, but also eliminate the need for heat ?xing. These com order to make available a permanent and stable image; positions make it possible after photographic exposure of to provide systems in the exposure, development and fix 50 dry ?lm to ultraviolet light to obtain an image which is ing stages which may be processed by totally dry tech niques; to provide means of ?xing which permits stabili zation of the image and the elimination of the sensitivity to ultraviolet light simply on exposure to air, preferably self-?xing simply by exposure of the pictorial image to still air, preferably moist, for a period of 8 to 10 hours, in which all portions of the ?lm have ready access to air. If the air is moving, the ?xing is completed within moist, in the absence of ultraviolet light; to provide two to three hours. means of stabilization of the preexposed surfaces so that condition whereby not only will the unexposed portion the desired color reactions take place only on exposure to radiation of speci?c nature; to provide means of sta bilization of the developed image so that once formed, it is sufficiently permanent for practical purposes; to pro vide means of stabilization of unexposed portions of the of the ?lm no longer fog on standing, but also a condi ultraviolet light. A further feature of this improvement resides in the fact that the solutions prior to deposition image so that on continued exposure to light after the on a suitable base are inde?nitely stable when placed in By the term "?xing" is means a tion wherein the exposed portions of the ?lm are no longer sensitive to development of color on exposure to ?rst images are formed, color and fogging does not de velop; to provide print-out systems which are sensitive a bottle in which the air has been substantially replaced with solvent fumes. If the bottle is brown colored and 65 to visible light: to provide a range of colored images kept tightly covered, an inde?nite stability is available. with respect to hue and tint: and, it is a further object Further, the prepared plate after spreading the composi of the invention to establish systems in which the de tion and drying the same is also inde?nitely stable on sired color is developed by exposure to light and the storage providing it is placed in a container which is facility for producing such color as a result of continued sealed against the intrusion of air. The adverse elfects exposure to light of a similar wavelength is destroyed by 70 of the intrusion of air may still further be minimized by exposure of the system (after the image has been once the deliberate addition of crystals of some of the agents developed) to moist air in a state of motion either in which are present in the raw photosensitive mix. Still 3,042,516 another important bene?t is the elimination of the heat ing step for ?xing purposes. Finally, in the referred to copending application, it is 4 There appears to be no real distinction between the various types of plastic materials which might be utilized as a base. The main requirements are that they be essen noted that certain of the halogenated hydrocarbons re tially neutral, that is, not exhibit distinctly acid or basic quired prestabilization in order to reduce their activity, and such prestabilization involved the deliberate addition resin systems may be dispersed on any substrate such as of weak alkalies to the mixture. It is a further advan tage of the present invention that the need for such pre characteristics, and that they be non-hygroscopic. These glass, paper, plastic ?lms, and the like. The second essential constituent of my composition is a halogenated hydrocarbon. The halogenated hydrocar stabilization additives has been obviated. Describing my invention ?rst in general terms, I have 10 bons useful for the purposes of my invention are those organic halogen compounds which when exposed to light found that certain secondary and tertiary amines and to of suitable wavelength are decomposed photochemically a very much lesser extent, primary amines, separately or to produce free radicals. As described in my earlier ?led in combination, when mixed with certain organic halo application Serial No. 787,112, the activation energy of gen compounds which may be alkyl or aryl derivatives formation of the halogen free-radical is the important de or mixtures thereof, plus an addition of certain sulfur termining factor and it appears that in order for the halo compounds which may be organic or inorganic in nature genated hydrocarbon to be effective in the present process will, depending on the nature of the amine, the organic halogen compound in question and the sulfur compound, produce brilliantly colored products on exposure to light it must have an energy of dissociation or in other words an energy of formation of the free halogen radical of Each of The images obtained may be 20 not less than 40 kilogram calories per mole. in times of a few seconds. either in the form of line copy or continuous tone by use of techniques as described later. In general the basic sensitivity of the system is in the ultraviolet becoming substantial at 4000 A. and less, the photographic speed increasing as shorter and shorter wavelength ultraviolet the halogen compounds hereinafter indicated as preferred, it will be noted, is a halogenated hydrocarbon in which at least one active halogen (cl, Br or I) is attached to a carbon atom having not more than one hydrogen atom attached thereto. The preferred halogenated hydrocar bons are carbon tetrabromide, iodoform, and tetrachloro is used as the exposing energy. Sensitivity to the visible tetrahydronaphthalene. Other halogenated hydrocarbons may be incorporated through the addition of certain which are effective but less useful either for reasons of azo-aniline type compounds which exhibit a yellow color solubility, volatility, or slow speed of development are in solution. While the color forming reaction may be effected by 30 bromoform, chloroform, carbon tetrachloride, tetrabrom butane, hexachlorethane, hexachlorbenzene, dichlorben exposure of solutions containing the above combination acne, and the like. It appears that these compounds of reactants to ultraviolet radiation, it has been found decompose under the in?uence of light and particularly preferable to deposit the several reactants in the form ultraviolet light through the formation of two free radi of a thin ?lm wherein they are dispersed in a suitable cals, one of which is a free radical halogen and a second base or hinder. In this way, a dry system is presented is a free radical residue. Thus, for example, the free for exposure, development and processing, with outstand radicals obtained as a result of photodecomposition of ing advantages noted above. carbon tetrabromide would be the bromine free radical All of the various ingredients of the light sensitive and the carbon tribrornide free radical. In the reactions in a suitable binder. More uniform results are obtained 40 to be described, it is not known which portion of the compositions of this invention are dispersed or dissolved if at least a portion and preferably all of the ingredients are soluble in the binder. The primary exception to this requirement is where insoluble pigments are utilized both for the development of continuous tone and as an active sul?ding agent. In addition to the solvents and residue is the active agent. The nature of the halogenated hydrocarbon has a some what speci?c effect on the nature of the color which forms. For example, carbon tetrabromide used as the photohalo genator for diphenylamine will on very short exposures plastic materials, plasticizing agents such as high boiling point liquids may also be utilized to improve the ?exi produce a blue, and as the exposure continues to be ex ers have been chosen with two requirements as the foun~ ing application. tended, the color becomes almost black. lodoform in the same degree of molecular equivalence ?rst produces bility of the ?lm and to still further improve the degree a greenish-yellow and the color on lengthy exposure is of solution of the active agents. The types of binders and recommended solvents for 50 green. The use and effectiveness of these halogenated hydrocarbons has been described in the aforesaid copend these binders are listed in Table 1. Solvents for the bind The third essential constituent of the color-forming sys tems of this invention is an aryl amine. Typical amines useful in the systems of present invention are listed below by way of example in Table 2. All of the amines listed are aryl amnies, and it is a requirement that the simple solvent is to insure as good solubility for other reagents or substituted amine grouping be a side chain attached as possible. to an aryl nucleus. Furthermore it has been found that TABLE 1 60 the color-producing action is more effective from the Plastic Bases (10% Solutions) standpoint of depth of color and speed on exposure to [All parts are by weight] light when the amine is substituted with complex sub stituents. Generally speaking, in the type of compositions Number 'Blnder Solvent which are being described, secondary amines appear to 65 be the most effective with respect to speed of develop 1 ........ ._ cellnlosi-ncetute _______ __ 30 methylene dichloride-{~70 acetone. ment of color. Tertiary amines are very slightly slower 2.. .. . cellulose nitrate _______ _. 30 ethyl aleohol+70 ethyl other. dation for the choice. The ?rst is the ability to produce a relatively low viscosity solution of the polymeric mate rial in question for concentrations of plastic in the range of 5 to 15%, and the second requirement imposed on the it ________ _. ehlerinatetlrnbb 4 ________ _. t-thyleellulose . 70t0lucne+30 act-tone. . .6 ________ _. polyethylene It ........ _. polynlethylmetllucry- _. 3t) acetone-+40 methyl alcohol. toluene+30 00to1uene+10aeetone 70acetone-Hi0ethylaeteate. to those obtained by use of secondary amines. late. 7 ________ __ . . \.l.___. tn. ., . polystyrene . . . _ . _ . _ _ . . _. 00tolnene+l0 acetone. IllllIv'VlllYltlt't'ttllt'. 40 methyl alcohol+~1tl acetone-l . '.10 toluene. |mlyvlnylehlortdt-_....._ 80 tetrahydroluran—l~20 acetone. [mlyvinylldtne chloride 80 tetrahytlrolm-nn+20 acetone. t-npolynler. in this respect and single primary amines are exceptionally slow. Signi?cantly, however, mixtures of primary amines yield unexpected results with speeds that are comparable For ex ample, in the compositions of the invention aniline used alone usually produces a very faint grayish color, whereas para-toluidine will produce a faint yellow. In both cases, 75 the photoreactions are relatively slow. If a mixture of 3,042,518 6 aniline, para-toluidine, and ortho-toluidine is employed in TABLE 4 the system, a very rapid photoreaction is available and deep red colors develop out. Preferred Composition Ranges of Ingredients Per 100 TABLE 2 Parts by Weight of Resin or Plastic Base 5 Number Active Amines 1 N um her Name 1 ______ __ Formula 10 l ______ __ tliphcnylaminc_...__. tlilwnlylmulne... it _._ N-N'~dlvtl1ylanilinn", ('?ll5N(c2II5)2 Call-.Nt?lla); t7 _ [HY-ninthylttnohlstN- (Cl11:)2NC5ll4CHzCiilI4N(Clls)g T . p-p'—ln-uzylidlnchls- HClIIO?NCBTiA'IQLilicnlls hunt. __ p-|1'-p"-Inotltylidint-~ is tristN-N'tltmnthyla 4 ______ __ PrOlCl'X't'tl ratio of orgat mixture lltllllllt' p-toluidine . _ _ . _ __ ._ _ l'roforrt'd ratio of _ 2 to 1. l to 30. 1' Between 1 to 1 and 30 to l. garlic suliur compound. S ______ __ 10 to '200. Between 0.5 to 1 and 7.._._ -_ Preferred ratio olaryl amino to lnor- 15 500 to 1,000. 10 to 100. . game sulfur compound. Between 10 to 1 and 3 to l. Phatoscusitlzvr t/o rlsible l__________ 0.1 to 1.0. ll_.______ Plastlrlzer I _____________ _. It] to 1m. 10 _____ __ Ultraviolet. absorber I _____________ __ 0.1 to 1.0. [(CXI3)2NCOII|]3CII 1 If present. ulliuu). 0.. Organic halogen compound._ Aryl amino. ___________ __ 6 ______ __ N-Nhdimvthylnnilinn. N'alimctltylaniline). tN-N'-tlilnvtl|yluui Solvent ___________________________ __ compound to :try] amino Sulfur ('Oil'lpOlllltL ((lqlhhN __ _ Range) 2 ______ __ tCttllmNll ,__, fl Parts by Weight 3 ______ __ tCttlM'llmNll triplu'nylnmiuv . Reagent p-CllsCalhNllz CallsNH-z Once the combination of reagents and solvent has been disposed on a suitable base, the solvent allowed to evap orate so that a dry ?lm is present and the surface ex posed to light so as to produce an image, ?xing is readily o-toluidiue.__ o-(JllsCslhNllz l 'l'hv amines are listed to (lt'l'lOlLt' the base structures which are active. it Hit' amine is t'oltlplt'xt'tl and still retains the same base structure it is 25 obtained by permitting the ?lm to be exposed to moving nlso active. air or oxygen containing moisture. The combination of air and moisture or oxygen and moisture appears to be a requirement. Another type of amine may be utilized in addition to the arylamine in order to extend the sensitivity of the over-all photoreaction to the visible. Compounds which Plasticizers may be advantageously added to the sys are most suitable for the purpose are yellow azo com- 30 tem in amounts of between 25% and 100% of the weight pounds such as N,N'-dimethylphenylazoaniline and 4 phcnylazodiphenylamine. These may be utilized in ex ?exibility of the dried ?lm and in certain cases to im ceptionally small percentages to impart sensitivity to the prove the solubility of agents whose solution is required of the resin present (dry basis) in order to improve the visible, generally as high up in the spectral range as green. in order for them to be effective. Suitable plasticizers The novel additions which distinguish the present in- 35 include: dioctylphthalate, tricresylphosphate, polyethyl vention from that described in Serial No. 787,112 and ene glycol, di(2 - ethylhexyl)maleate, di(2 — ethylhexyl) which make it possible for such systems to be self-?xing tetrahydrophthalate and tri(2-ethylhexyl)phosphate. on exposure to moist air and still retain stability on stor Further, and signi?cantly, true continuous tone effects age are sulfur compounds. Sulfur compounds which may be obtained through use of speci?c groups of the have been found to be effective for the purpose are listed sulfur compounds which have been mentioned previous m Table 3 and it is noted that these are both organic and ly. These are not only part of the active chemical sys inorganic in nature. In general, these comprise sulfur tem, but as the result of the reaction, ?nely divided in compounds taken from the class of thiols, organic disul soluble particles are retained in the ?lm so that develop ?des. thioureas. thioacetamides, and the like. Invariably ment of color in depth may be obtained as a function of these are sulfur compounds in which the sulfur is attached 5 the degree of exposure, thus leading to continuous tone. directly to a carbon atom. The inorganic sul?des which The usual improvements in photographic speed as a have been found to be effective are light colored or white result of exposure to ultraviolet light may also be obtained sul?des which are readily soluble in dilute acids and may by adding ultraviolet absorbers as is common in the . . . . 40 he used alone or in mixture. either with themselves or art. Such ultraviolet absorbers are benzil. stilbene de' with the organic sulfur compounds indicated in the table. 50 rivatives, phenylsalicylate. and the like. Usually amounts The organic sulfur compounds also may be used in of the order of one-tenth of a percent or less are suf mixture. ?cient for the purpose. The coating solution prior to deposition is inde?nitely TABLE 3 stable when stored in a tightly closed brown bottle in Stabilizer Sulfur Compounds 55 which all air has been displaced with solvent fumes. Aft er the coating composition is spread on a suitable sub strate and allowed to dry, the sensitive ?lm thus obtained Number Name Formula is inde?nitely stable if stored in the dark in the absence of air. One of the means for accomplishing this is to _ o-tuninolmnrr'ui-thiol ...... .. Nrncnnstr 60 place the ?lm in a polyethylene bag and replace the air llisltlimi-tlrrllliiwarlmmyll- [(L'llglgNCSlgSg with nitrogen, and then heat seal the polyethylene. Sta tlisult'nlv. bility for a period of months may also be obtained with Y l~ullyl-2-thiollrt-u._.._______. l'llxt'llCllzNlH'SNllg out the use of nitrogen, by using a rather thin gauge, poly lJt-tlit'lhH-ltlilourci ____ _- ('Ell5NlI('SN[l('2ll5 lllitlll?'ll . ._ , . . _____.__ Nllgf'h'Nllg tlollm'tutt'tltiol . r _ , s _ _ _ _ _. ClhH'llglnSll llliltllt't'tzllllitlt' ____ _. ('IMF-"N11; lhiotlt'ctltnilitlo.. ____ _. ('llgCSNllCgllb tltiolwm' ____ __ ('ellg?b'NlK'slls Ililtlt' l\tiot'ul'lmltilitlt' . ethylene bag material and wrapping the sensitive plates 65 tightly so as to squeeze out as much of the air as possible NtnCsNuNm before heat sealing. Each time a plate is removed from the bag for use, this squeezing out of the air followed by ZnS-(lrlS heat scaling is a requirement. ('?llbNllf'sNllcalls Z118 gas21193 111183 A still simpler techique is to store the sensitive plates in an air-tight container which 70 may be a box or a plastic bag in which a few crystals of carbon tetrabromide have been placed in the bottom of the bag. The extremely low but signi?cant volatility of the material gradually develops an atmosphere of carbon which these various ingredients may be mixed to produce the desired results. 75 tetrabromide, which apparently prevents the small amount in Table 4 are given the ranges of proportions in 3,042,510 7 8 of residual air from being clfcctive as a destroyer of the \inlct light indicated the permanency of ?xing, since no sensitivity of the plate. further coloration developed on such an exposure. A system has now been described comprising a plastic base or hinder, an aryl amine. a free radical producing organic halogen compound. a sulfur compound, with or without the addition of plasticizers, ultraviolet absorbers. and sensitizers to the visible. Such a system is dissolved or dispersed in a suitable solvent or mixture of solvents EXAMPLE :3 To the composition of Example 1 there was added 005 gram of N-N'-dimethylphenylazoaniline, 5 grams of dioetylphthalate, and 0.1 gram of phenylsalicylate. The resulting mixture was spread on a glass plate and allowed to dry, the spreading thickness being such that and is deposited on a suitable base such as glass, plastic. a ?nished dried thickness after all solvents have been paper. and the like or it may be prepared in the form 10 eliminated was of the order of one mil. It was then ex of a self supporting ?lm. After the solvent has been posed to a No. 2 re?ector photo?ood lamp at a distance eliminated by evaporation, the dry ?lm is then exposed of 10 inches for a period of 5 seconds and the dense to ultraviolet or visible light and such exposure will gen blue-black color obtained as in Example 1 was developed crally be in the range of l to 30 seconds. After exposure. out with a faintly yellow background. After exposure, the image is ?xed simply by permitting the exposed ?lm the image was ?xed by blowing air across the ?lm for to be exposed to moving ordinary air containing the mois a period of two hours. ture it normally contains in the range of 40 to 75% rela EXAMPLE 4 tive humidity for a period of 8 to 10 hours, preferably in the dark, though ordinary light containing no ultra violet may also be used if sensitizers to the visible are absent. The action is greatly accelerated if the air is moved rapidly across the surface in which case the ?x ing takes place in 2 to 3 hours. If moist oxygen is used, ?xing takes place in 30 to 60 minutes. After such treat ment. the exposed portions are insensitive to visible and A composition was formulated by adding 2.0 grams of para-para'-benzylidinebis(dimethylaniline), 5 grams of tetrachlorotetrahydronaphthalene, 0.5 gram of thi ourea, and 3.0 grams of tri(2~ethylhexyl) phosphate to 100 ccs. of a 10% solution of polystyrene in a mixture of toluene and acetone 90:10. After spreading the re sulting composition on a glass plate and permitting the ultraviolet light even on long exposure. The light sotlrce utilized for exposure purposes in this solvent to evaporate completely, a ?lm thickness of 1.5 speci?cation is the General Electric re?ector type sun lamp of 275 watts using a glass envelope. At a distance sunlamp at a distance of 10 inches for three seconds, of It) inches. exposure times of 1 to 30 seconds are ob taincd. Having described my invention, the following examples are indicative of specific methods of practice and are to be construed as illustrative rather than as limiting. EXA RIFLE 1 One hundred (100) ccs. of a solution containing 10 grams of a low molecular weight polyvinyl chloride in mils was obtained. This was exposed to a GB. 275 watt after which a rich deep green color was obtained in the This was allowed to stand in the dark box with ready access of air for a period of 10 hours to 30 light struck areas. complete the ?xing operation. EXA MI'LE 5 One hundred (l00) ccs. of a solution of polyvinyl ace tate in a mixture of methyl alcohol, acetone and toluene (40:40:20) was mixed with 2.0 grams of para-para' para"-methylidynetris(N-N'-dimethylaniline), 8.0 grams of carbon tetrabromide, 2.0 grams of thioacetamide, an 80:20 mixture of tetrahydrofuran and acetone was 10.0 grams of dioctylphthalate, 20 ccs. acetone, and mixed with It) grams of diphcnylamine, 15 grams of car 40 stirred vigorously until the solution of the ingredients bon tetrabromide, 2 grams of bis(dimcthylthi0car was complete. The resulting solution was spread on a bamylldisul?dc, and finally 20 ccs. of acetone. The mix paper base and a measurable thickness of 0.8 mil was ture was stirred until all of the ingredients were dis obtained. This was exposed to a GB. 275 watt sunlamp solved, after which the composition was spread on a glass plate so that a dried thickness of approximately 1 mil was obtained. After all solvent has evaporated. the sensitive surface at a distance of 10 inches for a period of 2 seconds on which exposure a deep royal blue developed out in the exposed areas. Air from a small fan was blown across the image for a period of 2 hours, after which reex was exposed to a 275 watt GE. sunlamp at a distance posure to ultraviolet light for a period of 2 minutes in of 10 inches for a period of 5 seconds, after which time 50 dicated no fogging. a dense bluc~black image was obtained. The exposed EXAMPLE 6 film was then placed in a dark cabinet fitted with means to permit the entry of air and therein retained for 10 hours. Subsequent exposure to ultraviolet light pro vided no noticeable effect even though the ultraviolet exposure comparable to the intensity indicated original ly extended for a period of 5 minutes. EXA M I'LE 2 One hundred (100) ccs. of a solution containing 10 grams of a low molecular weight polyvinyl chloride dis solved in an 80:20 mixture of tetrahydrofuran and ace tone was mixed with 4 grams of diphenylamine, 6 grams of carbon tetrabromide, 2.0 grams of dodecanethiol and ?nally 20 ccs. of acetone. The mixture was stirred until all the ingredients were dissolved, after which the com position was spread on glass with a doctor knife so that a dried thickness of 1 mil was obtained. One hundred (100) ccs. of a solution containing 10 grams of polystyrene dissolved in a 90: 10 toluene-acetone mixture was mixed with a solution of 2 grams of aniline, 4 grams of para-toluidine, and 4 grams of ortho-toluidine dissolved in 90 grams of toluene. To the resulting solu tion was added 10.0 grams of carbon tetrabromide, t.0 grams of thiosemicarbizide, 5.0 grams of tricresylphos phate, 0.1 gram of N-N'-dimethylphenylazoaniline, and 30 ccs. of acetone. The solution was stirred until all of the ingredients were completely dissolved and was then spread on a glass plate and a ?lm thickness of 1.2 mils was obtained. This was exposed for a period of 5 seconds and ?xed by storing in a dark cabinet in the presence of air for 12 hours. EXAMPLE 7 A coating composition was formulated consisting of The dry sensitive surface was exposed for 8 seconds 100 ccs. of a 10% solution of cellulose nitrate dissolved to the 275 wait (til. sunlamp at a distance of l0 inches giving an exposure color of deep blue-black. The ex in a mixture of ethyl alcohol and ethyl ether (30:70), powtl tilni was lixcd by exposing it to moist moving oxy _:~cu passed over at a rate of about 1 liter per minute for to which there was added 5.0 grams of zinc sul?de, 10 grams of carbon tetrabromide, 5.0 grams of diphenyl amine, 0.05 gram of phenylsalicylate, 0.02 gram of N N-dimethylphenylazoaniline, and 5 grams of dioctyl ~15 minutes. The moisture was obtained by bubbling the oxygen tluough water. Subsequent treatment with ultra_ 75 phthalate. After thorough mixing and grinding to disperse 3,042,510 10 4. The ?lm of claim 3 wherein the amount of said azo the zinc sul?de as completely as possible. the mixture was spread on a glass plate in sut?cicnt thickness to pro~ vide a dried ?lm after all solvent was eliminated approxi mately 1.5 mils in thickness. This was exposed to a gray step scale negative for a period of 20 seconds and the image was in a blue-black color. compound is from 0.001 to 0.02 part by weight per part of plastic. It was ?xed by re taining the exposed ?lm in a dark box in the presence of air for 12 hours. Of the thirty steps of gray on the negative, twenty were recorded on the photosensitive sur face. 10 EXAMPLE 8 7. The ?lm of claim 1 in which the arylamine is se lected from the group consisting of secondary amines, tertiary amines and mixtures of at least two primary amines. Twelve 4 x 5 glass plates were coated with the disper< sions of Example l. Separately another twelve plates were coated with the dispersions of Example 7. Six of the plates prepared in accordance with Example I and six of the plates prepared in accordance with Example 8. The ?lm of claim 1 containing in addition ?nely di vided insoluble pigment, dispersed in said plastic. 9. The ?lm of claim I in the form of a self-sustaining translucent ?lm. H]. A print-out member consisting of the ?lm of claim 24 on a support selected from the group consisting of glass, paper and plastic. ll. in a method of ?xing brilliantly colored images 7 were separately stored as follows: plates were stacked one on top of each other and clear glass plates were placed on the top plate. The packages were inserted in a polyethylene bag which was molded around the plate so as to squeeze out as much of the air as possible and produced in a photosensitive layer comprising an arylamine and an organic halogcnvcontaining compound by exposure the bag was then heat sealed. One month later, one of the plates was removed from the bag and exposed to of said layer to ultraviolet light, said exposure being un der such conditions that a free radical is produced by ultraviolet light in accordance with the teachings of the previous examples for a period of 6 seconds and a full density image obtained. 5. The ?lm of claim 1 containing in addition up to about 0.1% by weight of an ultraviolet absorber, dispersed in said ?lm-forming plastic. 6. The ?lm of claim 1 containing in addition between about 0.01 and l part by weight of a plasticizer per part by weight of plastic, dispersed in said plastic. decomposition of said halogen-containing organic com Repeating the same experi pound. said halogen~containing compound being selected ment after sealing the bag but with a three month lapse from the group consisting of halogenated hydrocarbons of time produced substantially the same results. In a having an energy of formation of the free halogen radical second series, six plates each were stored in separate and sealed polyethylene bags in which approximately one 30 of not less than about 40 kilogram calories per mol and is reacted with said arylamine to produce a brilliantly col gram of carbon tctrabromide was placed in the corner ored reaction product in the exposed portions of the layer; of the bag. These bags were opened six months later and again one of the plates was exposed as taught in the previous examples for a period of 5 seconds and again a full density image was obtained. Simultaneously the improvements which comprise: providing at least one sul?de selected from the group consisting of organic sul ?des in which the sulfur is attached directly to a carbon atom and inorganic sul?des in which the sulfur is at with the original preparation of these materials, plates prepared in accordance with Example l and Example 6 tached directly to a metal atom as an additional constituent in said photosensitive layer and ?xing the image compris ing said colored reaction product by exposing the surface after solvent elimination were stored in a dark cabinet with ready access of air for a period of 12 hours and of said sul?de-containing layer to a moist oxygen-cow after exposure to ultraviolet light, no noticeable image 40 raining gas, thereby stabilizing the brilliantly colored im was obtained. age against fading. I claim: 12. A method of developing stable brilliantly colored images which comprises preparing a composition consist< ing essentially of (ll a ?lm-forming plastic base material 1. A dry photographic ?lm producing a visible print out image by exposure to light of a suitable wave length and rendered insensitive to light by exposure to a moist oxygen-containing gas selected from the group consist selected from the group consisting of cellulose deriva tives and polymers of vinylidcne monomers. (2) at least one arylaminc. (3) at least one halogenated hydrocarbon compound having an energy of formation of the free least one arylamine; (2) at least one halogenated hydro halogen radical of not less than about 40 kilogram cal 50 carbon compound having an energy of formation of the ories per mol. selected from the group consisting of com free halogen radical of not less than about 40 kilogram pounds which produce free radicals upon exposure to light calories per mol, selected from the group consisting of of a suitable wave length and (4) at least one sulfur ing of oxygen and air, said ?lm consisting essentially of a ?lm-forming plastic having dispersed therein (1) at halogenated hydrocarbon compounds which produce free containing compound selected from the group consisting of organic sul?des in which the sulfur is attached directly and (3) at least one sulfur-containing compound selected 55 to a carbon atom and inorganic sul?des in which the sul from the group consisting of organic sulfides in which fur is attached directly to a metal atom; there being pres the sulfur is attached directly to a carbon atom and in ent in said ?lm between 0.l and 10 part of arylamine by organic sul?des in which the sulfur is attached directly weight, per part of ?lm-forming plastic. between 0.] and to a metal atom; there being present in said ?lm between 0.1 and 1.0 part of arylamine by weight. per part of ?lm 60 2.0 parts of halogenated hydrocarbon compound by weight. per part of ?lm—forming plastic and between 0.01 forming plastic. betweccn 0.] and 2.0 parts of halogenated and 0.3 part by weight of sulfur compound by weight. per hydrocarbon compound by weight. per part of ?lm-form part of ?lm-forming plastic: said composition being pre ing plastic and between 0.0l and 0.3 part by weight of pared in a solvent for the ?lm—forming plastic; depositing sul?de by weight. per part of ?lm-forming plastic. said radicals upon exposure to light of a suitable wave length; ?lm-forming plastic being selected from the group con 65 said composition on a support; evaporating said solvent. leaving a photosensitive ?lm wherein the arylamine. halo sisting of cellulose derivatives and polymers of vinylidenc genated hydrocarbon and sulfur-containing compounds monomers. are dispersed in said ?lm-forming plastic base material on 2. The lilm of claim I containing in addition an azo compound dispersed in said ?lm-forming plastic base ma< tcrial, to enhance the pholt'isensitivity of said ?lm to visible said support; exposing selected portions of the resulting 70 article to ultraviolet light; and thereafter ?xing the result ing brilliantly colored image by exposing the surface of light. said image bearing article to a moist oxygen-containing 3. The ?lm of claim 2 wherein the said azo compound is selected from the group consisting of azoanilines and axodiphcnylamincs, gas. 75 (References on following page) 3,042,510 12 11 References Cited in the file of this patent UNITED STATES PATENTS 1,574,357 1,587,272 1.587273 2,097,119 Beebe et al. Beebe et a1. Beebe et a1. Eggert et a1. __________ __ Feb. 23, __________ __ June 1, __________ __ June 1, __________ __ Oct. 26, 1926 1926 1926 1937 2.673.151 2,789.053 2905,556 Gcrhart ____________ -_ Mar. 23, 1954 Elliott ______________ __ Apr. 16, 1957 Fuchsman el al _______ __ Sept. 22, 1959 FOREIGN PATENTS 633,715 Germany ____________ __ July 16, 1936 UNITED STATES PATENT OFFICE CERTIFICATE OF CORRECTION Patent No. 3,042,516 July 3' 1962 Eugene Wainer It is hereby certified that error appears in the above numbered pat ent requiring correction and that the said Letters Patent should read as corrected below . Column 2 I inc 4 l ' line 6, for "comprsiing" read —— comprising -—; for "on" read —— of —-; meant ——; same column 2, line 23, line 55, for "means" read —" line 6'1'u strike out "the"; column 4, for "cl" read —— Cl —-; line 57, for "amnies" read — amines —~; column 8, line 58, for "grams", first occurrence, read —-- gram ~—; column lOI numeral "24" read —~— 1 line 19, for the claim reference —— Signed and sealed this 13th day of November 1962. (SEAL) Allest: EFNEST w. SWIDER DAVID L- LADD Aucsting Officer Commissioner of Patents


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The University of Central Florida women's soccer team, buoyed by a 1-0 upset at North Carolina State last weekend, jumped six spots to seventh place in the Intercollegiate Soccer Association of America poll, which was released Tuesday.
North Carolina (4-0) is No. 1.
UCF (2-0) opened the season in the Wolfpack Classic with a 1-0 victory over UNC-Greensboro before its victory over the Wolfpack, then ranked fifth.
N.C. State also was the last opponent in the top five that UCF had beaten. The Knights defeated the Wolfpack, 3-0, in the quarterfinals of the 1988 NCAA Tournament.
UCF will play its first home match Friday at 4 p.m. against Vanderbilt.


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The Pound Hill Medical Group will be asking a selection of our patients on a monthly basis if they would recommend the Practice to a Friend or Family Member and seeking positive and constructive feedback. If you would like to take part please follow this link:
August 2018
This month we had a return that 97% would definitely recommend or likely to recommend the Practice to a Friend of Family Member.
We would like to thank all of our patients for their patience while we have been implementing the Electronic Prescribing Service and would encourage any patient who has not yet singed up to speak to their pharmacist or the reception staff at the practice.
We are currently in the process of increasing the skills of our health care assistants here at the practice with the intention that the extra services they pick up will free up our practice nurses and therefore our
We would encourage any patient to sign up to our Online booking services where you can book appointments up to 4 weeks in advance with a GP of your choice.
Also we would like to remind all patients that we have an Acute Illness Clinic run by our trained Triage Nurses form 8:00AM to 12:00AM every morning who would call you back and be able to deal with any urgent medical issues on that day.


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from The American Heritage® Dictionary of the English Language, 4th Edition
- n. One who hangs something: a house painter who also works as a paperhanger.
- n. A contrivance to which something hangs or by which something is hung, as:
- n. A device around which a garment is draped for hanging from a hook or rod.
- n. A loop or strap by which something is hung.
- n. A bracket on the spring shackle of a motor vehicle, designed to hold it to the chassis.
- n. A decorative strip of cloth hung on a garment or wall.
- n. A short sword that may be hung from a belt.
from Wiktionary, Creative Commons Attribution/Share-Alike License
- n. One who hangs, or causes to be hanged; a hangman.
- n. That by which a thing is suspended. Especially:
- n. That which hangs or is suspended, as a sword worn at the side; especially, in the 18th century, a short, curved sword.
- n. A steep, wooded declivity.
from the GNU version of the Collaborative International Dictionary of English
- n. One who hangs, or causes to be hanged; a hangman.
- n. That by which a thing is suspended.
- n. A strap hung to the girdle, by which a dagger or sword is suspended.
- n. A part that suspends a journal box in which shafting runs. See Illust. of Countershaft.
- n. A bridle iron.
- n. That which hangs or is suspended, as a sword worn at the side; especially, in the 18th century, a short, curved sword.
- n. A steep, wooded declivity.
from The Century Dictionary and Cyclopedia
- n. One who hangs anything; one whose occupation is to hang something: as, a bell-hanger; a paper-hanger.
- n. One who hangs persons, or inflicts the penalty of hanging; a hangman.
- n. That which hangs or is suspended; specifically, a hanging or sloping wood or grove.
- n. A short cut-and-thrust sword, especially one worn by seamen and travelers.
- n. That from which something is hung or suspended.
- n. Specifically — A support for a line of shafting, consisting of a box for holding the shafting, an oiling device, etc., and supported by a bracket, by arms fixed to the ceiling, or on legs which rest on the floor. The term includes the whole apparatus, supports and all, whatever their shape.
- n. The lower part of the heddle of a loom.
- n. A chain or bent rod on which a pot or kettle is hung in the open fireplace of old-fashioned kitchens, by means of the pothook: hence used humorously in the phrase pothooks and hangers, the characters made by children in their first attempts to write.
- n. The arrangement of straps by which, in the sixteenth and seventeenth centuries, the rapier was hung from the belt: an appendage often made elaborate and ornamental.
- n. In tailoring, the loop or strap by which a coat or other garment is hung on a peg.
- n. In lace-making, one of those bobbins which lie straight down the cushion, as distinguished from the worker-bobbins, which are moved from side to side.
- n. The great seaweed, Laminaria digitata. The stem is woody, from 2 to 6 feet in length and from half an inch to nearly 2 inches in diameter. The frond is 6 or 8 feet in length and 2 feet broad, and olivaceous brown in color. When young the stems are sometimes eaten. It was once largely used in the manufacture of glass, supplying the alkali, but has now been superseded. It is also used for making handles for knives, for fuel, and for manure by the Highlanders. Also called tangle, sea-girdle, sea-staff, and sea-wand. See Laminaria.
- n. A vat in which skins are tanned by being suspended in the liquor.
- n. A long loop or looped rod which hangs from a transverse beam attached to a foundry crane, and which receives the trunnions of a molding-flask slung therefrom.
from WordNet 3.0 Copyright 2006 by Princeton University. All rights reserved.
- n. a worker who hangs something
- n. anything from which something can be hung
Sorry, no etymologies found.
Or if you want your name in B&C or P&Y record books, a wall hanger is a success.
How do you measure Success - something "In the Freezer" or "On the Wall"?
With the arm not inside the shirts, grab a hanger from the pile.
Speed Up Your Shirt-Hanging Routine With A Simple Trick | Lifehacker Australia
This silly hilarious coat hanger is simple and a little naughty, so Mr P entertains our office desks and accessorizes our homes in a unique, fun and memorable way!
The "Genius Lasts Longer than Beauty" clothes hanger is really cool: a statement mixed with something practical, a thing to reflect about on your way to work.
Do we all recall that Bush only made speech in "hanger's" telling the troops we are a Nation at War, and thank you so much for giving to your country.
& Design's "Frame hanger" is a huge, leaning cut-out of a silhouette of an artistic scene, intended to be used as a coat-hanger.
Does your opinion change with the sentence My striped hanger is unique?
Because as most women can tell you, men are rarely forthcoming about what they like in clothing, and the question, "What do you think of this shirt?" posed to a man while dangling it in front of him on a hanger is generally met with a blank stare.
As were the Hello Kitty shower curtain hanger things.
This pot-hanger is in the shape of the Chinese word for "luck," rendered in red steel.
Noun: The state or condition of being hangry. Pronounced with a hard g.
"8. A chain or bent rod on which a pot or kettle is hung in the open fireplace of old-fashioned kitchens, by means of the pothook: hence used humorously in the phrase pothooks and hangers, the characters made by children in their first attempts to write."
--Century Dictionary


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The Other Insect Societies. By James T. Costa. Harvard University Press, Cambridge, MA, 2006. 811 pp. $59.95, £38.95, €55.30. ISBN 0-674-02163-0.
The author reviews the social behavior and ecology of insects that fall outside the eusocial taxa (ants, wasps, bees, and termites).


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Asia's factual bosses track shift to local programming
The eighth edition of factual fest Asian Side of the Doc (ASD) wrapped in Bangkok at the end of January with a focus on the shift to local programming and lots of discussion around rising demand for digital content.
Delegates at the four-day event in the Thai capital also heard about what kinds of factual programming were working best in which markets in Asia.
Organisers counted 350 people through the door and said 35 countries were represented.
Pipope Panitchpakdi, deputy director of Thai PBS, talked about demand shifting from being "heavily westernised towards Eastwood", the right factual mix and the importance of building the culture of producers to prevent "documentary genre to become just another TV snack".
"It doesn't have to be only a feel-good kind of documentary that we welcome but things that make people think about; nature is always one of the high-viewed factual pieces, the development paradigm, mining activities," Panitchpakdi said.
Aileen Paredes, female specialty channels unit head for Philippines broadcaster ABS-CBN, pointed out how the dominant drama genre enhances the factual offering in the Philippines.
"By incorporating the elements of drama in presenting stories, it has proven to be more receptive to the Philippines audience," she said.
Paredes also talked about her greatest challenge – fulfilling production demand for a market expanding rapidly into digital/multiscreen. This has launched a hunt for factual content that can sit comfortably across multiple platforms.
A panel discussion on the rise of regional streaming services focused on what factual works best for which platform.
HOOQ's chief content officer, Jennifer Batty, noted a gap for factual entertainment on her line up, and said her audiences wanted easy viewing. "You can't just be movies and series," she added.
At the same time, "people are not coming to us for historical documentary, they are going to look for the History channel or their public broadcaster, so for us it's going to be a little bit more about light-hearted viewing, a bit more entertainment viewing, and when they walk away they're going to feel that they learned something. So, it's going to be factual that is a little bit light-hearted," Batty said.
Joe Suteestarpon, CEO of Thai's Mediaplex International agreed that factual was a critical part of a streaming/on-demand offering.
Mediaplex's OTT DOONEE offers more than 10,000 hours of content, including 800-1,000 hours of factual.
Artine S. Utomo, president director of Indonesia's four-year old private station, RTV (Rajawali Televisi Indonesia), highlighted demand for factual programming that was both entertaining and educational.
"We need documentaries delivered in such a way that is inspiring... and creates a change in the mindset of the mass audience to boost their way of life," Utomo said.
Relatability was also key, said Shamala Rajendran, commissioning editor for Mediacorp Singapore.
"There are many filmmakers, docu producers who have great stories but some of them tend to be too insular, or too specific to a place or situation. And our audience can't relate to them," said Rajendran.
Aegena Tay, director, programming development for regional distributor, Bomanbridge Media, said the range of factual programme demand in Asia was broad, and, in some markets, dictated to by content codes and regulations. Some services, for instance, preferred "happy, warm, friendly animal content" rather than predatory or "too much animal violence," she said.
TV Burabha, Thailand's international marketing content director, Nattanan Kulrapeekorn, said her priority for culture and wildlife content was timeless relevance.
"What we're doing is going to be relevant until the end of time because culture and wildlife projects stay forever. What is on the ticking clock are series on festivals that could last maybe 4 to 5 years," she said, adding: "Factual content can be watched a hundred years from now because the truth is the truth and it can be told a hundred times in different ways for any market."


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as the most popular and one of the most popular shoes, NIKE has published numerous various styles of Nike Dunk High Deluxe Edition, not only for the NIKE basketball shoes series a hehe exploits, even in line skate shoes also caused great repercussions. Now, the NBA battle shoes king is honored for you -- the latest Nike Dunk High NIKE.
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text: On May 12, 2004, RUTH M. JENKINS, beloved wife of the late George C. Jenkins, Sr.; devoted mother of George C. Jenkins, Jr., John E. Jenkins, Richard P. Jenkins, and Sharon Czajkowski; cherished grandmother of Rhonda & Richie Jenkins and numerous other grandchildren & great-grandchildren. Friends may call at the family owned Evans Chapel of Memories - Parkville Thursday 3 to 5 and 7 to 9 PM. A Funeral Service will be held 10AM Friday. Interment Moreland Memorial Park.


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Patients receiving cytotoxic drugs are at an increased risk of bacterial infection. Drug-induced leukopenia may be responsible for depression of host defenses; however, there is little information concerning the qualitative effects, if any, of cytotoxic agents on granulocyte antibacterial activity. Since methotrexate is now being used in massive doses in vivo, we investigated the effects of this drug on antibacterial and metabolic functions of normal polymorphonuclear leukocytes in vitro.
Phagocytosis, quantitative protein iodination, and staphylococcal killing of normal polymorphonuclear leukocytes were found to decrease with exposure to increasing concentrations of methotrexate. The effects of methotrexate on these cell functions were rapid in onset and readily reversed by washing the cells, suggesting a locus of action on the cell membrane rather than at the level of nucleic acid synthesis. Exposure of cells to similar concentrations of folic acid or folinic acid produced no impairment of bacterial phagocytosis, suggesting that the observed effects are specific for methotrexate. The concentrations of methotrexate that produced these impairments are readily achieved in vivo and may alter antibacterial defenses in patients receiving this therapy.
↵1 This work was supported by USPHS Grants R01 AI 10600, 2 R10 CA 11796, 5 T12 CA 08147, 1 PO 2 CA 14489, and R01 AI 13251; a considerable portion of the work was performed in the Department of Medicine, University of Pennsylvania.
↵3 Recipient of Research Career Development Award 5 K4 AI 70052 while at the University of Pennsylvania. To whom requests for reprints should be addressed, at Infectious Disease Section - 208 LCI, Yale University School of Medicine, 333 Cedar Street, New Haven, Conn. 06510.
- Received June 13, 1977.
- Accepted December 2, 1977.
- ©1978 American Association for Cancer Research.


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After the death of his father, T'Challa returns home to the African nation of Wakanda to take his rightful place as king. When a powerful enemy suddenly reappears, T'Challa's mettle as king -- and as Black Panther -- gets tested when he's drawn into a conflict that puts the fate of Wakanda and the entire world at risk. Faced with treachery and danger, the young king must rally his allies and release the full power of Black Panther to defeat his foes and secure the safety of his people. Read More


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BETH Tweddle and the GB women's gymnastics team are hoping to emulate the achievements of their male counterparts this afternoon.
Britain's men won bronze in yesterday's team final. It was Britain's first Olympic team medal in gymnastics for 100 years.
Today it is the turn of Tweddle, 27, of Bunbury, and her colleagues in the women's team to go for glory.
The action begins at 4.30pm in the North Greenwich Arena.
A busy morning at Eton Dorney saw three local rowers make finals.
Chris Bartley, of Farndon, was part of the men's lightweight four which won through to Thursday's final where they will be challenging for a gold medal.
In the repechage, the GB women's eight – containing Vicky Thornley and Olivia Whitlam – finished fourth, which was enough to book a place in the medal shoot-out on Thursday.
Last night saw the GB women's water polo team – including Chester's Fiona McCann – make their Olympic debut.
McCann, 25, scored in a 7-6 loss to three-time European champions Russia.
Pulford's James Fair played in the GB hockey team's 4-1 success over Argentina last night while Jo Leedham was the joint top-scorer for the women's basketball team in their 73-65 loss to Canada.


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1 definition found From The Free On-line Dictionary of Computing (13 Mar 01) [foldoc]: COMIT The first string-handling and {pattern-matching} language, designed in 1957-8 for applications in {natural language} translation. The user has a workspace organised into shelves. Strings are made of constituents (words), accessed by {subscript}. A program is a set of rules each of which has a pattern, a replacement and goto another rule ["COMIT Programmer's Reference Manual", V.H. Yngve MIT Press 1961]. [Sammet 1969, pp 416-436]. (1994-11-30)