WO2012038453A1 - Substance pour produire un marquage d'un objet ou d'un individu - Google Patents

Substance pour produire un marquage d'un objet ou d'un individu Download PDF

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Publication number
WO2012038453A1
WO2012038453A1 PCT/EP2011/066375 EP2011066375W WO2012038453A1 WO 2012038453 A1 WO2012038453 A1 WO 2012038453A1 EP 2011066375 W EP2011066375 W EP 2011066375W WO 2012038453 A1 WO2012038453 A1 WO 2012038453A1
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opening
nucleic acid
carbon nanotubes
substance
substance according
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PCT/EP2011/066375
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German (de)
English (en)
Inventor
Philipp CACHÉE
Christian PRÜFER
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Actc-Anti Crime Technology Corporation Gmbh
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Publication of WO2012038453A1 publication Critical patent/WO2012038453A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12Q—MEASURING OR TESTING PROCESSES INVOLVING ENZYMES, NUCLEIC ACIDS OR MICROORGANISMS; COMPOSITIONS OR TEST PAPERS THEREFOR; PROCESSES OF PREPARING SUCH COMPOSITIONS; CONDITION-RESPONSIVE CONTROL IN MICROBIOLOGICAL OR ENZYMOLOGICAL PROCESSES
    • C12Q1/00—Measuring or testing processes involving enzymes, nucleic acids or microorganisms; Compositions therefor; Processes of preparing such compositions
    • C12Q1/68—Measuring or testing processes involving enzymes, nucleic acids or microorganisms; Compositions therefor; Processes of preparing such compositions involving nucleic acids
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12Q—MEASURING OR TESTING PROCESSES INVOLVING ENZYMES, NUCLEIC ACIDS OR MICROORGANISMS; COMPOSITIONS OR TEST PAPERS THEREFOR; PROCESSES OF PREPARING SUCH COMPOSITIONS; CONDITION-RESPONSIVE CONTROL IN MICROBIOLOGICAL OR ENZYMOLOGICAL PROCESSES
    • C12Q1/00—Measuring or testing processes involving enzymes, nucleic acids or microorganisms; Compositions therefor; Processes of preparing such compositions
    • C12Q1/68—Measuring or testing processes involving enzymes, nucleic acids or microorganisms; Compositions therefor; Processes of preparing such compositions involving nucleic acids
    • C12Q1/6806—Preparing nucleic acids for analysis, e.g. for polymerase chain reaction [PCR] assay

Definitions

  • the present invention relates to a substance for producing a marking of an article or an individual according to the preamble of claim 1, the use of a corresponding substance according to the preambles of claims 11 or 12, a process for producing such a substance according to the preamble of claim 13 and a method for determining the identity or origin of an object or individual labeled with such a substance according to the preamble of claim 14.
  • EP 0 408 424 B1 discloses a hidden security marking method for protecting valuables in which an object chemical to be marked is applied with a target chemical compound capable of being detected later by a suitable detection means.
  • DE 197 38 816 A 1 relates to a method and a substance for labeling solid, liquid or gaseous substances, wherein the substance to be labeled is provided with a predetermined specifically designed nucleic acid sequence.
  • an ink which contains a nucleotide polymer and a release agent.
  • the release agent is used in an amount of 10 to 40 percent by mass.
  • US 5,763,176 A a method for marking an article is known, are used in the beads that carry nucleic acids. For each bead different nucleic acids can be used.
  • US 2010/0050901 A1 describes a marking consisting of several substances of different classes.
  • the use of DNA-coated carbon nanotubes is also provided.
  • Gao et al. "Spontaneous Insertion of DNA Oligonucleotides Into Carbon Nanotubes," Nano Letters 3 (2003), pages 471-473, describe computer simulations for incorporation of DNA into carbon nanotubes, but the problem of long-term retention of DNA in the carbon nanotubes does not arise
  • the invention is based on the object of further improving the possibilities of nucleic acid marking known from the prior art with regard to durability and manipulation resistance.
  • nucleic acid is meant in particular a single- or double-stranded ribonucleic acid (RNA) or deoxyribonucleic acid (DNA).
  • RNA ribonucleic acid
  • DNA deoxyribonucleic acid
  • the individual bases from which the corresponding nucleic acid is constructed may be modified or unmodified.
  • the substance preferably has exactly one single nucleic acid (that is to say a single type of nucleic acid having a specific sequence), a multiplicity of molecules of this nucleic acid being contained in the substance.
  • the carbon nanotubes have a first opening and a second opening facing the first opening in the longitudinal direction of the carbon nanotubes.
  • the carbon nanotubes thus consist - as is generally known to those skilled in the art - initially of a double-sided open carbon skeleton, which is a tube or tube-like Molecule forms.
  • the carbon nanotubes may be single-walled, double-walled or multi-walled.
  • the invention is characterized in that the individual nucleic acid molecules are completely accommodated in the carbon nanotubes and at least one of the two openings of the carbon nanotubes is closed by a closure.
  • This closure can be present in one of the two openings even before introducing the nucleic acid into the carbon nanotubes, so that in this case the nucleic acid is introduced into a single-sided closed carbon nanotube.
  • the nucleic acid molecules contained in the carbon nanotube are protected in a particularly advantageous manner from external influences. It has been found that it is not absolutely necessary to close both openings of the carbon nanotubes. Rather, the closing of a single opening is already sufficient to minimize or prevent an interaction of external substances with the nucleic acid molecules enclosed in the carbon nanotubes. However, even more effective encapsulation of the nucleic acid molecules contained in the carbon nanotubes from the environment can be achieved by closing both openings of the carbon nanotubes with a corresponding closure. Only when the corresponding closure is removed again can the nucleic acid molecules be used for further chemical analysis thereof. However, as long as the closure is at its intended location (ie in the region of the previously accessible opening of the carbon nanotubes), the nucleic acid molecules are stably and advantageously encapsulated from the environment.
  • the carbon nanotubes have both a width and a length of a few nanometers, wherein the extension in the longitudinal direction is preferably greater than that in the width direction.
  • the size of the carbon nanotubes is preferably adapted to the size of the nucleic acid to be introduced.
  • the nucleic acid has a length of from 20 to 200 bases, in particular from 30 to 180 bases, in particular from 40 to 160 bases, in particular from 50 to 150 bases.
  • Suitable upper limits for the length of the nucleic acid are also 70, 80, 90, 100, 110, 120, 130 or 140 bases.
  • a particularly suitable length comprises 54 up to 66 bases. If a double-stranded nucleic acid is used, the abovementioned lengths apply analogously to base pairs.
  • the closure of the first opening and / or the second opening of the carbon nanotubes are carbon atoms or carbon molecules that have been added to the carbon nanotubes so that they are attached to them or inserted into the openings.
  • the same closure type for the first opening and the second opening or different closure types for the two openings can be provided.
  • Suitable carbon molecules for forming a cap are fullerenes.
  • these spherical carbon constructions may be inserted into the openings of the carbon nanotubes as a kind of plug and thereby occlude the corresponding openings.
  • the fullerenes used are dimensioned so that a single fullerene molecule has a diameter which is adapted to the diameter of the opening of the carbon nanotube to be closed. As a result, a single fullerene molecule is sufficient to close a corresponding opening of the carbon nanotube.
  • the closure of the first opening and / or the second opening of the carbon nanotube is a sheathing of the carbon nanotubes.
  • This sheath can be configured, for example, with silicon or a silicon compound.
  • the openings of the carbon nanotubes are covered, so that also no unwanted access to the nucleic acid within the carbon nanotubes is possible.
  • the sheath can partially or completely surround the individual carbon nanotube. For example, it is possible to place a single, closed shell around the carbon nanotubes to equally close both openings of the carbon nanotubes. It is also possible to use a sheath designed as an end cap, which extends over an opening of the carbon nanotubes.
  • the carbon nanotubes and / or the closure are provided with a functional group.
  • Suitable functional groups are amines, carboxylic acids, carboxylic esters, alcohols, carboxylic acid amides, ketones and other organic compounds, but also inorganic molecules such as metal ions are conceivable.
  • the carbon nanotubes By means of functional groups on the carbon nanotubes it is possible to modify the reactivity of the two longitudinally opposite ends (openings) of the carbon nanotubes. In this way, it is possible to purposefully close only a single end of the carbon nanotubes with a closure, while the other end remains open.
  • the functional groups can also serve to facilitate reopening of the carbon nanotubes or to facilitate or enable detection of the carbon nanotubes.
  • the carbon nanotubes provided with the enclosed nucleic acid are designed in such a way that their surface is free of nucleic acid, that is, there are no nucleic acid-coated carbon nanotubes, but only carbon nanotubes, in the interior of which a nucleic acid is contained. Because nucleic acid molecules that are located on the surface of the carbon nanotubes are not protected by the carbon nanotubes themselves, but rather external environmental influences such as solutions with a high or a low pH, nucleic acid degrading enzymes such as nucleases or UV radiation such as sunlight or exposed to artificial UV radiation as generated by disinfection devices. against these environmental influences, the nucleic acids contained in the carbon nanotubes are protected.
  • nucleases or other nucleic acid-degrading enzymes makes it possible to free carbon nanotubes, on whose surface nucleic acid molecules should still adhere, from these nucleic acid molecules without damaging the DNA contained inside the carbon nanotubes; the nucleases provide for a corresponding nucleic acid degradation.
  • the substance has at least one quantified additive.
  • quantified is to be understood as meaning that the amount in which the additive is contained in the substance is known precisely, which means that the subsequent identification of an object by analysis of the corresponding substance makes it possible not only for coding information, those in the nucleic acid but also resort to secondary coding information resulting from the amount of additive.
  • the additive is a UV protecting agent, an antioxidant, a dye, a metal flake less than 1 mm in size, a polymer, or a pheromone.
  • the size of the metal platelets is to be understood as the greatest length expansion in one direction.
  • the metal platelets have a size of less than 500 ⁇ m, in particular of less than 400 ⁇ m, in particular of less than 300 ⁇ m and very particularly of less than 200 ⁇ m.
  • metal flakes having a size of about 200 ⁇ m to 500 ⁇ m are used.
  • the metal platelets are provided with an identification feature.
  • an identification feature may be, for example, a hologram, an alphanumeric code or a number. This identifier may be printed on the metal platelets or lasered or stamped into them.
  • the substance contains more than one additive, wherein the ratio of the individual additives to one another is precisely determined. This later enables a more accurate identification of a substance provided with the substance, if the ratio of the additives to each other in addition to the DNA coding information for identification is used.
  • the present invention also relates to the use of a substance according to the preceding explanations for determining the identity or origin of a substance or an individual labeled with the substance.
  • the substance can be used for example as a court-usable marker substance.
  • the invention further relates to the use of a substance according to the preceding explanations for medical or biochemical purposes.
  • the use of the substance in the context of gene therapy or for the (genetic) transformation of an organism or a cell (such as a bacterium or a plant cell) is provided.
  • the encapsulation in the carbon nanotubes can significantly increase the efficiency of nucleic acid transfer into an organism or cell, requiring fewer nucleic acid molecules for successful transformation.
  • nucleic acid contained in the carbon nanotubes into an organism or a cell, it is useful if the carbon nanotubes are opened after reaching their destination to allow exit of the nucleic acid contained them.
  • the nucleic acid can then be incorporated into the genome of the target organism or cell spontaneously or in other ways well known to those skilled in the art.
  • the nucleic acid introduced in this way can also interact (in particular with interference) with nucleic acid molecules present in the target organism or in the target cell in order, for example, to act on transcription or translation within the target organism or target cell.
  • the invention further relates to a method for producing a substance according to the previous explanations, which comprises the steps explained below.
  • a method for producing a substance which comprises the steps explained below.
  • carbon nanotubes and a variety of nucleic acid molecules of one type are provided in aqueous solution.
  • Each carbon nanotube has at least one first opening.
  • the aqueous solution is heated to at least 75 ° C.
  • the pressure acting on the solution is increased to at least 2 bar. Under these conditions, it is possible to introduce the nucleic acid into the carbon nanotubes.
  • the carbon nanotubes are preferably dimensioned such that exactly one single nucleic acid molecule fits into a carbon nanotube.
  • the carbon nanotubes may be sized larger to allow for easier introduction of the nucleic acid molecules into the carbon nanotubes or to allow the introduction of a plurality of nucleic acid molecules into a single carbon nanotube.
  • the first opening of the carbon nanotubes is closed. If a second or further opening is present, which preferably lies opposite the first opening in the longitudinal direction of the carbon nanotubes, these can also be closed. Alternatively, it is possible to leave the second or further opening open and to close only the first opening.
  • the aqueous solution is heated to at least 100.degree. C., in particular at least 110.degree. C., in particular at least 120.degree. C., in particular at least 130.degree. C., in particular at least 140.degree. C. and very particularly at least 150.degree.
  • the pressure for introducing the nucleic acid into the carbon nanotubes is preferably increased to at least 2.5 bar, in particular at least 3 bar, in particular at least 3.5 bar, in particular at least 4 bar, in particular at least 4.5 bar and especially at least 5 bar , Without one corresponding pressure increase, the pressure acting on the aqueous solution would correspond to the usual ambient pressure and be around 1 bar.
  • the selection of pressure and temperature is preferably made such that the aqueous solution does not begin to boil, but remains in the liquid state of matter.
  • the invention also provides a method for determining the identity or origin of an object or individual labeled with a substance according to one of the above explanations, which comprises the steps explained below.
  • the substance is isolated from the object or individual, wherein in the substance - in accordance with the above explanations - are contained carbon nanotubes whose first opening and / or second opening is closed with a closure and which contain a nucleic acid in its interior.
  • the shutter is opened. If both previously existing openings or ends of the carbon nanotubes are closed, either a single closure or both closures can be removed. If there is only a single closure, the step of opening the closure may be skipped or the single closure removed.
  • the nucleic acid is extracted from the carbon nanotubes.
  • techniques which are generally known to the person skilled in the art can be used.
  • the extracted nucleic acid is identified. Such an identification can be carried out for example by means of a sequencing of the nucleic acid. Before sequencing, it is possible to amplify the extracted nucleic acid. A suitable amplification technique is the polymerase chain reaction (PCR). This facilitates subsequent sequencing.
  • PCR polymerase chain reaction
  • the identified nucleic acid is compared with data, which are preferably stored in a database.
  • data which are preferably stored in a database.
  • the database stores those persons, organizations or locations to whom a specific nucleic acid has been made available or to which a specific nucleic acid has been used.
  • the concentration of this additive with data stored in the database can also be calibrated in the context of determining origin or identity, in order to achieve even more accurate assignment of the data to allow the substance labeled items or individuals.
  • Another aspect of the present invention is a combination of nucleic acid tagging (especially DNA coding) and quantifiable features of various natures in a marker substance in order to obtain the highest level of security with the claim of the court usability.
  • the substance is particularly advantageous usable as a court-proof substantive proof.
  • Evidence of the facts is material evidence of evidence of a crime or perpetration for the law enforcement authorities (police, prosecutors) and the competent court.
  • a substance for producing a court-usable marker comprising dissolved synthetically produced DNA and quantified additives such as protective agents and / or dyes and / or metal platelets ⁇ 1 mm in size and / or other additives such as quantified Mixtures / compounds of organic and / or inorganic substances (polymers or eg pheromones).
  • additives such as protective agents and / or dyes and / or metal platelets ⁇ 1 mm in size
  • additives such as quantified Mixtures / compounds of organic and / or inorganic substances (polymers or eg pheromones).
  • an embodiment of the marker substance as a gel or powder would be conceivable.
  • synthetic DNA is, according to current knowledge, only about 15 years stable. DNA can also be destroyed by other environmental factors, eg when exposed to acids.
  • the exactly quantified mixing of the additives thus results in a second coding (secondary coding) of the owner data, which can still be evaluated even after a long time.
  • this secondary coding can not be analyzed without knowledge of the preparation, or can only be analyzed with considerable effort, and thus manipulated. Marked objects, persons or crime scenes can thus be assigned to the owner, the act, the crime scene, etc., in a manner usable by the court, on the basis of the DNA coding contained in the marker substance according to the invention or at least via the secondary coding by the quantified additives.
  • the rightful owner can then prove ownership of the mark used in a database assigned to the rightful owner.
  • an offender may be assigned to a crime scene when used as a robbery trap / spray system, or an article, e.g. a bike or a laptop, the owner.
  • the substance according to the invention or the (primary and / or secondary) coding contained therein can thus be read on the one hand by a court-approved and publicly appointed expert or a crime lab.
  • a fraudulence, manipulation or emulation by fraudsters with reasonable certainty excluded as long as the recipe of the substance according to the invention or the assignment of owners to the unique recipe and DNA is kept secret.
  • DNA consists of four nucleobases linked to a chain.
  • a nucleon base chain with 60 nucleotides (A, C, G, T) provides a kind of fingerprint with 60 4 possibilities.
  • a liquid is used as described above, wherein the DNA contains 20 to 160 nucleotides, for example 20 to 100 nucleotides, preferably 40 to 80 nucleotides and in particular 54 to 66 nucleotides, in particular ca.
  • This high information capacity allows, for example, the storage of suitable owner data in coded form and thus an unambiguous assignment.
  • the owner data may take the form of a serial number assigned to the owner, stored in the selected ACGT encoding.
  • DNA is a relatively robust organic substance and therefore stable over long periods of time.
  • organic substances including DNA
  • DNA are subject to degradation under UV action.
  • the influence of this harmful radiation can be counteracted by adding a UV protective agent as additive to the substance.
  • DNA can also be destroyed and damaged by other environmental influences, such as, for example, an acid attack, which can be prevented or at least reduced by the addition of corresponding other protective agents for the DNA.
  • Suitable UV protectants are UV absorbers or antioxidants, which are disclosed, for example, in “Textile Chemicals: Environmental Data and Facts", Springer Verlag 2004, p. 357 et seq. Or in Römpp Lexikon "Paints and Printing Inks", Thieme Verlag 1997.
  • these agents preferably those combinations of which a synergistic effect is known, are blended and added.
  • the combination with UV absorbers and antioxidants increases the longevity of the DNA and thus the particularly highly encrypted, but also meaningful DNA coding.
  • the amount of the UV protection agents added is exactly quantified, one can also obtain a second coding (secondary coding) of the owner data alone, which can still be evaluated even after a long time.
  • a protective agent for the DNA not only against UV irradiation, but under certain circumstances also against other harmful influences, e.g. By an acid attack, carbon tubes (nanotubes) can be provided, in which the DNA is housed or closed to the environment.
  • dyes may be added to the substance.
  • Dyes in the context of the present invention are understood as meaning pigments and soluble dyes. Suitable dyes have proven to be those which fluoresce in the visible / non-visible light spectrum (for example: UV, IR range).
  • the dye in the case of a marker substance in the form of a liquid, the dye may be added in concrete dimension to the total dry matter.
  • the compound (s) added may be selected from an organic or inorganic pigment, a dye which is soluble in water or organic liquid, a reactive dye, a fluorescent dye or quantified mixtures thereof. Again, a quantifiable mixture of dyes can be used.
  • UV absorbers and / or antioxidants in addition to the protection of the DNA has the advantage that in the case of organic dyes whose integrity is maintained longer. Even in the case of the use of inorganic dyes, in particular pigments, usually gives a higher resistance to UV and light radiation.
  • metal flakes for example nickel
  • the metal platelets can also carry a punched-out number.
  • number carrier plates made of a different material, such as plastic can be used. This makes it easier for the authorities to allocate the item in the first attack become.
  • further alphanumeric markings or other pictorial representations may be applied.
  • different types of metal plates can be used. The mixture is quantified individually.
  • the metal plate may consist of an alloy produced in a quantified mixing ratio or other materials / mixtures.
  • quantified mixtures / compounds of organic and / or inorganic substances may also be added in order to still have a court-proof mark in the event of complete destruction of the DNA by chemical, biological or mechanical action.
  • odorous substances for example pheromones
  • an animal detection for example, by a domestic dog or electronic measurement method is also possible.
  • radioactive materials instead of or in addition to the admixture of the above-described quantified mixtures / compounds of organic and / or inorganic substances, it is also possible to add radioactive materials in order to be able to determine the age of a particular label based on the natural decay.
  • nanotubes it would also be conceivable to include instead of or in addition to individual DNA and an extract of the substance in the individual nanotubes, which reproduces the mixing ratio of the individual ingredients of the substance in the quantified ratio and thus to protect the secondary coding against environmental influences ,
  • a defined synthetic DNA of about 60 nucleotides is used.
  • the concrete sequence allows an unambiguous assignment of the marked object. 2.
  • the use of several different such DNA sequences, used in individually quantified Nukleinbasenstrangnic also increases security.
  • a combination of UV absorbers and / or antioxidants in a precisely quantified manner on the one hand forms a further safety factor with dimensioning that is unknown to the unauthorized person and, on the other hand, protects the DNA material used from UV radiation.
  • hologram platelets possibly with an alloy composition of the carrier plate, which has a quantified ratio, allows a rapid allocation of the object and provides a high hurdle, so that a manipulation of the marker is possible only under extremely complex measures.
  • a substance, in particular liquid for producing a court-usable marking on an object / person comprising dissolved or contained synthetically produced DNA and quantified additives, such as quantified protective agents and / or dyes and / or optionally metal platelets with a size x ⁇ 1 mm and / or other additives, such as quantified mixtures or compounds of organic and / or inorganic substances, e.g. Polymers, pheromones, isotopes.
  • additives such as quantified protective agents and / or dyes and / or optionally metal platelets with a size x ⁇ 1 mm and / or other additives, such as quantified mixtures or compounds of organic and / or inorganic substances, e.g. Polymers, pheromones, isotopes.
  • the DNA comprises 20 to 160 nucleotide bases.
  • the protective agent comprises a UV protection agent in concrete dimensioning to the total dry mass quantified amount comprises.
  • the protective agent comprises a UV protection agent, in particular a UV absorber and / or an antioxidant, wherein in the presence of both UV absorbers and antioxidants they are present in a precisely measured ratio.
  • the protective means comprises carbon tubes (nanotubes), in which the DNA or extracts from the substance housed and / or closed to the environment.
  • the substance comprises dyes in quantified amount, in particular one or more dyes, which fluoresce in the visible and / or non-visible light spectrum.
  • the dye is in concrete dimensioning to the total dry matter selected from an organic or inorganic pigment, a dye which is soluble in water or organic liquid, a reactive dye, a fluorescent dye or quantified mixtures.
  • the metal platelets ⁇ 500 ⁇ , in particular 500 ⁇ to 200 ⁇ large, and, if present in different sizes, in quantified amount, wherein the metal platelets in particular a hologram and / or a number printed / lasered / punched out, and wherein the metal is in particular an alloy with a quantified composition.
  • the substance is produced from a water-based or alcohol-based liquid or from an adhesive, wherein in the case of an adhesive, in particular a reactive diluent is used.
  • the substance is processed as a gel, a wax, a powder, a gas or a liquid solution for spraying / atomizing.
  • nonradioactive and / or radioactive isotopes and / or mixtures thereof are added as additives.

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  • Chemical Kinetics & Catalysis (AREA)
  • Measuring Or Testing Involving Enzymes Or Micro-Organisms (AREA)

Abstract

La présente invention concerne une substance pour produire un marquage d'un objet ou d'un individu, comprenant un acide nucléique et des nanotubes de carbone, chaque nanotube de carbone présentant une première ouverture et une deuxième ouverture opposée à la première ouverture dans la direction longitudinale du nanotube de carbone. Selon l'invention, l'acide nucléique est complètement logé dans les nanotubes de carbone et la première et/ou la deuxième ouverture des nanotubes de carbone individuels est/sont fermées par une fermeture. L'invention concerne également un procédé pour produire une telle substance et un procédé pour déterminer l'identité ou l'origine d'un objet ou d'un individu marqué avec une telle substance.
PCT/EP2011/066375 2010-09-22 2011-09-21 Substance pour produire un marquage d'un objet ou d'un individu WO2012038453A1 (fr)

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DE102010046047.8 2010-09-22
DE102010046047A DE102010046047A1 (de) 2010-09-22 2010-09-22 Substanz zur gerichtsverwertbaren Markierung

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DE102011011437A1 (de) 2011-02-16 2012-08-16 Philipp Cachée Vorrichtung und Verfahren zur Sicherung von Flüssigkraftstoff gegen Diebstahl
GB2530711B (en) * 2014-08-04 2021-05-26 Themis Risk Holdings Ltd Security composition and use thereof

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US5643728A (en) 1992-08-26 1997-07-01 Slater; James Howard Method of marking a liquid
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EP0408424B1 (fr) 1989-07-07 1994-05-04 Bioprobe Systems Procédé et dispositif de marquage crypté de haute securité pour la protection d'objets de valeur
US5643728A (en) 1992-08-26 1997-07-01 Slater; James Howard Method of marking a liquid
US5763176A (en) 1993-07-12 1998-06-09 Slater; James Howard Methods and devices for marking a solid and subsequently detecting the markings
DE19738816A1 (de) 1997-09-05 1999-03-11 November Ag Molekulare Medizin Verfahren zur Markierung von festen, flüssigen oder gasförmigen Substanzen
JP2004175924A (ja) 2002-11-27 2004-06-24 Toppan Forms Co Ltd ヌクレオチド重合体を含有する剥離性インキ
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WO2009046110A1 (fr) * 2007-10-01 2009-04-09 University Of Southern California Détection d'adn méthylé et de mutations d'adn
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