CN111326059B - Encryption and anti-counterfeiting method based on fluorescence or phosphorescence stimulation response - Google Patents
Encryption and anti-counterfeiting method based on fluorescence or phosphorescence stimulation response Download PDFInfo
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- CN111326059B CN111326059B CN202010109433.6A CN202010109433A CN111326059B CN 111326059 B CN111326059 B CN 111326059B CN 202010109433 A CN202010109433 A CN 202010109433A CN 111326059 B CN111326059 B CN 111326059B
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- G—PHYSICS
- G09—EDUCATION; CRYPTOGRAPHY; DISPLAY; ADVERTISING; SEALS
- G09F—DISPLAYING; ADVERTISING; SIGNS; LABELS OR NAME-PLATES; SEALS
- G09F3/00—Labels, tag tickets, or similar identification or indication means; Seals; Postage or like stamps
- G09F3/02—Forms or constructions
- G09F3/0291—Labels or tickets undergoing a change under particular conditions, e.g. heat, radiation, passage of time
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
- C09D11/00—Inks
- C09D11/50—Sympathetic, colour changing or similar inks
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- G—PHYSICS
- G09—EDUCATION; CRYPTOGRAPHY; DISPLAY; ADVERTISING; SEALS
- G09F—DISPLAYING; ADVERTISING; SIGNS; LABELS OR NAME-PLATES; SEALS
- G09F3/00—Labels, tag tickets, or similar identification or indication means; Seals; Postage or like stamps
- G09F3/02—Forms or constructions
- G09F2003/0208—Indicia
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Abstract
The invention belongs to the technical field of encryption and anti-counterfeiting, and particularly relates to an encryption and anti-counterfeiting method based on fluorescence or phosphorescence stimulation response. The method comprises the following steps: selecting a fluorescent anti-counterfeiting material by a combined chemical strategy; preparing a fluorescent anti-counterfeiting pattern; preparing a reading device of the fluorescent anti-counterfeiting pattern; and reading the encrypted information in the fluorescent anti-counterfeiting pattern. The invention prepares the fluorescent/phosphorescent luminescent material with stimulus response and the host material into the printable luminescent ink by the arrangement and combination mode; by using the characteristics that the luminescent material and the matrix material have thousands of combinations, and each combination has a uniquely determined nonlinear response behavior to a given concentration of stimulus, a high degree of safety is provided even in the case where the core fluorescent substance is broken. The invention solves the problem that the traditional encryption anti-counterfeiting technology depends heavily on the core luminescent material and is easy to forge and crack, and has important application in the anti-counterfeiting field with high security level.
Description
Technical Field
The invention belongs to the technical field of encryption and anti-counterfeiting, and particularly relates to an encryption and anti-counterfeiting method based on fluorescence or phosphorescence stimulation response.
Background
The information encryption and anti-counterfeiting technology is widely applied to various fields such as economy, military, daily life and the like. However, with the large-area flooding of counterfeit and shoddy products worldwide, governments and copyright owners of various countries are constantly increasing investments in information encryption and anti-counterfeiting technologies. In 2017, the market scale of the global anti-counterfeiting technology is 518 hundred million dollars, and the annual average composite growth rate is expected to be 11.7 percent from 2018 to 2025 (percent)Adv. Mater.2019, 1901430). The encryption technology based on the fluorescent material has the characteristics of simple use, convenient operation, low cost and quick and visual detection, and is widely applied to the fields of financial vouchers such as bank notes, stamps and commercial bills, and high-grade printed matter anti-counterfeiting marks such as cigarette and wine packages, medical packages and the like. The earliest fluorescent anti-counterfeiting technology printed the traditional single-color fluorescent material on a substrate material, and the encrypted information could be read by naked eyes under the irradiation of an ultraviolet lamp to distinguish the authenticity. But because a large number of fluorescent materials with similar characteristics exist in the marketTherefore, a counterfeiter can easily find a substitute completely matched with the characteristics of the traditional fluorescent material, so that the encryption anti-counterfeiting technology is easy to crack and counterfeit, the security level is low, and the security is difficult to ensure. With the development of material science, a novel multi-mode luminescent material with luminescent characteristics of multiple excitation wavelengths, multiple emission wavelengths, long afterglow and the like is synthesized and applied to the second-generation fluorescent anti-counterfeiting technology, so that the encryption security is improved. These new multimodal luminescent materials include up-conversion nanomaterials, carbon quantum dots, perovskite nanocrystals, etc. ((Adv. Mater.2019, 1901430.ACS Cent.Sci.2019, 5, 29-42). Recently, fluorescent substances based on external stimuli response such as light, heat, magnetism, etc. have been synthesized and used in the fields of encryption and anti-counterfeiting (ii)Adv. Mater.2018, 1800783. Adv. Funct. Mater.2019, 1906068.Chem. Soc. Rev.2015, 441585.) the prepared material can only display correct encryption information under the condition of external stimulation, thus greatly improving the security level of encryption and anti-counterfeiting technologies and becoming the typical characteristic of the third generation of fluorescent anti-counterfeiting technologies. However, even in the third generation fluorescent anti-counterfeiting technology, the core technology of anti-counterfeiting still highly depends on the luminescent material with stimulus response, and advanced counterfeiters can easily obtain the structure and composition information of the luminescent material through advanced characterization means. Once the composition and structure information of the luminescent material is obtained, a counterfeiter can easily forge the luminescent material by means of chemical synthesis, and a forged material which is identical to the original plate is prepared. In addition, the stimulus of the third generation fluorescent anti-counterfeiting technology can display correct information only when reaching a certain threshold value, and high-safety encryption cannot be realized by adjusting the composition of the stimulus.
Disclosure of Invention
The invention aims to provide an encryption and anti-counterfeiting method which has high safety, can be repeatedly checked and cannot be counterfeited, so as to solve the problem that the traditional encryption and anti-counterfeiting technology seriously depends on a core luminescent material and is easy to counterfeit and crack.
The encryption and anti-counterfeiting method provided by the invention is a high-security encryption anti-counterfeiting method based on fluorescence or phosphorescence stimulation response. The method specifically comprises the following four steps: (1) selecting a fluorescent anti-counterfeiting material by a combined chemical strategy; (2) preparing a fluorescent anti-counterfeiting pattern; (3) preparing a reading device of the fluorescent anti-counterfeiting pattern; (4) and reading the encrypted information in the fluorescent anti-counterfeiting pattern. Wherein the step (1), the step (3) and the step (4) are key.
The specific contents are as follows:
step (1), selecting a fluorescent anti-counterfeiting material: selecting a fluorescent/phosphorescent light-emitting material having a response behavior to a specific chemical stimulus; screening matrix materials for fixing the luminescent material, and researching the stimulus response behavior of the luminescent material in different matrix materials; the combination of the luminescent material and the substrate which has high sensitivity, good selectivity and nonlinear response curve is preferred;
step (2), preparation of the fluorescent anti-counterfeiting pattern: preparing the selected luminescent material and the substrate material into printable ink, and then drawing anti-counterfeiting patterns on the surfaces of materials (such as materials of bank notes, passports, document identity cards, commodity outer packages and the like) which need anti-counterfeiting or encryption by using various printing technologies such as ink-jet printing, handwriting, 3D printing, piezoelectric printing, silk-screen printing and the like;
preferably, the printed pattern cannot be obviously displayed under sunlight, and can display a bright fluorescent pattern under the irradiation of excitation light with a specific wavelength;
if necessary, luminescent substances with different colors or different fluorescent lives can be covered on the encrypted fluorescent patterns by adopting a fluorescent covering method so as to further cover the encrypted information and improve the difficulty of counterfeiting the encrypted patterns;
step (3), preparing a reading device of the fluorescent anti-counterfeiting pattern (as shown in the attached figure 1): the reading device mainly comprises the following four parts:
(a) the imaging component and the display component can realize fluorescence/phosphorescence lifetime measurement, the imaging component is arranged on the top surface of the interior of the reading device, and the display component is arranged on the top surface of the reading device or can be independently placed; if necessary, a filter with specific wavelength can be arranged in front of the imaging component;
(b) a light source capable of effectively exciting the luminescent material; the light source can be installed on the inner top surface or the inner side of the reading device;
(c) a component for creating a specific chemical environment, which can be arranged on the bottom surface inside the reading device, is made into a honeycomb-shaped object stage, or is made into a groove shape, and a stimulus with a specific concentration is introduced through a conduit;
(d) fluorescence/phosphorescence lifetime imaging analysis, input and control software, wherein the imaging and display component a, the light source b and the component c for creating a chemical environment are respectively controlled by the software;
and (4) reading the encrypted information in the fluorescent anti-counterfeiting pattern (as shown in the attached figure 2): placing the prepared fluorescent anti-counterfeiting pattern in a reading device, and introducing a chemical stimulus with specific concentration through a reading adjusting device to create a chemical atmosphere capable of accurately reading encrypted information in the information of the fluorescent anti-counterfeiting pattern; the information in the fluorescent anti-counterfeiting pattern is collected and analyzed through software, and then correct fluorescence/phosphorescence lifetime data or range is input in the software, so that correct encrypted information can be presented on a display device.
In the present invention, the stimulus response may be any chemical stimulus that causes a change in fluorescence/phosphorescence intensity or fluorescence/phosphorescence lifetime. Such chemical stimuli include, but are not limited to, oxygen, pH, temperature, carbon dioxide, ammonia, biogenic amines, ions, organic molecules, inorganic compounds, biomolecules, and the like.
In the present invention, the fluorescent/phosphorescent material includes, but is not limited to, an organic light emitting material, a metal organic complex material, a nano light emitting material, a long afterglow light emitting material, or a combination of several light emitting materials.
In the present invention, the matrix material includes, but is not limited to, organic polymers, inorganic materials, organic-inorganic hybrid materials, copolymers, or a mixture of several materials thereof.
In the invention, the imaging device and the display which can realize fluorescence/phosphorescence lifetime measurement in the reading device include, but are not limited to, cameras, mobile phones, imaging CCDs, image enhancement detectors ICCDs, CMOS, single photon detectors, phase sensitive detectors, and the like.
In the present invention, the excitation light source in the reading apparatus includes, but is not limited to, a laser, a fluorescent lamp, an ultraviolet lamp, a light emitting diode, and the like.
In the invention, the reading device can create a component with a specific chemical environment, and can accurately adjust the concentration of the chemical stimulus. The chemical environment can be liquid, gas or mixed gas and mixed solution, etc.
In the invention, the fluorescence/phosphorescence lifetime imaging analysis, input and control software equipped in the reading device has the functions of fluorescence/phosphorescence lifetime value analysis, imaging and display; having the function of inputting fluorescence/phosphorescence lifetime values or ranges; the function of displaying correct encrypted information on the display unit when correct information is inputted is provided.
The invention adopts a strategy of combinatorial chemistry, and prepares the fluorescent probe with stimulus response and the matrix material into the printable luminescent ink by an arrangement and combination mode. By utilizing the characteristics that the fluorescent/phosphorescent luminescent material and the matrix material have thousands of combinations, and each combination has a uniquely determined nonlinear response behavior for a given stimulus response, the encryption anti-counterfeiting technology still has high safety even under the condition that the core luminescent material is cracked. Since the counterfeiter needs to crack all the following information at the same time: (1) a properly aligned combination of luminescent material and host material; (2) enumerating and finding the correct chemical stimulus; (3) obtaining accurate concentration information of the chemical stimulus; (4) and the correct fluorescence/phosphorescence lifetime value or range is entered on the information reading device to obtain the correct encrypted information. More importantly, the information needing to be cracked presents a strict one-to-one correspondence, and the information is not easy to be cracked, so that the encryption anti-counterfeiting technology has high security of being incapable of being forged and cracked. Meanwhile, if the new generation of fluorescent encryption anti-counterfeiting technology provided by the invention adopts gas as a stimulus, the characteristics of no damage to the encryption material in the detection process are achieved, and the concentration of the gas can be conveniently controlled by a mass flow meter, so that the technology is very suitable for occasions needing nondestructive repeated inspection, such as passports, identity cards, checks or bank notes, and the like. More importantly, the encryption anti-counterfeiting technology can still carry out further safety confirmation by simply changing the concentration of the stimulus and the input fluorescence/phosphorescence lifetime value even under the worst condition (such as failure of all anti-counterfeiting strategies), thereby ensuring the safety of important information.
The invention can be used in the anti-counterfeiting field with high security level, and has important civil and military safety application. The high security level security fields include, but are not limited to, banknotes, checks, passports, identification cards, commercial labels, packaging materials, genuine labels, and confidential documents.
Drawings
Fig. 1 is a schematic diagram of an information encryption process and a fluorescent anti-counterfeiting information reading device mentioned in the invention.
Fig. 2 is a schematic diagram of the decryption and authentication steps according to embodiment 1 of the present invention.
FIG. 3 is a typical response curve of a fluorescent ink having oxygen response behavior according to example 1 of the present invention.
Reference numbers in the figures: 1 is an excitation light source, 2 is a display, 3 is a fluorescence life imaging setting key, 4 is a fluorescence life reading setting key, 5 is a chemical environment control setting key, and 6 is an object to be detected.
Detailed Description
The invention is further explained by the specific embodiment in the following with the attached drawings.
Example 1:
the present embodiment further illustrates the new generation of encryption and anti-counterfeiting method with high security by using the stimulus response behavior that oxygen molecules can quench phosphorescence of metal-organic complexes. The specific implementation mode is as follows:
oxygen-responsive fluorescent inks were prepared using a combinatorial chemistry strategy of choice by mixing a solution of the phosphorescent oxygen-sensitive probe platinum tetrakis (pentafluorophenyl) porphyrin (PtTFPP) in Tetrahydrofuran (THF), a matrix material of 5% D4 hydrogel, ethanol, glycerol in a 0.5: 1: 6: and 2.8, mixing uniformly to obtain the oxygen response fluorescent ink Y. Because the oxygen response fluorescent probes are various in types and sensing substrate materials with oxygen permeability are even numerous, the types of the oxygen sensing fluorescent inks obtained by free combination are varied and difficult to break. And simultaneously replacing the substrate material, namely, adding THF solution of PtTFPP, 5% Ethyl Cellulose (EC) of the substrate material, ethanol and glycerol into the mixture according to the weight ratio of 0.5: 1: 6: and 2.8, mixing uniformly to obtain the oxygen response fluorescent ink Y. And printing encrypted information by adopting an ink-jet printing mode, and respectively injecting the prepared Y and M fluorescent inks with the oxygen sensing characteristics into corresponding ink storage boxes of the color ink box of the commercial ink-jet printer. Printing is performed on paper material, and encrypted information (e.g., CHEM) is printed using Y ink, and other information is printed using M ink.
In order to further improve the security level, a substance with shorter fluorescence lifetime is covered on the fluorescent pattern by adopting a fluorescence covering method. An organic solution of a fluorescent substance without oxygen response, 6- (piperidin-1-yl) -2-undecyl-1H-benzo [ de ] isoquinoline-1, 3(2H) -dione (GD 2012), a base material of 5% EC, ethanol, glycerol, in a ratio of 0.5: 1: 6: and 2.8, uniformly mixing to obtain the oxygen-free response fluorescent ink C. Injecting the unresponsive C fluorescent ink into the corresponding ink storage box of the color ink box, and printing the pattern of the C color mark at the same position. The printed pattern is invisible in an air environment and under visible light irradiation. Under the ultraviolet lamp, the pattern printed by the C ink can be seen, the encrypted information is still invisible, and the printed fluorescent pattern has high resolution which is comparable to that of commercial ink. Even with the use of time-delay gated read techniques, the encrypted information is still protected.
And (3) using a fluorescent anti-counterfeiting information reading device to perform information decryption and authenticity identification (figure 2). The chemical environment of the reading apparatus was set to 5% oxygen concentration, the delayed photographing time was 600 ns, and the gate width was set to 100 μ s, and a fluorescence lifetime image was obtained. Setting the fluorescence lifetime reading to 44-47 mus allows reading the correct encryption CHEM. Since oxygen sensing exhibits non-linear characteristics, oxygen concentration and fluorescence lifetime value are in one-to-one correspondence (fig. 3). Since the counterfeiter needs to crack all the following information at the same time: (1) a properly aligned combination of light emitting material (PtTFPP) and host material (5% EC); (2) enumerate and find the correct chemical stimulus (oxygen); (3) obtaining accurate concentration information of chemical stimuli (5% oxygen chemical environment); (4) and the correct fluorescence/phosphorescence lifetime value or range (44-47 mus) is entered on the information reading device to obtain the correct encrypted information. The information needing to be cracked presents a strict one-to-one correspondence relationship, and the information is not easy to be cracked, so that the encryption anti-counterfeiting technology has high security of being incapable of being forged and cracked.
Example 2:
chloroform solution containing phosphorescent oxygen sensitive probe octaethyl porphin platinum (PtOEP), matrix material 5% Ethyl Cellulose (EC), ethanol, glycerol in a ratio of 0.7: 1: 5: 3, and uniformly mixing to obtain the oxygen response fluorescent ink M. A chloroform solution of PtOEP, a 5% D4 hydrogel as a base material, ethanol, glycerol, in a ratio of 0.7: 1: 5: 3, and uniformly mixing to obtain the oxygen response fluorescent ink Y. An organic solution of a fluorescent substance Fluorescein Isothiocyanate (FITC) without oxygen response, a base material 5% EC, ethanol and glycerol were mixed according to a ratio of 0.7: 1: 5: 3, and mixing uniformly to obtain the oxygen-free response fluorescent ink C.
Information encryption is performed by direct handwriting, encrypted information (CHEM) is written by using Y ink, other information is written by using M ink, and then the anti-counterfeiting pattern is drawn by using C ink at the same position. Under the irradiation of visible light in the air environment, the printed pattern is not visible. Under the ultraviolet lamp, the anti-counterfeiting pattern drawn by the C ink can be seen, and the encrypted information is invisible.
And (4) using a fluorescent anti-counterfeiting information reading device to decrypt information and authenticate true and false. The chemical environment of the reading device was set to 10% oxygen, the delayed photograph time was 600 ns, and the gate width was set to 100 μ s, and a fluorescence lifetime image was obtained. The encrypted information CHEM can be read by setting the fluorescence lifetime reading to 38-42 mus.
Claims (5)
1. An encryption and anti-counterfeiting method based on fluorescence or phosphorescence stimulation response is characterized by comprising the following specific steps:
step (1), selecting a fluorescent anti-counterfeiting material: selecting a fluorescent/phosphorescent light-emitting material having a response behavior to a specific chemical stimulus; screening matrix materials for fixing the luminescent material, and researching the stimulus response behavior of the luminescent material in different matrix materials;
step (2), preparation of the fluorescent anti-counterfeiting pattern: respectively preparing the selected luminescent material and the substrate material into printable ink, and then drawing an anti-counterfeiting pattern on the surface of the material to be anti-counterfeiting or encrypted by using a printing technology;
step (3), preparing a reading device of the fluorescent anti-counterfeiting pattern: the reading device mainly comprises the following four parts:
the imaging component and the display component can realize fluorescence/phosphorescence lifetime measurement, the imaging component is arranged on the top surface of the interior of the reading device, and the display component is arranged on the top surface of the reading device or can be independently placed;
a light source capable of effectively exciting the luminescent material, the light source being mounted on the top surface of the inner side or on the inner side of the reading device;
a component for creating a specific chemical environment, wherein the component is arranged on the bottom surface inside the reading device and is made into a honeycomb-shaped object stage or a groove shape, and a chemical stimulus with specific concentration is introduced through a conduit;
fluorescence/phosphorescence lifetime imaging analysis, input and control software, which respectively controls the imaging component and the display component, the light source and the component creating a specific chemical environment;
and (4) reading encrypted information in the fluorescent anti-counterfeiting pattern: placing the prepared fluorescent anti-counterfeiting pattern in a reading device, and introducing a chemical stimulus with specific concentration through the reading device to create a specific chemical environment capable of accurately reading encrypted information in the information of the fluorescent anti-counterfeiting pattern; collecting and analyzing the information in the fluorescent anti-counterfeiting pattern through software, and inputting a correct fluorescent/phosphorescent lifetime value or lifetime range in the software, namely displaying correct encrypted information on a display device;
the chemical stimulant is oxygen;
the phosphorescent luminescent material is an organic luminescent material containing a phosphorescent oxygen sensitive probe;
the substrate material is an organic polymer with oxygen permeability, an inorganic material with oxygen permeability, an organic-inorganic hybrid material or copolymer with oxygen permeability, or a mixture of several materials.
2. The encryption and anti-counterfeiting method based on fluorescence or phosphorescence stimulus response according to claim 1, wherein in the step (2), the printed pattern cannot be clearly displayed in sunlight, and can display a bright fluorescent pattern under the irradiation of excitation light with a specific wavelength.
3. The encryption and anti-counterfeiting method based on fluorescence or phosphorescence stimulation response as claimed in claim 1, wherein in the step (2), luminescent materials with different colors or different fluorescence lifetimes are covered on the encrypted fluorescence pattern by fluorescence masking to further mask the encrypted information.
4. The encryption and anti-counterfeiting method based on fluorescence or phosphorescence stimulation response according to claim 1, wherein the excitation light source in the reading device is a laser, a fluorescent lamp, an ultraviolet lamp or a light emitting diode.
5. The encryption and anti-counterfeiting method based on fluorescence or phosphorescence stimulation response according to claim 1, wherein the fluorescence/phosphorescence lifetime imaging analysis, input and control software provided in the reading device has the following functions: fluorescence/phosphorescence lifetime value analysis, imaging and display functions; a function of inputting fluorescence/phosphorescence lifetime values or ranges; the function of displaying correct encrypted information on a display part after correct information is input.
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| CN113121409A (en) * | 2021-03-03 | 2021-07-16 | 太原理工大学 | Organic fluorescent material with information deep hiding function, preparation and application |
| CN113234189B (en) * | 2021-06-01 | 2023-03-10 | 湖南科技大学 | Method for applying photoswitch polymorphic fluorescent polymer to data encryption |
| CN115019626A (en) * | 2022-07-07 | 2022-09-06 | 吉林大学 | Application of thermosensitive fluorescent material in anti-counterfeiting trademark |
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