CN114891368A - Magnetic optically variable pigment - Google Patents

Magnetic optically variable pigment Download PDF

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Publication number
CN114891368A
CN114891368A CN202210489739.8A CN202210489739A CN114891368A CN 114891368 A CN114891368 A CN 114891368A CN 202210489739 A CN202210489739 A CN 202210489739A CN 114891368 A CN114891368 A CN 114891368A
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refractive index
index layer
layer
high refractive
magnetic
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CN114891368B (en
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孙洪保
蔡宏亮
潘硕
陈章荣
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Huizhou Foryou Optical Technology Co ltd
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Huizhou Foryou Optical Technology Co ltd
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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
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C1/00—Treatment of specific inorganic materials other than fibrous fillers; Preparation of carbon black
    • C09C1/0015—Pigments exhibiting interference colours, e.g. transparent platelets of appropriate thinness or flaky substrates, e.g. mica, bearing appropriate thin transparent coatings
    • C09C1/0024—Pigments exhibiting interference colours, e.g. transparent platelets of appropriate thinness or flaky substrates, e.g. mica, bearing appropriate thin transparent coatings comprising a stack of coating layers with alternating high and low refractive indices, wherein the first coating layer on the core surface has the high refractive index
    • C09C1/003—Pigments exhibiting interference colours, e.g. transparent platelets of appropriate thinness or flaky substrates, e.g. mica, bearing appropriate thin transparent coatings comprising a stack of coating layers with alternating high and low refractive indices, wherein the first coating layer on the core surface has the high refractive index comprising at least one light-absorbing layer
    • C09C1/0033—Pigments exhibiting interference colours, e.g. transparent platelets of appropriate thinness or flaky substrates, e.g. mica, bearing appropriate thin transparent coatings comprising a stack of coating layers with alternating high and low refractive indices, wherein the first coating layer on the core surface has the high refractive index comprising at least one light-absorbing layer consisting of a metal or an alloy
    • 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
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C2200/00—Compositional and structural details of pigments exhibiting interference colours
    • C09C2200/20—Interference pigments comprising a layer with a concentration gradient or a gradient of the refractive index
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C2200/00—Compositional and structural details of pigments exhibiting interference colours
    • C09C2200/30—Interference pigments characterised by the thickness of the core or layers thereon or by the total thickness of the final pigment particle
    • C09C2200/301—Thickness of the core
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C2200/00—Compositional and structural details of pigments exhibiting interference colours
    • C09C2200/30—Interference pigments characterised by the thickness of the core or layers thereon or by the total thickness of the final pigment particle
    • C09C2200/302—Thickness of a layer with high refractive material
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C2200/00—Compositional and structural details of pigments exhibiting interference colours
    • C09C2200/30—Interference pigments characterised by the thickness of the core or layers thereon or by the total thickness of the final pigment particle
    • C09C2200/303—Thickness of a layer with low refractive material
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C2200/00—Compositional and structural details of pigments exhibiting interference colours
    • C09C2200/30—Interference pigments characterised by the thickness of the core or layers thereon or by the total thickness of the final pigment particle
    • C09C2200/306—Thickness of an absorbing layer
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C2210/00—Special effects or uses of interference pigments
    • C09C2210/50—Fluorescent, luminescent or photoluminescent properties

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Metallurgy (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Materials Engineering (AREA)
  • Wood Science & Technology (AREA)
  • Laminated Bodies (AREA)

Abstract

The application provides a magnetic optically variable pigment. The magnetic optically variable pigment comprises: the utility model provides a light-sensitive printing ink, including the membrane pile filter layer, the interference effect of membrane pile filter layer, this application is through the light scattering reinforcing characteristic who utilizes metal nanoparticle and membrane pile filter layer, use strong white light-induced plasma to the light variation field, obtain a neotype magnetic light-sensitive printing ink, this pigment has the effect of following the different colors of angle and light and shade dynamic change under ambient light, under strong white light, the dark space hidden color appears, simultaneously along with the visual angle rotates, bright zone colour and hidden color alternate change, make pigment have multiple anti-fake effect, improve anti-fake dynamics greatly.

Description

Magnetic optically variable pigment
Technical Field
The application relates to the technical field of anti-counterfeiting, in particular to a magnetic optically variable pigment.
Background
In the current society, counterfeit commodities flood the market, which not only destroys the normal market order, but also infringes the rights and interests of consumers and the economic benefits of production enterprises. In order to prevent and fight against counterfeit activities, various anti-counterfeit technologies have been researched and developed. In recent years, optically variable pigments are being widely used in the high-end anti-counterfeiting field.
The magnetic optically variable pigment integrates two physical properties of magnetism and optically variable, and the pigment can complete the control of the position of the pigment flakes through the action of a magnetic field in the ink layer. The pattern after the fixed magnetism can present the characteristics such as color change, flow effect and light and shade change along with the change of the visual angle of the naked eyes of an observer. The technology is applied to the anti-counterfeiting fields of bank notes, passports, bank checks and the like, and is a more advanced 'first-line anti-counterfeiting' technology before a project.
The structure and the realization principle of the existing magnetic optically variable pigment are reported in a large number, for example, the technical principle, the structural design and the preparation process of the magnetic optically variable film are studied in detail in the article "research and application of the magnetic optically variable anti-counterfeiting film" of the university of mansion university Master graduation. In addition, some counterfeit money or counterfeit goods are occasionally packaged with interference type optically variable pigments, so that the traditional interference type optically variable pigments are gradually losing the public confidence as a first-line anti-counterfeiting means for identifying the authenticity. Therefore, the search and preparation of new anti-counterfeiting magnetic pigments are urgently needed.
Disclosure of Invention
The application provides a magnetism light becomes pigment, this magnetism light becomes pigment utilizes plasma metal nanoparticle's light scattering reinforcing characteristic and the interference effect of membrane pile filter layer, makes magnetism light become raw materials and has multiple anti-fake effect, and in addition, the magnetism light becomes pigment of this application carries out configuration optimization, makes this magnetism light become pigment's saturation higher.
In order to solve the technical problem, the application adopts a technical scheme that: provided is a magnetic optically variable pigment, including: the structure of the film stack filter layer is (a) 1 H 1 a 2 L 1 a 3 H 2 ) n1 bN(a 4 H 3 a 5 L 2 a 6 H 4 ) n2 cM, wherein H 1 Is a first high refractive index layer, L 1 Is a first low refractive index layer, H 2 Is the second high refractive index layer, H 3 Is a thirdHigh refractive index layer, L 2 Is a second low refractive index layer, H 4 Is a fourth high refractive index layer, N is an absorption layer, M is a magnetic core layer containing a magnetic material, a 1 Film thickness coefficient, a, of the first high refractive index layer 2 Film layer thickness coefficient of first low refractive index layer, a 3 Is the film thickness coefficient of the second high refractive index layer, a 4 Is the film thickness coefficient of the third high refractive index layer, a 5 Is the film thickness coefficient of the second low refractive index layer, a 6 Is the film thickness coefficient of the fourth high refractive index layer, b is the film thickness coefficient of the absorption layer, c is the film thickness coefficient of the magnetic core layer, n1 and n2 are the corresponding dielectric film stack period numbers, and wherein 0 < a 1 ≤5、0≤a 2 ≤5、0≤a 3 ≤5、0≤a 4 ≤5、0≤a 5 ≤5、0≤a 6 B is more than or equal to 5, b is more than 0 and less than or equal to 3, c is more than 0 and less than or equal to 3, and n1 and n2 are corresponding medium film stack period numbers.
Further, the magnetic optically variable pigment includes: the film stack filtering layer is provided with a magnetic material and a plurality of metal nano-particles arranged on the surface of the film stack filtering layer; the structure of the film stack filter layer is (a) 1 H 1 a 2 L 1 a 3 H 2 ) n1 bN(a 4 H 3 a 5 L 2 a 6 H 4 ) n2 cM(a 6 H 4 a 5 L 2 a 4 H 3 ) n2 bN(a 3 H 2 a 2 L 1 a 1 H 1 ) n1 Wherein H is 1 Is a first high refractive index layer, L 1 Is a first low refractive index layer, H 2 Is the second high refractive index layer, H 3 Is a third high refractive index layer, L 2 Is a second low refractive index layer, H 4 Is a fourth high refractive index layer, N is an absorption layer, M is a magnetic core layer containing a magnetic material, a 1 Is the film thickness coefficient of the first high refractive index layer, a 2 Is the film thickness coefficient of the first low refractive index layer, a 3 Is the film thickness coefficient of the second high refractive index layer, a 4 Is the film thickness coefficient of the third high refractive index layer, a 5 Is the film thickness coefficient of the second low refractive index layer, a 6 Is the film thickness coefficient of the fourth high refractive index layer, b is the film thickness coefficient of the absorption layer, and c is the film thickness coefficient of the magnetic core layer, wherein 0 < a 1 ≤5、0≤a 2 ≤5、0≤a 3 ≤5、0≤a 4 ≤5、0≤a 5 ≤5、0≤a 6 B is more than 0 and less than or equal to 5, b is more than 0 and less than or equal to 3, c is more than 0 and less than or equal to 3, and n1 and n2 are the corresponding stacking period number of the dielectric film.
Furthermore, the film stack filter layer has a first main surface and a second main surface which are opposite to each other, and a plurality of metal nano-particles are arranged on the first main surface and the second main surface, so that the magnetic optically variable pigment is in a symmetrical structure taking the film stack filter layer as a center, or the plurality of metal nano-particles are arranged on the first main surface or the second main surface.
Further, the materials of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer and the fourth high refractive index layer are all materials with refractive indexes larger than 1.65; the materials of the first low-refractive-index layer and the second low-refractive-index layer are both materials with refractive indexes less than or equal to 1.65.
Further, the materials of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer and the fourth high refractive index layer are the same, or at least two of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer and the fourth high refractive index layer are different.
Further, the materials of the first high refractive-index layer, the second high refractive-index layer, the third high refractive-index layer, and the fourth high refractive-index layer include: lanthanum titanate, titanium oxide, niobium pentoxide, zinc sulfide, zinc oxide, zirconium oxide, titanium dioxide, carbon, indium oxide, indium tin oxide, tantalum pentoxide, cerium oxide, yttrium oxide, europium oxide, iron oxide, triiron tetroxide, hafnium nitride, hafnium carbide, hafnium oxide, lanthanum oxide, magnesium oxide, neodymium oxide, praseodymium oxide, samarium oxide, antimony trioxide, silicon carbide, silicon nitride, silicon monoxide, selenium trioxide, tin oxide, and tungsten trioxide.
Further, the materials of the first low refractive index layer and the second low refractive index layer are the same, or the materials of the first low refractive index layer and the second low refractive index layer are different.
Further, the materials of the first low refractive index layer and the second low refractive index layer include: at least one of silica, alumina, magnesium fluoride, aluminum fluoride, cerium fluoride, lanthanum fluoride, neodymium fluoride, samarium fluoride, barium fluoride, calcium fluoride, lithium fluoride polystyrene, polyethylene, polymethyl methacrylate, polyamideimide, polyperfluoroethylpropylene, tetrafluoroethylene, chlorotrifluoroethylene, cellulose propionate, cellulose acetate butyrate, methylpentene polymer, homopolyformaldehyde, acrylic resin, cellulose nitrate, ethyl cellulose, polypropylene, polysulfone, polyethersulfone, mica, a heteroisomorphous polymer, polybutene, an ionomer, an acrylic copolymer, styrene butadiene, polyvinyl chloride, urea formaldehyde, styrene acrylonitrile, and polycarbonate.
Further, the material of the absorption layer includes: one or an alloy of at least two of titanium, aluminum, chromium, nickel, palladium, titanium, silicon, vanadium, cobalt, iron, carbon, tin, tungsten, molybdenum, rhodium, niobium, and carbon.
Further, the physical thickness of the absorption layer is 5nm to 100 nm.
Further, the magnetic core layer is of a single-layer structure; the materials of the magnetic core layer include: at least one of iron, cobalt, nickel, gadolinium, terbium, dysprosium, and erbium or an oxide of at least one or an alloy of at least two; alternatively, the material of the magnetic core layer includes: at least one of an iron-silicon alloy, an iron-aluminum alloy, an iron-silicon-chromium alloy, and an iron-nickel-molybdenum alloy.
Further, the magnetic core layer is of a multilayer structure, and the structure of the magnetic core layer is as follows: m 1 M 0 M 2 、M 0 M 1 M 0 、M 0 M 1 、M 1 D 1 M 0 D 2 M 2 、M 0 D 1 M 1 D 2 M 0 Or M 1 D 1 M 0 Wherein M is 0 Is a magnetic film layer, M 1 And M 2 Is a metal film layer, D 1 And D 2 Is a dielectric film layer.
Further, the material of the magnetic film layer comprises: at least one of iron, cobalt, nickel, gadolinium, terbium, dysprosium and erbium or at least one of oxides or at least two of alloys thereof, or the material of the magnetic film layer comprises at least one of iron-silicon alloy, iron-aluminum alloy, iron-silicon-chromium alloy and iron-nickel-molybdenum alloy; the metal film layer comprises the following materials: at least one or an alloy of at least two of aluminum, silver, gold, copper, platinum, tin, titanium, palladium, rhodium, niobium, and chromium; the material of the dielectric film layer comprises: at least one of silicon dioxide, aluminum oxide, magnesium fluoride, aluminum fluoride, cerium fluoride, lanthanum fluoride, neodymium fluoride, samarium fluoride, barium fluoride, and calcium fluoride.
Further, the plurality of metal nanoparticles are distributed at intervals, and the gap between the plurality of metal nanoparticles is 2nm-1 mm.
Further, the material of the metal nanoparticles includes: at least one of aluminum, silver, gold, copper, platinum, ruthenium, palladium, rhodium, cobalt, iron, nickel, lead, osmium, and iridium, or an alloy of at least two thereof.
The beneficial effects of the embodiment of the application are that: in distinction from the state of the art, the magnetic optically variable pigments of the present application comprise: the utility model provides a film pile filter layer with magnetic material and locate a plurality of metal nanoparticle on film pile filter layer surface, this application is through the interference effect that utilizes metal nanoparticle's light scattering reinforcing characteristic and film pile filter layer, use strong white light plasma to the light variation field, obtain a neotype magnetic light variation pigment, this pigment has the effect of following the different colors of angle and light and shade dynamic change under ambient light, under strong white light, the dark space hidden color appears, simultaneously along with the visual angle rotates, bright zone colour and hidden color alternate change, make pigment have multiple anti-fake effect, improve anti-fake dynamics greatly, and this pigment has higher saturation and richer colour gamut space.
Drawings
In order to more clearly illustrate the technical solutions in the embodiments of the present application, the drawings needed to be used in the description of the embodiments are briefly introduced below, and it is obvious that the drawings in the following description are only some embodiments of the present application, and it is obvious for those skilled in the art to obtain other drawings based on these drawings without creative efforts.
Fig. 1 is a schematic structural diagram of an embodiment of a magnetic optically variable pigment provided herein;
fig. 2 is a schematic structural diagram of an embodiment of a film stack filter layer in the magnetic optically variable pigment shown in fig. 1.
Detailed Description
The present application will now be described in detail with reference to specific embodiments thereof as illustrated in the accompanying drawings. These embodiments are not intended to limit the present application, and structural, methodological, or functional changes made by those skilled in the art according to these embodiments are included in the scope of the present application.
In addition, if there is a description of "first", "second", etc. in the embodiments of the present application, the description of "first", "second", etc. is for descriptive purposes only and is not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include at least one such feature. In addition, technical solutions between various embodiments may be combined with each other, but must be realized by a person skilled in the art, and when the technical solutions are contradictory or cannot be realized, such a combination should not be considered to exist, and is not within the protection scope of the present application.
The application provides a magnetic optically variable pigment, which adopts a special arrangement structure, utilizes the scattered light enhancement characteristic under the local plasma resonance of metal nanoparticles, and improves an F-P (Fabry-Perot) interference cavity structure, so that the magnetic optically variable pigment has a multiple optical color change effect, the anti-counterfeiting strength is greatly increased, and the color saturation of the pigment is further improved.
As shown in fig. 1, fig. 1 is a schematic structural diagram of an embodiment of a magnetic optically variable pigment provided in the present application, where the magnetic optically variable pigment 10 includes: a stack filter layer 11 having a magnetic material and a plurality of metal nanoparticles 12 disposed on a surface of the stack filter layer 11.
Specifically, the structure of the film stack filter layer 11 is (a) 1 H 1 a 2 L 1 a 3 H 2 ) n1 bN(a 4 H 3 a 5 L 2 a 6 H 4 ) n2 cM, wherein H 1 Is a first high refractive index layer, L 1 Is a first low refractive index layer, H 2 Is the second high refractive index layer, H 3 Is a third high refractive index layer, L 2 Is a second low refractive index layer, H 4 Is a fourth high refractive index layer, N is an absorption layer, M is a magnetic core layer containing a magnetic material, a 1 Film thickness coefficient, a, of the first high refractive index layer 2 Film thickness coefficient of first low refractive index layer, a 3 Is the film thickness coefficient of the second high refractive index layer, a 4 Is the film thickness coefficient of the third high refractive index layer, a 5 Is the film thickness coefficient of the second low refractive index layer, a 6 Is the film thickness coefficient of the fourth high refractive index layer, b is the film thickness coefficient of the absorption layer, c is the film thickness coefficient of the magnetic core layer, n1 and n2 are the corresponding dielectric film stack period numbers, wherein, a is more than 0 1 ≤5、0≤a 2 ≤5、0≤a 3 ≤5、0≤a 4 ≤5、0≤a 5 ≤5、0≤a 6 B is more than or equal to 5, b is more than 0 and less than or equal to 3, c is more than 0 and less than or equal to 3, and n1 and n2 are corresponding medium film stack period numbers.
For example, a 1 ＝1，a 2 ＝1，a 3 ＝1，a 4 ＝1，a 5 ＝1，a 6 1, 1 for b, 1 for c, 1 for n1, 1 for n2, and the structure of the corresponding stack filter layer 11 is H 1 L 1 H 2 NH 3 L 2 H 4 M, that is, the film thickness coefficient of the first high refractive index layer is 1, the film thickness coefficient of the first low refractive index layer is 1, the film thickness coefficient of the second high refractive index layer is 1, the film thickness coefficient of the third high refractive index layer is 1, the film thickness coefficient of the second low refractive index layer is 1, the film thickness coefficient of the fourth high refractive index layer is 1, the film thickness coefficient of the absorption layer is 1, and the film thickness coefficient of the magnetic core layer containing a magnetic material is 1. As shown in FIG. 2, the structure of the in-film filter layer 11 is a first high refractive index layer sequentially stackedA refractive index layer 111, a first low refractive index layer 112, a second high refractive index layer 113, an absorption layer 114, a third high refractive index layer 115, a second low refractive index layer 116, a fourth high refractive index layer 117, and a magnetic core layer 118 containing a magnetic material.
In another embodiment, the magnetic optically variable pigment 10 includes an ild layer 11 having a magnetic material and a plurality of metal nanoparticles 12 disposed on a surface of the ild layer 11.
Wherein the structure of the film stack filter layer 11 is (a) 1 H 1 a 2 L 1 a 3 H 2 ) n1 bN(a 4 H 3 a 5 L 2 a 6 H 4 ) n2 cM(a 6 H 4 a 5 L 2 a 4 H 3 ) n2 bN(a 3 H 2 a 2 L 1 a 1 H 1 ) n1 . Wherein H 1 Is a first high refractive index layer, L 1 Is a first low refractive index layer, H 2 Is the second high refractive index layer, H 3 Is a third high refractive index layer, L 2 Is a second low refractive index layer, H 4 Is a fourth high refractive index layer, N is an absorption layer, M is a magnetic core layer containing a magnetic material, a 1 Is the film thickness coefficient of the first high refractive index layer, a 2 Is the film thickness coefficient of the first low refractive index layer, a 3 Is the film thickness coefficient of the second high refractive index layer, a 4 Is the film thickness coefficient of the third high refractive index layer, a 5 Is the film thickness coefficient of the second low refractive index layer, a 6 Is the film thickness coefficient of the fourth high refractive index layer, b is the film thickness coefficient of the absorption layer, and c is the film thickness coefficient of the magnetic core layer, wherein 0 < a 1 ≤5、0≤a 2 ≤5、0≤a 3 ≤5、0≤a 4 ≤5、0≤a 5 ≤5、0≤a 6 B is more than or equal to 5, b is more than 0 and less than or equal to 3, c is more than 0 and less than or equal to 3, and n1 and n2 are corresponding medium film stack period numbers.
For example, a 1 ＝1，a 2 ＝1，a 3 ＝1，a 4 ＝1，a 5 ＝1，a 6 1, and 1, the structure of the corresponding stack filter layer 11 is H 1 L 1 H 2 NH 3 L 2 H 4 MH 4 L 2 H 3 NH 2 L 1 H 1 . That is, the film-on-film filter layer 11 has a structure of a first high refractive index layer/a first low refractive index layer/a second high refractive index layer/an absorber layer/a third high refractive index layer/a second low refractive index layer/a fourth high refractive index layer/a core layer/a fourth high refractive index layer/a second low refractive index layer/a third high refractive index layer/an absorber layer/a second high refractive index layer/a first low refractive index layer/a first high refractive index layer which are laminated in this order. That is, the magnetic optically variable pigments 10 of the present embodiment are symmetrically disposed along the center of the magnetic core layer 118.
The film stack filter layer 11 in the magnetic optically variable pigment 10 of the above embodiment contains a magnetic material, and utilizes the interaction between the magnetic material and a magnetic field, so that the pigment is directionally arranged in the printing process, and has the effect of color variation along with the angle and dynamic change of light and shade under ambient light, and hidden colors (third colors) appear in dark area colors under strong white light, and simultaneously along with the rotation of the visual angle, the novel optically variable effect of alternate change of bright area colors and hidden colors makes the magnetic optically variable pigment 10 have a multiple optically variable effect, and the anti-counterfeiting strength is greatly increased. For example, the authenticity identification can be completed by using a household flashlight or a mobile phone flashlight to visually inspect color changes, and the method is a novel simple and efficient one-line anti-counterfeiting technology.
Further, as shown in fig. 1, the stack filter layer 11 has a first main surface 101 and a second main surface 102 opposite to each other, and a plurality of metal nanoparticles 12 are disposed on both the first main surface 101 and the second main surface 102, so that the magnetic optically variable pigment 10 has a symmetrical structure with the stack filter layer 11 as a center.
Alternatively, in another embodiment, the magnetic optically variable pigment 10 may also be an asymmetric structure, for example, the metal nanoparticles 12 are provided only on the first main surface 101 of the stack filter layer 11, or the metal nanoparticles 12 are provided only on the second main surface 102 of the stack filter layer 11.
Further, the materials of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer and the fourth high refractive index layer are all materials with refractive indexes larger than 1.65, for example, the refractive indexes of the materials are 1.7, 1.75, 1.8 or 1.9, etc.; the materials of the first low refractive index layer and the second low refractive index layer are both materials having a refractive index of 1.65 or less, for example, the materials have refractive indices of 1.1, 1.3, 1.6, 1.65, and the like.
Specifically, the materials of the first high refractive-index layer, the second high refractive-index layer, the third high refractive-index layer, and the fourth high refractive-index layer include: lanthanum titanate, titanium oxide, niobium pentoxide, zinc sulfide, zinc oxide, zirconium oxide, titanium dioxide, carbon, indium oxide, indium tin oxide, tantalum pentoxide, cerium oxide, yttrium oxide, europium oxide, iron oxide, triiron tetroxide, hafnium nitride, hafnium carbide, hafnium oxide, lanthanum oxide, magnesium oxide, neodymium oxide, praseodymium oxide, samarium oxide, antimony trioxide, silicon carbide, silicon nitride, silicon monoxide, selenium trioxide, tin oxide, and tungsten trioxide.
It should be noted that, in a specific embodiment of the present invention, the materials of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer and the fourth high refractive index layer may be completely the same, or not completely the same, that is, the materials of at least two of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer and the fourth high refractive index layer are different, which is not limited herein.
Specifically, the materials of the first low refractive index layer and the second low refractive index layer include: at least one of silica, alumina, magnesium fluoride, aluminum fluoride, cerium fluoride, lanthanum fluoride, neodymium fluoride, samarium fluoride, barium fluoride, calcium fluoride, lithium fluoride polystyrene, polyethylene, polymethyl methacrylate, polyamideimide, polyperfluoroethylpropylene, tetrafluoroethylene, chlorotrifluoroethylene, cellulose propionate, cellulose acetate butyrate, methylpentene polymer, homopolyformaldehyde, acrylic resin, cellulose nitrate, ethyl cellulose, polypropylene, polysulfone, polyethersulfone, mica, a heteroisomorphous polymer, polybutene, an ionomer, an acrylic copolymer, styrene butadiene, polyvinyl chloride, urea formaldehyde, styrene acrylonitrile, and polycarbonate.
It should be noted that, in a specific embodiment of the present invention, the materials of the first low refractive index layer and the second low refractive index layer may be the same, or the materials of the first low refractive index layer and the second low refractive index layer are different, and are not limited herein.
Further, the material of the absorption layer includes: one or an alloy of at least two of titanium, aluminum, chromium, nickel, palladium, titanium, silicon, vanadium, cobalt, iron, carbon, tin, tungsten, molybdenum, rhodium, niobium, and carbon.
The physical thickness of the absorption layer is 5nm-100 nm. For example, the physical thickness of the absorption layer may be 5nm, 7nm, 20nm, 50nm, 70nm, 90nm, 100nm, or the like.
Alternatively, the magnetic core layer may be a single layer structure. The materials of the magnetic core layer include: at least one of iron, cobalt, nickel, gadolinium, terbium, dysprosium, and erbium, or an oxide of at least one of them, or an alloy of at least two of them. Or the magnetic material in the magnetic core layer comprises: at least one of an iron-silicon alloy, an iron-aluminum alloy, an iron-silicon-chromium alloy, and an iron-nickel-molybdenum alloy.
Alternatively, the magnetic core layer may also be a multilayer structure, for example, the structure of the magnetic core layer: m 1 M 0 M 2 、M 0 M 1 M 0 、M 0 M 1 、M 1 D 1 M 0 D 2 M 2 、M 0 D 1 M 1 D 2 M 0 Or M 1 D 1 M 0 Wherein M is 0 Is a magnetic film layer, M 1 And M 2 Is a metal film layer, D 1 And D 2 Is a dielectric film layer.
Specifically, the material of the magnetic film layer includes: at least one of iron, cobalt, nickel, gadolinium, terbium, dysprosium, erbium, or an oxide of at least one of them, or an alloy of at least two of them, or the material of the magnetic film layer includes at least one of an iron-silicon alloy, an iron-aluminum alloy, an iron-silicon-chromium alloy, and an iron-nickel-molybdenum alloy.
The metal film layer comprises the following materials: at least one of aluminum, silver, gold, copper, platinum, tin, titanium, palladium, rhodium, niobium, and chromium, or an alloy of at least two thereof.
The dielectric film layer comprises the following materials: at least one of silicon dioxide, aluminum oxide, magnesium fluoride, aluminum fluoride, cerium fluoride, lanthanum fluoride, neodymium fluoride, samarium fluoride, barium fluoride, and calcium fluoride.
In this embodiment, the plurality of metal nanoparticles 12 are spaced apart from each other, and the gap between the plurality of metal nanoparticles 12 is 2nm to 1 mm. For example, the gaps between the metal nanoparticles 12 may be 2nm, 200nm, 1000nm, 20000nm, 100000nm, 1mm, or the like.
Specifically, the material of the metal nanoparticles 12 includes: at least one of aluminum, silver, gold, copper, platinum, ruthenium, palladium, rhodium, cobalt, iron, nickel, lead, osmium, and iridium, or an alloy of at least two thereof.
Specifically, the shape of the metal nanoparticles 12 may be any shape, such as a sphere, a hemisphere, an ellipsoid, a cube, a cuboid, an octahedron, a dodecahedron, a hexadecahedron, a rod, a star, a cone, a triangle, a cylinder, or the like. The shape of the metal nanoparticles 12 may be the same shape or a mixture of shapes.
Unlike absorption color development by localized plasmon resonance (LSPR), the color development of the metal nanoparticles 12 in this application under high intensity white light is the color of the scattered light enhanced by the LSPR, and the high intensity white light color-changing effect is only achieved when the film layer (the outermost film layer of the interference film stack) in direct contact with the metal particles is a high refractive index film layer (n > 1.75).
For example, a layer of Ag NPs is arranged on a SiO2 film layer or a layer of Ag NPs is arranged on the surface of a MgF2/AL2O3/MgF2 film stack, and the structure can generate color due to light absorption of LSPR wavelength selectivity of the Ag NPs, but cannot generate color change due to illumination under strong white light. And the Ag NPs arranged on the surface of the single-layer ZrO2 film layer also cannot generate high light discoloration. In the prior art, the vast majority of plasma rendering devices utilize LSPR light absorption, while the LSPR light scattering enhancement feature is rarely used.
Macroscopic diffuse color realization has strict requirements on the F-P film stack structure. Similarly, the scattering type optically variable pigment has certain requirements on ambient light, and different from the traditional interference type optically variable pigment, the bright color of the pigment needs to be observed in a bright environment, and the scattering type optically variable pigment in the application needs to be irradiated by white light (high-intensity white light) with preset intensity in a dark field environment to have a photochromic effect. Specifically, the ambient light illumination is less than 300lx, the light source illumination is more than 3000lx, preferably, the light source illumination is more than 5000lx, and the magnetic optically variable pigment 10 has a good high photochromic effect. And in outdoor environment of sunny day, if the ambient light illumination is more than 3000lx, the sample does not have the high photochromic effect.
Therefore, the magnetic optically variable pigment 10 provided by the present application is a strong white color-changing pigment in dark field environment, which is very different from the conventional pigment. The color change is essentially the conversion of the reflected color under ambient light to the scattered color under high white and strong light.
Moreover, the magnetic optically variable pigment 10 has higher color saturation and richer color gamut space by adjusting the interference film stack in the pigment film system and specially selecting some materials.
It should be understood that although the present description refers to embodiments, not every embodiment may contain only a single embodiment, and such description is for clarity only, and those skilled in the art will be able to make the description as a whole, and the embodiments may be appropriately combined to form other embodiments as will be appreciated by those skilled in the art. The above detailed description is given for the purpose of illustrating a practical embodiment of the present application and is not to be construed as limiting the scope of the present application, and any equivalent embodiments or modifications that do not depart from the technical spirit of the present application are intended to be included therein.

Claims (15)

1. A magnetic optically variable pigment, characterized in that it comprises: a film stack filtering layer with magnetic material and a plurality of metal nano-particles arranged on the surface of the film stack filtering layer,
the structure of the film stack filter layer is (a) 1 H 1 a 2 L 1 a 3 H 2 ) n1 bN(a 4 H 3 a 5 L 2 a 6 H 4 ) n2 cM, wherein H 1 Is a first high refractive index layer, L 1 Is a first low refractive index layer, H 2 Is the second high refractive index layer, H 3 Is a third high refractive index layer, L 2 Is a second low refractive index layer, H 4 Is a fourth high refractive index layer, N is an absorption layer, M is a magnetic core layer containing a magnetic material, a 1 Is the film thickness coefficient, a, of the first high refractive index layer 2 Film layer thickness coefficient, a, of the first low refractive index layer 3 Is a film thickness coefficient of the second high refractive index layer, a 4 Is the film thickness coefficient of the third high refractive index layer, a 5 Is the film layer thickness coefficient of the second low refractive index layer, a 6 Is the film thickness coefficient of the fourth high refractive index layer, b is the film thickness coefficient of the absorption layer, c is the film thickness coefficient of the magnetic core layer, n1 and n2 are the corresponding dielectric film stack period numbers, and wherein 0 < a 1 ≤5、0≤a 2 ≤5、0≤a 3 ≤5、0≤a 4 ≤5、0≤a 5 ≤5、0≤a 6 B is more than or equal to 5, b is more than 0 and less than or equal to 3, c is more than 0 and less than or equal to 3, and n1 and n2 are corresponding medium film stack period numbers.
2. A magnetic optically variable pigment, characterized in that it comprises: the film stack filtering layer is provided with a magnetic material and a plurality of metal nano-particles arranged on the surface of the film stack filtering layer;
the structure of the film stack filter layer is (a) 1 H 1 a 2 L 1 a 3 H 2 ) n1 bN(a 4 H 3 a 5 L 2 a 6 H 4 ) n2 cM(a 6 H 4 a 5 L 2 a 4 H 3 ) n2 bN(a 3 H 2 a 2 L 1 a 1 H 1 ) n1 ，
Wherein H 1 Is a first high refractive index layer, L 1 Is a first low refractive index layer, H 2 Is the second high refractive index layer, H 3 Is a third high refractive index layer, L 2 Is a second low refractive index layer, H 4 Is a fourth high refractive index layer, N is an absorption layer, M is a magnetic core layer containing a magnetic material, a 1 Is a film thickness coefficient of the first high refractive index layer, a 2 Is the film layer thickness coefficient of the first low refractive index layer, a 3 Is the film thickness coefficient of the second high refractive index layer, a 4 Is the film thickness coefficient of the third high refractive index layer, a 5 Is the film layer thickness coefficient of the second low refractive index layer, a 6 Is the film thickness coefficient of the fourth high refractive index layer, b is the film thickness coefficient of the absorption layer, and c is the film thickness coefficient of the magnetic core layer, wherein 0 < a 1 ≤5、0≤a 2 ≤5、0≤a 3 ≤5、0≤a 4 ≤5、0≤a 5 ≤5、0≤a 6 B is more than or equal to 5, b is more than 0 and less than or equal to 3, c is more than 0 and less than or equal to 3, and n1 and n2 are corresponding medium film stack period numbers.
3. A magnetic optically variable pigment according to claim 1 or 2, wherein the on-film filter layer has a first main surface and a second main surface opposite to each other,
the first main surface and the second main surface are both provided with a plurality of metal nano-particles so that the magnetic optically variable pigment is in a symmetrical structure with the membrane stack filter layer as the center, or,
a number of the metal nanoparticles are disposed on the first major surface or the second major surface.
4. The magnetic optically variable pigment according to claim 1 or 2, wherein the materials of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer and the fourth high refractive index layer are all materials with a refractive index of more than 1.65; the materials of the first low-refractive-index layer and the second low-refractive-index layer are both materials with refractive indexes smaller than or equal to 1.65.
5. The magnetic optically variable pigment according to claim 4, wherein the materials of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer and the fourth high refractive index layer are the same, or,
at least two of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer, and the fourth high refractive index layer are made of different materials.
6. The magnetic optically variable pigment of claim 5, wherein the materials of the first high refractive index layer, the second high refractive index layer, the third high refractive index layer and the fourth high refractive index layer comprise: lanthanum titanate, titanium oxide, niobium pentoxide, zinc sulfide, zinc oxide, zirconium oxide, titanium dioxide, carbon, indium oxide, indium tin oxide, tantalum pentoxide, cerium oxide, yttrium oxide, europium oxide, iron oxide, triiron tetroxide, hafnium nitride, hafnium carbide, hafnium oxide, lanthanum oxide, magnesium oxide, neodymium oxide, praseodymium oxide, samarium oxide, antimony trioxide, silicon carbide, silicon nitride, silicon monoxide, selenium trioxide, tin oxide, and tungsten trioxide.
7. A magnetic optically variable pigment according to claim 4, wherein the first low refractive index layer and the second low refractive index layer are of the same material, or,
the first low refractive index layer and the second low refractive index layer are different in material.
8. The magnetic optically variable pigment according to claim 7, wherein the material of the first low refractive index layer and the second low refractive index layer comprises: at least one of silica, alumina, magnesium fluoride, aluminum fluoride, cerium fluoride, lanthanum fluoride, neodymium fluoride, samarium fluoride, barium fluoride, calcium fluoride, lithium fluoride polystyrene, polyethylene, polymethyl methacrylate, polyamideimide, polyperfluoroethylpropylene, tetrafluoroethylene, chlorotrifluoroethylene, cellulose propionate, cellulose acetate butyrate, methylpentene polymer, homopolyformaldehyde, acrylic resin, cellulose nitrate, ethyl cellulose, polypropylene, polysulfone, polyethersulfone, mica, a heteroisomorphous polymer, polybutene, an ionomer, an acrylic copolymer, styrene butadiene, polyvinyl chloride, urea formaldehyde, styrene acrylonitrile, and polycarbonate.
9. A magnetic optically variable pigment according to claim 1 or 2, wherein the material of the absorption layer comprises: one or an alloy of at least two of titanium, aluminum, chromium, nickel, palladium, titanium, silicon, vanadium, cobalt, iron, carbon, tin, tungsten, molybdenum, rhodium, niobium, and carbon.
10. A magnetic optically variable pigment according to claim 1 or 2, wherein the physical thickness of the absorption layer is 5nm to 100 nm.
11. The magnetic optically variable pigment according to claim 1 or 2, wherein the magnetic core layer has a single-layer structure;
the material of the magnetic core layer comprises: at least one of iron, cobalt, nickel, gadolinium, terbium, dysprosium, and erbium or an oxide of at least one or an alloy of at least two; alternatively, the first and second electrodes may be,
the material of the magnetic core layer comprises: at least one of an iron-silicon alloy, an iron-aluminum alloy, an iron-silicon-chromium alloy, and an iron-nickel-molybdenum alloy.
12. A magnetic optically variable pigment according to claim 1 or 2, characterized in that: the magnetic core layer is of a multilayer structure, and the structure of the magnetic core layer is as follows: m 1 M 0 M 2 、M 0 M 1 M 0 、M 0 M 1 、M 1 D 1 M 0 D 2 M 2 、M 0 D 1 M 1 D 2 M 0 Or M 1 D 1 M 0 Wherein M is 0 Is a magnetic film layer, M 1 And M 2 Is a metal film layer, D 1 And D 2 Is a dielectric film layer.
13. The magnetic optically variable pigment of claim 12, wherein the material of the magnetic film layer comprises: at least one of iron, cobalt, nickel, gadolinium, terbium, dysprosium and erbium or an oxide of at least one of iron, cobalt, nickel, gadolinium, terbium, dysprosium and erbium or an alloy of at least two of them, or the material of the magnetic film layer comprises at least one of an iron-silicon alloy, an iron-aluminum alloy, an iron-silicon-chromium alloy and an iron-nickel-molybdenum alloy;
the metal film layer comprises the following materials: at least one or an alloy of at least two of aluminum, silver, gold, copper, platinum, tin, titanium, palladium, rhodium, niobium, and chromium;
the material of the dielectric film layer comprises: at least one of silicon dioxide, aluminum oxide, magnesium fluoride, aluminum fluoride, cerium fluoride, lanthanum fluoride, neodymium fluoride, samarium fluoride, barium fluoride, and calcium fluoride.
14. The magnetic optically variable pigment according to claim 1 or 2, wherein a plurality of the metal nanoparticles are spaced apart from each other, and the gap between a plurality of the metal nanoparticles is 2nm to 1 mm.
15. A magnetic optically variable pigment according to claim 1 or 2, wherein the material of the metal nanoparticles comprises: at least one of aluminum, silver, gold, copper, platinum, ruthenium, palladium, rhodium, cobalt, iron, nickel, lead, osmium, and iridium, or an alloy of at least two thereof.
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