CN107523139A - A kind of photonic crystal color inks and application - Google Patents
A kind of photonic crystal color inks and application Download PDFInfo
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- CN107523139A CN107523139A CN201710991747.1A CN201710991747A CN107523139A CN 107523139 A CN107523139 A CN 107523139A CN 201710991747 A CN201710991747 A CN 201710991747A CN 107523139 A CN107523139 A CN 107523139A
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- photonic crystal
- color inks
- color
- crystal color
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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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- 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
- C09D11/16—Writing inks
-
- 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
- C09D11/30—Inkjet printing inks
- C09D11/38—Inkjet printing inks characterised by non-macromolecular additives other than solvents, pigments or dyes
-
- 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
- C09D11/30—Inkjet printing inks
- C09D11/40—Ink-sets specially adapted for multi-colour inkjet printing
Abstract
The present invention provides a kind of photonic crystal color inks, including photonic crystal particle and solvent；The photonic crystal particle is that Surface coating has SiO2The particles of magnetic material of layer；The particles of magnetic material is shaped as elliposoidal, bar-shaped, spherocylinder or round platform.The color of color inks in the present invention is shown that different structural cycles shows different colours by the schemochrome of its three-D photon crystal formed.Control the structural cycle of three-D photon crystal to produce continuity by externally-applied magnetic field to change, so that ink obtains different color, and color gamut is wide and continuously adjustabe, can show from purple, blueness, green, yellow, orange, red etc..Present invention also offers a kind of application of photonic crystal color inks.
Description
Technical field
The invention belongs to new material and photonic crystal technical field, more particularly to a kind of photonic crystal color inks and should
With.
Background technology
Photonic crystal (Photonic Crystal) be 1987 by S.John and E.Yablonovitch independently
It is proposed, be the artificial micro-structure formed by the medium period arrangement of different refractivity.Photonic crystal is forbidden photon band material, from
Seen on material structure, photonic crystal is the crystalline substance of a kind of engineer on optics yardstick with periodic dielectric structures and manufacture
Body.Similar with modulation of the semiconductor lattice to electron wave function, photonic bandgap material can modulate the electricity with respective wavelength
Magnetic wave --- when electromagnetic wave is propagated in photonic bandgap material, electromagnetic wave energy modulated due to Bragg diffraction be present
Form band structure.Band gap, i.e. photon band gap can occur between band and energy band.Had energy is in the photon in photon band gap,
The crystal can not be entered.Photonic crystal and semiconductor have many similarities on basic model and Research Thinking, in principle people
The purpose of control photon motion by designing and manufacture photonic crystal and its device, can be reached.Photonic crystal (also known as photon
Forbidden band material) appearance, make it possible people manipulate and control photon dream.Briefly, photonic crystal has wavelength
The function of selection, it can selectively make the light of some wave band by preventing the light of other wavelength from passing through wherein.
The property of this structure control reflection wavelength is applicable as colored display, sensing, wave filter etc..The application is by light
Sub- crystal carries out colour writing, printing as ink.Now contrast prior art：
1) conventional color ink：
Mainly include paint ink and dye ink.Dyestuff is water-base ink, and its advantage is：Ink gun, color will not be blocked
Color gorgeous, cost is low；Shortcoming is：Non-watertight, irradiation dyestuff can be decomposed so as to fade under light.Pigment is oily ink, and its is excellent
Point is that fading rate is slow, and will not spread and sink in ink, more water-fast；Its shortcoming is that print surface is uneven, and image is matt, and cost is higher.
2) photon ink：
The characteristics of having benefited from structure coloring, photon ink have many advantages relative to conventional inks, e.g., can the holding time more
Length is not faded, will not dazzle etc. under strong illumination.As SuliWu is reported with different size CdS beads printing false-proof icons
(J.Phys.Chem.Lett.2017,8,2835)；Yanlin Song report to be entered by the use of different size PS beads as ink
Row printing (ACS Appl.Mater.Interfaces 2014,6,13344, J.Mater.Chem., 2009,19,5499).
But above-mentioned photon ink has the following disadvantages：A kind of particle of size is only capable of displaying a kind of color, if will
Doing multi-color just needs to prepare various sizes of particle ink, and color is discontinuous, is only capable of displaying several specific colors.
The content of the invention
It is an object of the invention to provide a kind of photonic crystal color inks and application, a kind of light of size in the present invention
Sub- crystal color ink can show multiple color, and all inorganic material of raw material.
The present invention provides a kind of photonic crystal color inks, including photonic crystal particle and solvent；
The photonic crystal particle is that Surface coating has SiO2The particles of magnetic material of layer；
The particles of magnetic material is shaped as elliposoidal, bar-shaped, spherocylinder or round platform.
Preferably, the major axis dimension of the particles of magnetic material is 100~200nm；
The minor axis dimension of the particles of magnetic material is 20~50nm.
Preferably, the magnetic material is Fe3O4、γ-Fe2O3, Ni, the one or more in Co and Fe.
Preferably, the mass fraction of the photonic crystal color inks is 10~30%.
Preferably, the SiO2The thickness of layer is 15~100nm.
Preferably, the solvent is the one or more in water, ethanol and ethylene glycol.
The present invention provides a kind of application of photonic crystal color inks, it is characterised in that by above-mentioned photonic crystal color ink
Water is write under magnetic field, by controlling magnetic direction to obtain different colours during drying.
Preferably, the intensity in the magnetic field is 100~2000 Gausses.
Preferably, the temperature of the drying is 10~80 DEG C.
The present invention provides a kind of photonic crystal color inks, including photonic crystal particle and solvent；The photonic crystal
Grain has SiO for Surface coating2The particles of magnetic material of layer；The particles of magnetic material is shaped as elliposoidal, bar-shaped, spherocylinder
Or round platform.The color of color inks in the present invention shows by the schemochrome of its three-D photon crystal formed, different structures
Cycle shows different colours.Control the structural cycle of three-D photon crystal to produce continuity by externally-applied magnetic field to change, so that
Ink obtains different color, and color gamut is wide and continuously adjustabe, from purple, blueness, green, yellow, orange, red etc.
It can show.
In addition, the photonic crystal color inks in the present invention have further the advantage that：
A kind of particle can realize multiple color；Color continuously adjustabe, covering total visible light spectrum；It is colour-fast；Recyclable repetition
Utilize；Ink is full-inorganic material, and component (iron, silicon, oxygen) is non-toxic；It is assembled into three-D photon crystal, bright-colored,
It is bright；Writing is easy, it is only necessary to is dried under magnetic field；It is simple to form different colours manipulation, it is only necessary to change magnetic direction；Can be in difference
Write or print on material.
Brief description of the drawings
In order to illustrate more clearly about the embodiment of the present invention or technical scheme of the prior art, below will be to embodiment or existing
There is the required accompanying drawing used in technology description to be briefly described, it should be apparent that, drawings in the following description are only this
The embodiment of invention, for those of ordinary skill in the art, on the premise of not paying creative work, can also basis
The accompanying drawing of offer obtains other accompanying drawings.
Fig. 1 is the colour developing principle of photonic crystal color inks in the present invention；
Fig. 2 is elliposoidal α-Fe in the embodiment of the present invention 22O3The TEM pictures of particle；
Fig. 3 is SiO in the embodiment of the present invention 22Coat Fe3O4Ellipsoidal particle TEM pictures；
Fig. 4 is the writing effect of the ink inside of the embodiment of the present invention 2；
Fig. 5 is the wavelength corresponding to two kinds of colors in Fig. 4 of the present invention.
Embodiment
The invention provides a kind of photonic crystal color inks, including photonic crystal particle and solvent；
The photonic crystal particle is that Surface coating has SiO2The particles of magnetic material of layer；
The particles of magnetic material is shaped as elliposoidal, bar-shaped, spherocylinder or round platform.
This application provides one kind writing, printing color inks, it is used as light using having magnetic anisotropic particle
Sub- crystal color ink, the theory of different colours is obtained especially by regulation and control externally-applied magnetic field direction.Ink-manufacturing method letter
Just, nontoxic, cost is low, easy prepare with scale.
In the present invention, the magnetic material is preferably Fe3O4、γ-Fe2O3, Ni, the one or more in Co and Fe；Institute
It is the three-dimensional shape with major axis and short axle to state magnetic material, can be elliposoidal, bar-shaped, spherocylinder or round platform e.g.；The magnetic
The major axis of property material granule is preferably dimensioned to be 100~200nm, more preferably 150~160nm；The particles of magnetic material
Short axle is preferably dimensioned to be 20~50nm, more preferably 30~40nm.
In the present invention, the color of the photonic crystal color inks is shown by the schemochrome of its three-D photon crystal formed
Show, different structural cycles shows different colours.As shown in Figure 1, Fig. 1 is photonic crystal color inks in the present invention to its principle
Colour developing principle.Externally-applied magnetic field can control the orientation of magnetic ellipsoidal particle (major axis of particle can be along magnetic direction).Not
The ink dried under equidirectional magnetic field, the structure of different cycles can be formed.Application level magnetic field, angle magnetic field and perpendicular magnetic place
The periodic structure that can be formed is respectively d1, d2 and d3, and the most short cycle that d1 can be formed for this particles of ink, d3 are most long week
Phase.One corresponding relation is had according to this periodic structure of Bragg equation and wavelength：(λ is diffraction wavelength to λ=2ndsin θ, and n is folding
Rate, d interplanar distances are penetrated, θ is Bragg angle).The periodic structure of formation is different, so different colours are shown, the ripple of color
Long λ and the positive correlation of cycle d.Different colours can be obtained so as to apply different directions magnetic field in ink curing processes.Color gamut
Wide and continuously adjustabe, can show from purple, blueness, green, yellow, orange, red etc..
In the present invention, the SiO2The thickness of layer is preferably 15~100nm, more preferably 30~80nm, is most preferably
40~70nm, specifically, can be 60nm or 65nm in an embodiment of the present invention.The SiO2Layer has equilibrium magnetism
Function, particles of magnetic material non-agglomerate under the influence of a magnetic field can be made, still be able to it is dispersed in a solvent.
In the present invention, the solvent is preferably the one or more in water, ethanol and ethylene glycol.The photonic crystal is color
The mass fraction of chromatic ink is preferably 10~30%, and more preferably 15~25%.
In the present invention, the photonic crystal particle is photonic crystal particle described in the homogeneous monodisperse particles of dimensional height
Major axis be preferably dimensioned to be 150~350nm, more preferably 220~300nm；The size of the short axle of the photonic crystal particle
Preferably 50~200nm, more preferably 120~180nm.In the present invention, the particles of magnetic material is preferably according to document
J.Am.Chem.Soc.2012, the method that molysite is hydrolyzed in 134,11864-11867 are prepared, and e.g., chlorine are hydrated by 0.7 gram six
Change iron and 3.5 milligrams of sodium dihydrogen phosphates are dissolved in 200 milliliters of water, 2 days are stood in 100 degree of baking ovens, can obtain size as length
Axle 150nm, short axle 40nm elliposoidal α-Fe2O3Particle, by the composition and reaction temperature that adjust reaction solution, you can obtain
Different sizes, particles of magnetic material of different shapes.
Present invention preferably employs stober methods SiO is wrapped up on the particles of magnetic material surface2Layer, is concretely comprised the following steps：On
Particles of magnetic material is stated after centrifuge washing, takes 50 milligrams to be scattered in 30 milliliters of ethanol, then 5 milliliters of water and 2 millis are added to it
Ammoniacal liquor is risen, 2000 microlitres of tetraethyl orthosilicate is added under agitation and (adds in ten times, 200 microlitres every time, be spaced 30 points
Clock), you can SiO thick parcel 60nm2Layer.
Then above-mentioned product is collected by centrifugation, after 60 degree of oven dried overnights, be positioned in hydrogen under 400 degrees Celsius also
Original, makes particle have magnetic, and size does not change.A certain amount of solvent is added thereto, and this hair is obtained after ultrasonic disperse
Photonic crystal ink in bright.
Present invention also offers a kind of application of photonic crystal color inks, by above-mentioned photonic crystal color inks in magnetic field
Lower writing, in the drying process by controlling the direction in magnetic field to obtain different colours.
In the present invention, the magnetic field can be provided by magnet or electromagnet, and the intensity in the magnetic field is preferably 100~
2000 Gausses, more preferably 300~1800 Gausses, most preferably 500~1500 Gausses；The temperature of the drying can be room
Arbitrary temp in the range of temperature, or 10~80 DEG C, preferably 20~70 DEG C, most preferably 25~50 DEG C.
Prepared monodispersed ellipsoidal particle is scattered in the mixed liquor of water or water and ethanol by the application, as ink
Water, magnetic ellipsoid particle solution is written on paper by writing implements such as pen, writing brushes, or utilizes ink jet printing device by ellipsoid
Particle solution is printed on paper, by additional different magnetic field, it is shown different structure color in the drying process.Also can incite somebody to action
Miniature magnet is integrated on ink-jet printer, is controlled magnetic direction using computer program, is obtained more fine color printing effect.
The present invention provides a kind of photonic crystal color inks, including photonic crystal particle and solvent；The photonic crystal
Grain has SiO for Surface coating2The particles of magnetic material of layer；The particles of magnetic material is shaped as elliposoidal, bar-shaped, spherocylinder
Or round platform.The color of color inks in the present invention shows by the schemochrome of its three-D photon crystal formed, different structures
Cycle shows different colours.Control the structural cycle of three-D photon crystal to produce continuity by externally-applied magnetic field to change, so that
Ink obtains different color, and color gamut is wide and continuously adjustabe, from purple, blueness, green, yellow, orange, red etc.
It can show.
In addition, the photonic crystal color inks in the present invention have further the advantage that：
A kind of particle can realize multiple color；Color continuously adjustabe, covering total visible light spectrum；It is colour-fast；Recyclable repetition
Utilize；Ink is full-inorganic material, and component (iron, silicon, oxygen) is non-toxic；It is assembled into three-D photon crystal, bright-colored,
It is bright；Writing is easy, it is only necessary to is dried under magnetic field；It is simple to form different colours manipulation, it is only necessary to change magnetic direction；Can be in difference
Write or print on material.
In order to further illustrate the present invention, with reference to embodiments to a kind of photonic crystal color inks provided by the invention
And its application is described in detail, but limiting the scope of the present invention can not be understood as.
Embodiment 1
Method by hydrolyzing molysite, 0.7 gram of ferric chloride hexahydrate and 3.5 milligrams of sodium dihydrogen phosphates are dissolved in 200 millis
Rise in water, 2 days are stood in 100 degree of baking ovens, obtain size as 150 nanometers of major axis, the elliposoidal α-Fe of 40 nanometers of short axle2O3
Particle.The silica of 65 nanometer thickness is wrapped up using stober methods, detailed process is：α-Fe2O3After centrifuge washing, 50 milligrams are taken
It is scattered in 30 milliliters of ethanol, then 5 milliliters of water and 2 milliliters of ammoniacal liquor is added to it, adds tetraethyl orthosilicate under agitation
2000 microlitres (adding in ten times, 200 microlitres every time, be spaced 30 minutes), are collected by centrifugation, after 60 degree of oven dried overnights, put
It is placed in hydrogen and is restored to Fe under 400 degrees Celsius3O4@SiO2, make particle that there is magnetic, size does not change to be received for major axis 280
The ellipsoidal particle of 170 nanometers of short axle of rice.A certain amount of water (granular mass fraction be 15%) is added thereto, after ultrasonic disperse
I.e. arrive ink.Write under different magnetic field, the word of the color of blueness, green, red etc. can be write out.
Embodiment 2
Method by hydrolyzing molysite, after the composition of regulation reaction solution, size is obtained as 100 nanometers of major axis, short axle
50 nanometers of elliposoidal α-Fe2O3Particle, after the silica of 60 nanometer thickness is wrapped up, it is restored in hydrogen under 400 degrees Celsius
Fe3O4@SiO2, make particle that there is magnetic, size does not change as the ellipsoidal particle of 220 nanometers of major axis, 170 nanometers of short axle.
A certain amount of water (granular mass fraction is 15%) is added thereto, and be after ultrasonic disperse arrives ink.The book under different magnetic field
Write, the word of the color of blueness, cyan, green etc. can be write out.
Fig. 2 is elliposoidal α-Fe in the embodiment of the present invention 22O3The TEM pictures of particle, major axis 100nm, short axle 50nm.
Fig. 3 is SiO in the embodiment of the present invention 22Coat Fe3O4Ellipsoidal particle TEM pictures, SiO2Thickness is received for 60
Rice, particle entirety major axis are 220 nanometers, and short axle is 170 nanometers.
Fig. 4 is the writing effect of the ink inside of the embodiment of the present invention 2.Wherein, " S " letter in left side be in the horizontal direction, 500
Writing obtains under the magnetic field of gaussian intensity, for blueness；" U " letter on right side be vertical direction, 500 gaussian intensities magnetic field under
Writing obtains, for green.
Fig. 5 is the wavelength corresponding to two kinds of colors in Fig. 4 of the present invention, and blue " S " letter is 450nm, green " U " word
Mother is 550nm.
Embodiment 3
Method by hydrolyzing molysite, after the composition of regulation reaction solution and reaction temperature, it is major axis to obtain size
200 nanometers, the bar-shaped FeOOH particles of 20 nanometers of short axle, after the silica of 60 nanometer thickness is wrapped up, 350 is Celsius in hydrogen
Fe is restored under degree3O4@SiO2, make particle that there is magnetic, size does not change as the ellipse of 320 nanometers of major axis, 140 nanometers of short axle
Spheric granules.A certain amount of water (granular mass fraction is 15%) is added thereto, and be after ultrasonic disperse arrives ink.In difference
Write under magnetic field, the word of the color of purple, green, red etc. can be write out.
Described above is only the preferred embodiment of the present invention, it is noted that for the ordinary skill people of the art
For member, under the premise without departing from the principles of the invention, some improvements and modifications can also be made, these improvements and modifications also should
It is considered as protection scope of the present invention.
Claims (9)
1. a kind of photonic crystal color inks, including photonic crystal particle and solvent；
The photonic crystal particle is that Surface coating has SiO2The particles of magnetic material of layer；
The particles of magnetic material is shaped as elliposoidal, bar-shaped, spherocylinder or round platform.
2. photonic crystal color inks according to claim 1, it is characterised in that the major axis chi of the particles of magnetic material
Very little is 100~200nm；
The minor axis dimension of the particles of magnetic material is 20~50nm.
3. photonic crystal color inks according to claim 1, it is characterised in that the magnetic material is Fe3O4、γ-
Fe2O3, Ni, the one or more in Co and Fe.
4. photonic crystal color inks according to claim 1, it is characterised in that the matter of the photonic crystal color inks
It is 10~30% to measure fraction.
5. photonic crystal color inks according to claim 1, it is characterised in that the SiO2The thickness of layer for 15~
100nm。
6. photonic crystal color inks according to claim 1, it is characterised in that the solvent is water, ethanol and second two
One or more in alcohol.
7. a kind of application of photonic crystal color inks, it is characterised in that by the photon described in claim 1~6 any one
Crystal color ink is write under magnetic field, by controlling magnetic direction to obtain different colours during drying.
8. application according to claim 7, it is characterised in that the intensity in the magnetic field is 100~2000 Gausses.
9. application according to claim 7, it is characterised in that the temperature of the drying is 10~80 DEG C.
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Cited By (7)
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| CN108803089A (en) * | 2018-06-08 | 2018-11-13 | 苏州大学 | A kind of SMART OPTICS and preparation method thereof and application |
| CN109435514A (en) * | 2018-10-24 | 2019-03-08 | 中丰田光电科技(珠海)有限公司 | A kind of production technology and radium-shine material of aluminizing laser material |
| CN110109197A (en) * | 2018-05-14 | 2019-08-09 | 广东聚华印刷显示技术有限公司 | Photon crystal material and preparation method thereof and photonic crystal ink and its application |
| CN111464696A (en) * | 2020-03-31 | 2020-07-28 | Oppo广东移动通信有限公司 | Information prompting method and device, storage medium and full-screen electronic equipment |
| CN111484769A (en) * | 2019-05-14 | 2020-08-04 | 广东聚华印刷显示技术有限公司 | Composite material, method for preparing same, ink containing same, and film forming method |
| CN113416450A (en) * | 2021-07-05 | 2021-09-21 | 中钞印制技术研究院有限公司 | Anti-counterfeiting ink and preparation method thereof, anti-counterfeiting layer and preparation method thereof |
| CN113442618A (en) * | 2020-03-24 | 2021-09-28 | 鹰酷斯达有限公司 | Photonic crystal color printing method and photonic crystal color printed matter |
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| CN110109197A (en) * | 2018-05-14 | 2019-08-09 | 广东聚华印刷显示技术有限公司 | Photon crystal material and preparation method thereof and photonic crystal ink and its application |
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| CN108803089B (en) * | 2018-06-08 | 2021-11-05 | 苏州大学 | Intelligent optical material and preparation method and application thereof |
| CN109435514A (en) * | 2018-10-24 | 2019-03-08 | 中丰田光电科技(珠海)有限公司 | A kind of production technology and radium-shine material of aluminizing laser material |
| CN111484769A (en) * | 2019-05-14 | 2020-08-04 | 广东聚华印刷显示技术有限公司 | Composite material, method for preparing same, ink containing same, and film forming method |
| CN113442618A (en) * | 2020-03-24 | 2021-09-28 | 鹰酷斯达有限公司 | Photonic crystal color printing method and photonic crystal color printed matter |
| CN113442618B (en) * | 2020-03-24 | 2023-06-30 | 鹰酷斯达有限公司 | Photonic crystal color printing method and photonic crystal color printed matter |
| CN111464696A (en) * | 2020-03-31 | 2020-07-28 | Oppo广东移动通信有限公司 | Information prompting method and device, storage medium and full-screen electronic equipment |
| CN113416450A (en) * | 2021-07-05 | 2021-09-21 | 中钞印制技术研究院有限公司 | Anti-counterfeiting ink and preparation method thereof, anti-counterfeiting layer and preparation method thereof |
| CN113416450B (en) * | 2021-07-05 | 2022-11-04 | 中钞印制技术研究院有限公司 | Anti-counterfeiting ink and preparation method thereof, anti-counterfeiting layer and preparation method thereof |
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