JP2005153192A - Color developing body and its manufacturing method - Google Patents
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Abstract
Description
この発明は、発色体、特に構造色を発する発色体とその製造方法に属する。 The present invention belongs to a color former, particularly a color former that emits a structural color, and a method for producing the same.
分子や固体そのものの電子的な性質により発色する色素と異なり、それ自体には色が無く光の反射、干渉、回折などの作用で発色する構造体は、紫外線による経時変化が少なく且つ光沢が出やすい等の利点を有することから、自動車の塗装方法や繊維への着色手段として期待されている。
このような発色構造体として、例えば屈折率の異なる2種の高分子物質を交互に積層した構造を有するもの(特許文献1、特許文献2)や、ラメラを備えたもの(特許文献3)が提案されている。また、発明者等も高屈折率層と低屈折率層とが交互に積層した複数の積層体を所定の間隔で基材上に平面方向に配列したものを開示した(特許文献4)。
As such a coloring structure, for example, one having a structure in which two kinds of polymer substances having different refractive indexes are alternately laminated (
しかし、特許文献1〜3で提案された発色構造体には、構造色を有する自然物として有名なモルフォチョウに匹敵するほど強く反射したり、きらきらと輝いたりするものは無い。また、特許文献4に開示された発色体の場合、隣り合う微細な積層体の間の溝を所定の幅で形成するのが困難であり、コストが高い。
それ故、この発明の課題は、モルフォチョウのように眺める角度変化によって色が緩やかに変化し、且つ緩やかな波長分散、奥行きのある色合い及び高い反射率を有する発色体を安価に提供することにある。
However, none of the color developing structures proposed in
SUMMARY OF THE INVENTION Therefore, an object of the present invention is to provide, at a low cost, a chromophore that has a gradual chromatic dispersion, a deep hue, and a high reflectivity, in which the color changes slowly according to a change in the viewing angle like a morpho butterfly. is there.
その課題を解決するために、この発明の発色体は、
一主面にX方向の幅が500nm以下でY方向に比べて均一、Y方向の長さが不定、Z方向の高さ又は深さが10nm以上の多数の平面視方形の凸部又は凹部がXY方向に配列して形成された基材と、
高い屈折率を有する高屈折率層と、低い屈折率を有する低屈折率層とが前記基材の主面に倣うようにZ方向に交互に積層された積層体と
を備えることを特徴とする。
In order to solve the problem, the color former of the present invention is
A number of planar projections or depressions having a width in the X direction of 500 nm or less, uniform in the Y direction, an indefinite length in the Y direction, and a height or depth in the Z direction of 10 nm or more on one main surface. A substrate formed by being arranged in the XY direction;
A high-refractive index layer having a high refractive index and a low-refractive index layer having a low refractive index are provided with a laminated body that is alternately laminated in the Z direction so as to follow the main surface of the substrate. .
ここで高屈折率層と低屈折率層とが基材の主面に倣うように積層されるとは、積層体のうち凸部(又は凹部)上に設けられた部分は、その最上面も凸部(凹部)となることをいう。この発明の発色体は、高屈折率層と低屈折率層とが交互に積層された積層体を有するので、入射光が各段の高屈折率層で反射し、その反射光のうち、高屈折率層及び低屈折率層の各屈折率及び厚さとによって定まる特定波長の光が干渉によって強められたり打ち消し合ったりする。即ち、高屈折率層の屈折率をn1、厚さをd1、低屈折率層の屈折率をn2、厚さをd2とするとき、波長λ=2(n1*d1+n2*d2)で定まる波長の光が選択的に強められる。 Here, the high refractive index layer and the low refractive index layer are laminated so as to follow the main surface of the substrate. The portion of the laminated body provided on the convex portion (or concave portion) is also the uppermost surface. It means that it becomes a convex part (concave part). Since the color body of the present invention has a laminate in which high refractive index layers and low refractive index layers are alternately laminated, incident light is reflected by the high refractive index layers at each stage, and among the reflected light, Light having a specific wavelength determined by the refractive index and thickness of the refractive index layer and the low refractive index layer is intensified or canceled by interference. That is, when the refractive index of the high refractive index layer is n1, the thickness is d1, the refractive index of the low refractive index layer is n2, and the thickness is d2, the wavelength is determined by wavelength λ = 2 (n1 * d1 + n2 * d2). Light is selectively enhanced.
しかも積層体の最上面のX方向の凹凸の間隔が500nm以下即ち大部分の可視光の波長より小さく且つY方向に比べて均一であるので、強められた反射光が回折効果によって空間的に広がるとともに、光波動場の膜内への侵入を制限する効果により高い反射率が得られる。よって、高い反射率を有しつつ、XZ間の角度方向から眺めると眺める角度によって色が緩やかに変化する。 In addition, since the interval between the concaves and convexes in the X direction on the top surface of the laminate is 500 nm or less, that is, smaller than the wavelength of most visible light and uniform compared to the Y direction, the enhanced reflected light spreads spatially by the diffraction effect. At the same time, a high reflectance can be obtained by the effect of limiting the penetration of the light wave field into the film. Therefore, when viewed from the angle direction between XZ while having a high reflectance, the color gradually changes depending on the viewing angle.
また、2次元全方位の乱反射による反射率低下を防止するために、前記多数の凸部又は凹部は、X方向に互いに同一の幅とし、Y方向長さがX方向の幅より大きくX方向幅の2倍以下の偏差をもつ統計分布をなすように設計することにより、配列に一次元の規則性をもたせるのが好ましい。この一次元異方性により、反射光が全方位に散乱することを防ぎ、空間的に集中して反射強度が高くなるからである。
尚、凸部又は凹部の高さ又は深さが10nmよりも小さいと積層体の最上面のレベルが近似的に同じになって回折効果による光の広がりが得られないので、Z方向の寸法を上記の通りに限定した。凸部又は凹部の高さ又は深さの上限は定めないが、通常1μm以下である。
In order to prevent a decrease in reflectance due to two-dimensional omnidirectional irregular reflection, the plurality of convex portions or concave portions have the same width in the X direction, the Y direction length is larger than the X direction width, and the X direction width. It is preferable to give the array a one-dimensional regularity by designing it so as to form a statistical distribution having a deviation equal to or less than twice. This is because the one-dimensional anisotropy prevents the reflected light from being scattered in all directions and is concentrated spatially to increase the reflection intensity.
In addition, if the height or depth of the convex portion or the concave portion is smaller than 10 nm, the level of the uppermost surface of the laminated body is approximately the same and the light spread due to the diffraction effect cannot be obtained. Limited to the above. The upper limit of the height or depth of the convex portion or the concave portion is not defined, but is usually 1 μm or less.
屈折率と波長との前記関係式で定まる波長が可視光の範囲となるように、高屈折率層の厚さを30〜120nm、低屈折率層の厚さを60〜300nmに設定するのが好ましい。各層の光学距離を同等にするために高屈折率層よりも低屈折率層を厚くするのが好ましい。基材としては積層体を所定の配列で固定できる物であれば良く、限定されない。例えば各層が後述の無機質誘電体薄膜からなる場合、基材をガラス基板とすることにより発色体を完全に固体無機材料で構成することができる。 The thickness of the high refractive index layer is set to 30 to 120 nm, and the thickness of the low refractive index layer is set to 60 to 300 nm so that the wavelength determined by the relational expression of the refractive index and the wavelength is in the visible light range. preferable. In order to make the optical distances of the respective layers equal, it is preferable to make the low refractive index layer thicker than the high refractive index layer. The substrate is not limited as long as it can fix the laminate in a predetermined arrangement. For example, when each layer is made of an inorganic dielectric thin film, which will be described later, the color former can be completely composed of a solid inorganic material by using a glass substrate as the base material.
前記高屈折率層又は低屈折率層を構成する材質としては、Al2O3、SiO2、SiO、SnO2、Sb2O3、PbCl2、PbO、TiO2、TiO、ZrO2、CeO2、CeF3、ZnS、MgO、NaF、MgF2などの無機質誘電体薄膜のうちから選ばれる1種以上からなるものが挙げられ、このように無機質で構成することで耐熱性及び耐光性が向上し、また屈折率の範囲も広がる。これらのうちで屈折率比を大きくして反射率を高めるために、高屈折率層がCeO2、PbO、Sb2O3、PbCl2、TiO2、ZnS、低屈折率層がSiO2、MgF2の組み合わせが好ましい。また、各屈折率層は、PMMA、CR−39、MMA、ポリアリルメタクリレート、ポリジアリルフタレート、ポリカーボネート、ポリスチレン、ポリビニルナフタレンなどの合成樹脂膜のうちから選ばれる1種以上であってもよい。
更に前記積層体と基材との間に光吸収体が形成されていると、特定波長の光のみを吸収するので、色合いを変化させることができる。更に、その光吸収体をアルミニウム、金、銅、クロムなどからなる金属薄膜とすると、反射光に光沢が加わる。
Examples of the material constituting the high refractive index layer or the low refractive index layer include Al 2 O 3 , SiO 2 , SiO, SnO 2 , Sb 2 O 3 , PbCl 2 , PbO, TiO 2 , TiO, ZrO 2 , and CeO 2. , CeF 3 , ZnS, MgO, NaF, MgF 2 and other inorganic dielectric thin films are selected from the above, and the heat resistance and light resistance can be improved by using inorganic material. In addition, the range of refractive index is expanded. Among these, in order to increase the refractive index ratio and increase the reflectance, the high refractive index layer is CeO 2 , PbO, Sb 2 O 3 , PbCl 2 , TiO 2 , ZnS, and the low refractive index layer is SiO 2 , MgF. A combination of 2 is preferred. Each refractive index layer may be one or more selected from synthetic resin films such as PMMA, CR-39, MMA, polyallyl methacrylate, polydiallyl phthalate, polycarbonate, polystyrene, and polyvinyl naphthalene.
Furthermore, when a light absorber is formed between the laminate and the base material, only light of a specific wavelength is absorbed, so that the hue can be changed. Further, when the light absorber is a metal thin film made of aluminum, gold, copper, chromium, etc., gloss is added to the reflected light.
この発明の発色体を製造する適切な方法は、
基材の一主面に、X方向の幅が500nm以下でY方向に比べて均一、Y方向の長さが不定、Z方向の高さ又は深さが10nm以上の多数の平面視方形の凸部又は凹部をXY方向に配列して形成する工程と、
前記基材の主面に、高い屈折率を有する高屈折率層と、低い屈折率を有する低屈折率層とをZ方向に交互に積層する工程と
を備えることを特徴とする。
この方法によれば、高屈折率層と低屈折率層とが基材の主面に倣って凹凸をなすように積層される。前記各凸部又は凹部のY方向の長さは乱数を用いて決定するとよい。
A suitable method for producing the color former of this invention is:
On one main surface of the substrate, a number of square-shaped projections having a width in the X direction of 500 nm or less, uniform compared to the Y direction, an indefinite length in the Y direction, and a height or depth in the Z direction of 10 nm or more. Forming a portion or a recess in an XY direction; and
And a step of alternately laminating a high refractive index layer having a high refractive index and a low refractive index layer having a low refractive index on the main surface of the base material in the Z direction.
According to this method, the high-refractive index layer and the low-refractive index layer are laminated so as to be uneven according to the main surface of the substrate. The length of each convex portion or concave portion in the Y direction may be determined using a random number.
以上のように、この発明の発色体によれば、モルフォチョウのごとくある波長領域の色を主体としつつバンド幅を有する、奥行きのある色合いを発し、高い反射率を有するのでデザイン性に優れ、各種デザイン分野で有益である。 As described above, according to the color body of the present invention, the color has a bandwidth while having mainly a color in a certain wavelength region like a morpho butterfly, emits a hue with a depth, and has high reflectivity, so it has excellent designability. Useful in various design fields.
この発明の実施形態を図面と共に説明する。図1は実施形態の発色体に用いる基材をX軸に沿って切断したところを示す断面図、図2はその発色体を示す断面図である。
発色体を製造するには、先ず平坦な主面を有する基材1を準備し、その主面をフォトリソ技術で図1に示すように凹凸に加工する。この凹凸は、X方向に一様な幅d、Y方向にはdを下限とするばらつきを有するように形成する。従って、平面視ではX方向の長さがdで種々のアスペクト比を有する縦長の四辺形がY方向を向いて多数配列していることになる。図1で幅が2d、3dをなす凹凸が見られるのは、この断面において隣接する凸部同士あるいは凹部同士が連なっていることを示す。凹凸のY方向長さ及び配列は、電子ビーム描画にて、高さ(深さ)はエッチング時間等のエッチング条件にて実現可能である。エッチングはドライエッチングが良い。
次に、高屈折率層2及び低屈折率層3を交互に電子ビーム蒸着し、最上層を高屈折率層2とする。こうして発色体10が得られる。
An embodiment of the present invention will be described with reference to the drawings. FIG. 1 is a cross-sectional view showing a substrate used for the color body of the embodiment cut along the X axis, and FIG. 2 is a cross-sectional view showing the color body.
In order to produce a color body, first, a
Next, the high-
図1における基材1として厚さ1.1mmの石英ガラス基板を準備した。この基板の一主面にフォトレジスト(住友化学工業株式会社製NEB−22A2)を塗布し、加熱硬化した。その後、帯電防止剤(昭和電工株式会社製エスペイサー300N2)を塗布し、加熱硬化した。別途、X方向寸法が0.3μmで一様、Y方向寸法が2.0μmを中心とする標準偏差0.5μmの正規分布をなす多数の長方形がXY2次元面内に乱数配置された擬1次元的パターンを電子ビーム描画装置(日本電子株式会社製JBX−5000SI)に記憶させた。そして、記憶したパターンに従って上記のフォトレジストに電子ビームを照射した。電子ビームの加速電圧は50kV、描画電流値は100pA、照射電子ビーム量は4.75μC/cm2とした。露光及び現像後、エッチング装置(アルバック社製NLD−800)にてドライエッチングすることにより、高さ(又は深さ)0.34μmの凹凸を形成した。残ったフォトレジストを除去することにより基材1を得た。得られた基材1の上記主面をX軸に対して直交し、Y軸及びZ軸に対して鋭角をなす方向から眺めた電子顕微鏡写真を図3に示す。
A quartz glass substrate having a thickness of 1.1 mm was prepared as the
次に、高屈折率層2として酸化チタン、低屈折率層3として酸化ケイ素を各々電子ビーム蒸着した。各層の厚さ及び層数は高屈折率層2が厚さ80nmのものを合計7層、低屈折率層3が厚さ150nmのものを合計7層とした。
こうして得られた発色体に白色光を垂直入射し、反射強度の角度依存性をステッピングモータ回転ステージ(オリエンタルモーター社製PK245−01A)付きのCCD分光器システム(Ocean Optics 社製USB2000)で測定した。測定結果を図4に示す。図4に見られるように、垂直方向への反射は560nmが最も強いが、この波長は5度を超えた途端に弱くなった。それに対して520nm以下の波長の光は垂直方向へはほとんど反射しないが、8度付近で強く反射した。実際に肉眼で観察したところ、垂直から10度前後まで基板が青色に輝いて見えた。また、異方性も再現された。
Next, titanium oxide was deposited as the high
White light was vertically incident on the color former thus obtained, and the angle dependence of the reflection intensity was measured with a CCD spectrometer system (USB2000 manufactured by Ocean Optics) equipped with a stepping motor rotating stage (PK245-01A manufactured by Oriental Motor Co.). . The measurement results are shown in FIG. As can be seen in FIG. 4, the reflection in the vertical direction is the strongest at 560 nm, but this wavelength became weak as soon as it exceeded 5 degrees. In contrast, light having a wavelength of 520 nm or less hardly reflected in the vertical direction, but strongly reflected in the vicinity of 8 degrees. When actually observed with the naked eye, the substrate appeared to shine in blue from the vertical to around 10 degrees. Anisotropy was also reproduced.
この発明の発色体によれば、様々な方向から眺めても特定の色を輝かせることができるので、装飾や塗装などの分野での利用が期待される。さらに、酸化物や人工樹脂を多層膜に用いた場合、耐熱性、強度などにおいて、たんぱく質でできた自然の発色体にはない長所を有することができる。 According to the color body of the present invention, it is possible to make a specific color shine even when viewed from various directions, so that it is expected to be used in fields such as decoration and painting. Furthermore, when an oxide or an artificial resin is used for the multilayer film, it can have advantages in heat resistance, strength, etc. that are not found in natural color bodies made of protein.
基材 1
高屈折率層 2
低屈折率層 3
High
Low
Claims (7)
高い屈折率を有する高屈折率層と、低い屈折率を有する低屈折率層とが前記基材の主面に倣うようにZ方向に交互に積層された積層体と
を備えることを特徴とする発色体。 A number of planar projections or depressions having a width in the X direction of 500 nm or less, uniform in the Y direction, an indefinite length in the Y direction, and a height or depth in the Z direction of 10 nm or more on one main surface. A substrate formed by being arranged in the XY direction;
A high-refractive index layer having a high refractive index and a low-refractive index layer having a low refractive index are provided with a laminated body that is alternately laminated in the Z direction so as to follow the main surface of the substrate. Colored body.
前記基材の主面に、高い屈折率を有する高屈折率層と、低い屈折率を有する低屈折率層とをZ方向に交互に積層する工程と
を備えることを特徴とする請求項1〜5のいずれかに記載の発色体の製造方法。 On one main surface of the substrate, a number of square-shaped projections having a width in the X direction of 500 nm or less, uniform compared to the Y direction, an indefinite length in the Y direction, and a height or depth in the Z direction of 10 nm or more. Forming a portion or a recess in an XY direction; and
The main surface of the substrate comprises a step of alternately laminating a high refractive index layer having a high refractive index and a low refractive index layer having a low refractive index in the Z direction. 6. A method for producing a color former according to any one of 5 above.
The method according to claim 6, wherein the length of each convex part or concave part in the Y direction is determined by a random number.
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