WO2003042325A1 - Materiau fonctionnel optique utilisant des complexes des terres rares et dispositif emetteur de lumiere - Google Patents

Materiau fonctionnel optique utilisant des complexes des terres rares et dispositif emetteur de lumiere Download PDF

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Publication number
WO2003042325A1
WO2003042325A1 PCT/JP2002/011748 JP0211748W WO03042325A1 WO 2003042325 A1 WO2003042325 A1 WO 2003042325A1 JP 0211748 W JP0211748 W JP 0211748W WO 03042325 A1 WO03042325 A1 WO 03042325A1
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Prior art keywords
complex
group
light
emitting device
formula
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PCT/JP2002/011748
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English (en)
Japanese (ja)
Inventor
Yasuchika Hasegawa
Shozo Yanagida
Yuji Wada
Junichi Shimada
Yoichi Kawakami
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Kansai Technology Licensing Organization Co., Ltd.
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Publication of WO2003042325A1 publication Critical patent/WO2003042325A1/fr

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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
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
    • C09K11/06—Luminescent, e.g. electroluminescent, chemiluminescent materials containing organic luminescent materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/50—Wavelength conversion elements
    • H01L33/501—Wavelength conversion elements characterised by the materials, e.g. binder
    • H01L33/502—Wavelength conversion materials
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02B—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO BUILDINGS, e.g. HOUSING, HOUSE APPLIANCES OR RELATED END-USER APPLICATIONS
    • Y02B20/00—Energy efficient lighting technologies, e.g. halogen lamps or gas discharge lamps

Definitions

  • the present invention relates to a light emitting device in which an optical functional material composed of a wavelength conversion material containing an organic phosphor composed of a rare earth complex is combined with a light emitting diode or a semiconductor laser that excites the organic phosphor.
  • the light emitting device according to the present invention can be used as a white light source having high color rendering properties or a light emitting device capable of emitting an arbitrary color.
  • LEDs light-emitting diodes
  • RGB red
  • G green
  • B blue
  • the display color is arbitrarily controlled by the intensity ratio of each RGB color.
  • LEDs still have many problems when viewed as lighting devices rather than as display devices.
  • white light can be obtained by using a device in which RGB LED light emitters are arranged and setting the intensity ratio of each RGB color appropriately, but when viewed as a lighting device, a conventional lighting device Compared with incandescent lamps and fluorescent lamps, (1) when you look closely, you can see the mixture of the three primary colors, (2) you must control each RGB color independently, (3) the device becomes a dog (4) Poor color rendering properties.
  • color rendering refers to the nature of the light source, such as what color the object looks like when the object is illuminated by the light source.
  • CIE Commission Internationale de l'Eclairage, International Commission on Illumination
  • a perfect radiator is used for color temperatures of 5000K or less, and a calculated value of the spectral distribution of daylight (referred to as synthetic daylight) is used for temperatures exceeding 5000K.
  • synthetic daylight a calculated value of the spectral distribution of daylight
  • eight colors having a predetermined spectral reflectance are selected for general use, and the color rendering index calculated by this is called an average color rendering index.
  • seven colors are selected for special purposes, including the Japanese skin color.
  • the color rendering index calculated in this way is called a special color rendering index.
  • Lighting Engineering (edited by The Institute of Electrical Engineers of Japan, published by Ohmsha, p. 36). ) Is close to the light of a perfect radiator.
  • the light emitted by the perfect radiator includes light of each wavelength continuously. Since the color of the object is determined by the light reflectance (spectral reflectance) for each wavelength of the object, light of each wavelength is continuously included in the spectral distribution of the illumination light (luminous body), and However, if the intensity distribution is close to that of a perfect radiator, the color appearance of the object will be similar to that under natural light. However, even if the LED white light emitter composed of RGB emits white light as a whole by adjusting the intensity ratio of each color, its spectral distribution is not continuous, and R (red), G ( It is discontinuous with narrow peaks only at three wavelengths, green (green) and B (blue). Due to this discontinuity, RGB-LED emitters cannot have sufficient color rendering properties as lighting devices.
  • a gallium nitride blue LED covered (or coated) with a YAG phosphor As a light source for white illumination using a single LED, a gallium nitride blue LED covered (or coated) with a YAG phosphor has been devised (see Japanese Patent Application Laid-Open No. 5-152609). This is because the YAG phosphor is photo-excited using blue light (wavelength 46 Onm) from the InGaN active layer of a gallium nitride blue LED, and the color mixture of the yellow emission, which is the fluorescence from the phosphor, and the blue from the LED. To obtain white light.
  • blue light wavelength 46 Onm
  • YAG phosphor white LED made of coated gallium nitride blue LED (correlated color temperature: 6500K) and scan Bae spectrum of a standard light D 65 (correlated color temperature: 6504 K) shows the scan Bae spectrum of You.
  • the standard light D 65 a color rendering index for a standard light representing the daylight color temperature 6504 K
  • Figure 2 shows the performance of the white LED. Although the color evaluation numbers are shown, it can be seen that the special color rendering numbers for blue-violet, green, and red are inferior to the spectral distribution. Therefore, it is necessary to reinforce the spectral components required in some fields to improve the color rendering of the object.
  • the color temperature can be controlled by increasing the amount of YAG phosphor applied and changing the light-emitting component (emission amount) from the phosphor. (See Figure 5).
  • the color temperature around 6500K which is often used at present, there are the following two problems in lowering the color temperature by increasing the number of light emitting components from the phosphor.
  • the YAG phosphor Since the YAG phosphor has a strong yellow component and a weak red color component, it has an unnatural white color with a strong yellow color and poor red color rendering.
  • the white LED was difficult to distinguish between arteries (clear red) and venous blood vessels (dark red) during the above operation. This is due to the problem of the color rendering properties of the used white LEDs in the red region, and by increasing the spectrum in the reddish orange of 597 to 640 nm and the red region of 640 to 780 nm. It can be resolved.
  • the easiest way to increase the spectrum in the red region without causing the above problems is to apply a phosphor emitting in the red region to a current white LED.
  • the red phosphor has high efficiency but high stability.
  • 11-62298 Japanese Patent Application No.2000- 256251). These complexes are stable even at a high temperature of 350 ° C, and are unlikely to undergo photodegradation, and overturn the conventional wisdom that organic compounds are easily degraded by heat or light irradiation. In addition, it has high affinity with resin-based host materials such as plastics and polymers, and is expected to be a next-generation optical device in combination with easy processability.
  • the present invention has realized a white light-emitting device having high color rendering properties by first selecting and using a substance suitable for the purpose among these complexes.
  • the present invention is not limited to a simple white light emitting device, and may be a device that emits light of any color. Disclosure of the invention
  • An optical functional material according to the present invention made to solve the above-mentioned problem has a structural formula of any of the following general formulas (I) to (VI I), and a central ion M is Eu (europium).
  • a transparent solid support comprising a first complex and a second complex also having any one of the general formulas (I) to (VI I) and having a central ion M of Tb (terbium).
  • nl represents 2 or 3.
  • n2 represents 2, 3 or 4.
  • Rf 1 and Rf 2 are the same or different and do not contain a hydrogen atom.
  • X 1 and X 2 are the same or different IVA ZokuHara Indicate any of group VIA atoms excluding nitrogen, nitrogen, and VIA group atoms excluding oxygen.
  • n3 and n4 represent 0 or 1.
  • Y represents C— ⁇ ′ ( ⁇ ′ does not contain a deuterium, a halogen atom or a hydrogen atom ( ⁇ represents an aliphatic group of 22 ), and represents N, P, As, Sb or Bi.
  • X 1 is-out bets carbon atoms n3 is 0, when X 2 is a carbon atom n4 is 0, X 1 and X 2 and at the same time if the carbon atom, at least one of hydrogen atoms of Rf Rf 2 Is an aromatic group not containing.
  • nl and n2 are as defined above.
  • Rf 3 does not contain a hydrogen atom.
  • X 3 represents any one of a group IVA atom excluding carbon, a group VA atom excluding nitrogen, and a group V atom excluding oxygen.
  • N5 represents 0 or 1.
  • nl and n2 are as described above. Represents a hydrogen atom or Z ′ (Z ′ is the same as above.) Rf 4 and Rf 5 are the same or different, and do not contain a hydrogen atom. , To C 22 aliphatic groups, hydrogen-free aromatic groups or hydrogen-free heterocyclic groups. Show. )
  • nl represents 2 or 3.
  • n2 represents 1 or 2.
  • n3 represents 1, 2, 3, or 4.
  • X is the same or different, and is a hydrogen atom, a deuterium atom, or a halogen atom.
  • a hydroxyl group, a nitro group, an amino group, a sulfonyl group, a cyano group, a silyl group, a phosphonic acid group, a diazo group, and a mercapto group wherein Y is the same or different, a group of ⁇ ⁇ , a hydroxyl group, A nitro group, an amino group, a sulfonyl group, a cyano group, a silyl group, a phosphonic acid group, a diazo group, or a mercapto group, and Z represents a hydrogen atom or a deuterium atom.
  • a third complex having the same
  • Eu is an element with atomic number 63 belonging to the lanthanoid, and its trivalent ion Eu 3+ can increase the excitation energy of the f_f transition at wavelengths around 394, 420, and 465 nm (all blue) by properly designing the ligand.
  • the radiant energy can be set to around 600-700 ⁇ (red light).
  • excitation at a wavelength of 394 nm has particularly high luminous efficiency.
  • Tb is also an element with an atomic number of 65 belonging to the lanthanoid, and its trivalent ion Tb 3+ has an excitation energy of the ff transition near the wavelength of 300 to 380 nm (all of which are blue), and especially excitation at 380 nm.
  • the resulting light emission is 488 nm, 543 nm, 581 nm, 618 nm, 652 nm, etc. Of these, the emission intensity ratio of 543 nm (green light) is extremely high.
  • Tm is also an element of atomic number 69 belonging to the lanthanide, and its trivalent ion Tm 3+ has an excitation wavelength of 400 nm or less, and has an excitation wavelength of 362 nm in the ff transition. Tm emission is strongest at a wavelength of 453 nm (blue light).
  • the wavelength refers to the wavelength of the excitation light of the rare-earth complex
  • the width is narrow, not more than lnm, regardless of the type of ligand physicochemically, but several nm in consideration of measurement technology, etc. It includes the width of the degree.
  • the wavelength of the fluorescence emission may include a large number of interlevel transitions physicochemically, so that the width may reach lOnm or more.
  • the color coordinates on the chromaticity diagram of the red emission of the above complex (first complex) with Eu as the central ion are about (0.666, 0.333), and the central ion is Tb.
  • the color coordinates of the complex (second complex) are approximately (0.313, 0.631). And the color coordinates of those excited blue lights are about (0.147, 0.064).
  • RGB emission can be achieved only with the complex by combining with a near-ultraviolet LED or semiconductor laser.
  • a light-emitting device that emits white light of any color temperature or light of any color can be realized.
  • FIG. 4 shows a spectrum when a sample in which the first complex and the second complex are mixed at an appropriate ratio in a polymer plastic is covered with an InGaN_LED which emits blue light of 440 nm to form a luminous body.
  • the RGB emission from each layer is mixed to achieve a pastel color tone that is slightly pinkish and close to white.
  • the light emitting device may be configured by placing the light emitting device.
  • the emission color can be arbitrarily set by appropriately adjusting the concentration of the complex in each layer (each transparent fixed carrier) or the thickness of each layer.
  • white of any color temperature for example, 6500K (daylight), 5000K (daylight), 4200K (white), 3500K (warm white), 3000K (bulb)
  • Color light source for fluorescent lamp light source, for example, Paroc (registered trademark of Matsushita Electric Industrial Co., Ltd.)) cool [for study room], natural living room and study], warm [for living and dining] ))
  • LEDs can also be realized with LEDs. Since the fluorescent efficiency of the complex used is as high as 40% to 70%, it is a big point that the luminous efficiency higher than that of the conventional technology can be realized even with low color temperature white light.
  • a sensitizing dye capable of selectively exciting each central ion (Eu and Tb) may be simultaneously contained in each transparent fixing carrier, and thereby the emission color may be controlled.
  • the complex is preliminarily supported on a host-guest complex having an average particle size of nano-size, and then the transparent It may be a method of mixing in a fixed carrier.
  • the type and production method of the nano-sized host-guest complex supporting the rare earth complex It is described in detail in JP-A-2000-256251.
  • the excitation light source for producing a white or arbitrary color light emitting device by combining with the optical functional material according to the present invention is represented by a general formula
  • a light emitting diode or a semiconductor laser having a nitride light emitting layer represented by OKx (1) is desirable.
  • a semiconductor LED or semiconductor laser having this light-emitting layer can emit light of any wavelength in the blue to ultraviolet range by controlling the component variable X.However, when a Eu complex is used as a rare earth complex, Is the component variable X for generating the excitation light near the wavelengths 394, 420, and 465 nm. It is about 0.5.
  • the component variable X for generating excitation light having a wavelength of about 360 to 380 nm is about 0 to 0.1. Since the light emitting device according to the present invention does not include three separate color light sources arranged side by side, even if it is viewed in detail, each color does not appear separately and a completely homogeneous white light source is obtained. Further, the problem of interference fringes does not occur at the time of photographing or the like. Furthermore, since the intensity of each color of RGB is fixed by the concentration and layer thickness of each complex, there is almost no change over time, and a long-term stable white light source can be obtained. In addition, since the light emitting device includes only the light source and the transparent fixing member disposed on the front surface thereof, the device itself can be made very compact. BRIEF DESCRIPTION OF THE FIGURES
  • White LED (correlated color temperature: 6500K) comprising a first drawing YAG phosphor coated with nitride Gariumu based blue LED and scan Bae spectrum of a standard light D 65 (correlated color temperature: 6504 K) scan Bae spectrum Dara off of.
  • Fig. 2 Table of color rendering index of white LEDs and other white light sources.
  • FIG. 4 is a spectrum diagram when a luminous body is formed by covering a sample in which a first complex and a second complex are mixed at an appropriate ratio in a polymer plastic over an InGaN-LED light source.
  • Fig. 5 Graph of chromaticity coordinates and correlated color temperature covered by InGaN blue LED + YAG phosphor white LED.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Led Device Packages (AREA)
  • Led Devices (AREA)
  • Semiconductor Lasers (AREA)
  • Luminescent Compositions (AREA)

Abstract

L'invention se rapporte à un dispositif émetteur de lumière doté de propriétés de rendu de couleurs intenses et à un dispositif émetteur de lumière qui émet une lumière de couleur arbitraire obtenue par combinaison d'un dispositif émetteur de lumière à semi-conducteur et d'un support de conversion de longueur d'ondes transparent, recouvrant le dispositif. Un premier complexe présente les formules structurelles générales (I) - (VIII) et un ion central M de Eu, et un second complexe présente les formules structurelles générales identiques (I) (VIII) et un ion central M de Tb, sont mélangés dans un support solide, par exemple un plastique transparent, et combinés à un dispositif émetteur de lumière à semi-conducteur qui émet de la lumière bleue sur la bande d'excitation de Eu et Tb. Une couche de porteur fixe transparent contenant le second complexe peut être disposée en couches. Un dispositif émetteur de lumière émet une lumière de couleur arbitraire qui peut être obtenue par régulation des intensités d'émission de lumière rouge issue du porteur fixe transparent contenant le premier complexe, de lumière verte issue du porteur fixe transparent contenant le second complexe, et de lumière bleue issue du dispositif émetteur de lumière à semi-conducteur.
PCT/JP2002/011748 2001-11-15 2002-11-11 Materiau fonctionnel optique utilisant des complexes des terres rares et dispositif emetteur de lumiere WO2003042325A1 (fr)

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JP2001350723A JP2003147346A (ja) 2001-11-15 2001-11-15 希土類錯体を用いた光機能材料及び発光装置
JP2001-350723 2001-11-15

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102827599A (zh) * 2012-08-20 2012-12-19 太原理工大学 一种红绿蓝共混白光荧光粉的制备方法
CN102887973A (zh) * 2012-09-19 2013-01-23 太原理工大学 一种含铕铽铍聚合物的白光荧光粉的制备方法

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WO2004104136A1 (fr) * 2003-05-22 2004-12-02 Mitsubishi Chemical Corporation Dispositif electroluminescent et phosphore
JP4238666B2 (ja) * 2003-07-17 2009-03-18 豊田合成株式会社 発光装置の製造方法
WO2005075598A1 (fr) * 2004-02-06 2005-08-18 Mitsubishi Chemical Corporation Dispositif luminescent et dispositif d’eclairage l’utilisant, unite d’affichage d’images
WO2006004187A1 (fr) 2004-07-05 2006-01-12 Kri, Inc. Composite organique/inorganique
JP4817632B2 (ja) * 2004-09-27 2011-11-16 京セラ株式会社 Ｌｅｄファイバ光源装置及びそれを用いた内視鏡
JP2006222403A (ja) * 2005-02-14 2006-08-24 Kri Inc 光増幅素器
JP5130512B2 (ja) * 2006-02-07 2013-01-30 国立大学法人秋田大学 カルボン酸−ジケトン複合系希土類金属錯体
JP5574646B2 (ja) * 2009-09-09 2014-08-20 株式会社東芝 アモルファス発光材料及びアモルファス発光材料を用いた発光素子
JP6314518B2 (ja) * 2014-02-10 2018-04-25 ソニー株式会社 画像表示装置及び表示装置
JP6679755B2 (ja) * 2016-12-19 2020-04-15 富士フイルム株式会社 波長変換用発光性樹脂組成物及びその製造方法、並びに波長変換部材及び発光素子

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CN102827599A (zh) * 2012-08-20 2012-12-19 太原理工大学 一种红绿蓝共混白光荧光粉的制备方法
CN102887973A (zh) * 2012-09-19 2013-01-23 太原理工大学 一种含铕铽铍聚合物的白光荧光粉的制备方法

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