JP2018109664A - Joined body for wavelength conversion - Google Patents
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- JP2018109664A JP2018109664A JP2016256312A JP2016256312A JP2018109664A JP 2018109664 A JP2018109664 A JP 2018109664A JP 2016256312 A JP2016256312 A JP 2016256312A JP 2016256312 A JP2016256312 A JP 2016256312A JP 2018109664 A JP2018109664 A JP 2018109664A
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- 238000006243 chemical reaction Methods 0.000 title claims abstract description 20
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims abstract description 57
- 229910052594 sapphire Inorganic materials 0.000 claims abstract description 39
- 239000010980 sapphire Substances 0.000 claims abstract description 39
- 239000000758 substrate Substances 0.000 claims abstract description 39
- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims description 55
- 239000013078 crystal Substances 0.000 claims description 11
- 229910019990 cerium-doped yttrium aluminum garnet Inorganic materials 0.000 abstract 1
- 239000000919 ceramic Substances 0.000 description 13
- 239000000843 powder Substances 0.000 description 12
- 239000002245 particle Substances 0.000 description 10
- 238000000034 method Methods 0.000 description 9
- 238000002834 transmittance Methods 0.000 description 7
- 239000000463 material Substances 0.000 description 6
- 239000002994 raw material Substances 0.000 description 6
- 239000002002 slurry Substances 0.000 description 6
- 238000004519 manufacturing process Methods 0.000 description 5
- 238000005498 polishing Methods 0.000 description 5
- 239000004065 semiconductor Substances 0.000 description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 4
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 description 4
- 230000005540 biological transmission Effects 0.000 description 4
- 238000011156 evaluation Methods 0.000 description 4
- 150000002500 ions Chemical class 0.000 description 4
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 4
- 238000005245 sintering Methods 0.000 description 4
- 239000011230 binding agent Substances 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 238000007606 doctor blade method Methods 0.000 description 3
- 229910000420 cerium oxide Inorganic materials 0.000 description 2
- 229910003460 diamond Inorganic materials 0.000 description 2
- 239000010432 diamond Substances 0.000 description 2
- 235000011187 glycerol Nutrition 0.000 description 2
- 238000005286 illumination Methods 0.000 description 2
- 230000003287 optical effect Effects 0.000 description 2
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 2
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 2
- 239000004014 plasticizer Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910052684 Cerium Inorganic materials 0.000 description 1
- 238000000137 annealing Methods 0.000 description 1
- 238000000149 argon plasma sintering Methods 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000000634 powder X-ray diffraction Methods 0.000 description 1
- 230000002250 progressing effect Effects 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 238000011282 treatment Methods 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
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Abstract
Description
本発明は、発光ダイオード（ＬＥＤ）やレーザーダイオード（ＬＤ）などの半導体発光デバイスに用いられる波長変換用接合体に関する。 The present invention relates to a wavelength conversion joint used in a semiconductor light emitting device such as a light emitting diode (LED) or a laser diode (LD).
青色ＬＥＤチップと、青色光を黄色に変換するＹＡＧとを組み合わせた白色ＬＥＤ照明装置が知られている。このような照明装置は、白熱電球などに比べて発光効率が高く、長寿命でかつ装置の小型化や消費電力の削減が可能であり、さらなる効率・信頼性の向上や、高出力化に向けて開発が進んでいる。 There is known a white LED illumination device in which a blue LED chip and a YAG that converts blue light into yellow are combined. Such lighting devices have higher luminous efficiency than incandescent bulbs, etc., have a long life span, and can reduce the size and power consumption of the device, further improving efficiency and reliability, and increasing output. Development is progressing.
また、パソコンやメモリカードからの画像データをスクリーンに投影するためのプロジェクタにおいても、従来は高輝度の放電ランプを光源とするものが主流であったが、近年、ＬＥＤやＬＤを用いた装置が開発されている。なかでも、ＬＤは、ＬＥＤのように波長や振幅にバラつきがなく、可視光線から中赤外線までの様々な波長領域において光を出力できることから、発光効率の高い光源として開発されている。ただし、波長５００〜６００ｎｍの可視光線、および波長２〜５μｍの近赤外線から中赤外線までの波長領域では、ＬＤ光源から直接光を発生することが困難であるため、非線形光学効果を利用した波長変換が用いられている。 In addition, projectors for projecting image data from a personal computer or a memory card onto a screen have conventionally been mainly using a high-intensity discharge lamp as a light source. Recently, however, devices using LEDs or LDs have been used. Has been developed. Among them, the LD has been developed as a light source with high luminous efficiency because it has no variation in wavelength and amplitude like an LED and can output light in various wavelength regions from visible light to mid-infrared. However, it is difficult to generate light directly from the LD light source in the visible light having a wavelength of 500 to 600 nm, and in the wavelength region from near infrared to mid-infrared having a wavelength of 2 to 5 μm. Is used.
これまでに様々な形態の波長変換素子が報告されているが、例えば、特許文献１には、ｎ−型領域とｐ−型領域との間に発光層を有し、さらに、該発光層によって放射される光の光路にセラミック層が組み合わされた半導体発光装置において、サファイアの成長基板上にＹＡＧ：Ｃｅセラミック層が形成された波長変換素子が開示されている。特許文献１では、サファイアの成長基板上にＹＡＧ：Ｃｅセラミック層をキャストしてセラミック生形体を得た後、この成形体を焼結することで、成長基板とセラミック層とを一体化させている。 Various types of wavelength conversion elements have been reported so far. For example, Patent Document 1 has a light-emitting layer between an n-type region and a p-type region, and further includes a light-emitting layer. In a semiconductor light emitting device in which a ceramic layer is combined with an optical path of emitted light, a wavelength conversion element in which a YAG: Ce ceramic layer is formed on a sapphire growth substrate is disclosed. In Patent Document 1, after a YAG: Ce ceramic layer is cast on a sapphire growth substrate to obtain a ceramic green body, the growth substrate and the ceramic layer are integrated by sintering the formed body. .
特許文献２には、成長基板の上に、ｎ−型領域とｐ−型領域との間に堆積された発光層を含む半導体構造体を成長させ、該半導体構造体の上に、さらに、ホストと発光材料を含むセラミック層とを含む複合基板を接合した波長変換素子が開示されている。特許文献２では、ＹＡＧ：Ｃｅセラミックグリーン体をサファイア・ホスト材料と重ね、セラミック・バインダを５００〜６００℃の温度下に空気中で燃焼させ、次いで、スタックを加圧ダイに送った後、１５００〜１８００℃で２〜１２時間、真空加圧して発光セラミックとホストとの接合体を形成している。 In Patent Document 2, a semiconductor structure including a light emitting layer deposited between an n-type region and a p-type region is grown on a growth substrate, and a host is further formed on the semiconductor structure. And a wavelength conversion element in which a composite substrate including a ceramic layer containing a light emitting material is bonded. In Patent Document 2, a YAG: Ce ceramic green body is overlapped with a sapphire host material, a ceramic binder is burned in air at a temperature of 500 to 600 ° C., and then the stack is sent to a pressure die, and then 1500 Vacuum bonding is performed at ˜1800 ° C. for 2 to 12 hours to form a joined body of the luminescent ceramic and the host.
しかしながら、特許文献１では、ＹＡＧ：Ｃｅセラミック成形体を焼結させるために、焼結後、サファイアの成長基板に比べて、ＹＡＧ：Ｃｅセラミック層が大きく収縮するために、成長基板とセラミック層とを一体化させた後、波長変換素子に歪みが生じ、これが反りの発生、強度の低下の原因となっていた。 However, in Patent Document 1, in order to sinter the YAG: Ce ceramic molded body, the YAG: Ce ceramic layer contracts more greatly after sintering than the sapphire growth substrate. After being integrated, the wavelength conversion element was distorted, which caused warpage and reduced strength.
また、特許文献２では、ＹＡＧ：Ｃｅセラミックグリーン体とサファイア・ホスト材料とを加圧しながら共焼成するために、ＹＡＧ：Ｃｅセラミックグリーン体とサファイア・ホスト材料との間の接触面積は大きくなるものの、得られる接合体の機械的強度や光学的特性を改善するのに、必要に応じて、アニーリングや表面研磨等の処理がさらに必要であり、改善の余地があった。 In Patent Document 2, since the YAG: Ce ceramic green body and the sapphire host material are co-fired while being pressurized, the contact area between the YAG: Ce ceramic green body and the sapphire host material is increased. In order to improve the mechanical strength and optical characteristics of the obtained bonded body, further treatments such as annealing and surface polishing are necessary as needed, and there is room for improvement.
本発明は、上記した従来技術の問題に鑑みてなされたものであり、高い光透過性を有し、かつ、焼結しても強度を維持することができる波長変換用接合体を提供することを課題とする。 The present invention has been made in view of the above-described problems of the prior art, and provides a wavelength conversion bonded body having high light transmittance and capable of maintaining strength even when sintered. Is an issue.
本発明の波長変換用接合体は、Ａｌ2Ｏ3およびＹＡＧ：Ｃｅからなる多結晶蛍光体と、サファイア基板との接合体であって、前記多結晶蛍光体が、厚さ５０〜１０００μｍであり、前記多結晶蛍光体と前記サファイア基板との接合界面から多結晶蛍光体の厚さ方向の２０〜５０％の領域にＡｌ2Ｏ3配向度が６０％以上であるＡｌ2Ｏ3配向化層を有することを特徴とする。 The joined body for wavelength conversion of the present invention is a joined body of a polycrystalline phosphor composed of Al 2 O 3 and YAG: Ce and a sapphire substrate, and the polycrystalline phosphor has a thickness of 50 to 1000 μm. An Al 2 O 3 oriented layer having an Al 2 O 3 orientation degree of 60% or more in a region of 20 to 50% in the thickness direction of the polycrystalline phosphor from the junction interface between the polycrystalline phosphor and the sapphire substrate It is characterized by having.
上記の構成を有することで、本発明の波長変換用接合体は、高い透明性を有し、かつ、多結晶蛍光体層とサファイア基板との熱膨張の差が小さいため、該多結晶蛍光体層と該サファイア基板とを焼結により接合しても、割れ難く、強度を維持することができる。 By having the above structure, the wavelength conversion assembly of the present invention has high transparency, and the difference in thermal expansion between the polycrystalline phosphor layer and the sapphire substrate is small. Even if the layer and the sapphire substrate are joined by sintering, it is difficult to break and the strength can be maintained.
さらに、前記Ａｌ2Ｏ3配向化層の直上にＡｌ2Ｏ3配向度が３０％以下であるＡｌ2Ｏ3非配向化層を有することが好ましい。 Further, it is preferable with Al 2 O 3 unoriented layer Al 2 O 3 orientation degree is 30% or less immediately above the Al 2 O 3 textured layer.
このようなＡｌ2Ｏ3非配向化層をＡｌ2Ｏ3配向化層上に有することで、該非配向化層が光を適度に散乱させ、所望の光透過性を波長変換用接合体に付与することができる。 By having such an Al 2 O 3 non-oriented layer on the Al 2 O 3 oriented layer, the non-oriented layer appropriately scatters light and imparts desired light transmittance to the wavelength conversion joint. can do.
前記Ａｌ2Ｏ3配向化層中のＡｌ2Ｏ3の平均結晶粒径は１〜１０μｍであることが好ましい。
前記多結晶蛍光体中、Ａｌ2Ｏ3とＹＡＧ：Ｃｅとの含有比率が体積比で９０：１０〜５０：５０であることが好ましい。
The average crystal grain size of Al 2 O 3 in the Al 2 O 3 oriented layer is preferably 1 to 10 μm.
In the polycrystalline phosphor, the content ratio of Al 2 O 3 and YAG: Ce is preferably 90:10 to 50:50 by volume.
かかる構成を有することで、本発明の波長変換用接合体は透明性を有し、加えて、従来の波長変換部材に比べて、良好な強度を有することができる。 By having such a structure, the bonded body for wavelength conversion of the present invention has transparency, and in addition, can have better strength than conventional wavelength conversion members.
本発明の波長変換用接合体は、高い光透過性、すなわち、透明性を有し、かつ、製造時に焼結しても、応力による歪みが生じず、強度を維持することができる。このため、例えば、発光ダイオード（ＬＥＤ）やレーザーダイオード（ＬＤ）、特にレーザーダイオード（ＬＤ）の半導体発光デバイスの用途に好適に用いられる。 The bonded body for wavelength conversion of the present invention has high light transmittance, that is, transparency, and even when sintered at the time of manufacture, distortion due to stress does not occur and strength can be maintained. For this reason, for example, it is used suitably for the use of the semiconductor light-emitting device of a light emitting diode (LED), a laser diode (LD), especially a laser diode (LD).
本発明の波長変換用接合体（以下単に「接合体」ともいう。）は、Ａｌ2Ｏ3およびＹＡＧ：Ｃｅからなる多結晶蛍光体と、サファイア基板との接合体であって、前記多結晶蛍光体が、厚さ５０〜１０００μｍであり、前記多結晶蛍光体と前記サファイア基板との接合界面から多結晶蛍光体の厚さ方向の２０〜５０％の領域にＡｌ2Ｏ3配向度が６０％以上であるＡｌ2Ｏ3配向化層を有する。
上記接合体の各構成要素について詳細に説明する。
The wavelength conversion bonded body (hereinafter also simply referred to as “bonded body”) of the present invention is a bonded body of a polycrystalline phosphor composed of Al 2 O 3 and YAG: Ce and a sapphire substrate. The phosphor has a thickness of 50 to 1000 μm, and an Al 2 O 3 orientation degree of 60 is in a region of 20 to 50% in the thickness direction of the polycrystalline phosphor from the junction interface between the polycrystalline phosphor and the sapphire substrate. % Of Al 2 O 3 orientation layer.
Each component of the joined body will be described in detail.
上記多結晶蛍光体は、Ａｌ2Ｏ3およびＹＡＧ：Ｃｅからなる。
ＹＡＧ：Ｃｅは、黄緑色の範囲の光を放出する蛍光体である。ＹＡＧ：Ｃｅは、Ｙ3Ａｌ5Ｏ12のＹの格子位置を希土類元素であるＣｅで置換した化合物であり、（Ｙ，Ｃｅ）3Ａｌ5Ｏ12またはＹ3Ａｌ5Ｏ12：Ｃｅ3+とも表される。
蛍光体は、母体となる結晶と、それに固溶させる金属イオン（付活イオン）との組み合わせで発光色が決まる。付活イオンは、発光中心として機能するイオンである。本発明では、母体であるＹＡＧ結晶に、付活イオンＣｅ3+をドープすることによって、ＹＡＧ：Ｃｅが青色光によって励起され、黄緑色光を発する。なお、化学組成が同じであっても結晶構造が異なる場合、母体結晶が異なることにより発光特性や安定性が異なるため、異なる蛍光体となる。
ＣｅはＹＡＧに対して、０．１〜３．０ｍｏｌ％添加する。Ｃｅの添加量が前記範囲内であるとき、単一相のＹＡＧが得られることが粉末Ｘ線回折パターンからわかっている。
The polycrystalline phosphor is made of Al 2 O 3 and YAG: Ce.
YAG: Ce is a phosphor that emits light in the yellow-green range. YAG: Ce is a compound in which the Y lattice position of Y 3 Al 5 O 12 is substituted with Ce, which is a rare earth element, and (Y, Ce) 3 Al 5 O 12 or Y 3 Al 5 O 12 : Ce 3+ It is also expressed.
The phosphor emits light with a combination of a crystal serving as a base and a metal ion (activated ion) to be dissolved therein. An activated ion is an ion that functions as a luminescent center. In the present invention, YAG: Ce is excited by blue light and emits yellow-green light by doping the active ion Ce 3+ into the base YAG crystal. In addition, even if the chemical composition is the same, when the crystal structure is different, the emission characteristics and stability differ due to the difference in the host crystal, resulting in different phosphors.
Ce is added in an amount of 0.1 to 3.0 mol% with respect to YAG. It is known from the powder X-ray diffraction pattern that when the addition amount of Ce is within the above range, single-phase YAG is obtained.
Ａｌ2Ｏ3には、単結晶Ａｌ2Ｏ3および多結晶Ａｌ2Ｏ3のいずれも用いることができる。このようなＡｌ2Ｏ3の平均粒径は、通常１〜１０μｍである。Ａｌ2Ｏ3は、多結晶蛍光体において光の散乱および熱の伝搬の働きをする。 As Al 2 O 3 , both single crystal Al 2 O 3 and polycrystalline Al 2 O 3 can be used. The average particle diameter of such Al 2 O 3 is usually 1 to 10 μm. Al 2 O 3 functions as light scattering and heat propagation in the polycrystalline phosphor.
上記多結晶蛍光体において、Ａｌ2Ｏ3およびＹＡＧ：Ｃｅは、体積比で９０：１０〜５０：５０で含まれることが好ましく、７８：２２〜７０：３０で含まれることがより好ましい。ＹＡＧ：Ｃｅの含有比が２０ｖｏｌ％未満であると、蛍光体として実用に耐える機能を発揮できないことがある。一方、ＹＡＧ：Ｃｅの含有比が５０ｖｏｌ％を超えると、熱伝導率が低下し、放熱効果が低下することがある。 In the polycrystalline phosphor, Al 2 O 3 and YAG: Ce are preferably included in a volume ratio of 90:10 to 50:50, and more preferably 78:22 to 70:30. When the content ratio of YAG: Ce is less than 20 vol%, the phosphor may not be able to exhibit a function that can withstand practical use. On the other hand, when the content ratio of YAG: Ce exceeds 50 vol%, the thermal conductivity may be reduced, and the heat dissipation effect may be reduced.
多結晶蛍光体は、ドクターブレード法を用いた反応焼結法により作製することができる。
このような多結晶蛍光体の厚さは５０〜１０００μｍ、好ましくは１００〜３００μｍである。多結晶蛍光体の厚さが上記範囲内にあると、散乱特性が適性化し、配光特性、発光効率が良化するため好ましい。
The polycrystalline phosphor can be produced by a reactive sintering method using a doctor blade method.
The thickness of such a polycrystalline phosphor is 50 to 1000 μm, preferably 100 to 300 μm. It is preferable that the thickness of the polycrystalline phosphor is in the above range because the scattering characteristics are optimized and the light distribution characteristics and the light emission efficiency are improved.
本発明では、多結晶蛍光体を形成させるための成長基板として、サファイア基板が用いられる。成長基板を形成する材料としては、熱伝導率および透明性の高いものであれば、制限はないといえるが、サファイア、特に単結晶サファイアは、機械的および熱的特性、化学的安定性、並びに光透過性に優れることから、本発明において、多結晶蛍光体を成長させるための成長基板として好適に用いられる。 In the present invention, a sapphire substrate is used as a growth substrate for forming a polycrystalline phosphor. The material for forming the growth substrate is not limited as long as it has high thermal conductivity and transparency, but sapphire, particularly single crystal sapphire, has mechanical and thermal properties, chemical stability, and Since it is excellent in light transmittance, in the present invention, it is suitably used as a growth substrate for growing a polycrystalline phosphor.
サファイア基板は、公知の方法により作製してもよいし、例えば、ＣＺ法にて作製した市販品を用いてもよい。
このようなサファイア基板の厚みは、通常１００〜１０００μｍである。
The sapphire substrate may be produced by a known method, for example, a commercially available product produced by the CZ method may be used.
The thickness of such a sapphire substrate is usually 100 to 1000 μm.
次に、本発明の接合体の製造方法として、上記多結晶蛍光体をサファイア基板の表面に形成する方法を説明する。 Next, a method for forming the polycrystalline phosphor on the surface of the sapphire substrate will be described as a method for producing the joined body of the present invention.
まず、サファイア基板および多結晶蛍光体をラップ研磨等の方法により研磨する。サファイア基板および多結晶蛍光のそれぞれの研磨面を重ね合わせ、減圧〜常圧下、１６００〜１７００℃で１０〜３０分間焼成することで、サファイア基板および多結晶蛍光体を一体化させる。なお、この焼成では徐々に１６００℃まで昇温することを要しない。
このようにして得られる本発明の接合体では、多結晶蛍光体とサファイア基板との接合界面から多結晶蛍光体の厚さ方向の２０〜５０％の領域に、Ａｌ2Ｏ3配向度が６０％以上であるＡｌ2Ｏ3配向化層を有している。
First, the sapphire substrate and the polycrystalline phosphor are polished by a method such as lapping. The polished surfaces of the sapphire substrate and the polycrystalline fluorescent material are overlapped and fired at 1600 to 1700 ° C. for 10 to 30 minutes under reduced pressure to normal pressure, thereby integrating the sapphire substrate and the polycrystalline phosphor. In this baking, it is not necessary to gradually raise the temperature to 1600 ° C.
In the joined body of the present invention thus obtained, the Al 2 O 3 orientation degree is 60 in the region of 20 to 50% in the thickness direction of the polycrystalline phosphor from the joined interface between the polycrystalline phosphor and the sapphire substrate. % Of Al 2 O 3 orientation layer.
つまり、本発明の製造方法では、まず、サファイア基板および多結晶蛍光体を別途作製し、それぞれ表面を研磨し、該サファイア基板の研磨面に該多結晶蛍光体の研磨面を重ねて、加圧せずに焼成することで、応力による歪みが生じることなく両者が一体化し、多結晶蛍光体とサファイア基板との接合界面付近のＡｌ2Ｏ3層を配向させることができる。 That is, in the manufacturing method of the present invention, first, a sapphire substrate and a polycrystalline phosphor are separately prepared, the surfaces are polished, and the polishing surface of the polycrystalline phosphor is overlaid on the polishing surface of the sapphire substrate, and then the pressure is applied. By baking without applying the stress, the two can be integrated without causing stress distortion, and the Al 2 O 3 layer in the vicinity of the bonding interface between the polycrystalline phosphor and the sapphire substrate can be oriented.
上記接合体において、Ａｌ2Ｏ3配向化層中のＡｌ2Ｏ3配向度が６０％未満であると、発光強度が小さく、波長変換体としての実用に耐える機能を発揮できないことがある。 When the Al 2 O 3 orientation degree in the Al 2 O 3 orientation layer is less than 60% in the above joined body, the light emission intensity is small, and the function to withstand practical use as a wavelength converter may not be exhibited.
さらに、上記接合体では、前記Ａｌ2Ｏ3配向化層の直上、すなわち、上記接合界面から多結晶蛍光体の厚さ方向５０％を超える領域に、Ａｌ2Ｏ3配向度が３０％以下であるＡｌ2Ｏ3非配向化層を有することが好ましい。 Furthermore, in the joined body, the Al 2 O 3 orientation degree is 30% or less immediately above the Al 2 O 3 oriented layer, that is, in a region exceeding 50% in the thickness direction of the polycrystalline phosphor from the joined interface. It is preferable to have a certain Al 2 O 3 non-oriented layer.
このような層をＡｌ2Ｏ3配向化層の上に有することで、多結晶蛍光体中を光が過度に通り抜けるのを防止することができる。 By having such a layer on the Al 2 O 3 oriented layer, it is possible to prevent light from passing through the polycrystalline phosphor excessively.
上記接合体中、Ａｌ2Ｏ3配向層中のＡｌ2Ｏ3の平均粒径は、１〜１０μｍであることが好ましい。Ａｌ2Ｏ3の平均粒径が１μｍ未満であると、多結晶蛍光体の結晶性が向上せず、発光効率が低下することがある。一方、Ａｌ2Ｏ3の平均粒径が１０μｍを超えると、発光ムラが生じたり、強度の低下に繋がることがある。 During the assembly, the average particle size of the Al 2 O 3 of Al 2 O 3 alignment layer is preferably 1 to 10 [mu] m. When the average particle diameter of Al 2 O 3 is less than 1 μm, the crystallinity of the polycrystalline phosphor is not improved, and the light emission efficiency may be lowered. On the other hand, if the average particle size of Al 2 O 3 exceeds 10 μm, uneven light emission may occur or the strength may be reduced.
以上のとおり、本発明の接合体は、高い光透過性を有し、かつ、製造時に焼結しても、応力による歪みが生じることがないため、強度を維持することができる。このため、上記接合体は、発光ダイオード（ＬＥＤ）およびレーザーダイオード（ＬＤ）、特にレーザーダイオード（ＬＤ）の照明用途に好適である。 As described above, the joined body of the present invention has high light transmittance, and even when sintered at the time of manufacturing, distortion due to stress does not occur, so that the strength can be maintained. For this reason, the said conjugate | zygote is suitable for the illumination use of a light emitting diode (LED) and a laser diode (LD), especially a laser diode (LD).
以下、本発明を実施例に基づき、さらに具体的に説明するが、本発明は下記の実施例により制限されるものではない。 EXAMPLES Hereinafter, although this invention is demonstrated further more concretely based on an Example, this invention is not restrict | limited by the following Example.
［実施例１］
平均粒径０．５μｍで純度９９．９％の酸化セリウム粉末、純度９９．９％、所定粒子径の酸化イットリウム粉末、純度９９．９％、所定粒子径の酸化アルミニウム粉末を所定量配合し、原料粉末を得た。
前記原料粉末に対してエタノール、ＰＶＢ系バインダーおよびグリセリン系可塑剤を原料粉末に対して添加し、酸化アルミニウムボールを用いたボールミルによって１０時間粉砕混合を行い、スラリーを作製した。
そして、得られたスラリーから、ドクターブレード法により、表１に示す所定厚みのグリーンシートを作製した。次に、作製したグリーンシートを口１００ｍｍに打ち抜き加工した後、大気中で脱脂仮焼、真空雰囲気下で焼結し、多結晶蛍光体を得た。
サファイア基板および多結晶蛍光体を３μｍのダイヤモンドスラリーを用い研磨加工後、研磨面を重ね合わせ、常圧下、１６００℃で３０分間焼成し、サファイア基板および多結晶蛍光体を一体化させた。
得られた接合体は、前記多結晶蛍光体中のＡｌ2Ｏ3とＹＡＧ：Ｃｅとの含有比率が体積比で７５：２５の焼結体からなり、前記多結晶蛍光体層の厚さが５００μｍであった。
また、前記サファイア基板との界面から２００μｍの厚さ領域およびこの直上から外表面までの領域における前記多結晶蛍光体層のＡｌ2Ｏ3の配向度をＥＢＳＰ装置を用い測定を行った。その結果得られた配向度はいずれも６５％であった。前記２００μｍの厚さ領域のＡｌ2Ｏ3配向化層中のＡｌ2Ｏ3の平均結晶粒径をインターセプト法により測定したところ４．５μｍであった。
[Example 1]
A predetermined amount of a cerium oxide powder having an average particle size of 0.5 μm and a purity of 99.9%, a purity of 99.9%, an yttrium oxide powder having a predetermined particle size, a purity of 99.9% and an aluminum oxide powder having a predetermined particle size, Raw material powder was obtained.
Ethanol, a PVB binder and a glycerin plasticizer were added to the raw material powder to the raw material powder, and pulverized and mixed by a ball mill using aluminum oxide balls for 10 hours to prepare a slurry.
And the green sheet of the predetermined thickness shown in Table 1 was produced from the obtained slurry by the doctor blade method. Next, the produced green sheet was punched into a 100 mm opening, and then degreased and calcined in the atmosphere and sintered in a vacuum atmosphere to obtain a polycrystalline phosphor.
After polishing the sapphire substrate and the polycrystalline phosphor using a 3 μm diamond slurry, the polished surfaces were overlaid and fired at 1600 ° C. for 30 minutes under normal pressure to integrate the sapphire substrate and the polycrystalline phosphor.
The obtained joined body is a sintered body in which the content ratio of Al 2 O 3 and YAG: Ce in the polycrystalline phosphor is 75:25 by volume, and the thickness of the polycrystalline phosphor layer is It was 500 μm.
Further, the degree of orientation of Al 2 O 3 of the polycrystalline phosphor layer in the 200 μm thick region from the interface with the sapphire substrate and the region from directly above to the outer surface was measured using an EBSP apparatus. As a result, the degree of orientation obtained was 65%. The average crystal grain size of Al 2 O 3 in the 200 μm thick Al 2 O 3 oriented layer was measured by the intercept method and found to be 4.5 μm.
［実施例２］
平均粒径０．５μｍで純度９９．９％の酸化セリウム粉末、純度９９．９％、所定粒子径の酸化イットリウム粉末、純度９９．９％、所定粒子径の酸化アルミニウム粉末を所定量配合し、原料粉末を得た。
前記原料粉末に対してエタノール、ＰＶＢ系バインダーおよびグリセリン系可塑剤を原料粉末に対して添加し、酸化アルミニウムボールを用いたボールミルによって１０時間粉砕混合を行い、スラリーを作製した。
そして、得られたスラリーから、ドクターブレード法により、表１に示す所定厚みのグリーンシートを作製した。次に、作製したグリーンシートを口１００ｍｍに打ち抜き加工した後、大気中で脱脂仮焼、真空雰囲気下で焼結し、多結晶蛍光体を得た。
サファイア基板および多結晶蛍光体を３μｍのダイヤモンドスラリーを用い研磨加工後、研磨面を重ね合わせ、真空雰囲気下、１７００℃で１０分間焼成し、サファイア基板および多結晶蛍光体を一体化させた。
得られた接合体は、前記多結晶蛍光体中のＡｌ2Ｏ3とＹＡＧ：Ｃｅとの含有比率が体積比で７０：３０の焼結体からなり、前記多結晶蛍光体層の厚さが４００μｍであった。
また、前記サファイア基板との界面から２００μｍの厚さ領域およびこの直上から外表面までの領域における前記多結晶蛍光体層のＡｌ2Ｏ3の配向度をＥＢＳＰ装置を用い測定を行った。その結果得られた配向度は、前者領域が７０％であり、後者領域が２５％であった。前記２００μｍの厚さ領域のＡｌ2Ｏ3配向化層中のＡｌ2Ｏ3の平均結晶粒径をインターセプト法により測定したところ３．２μｍであった。
[Example 2]
A predetermined amount of a cerium oxide powder having an average particle size of 0.5 μm and a purity of 99.9%, a purity of 99.9%, an yttrium oxide powder having a predetermined particle size, a purity of 99.9% and an aluminum oxide powder having a predetermined particle size, Raw material powder was obtained.
Ethanol, a PVB binder and a glycerin plasticizer were added to the raw material powder to the raw material powder, and pulverized and mixed by a ball mill using aluminum oxide balls for 10 hours to prepare a slurry.
And the green sheet of the predetermined thickness shown in Table 1 was produced from the obtained slurry by the doctor blade method. Next, the produced green sheet was punched into a 100 mm opening, and then degreased and calcined in the atmosphere and sintered in a vacuum atmosphere to obtain a polycrystalline phosphor.
After polishing the sapphire substrate and the polycrystalline phosphor using a 3 μm diamond slurry, the polished surfaces were overlapped and baked at 1700 ° C. for 10 minutes in a vacuum atmosphere to integrate the sapphire substrate and the polycrystalline phosphor.
The obtained joined body is a sintered body in which the content ratio of Al 2 O 3 and YAG: Ce in the polycrystalline phosphor is 70:30 by volume, and the thickness of the polycrystalline phosphor layer is It was 400 μm.
Further, the degree of orientation of Al 2 O 3 of the polycrystalline phosphor layer in the 200 μm thick region from the interface with the sapphire substrate and the region from directly above to the outer surface was measured using an EBSP apparatus. As a result, the degree of orientation obtained was 70% in the former region and 25% in the latter region. The average crystal grain size of Al 2 O 3 in the 200 μm-thickness Al 2 O 3 oriented layer was measured by the intercept method and found to be 3.2 μm.
［比較例１］
上記実施例１の製造方法のうち、接合について、接合条件を常圧下、１５００℃で１８０分間焼成としたこと以外は同様に接合体を製造した。
得られた接合体は、前記多結晶蛍光体中のＡｌ2Ｏ3とＹＡＧ：Ｃｅとの含有比率が体積比で７５：２５の焼結体からなり、前記多結晶蛍光体層の厚さが５００μｍであった。
また、前記サファイア基板との界面から２００μｍの厚さ領域およびこの直上から外表面までの領域における前記多結晶蛍光体層のＡｌ2Ｏ3の配向度をＥＢＳＰ装置を用い測定を行った。その結果得られた配向度はいずれも５５％であった。前記２００μｍの厚さ領域のＡｌ2Ｏ3配向化層中のＡｌ2Ｏ3の平均結晶粒径をインターセプト法により測定したところ１．５μｍであった。
[Comparative Example 1]
In the manufacturing method of Example 1 described above, a bonded body was manufactured in the same manner except that the bonding condition was firing at 1500 ° C. for 180 minutes under normal pressure.
The obtained joined body is a sintered body in which the content ratio of Al 2 O 3 and YAG: Ce in the polycrystalline phosphor is 75:25 by volume, and the thickness of the polycrystalline phosphor layer is It was 500 μm.
Further, the degree of orientation of Al 2 O 3 of the polycrystalline phosphor layer in the 200 μm thick region from the interface with the sapphire substrate and the region from directly above to the outer surface was measured using an EBSP apparatus. As a result, the degree of orientation obtained was 55%. When the average crystal grain size of Al 2 O 3 in the 200 μm thick Al 2 O 3 oriented layer was measured by the intercept method, it was 1.5 μm.
［評価］
前記実施例１、実施例２および比較例１について、次の方法により光透過特性および機械的強度特性の評価を行った。
〈光透過特性の評価法〉
サファイア基板、およびそれぞれの接合体の背面より赤色ＬＤ光を照射し、前方透過光の出力を測定し、接合体の透過率／サファイア基板の透過率を算出し、光の透過特性を評価した。
〈機械的強度特性の評価法〉
接合強度の評価はサファイア、多結晶蛍光体にプラグを設置し、引っ張り強度にて測定した。
[Evaluation]
About the said Example 1, Example 2, and the comparative example 1, the light transmission characteristic and the mechanical strength characteristic were evaluated with the following method.
<Evaluation method of light transmission characteristics>
Red LD light was irradiated from the back surface of the sapphire substrate and each joined body, the output of forward transmitted light was measured, the transmittance of the joined body / the transmittance of the sapphire substrate was calculated, and the light transmission characteristics were evaluated.
<Evaluation method of mechanical strength characteristics>
The bonding strength was evaluated by measuring the tensile strength by installing a plug on sapphire or polycrystalline phosphor.
［評価］
上記の通り、光透過特性および機械的強度において、実施例１および実施例２の波長変換用接合体は、比較例１のものに比べ、優れた特性が得られることが確認された。
[Evaluation]
As described above, it was confirmed that in the light transmission characteristics and the mechanical strength, the wavelength conversion joints of Example 1 and Example 2 obtained superior characteristics as compared with those of Comparative Example 1.
Claims (4)
前記多結晶蛍光体が、厚さ５０〜１０００μｍであり、
前記多結晶蛍光体と前記サファイア基板との接合界面から多結晶蛍光体の厚さ方向の２０〜５０％の領域にＡｌ2Ｏ3配向度が６０％以上であるＡｌ2Ｏ3配向化層を有することを特徴とする波長変換用接合体。 A joined body of a polycrystalline phosphor composed of Al 2 O 3 and YAG: Ce and a sapphire substrate,
The polycrystalline phosphor has a thickness of 50 to 1000 μm;
An Al 2 O 3 orientation layer having an Al 2 O 3 orientation degree of 60% or more is formed in a region of 20 to 50% in the thickness direction of the polycrystalline phosphor from the junction interface between the polycrystalline phosphor and the sapphire substrate. A joined body for wavelength conversion, comprising:
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| WO2020026819A1 (en) * | 2018-07-31 | 2020-02-06 | 日本特殊陶業株式会社 | Light wavelength conversion member and light-emitting device |
| WO2023153241A1 (en) * | 2022-02-09 | 2023-08-17 | 日亜化学工業株式会社 | Wavelength conversion module, light emission device, and method for manufacturing wavelength conversion module |
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| WO2007018222A1 (en) * | 2005-08-10 | 2007-02-15 | Ube Industries, Ltd. | Substrate for light emitting diode and light emitting diode |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2020026819A1 (en) * | 2018-07-31 | 2020-02-06 | 日本特殊陶業株式会社 | Light wavelength conversion member and light-emitting device |
| JPWO2020026819A1 (en) * | 2018-07-31 | 2020-08-06 | 日本特殊陶業株式会社 | Light wavelength conversion member and light emitting device |
| TWI716050B (en) * | 2018-07-31 | 2021-01-11 | 日商日本特殊陶業股份有限公司 | Light wavelength conversion member and light emitting device |
| CN112470044A (en) * | 2018-07-31 | 2021-03-09 | 日本特殊陶业株式会社 | Optical wavelength conversion member and light emitting device |
| US20210324266A1 (en) * | 2018-07-31 | 2021-10-21 | Ngk Spark Plug Co., Ltd. | Light wavelength conversion member and light-emitting device |
| EP3832360A4 (en) * | 2018-07-31 | 2022-04-20 | NGK Spark Plug Co., Ltd. | Light wavelength conversion member and light-emitting device |
| US11945987B2 (en) | 2018-07-31 | 2024-04-02 | Niterra Co., Ltd. | Light wavelength conversion member and light-emitting device |
| WO2023153241A1 (en) * | 2022-02-09 | 2023-08-17 | 日亜化学工業株式会社 | Wavelength conversion module, light emission device, and method for manufacturing wavelength conversion module |
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