發(fā)布時間：2018-06-05 14:31

  本文選題：YAG熒光膜 + 白光LED��； 參考：《電子科技大學》2016年博士論文

【摘要】：YAG:Ce~(3+)熒光材料轉(zhuǎn)換白光LED具有發(fā)光效率高、能耗低、壽命長和安全可靠等優(yōu)點,是新一代全固態(tài)照明光源,在照明市場中占據(jù)不可代替的地位。但是,商業(yè)YAG:Ce~(3+)熒光粉體顆粒較大且形貌不規(guī)則分布不均勻,不可避免地產(chǎn)生背反射與背散射,導致能量轉(zhuǎn)換效率下降;此外,熒光粉/環(huán)氧樹脂層的差導熱性會引起熒光材料溫度猝滅,環(huán)氧樹脂層受長時間的熱輻射會泛黃或發(fā)生脫落,降低白光LED使用的穩(wěn)定性與壽命。透明YAG:Ce~(3+)熒光膜有著更小與更均勻的顆粒尺寸、更強的附著力、更好的導熱性、特別是有著較小的背反射與背散射效應,被認為是作為白光LED良好熒光轉(zhuǎn)換層,受廣泛研究者所關(guān)注。論文研究的出發(fā)點是制備可應用在白光LED上的高效發(fā)光性能的稀土摻雜YAG熒光膜,研究所取得結(jié)果如下:1.采用粉末靶材在石英基片上制備YAG:3.3%Ce~(3+)熒光膜,對濺射過程中的濺射功率、氧氣含量與退火工藝對沉積速率及性能的影響進行系統(tǒng)研究。由于粉末靶原子的表面結(jié)合能低于傳統(tǒng)高溫燒結(jié)陶瓷靶,薄膜的沉積速率得到了提高,達1.2μm/h。在最佳工藝條件下濺射2h,沉積薄膜厚度達2.92μm,經(jīng)在H2/Ar還原氣氛1100℃燒結(jié)10 h,薄膜為純相YAG膜,在450 nm激發(fā)下,發(fā)光量子產(chǎn)率達23%。2.采用具有高溶解能力的乙二醇作為溶膠的溶劑,實現(xiàn)了高濃度溶膠下制備YAG:3.3%Ce~(3+)熒光膜,涂膜40層,所制備YAG:Ce~(3+)熒光膜為80 nm顆粒緊密堆積而成,厚度達4.3μm。所制備YAG:Ce~(3+)熒光膜在可見光區(qū)域有著良好的透光性的同時,在藍光區(qū)有著強吸收峰,發(fā)光量子產(chǎn)率達47%,可作為在白光LED的熒光轉(zhuǎn)換層。3.以硝酸鹽為原材料、尿素與氨基乙酸為輔助燃料采用溶膠燃燒法在較低溫條件下制備了YAG:3.3%Ce~(3+)熒光膜,在40層重復涂膜,膜層為大小約50 nm顆粒緊密堆積而成,膜厚達5.1μm。所制備的YAG:3.3%Ce~(3+)熒光膜在藍光區(qū)有著強吸收峰,波長大于500 nm處有著良好的透光性,發(fā)光量子產(chǎn)率達56%。所YAG:3.3%Ce~(3+)熒光膜可應用在白光LED的封裝,在8V電壓,100 m A電流驅(qū)動下,發(fā)光效率為82 lm/W,色溫為4536K,顯色指數(shù)為75.6。4.研究了石榴石母體結(jié)構(gòu)對Ce~(3+)發(fā)光特性的影響。利用更大離子半徑的Tb~(3+)與Gd~(3+)取代Y~(3+)所在12面體位置,會增大晶體的晶場分裂能與晶格畸變效應,因此Ce~(3+)的發(fā)光光譜半峰寬與峰值波長呈現(xiàn)了寬化與紅移。以鈧離子取代鋁離子,發(fā)光光譜半峰寬呈現(xiàn)了寬化,但沒有發(fā)生紅移。適當增大石榴石的晶胞體積可減小Ce~(3+)發(fā)生熒光猝滅的概率從而提高發(fā)Ce~(3+)的發(fā)光強度;Ce~(3+)發(fā)光峰的寬化與紅移有效改善白光LED的發(fā)光性能,以TAG:3.3%Ce~(3+)熒光膜所封裝的白光LED的發(fā)光效率達72 lm/W,色溫為4888 K,顯色指數(shù)79.2;以(Y0.7Gd0.3)3Al5O12:3.3%Ce~(3+)熒光膜所封裝的白光LED的發(fā)光效率為88 lm/W,色溫為4356 K,顯色指數(shù)達78.3,而以(Y0.25Gd0.75)3Al5O12:3.3%Ce~(3+)熒光膜所封裝的白光LED,有著更高的顯色指數(shù)81.2。5.論文研究了在YAG母體中Ce~(3+)→Eu~(3+)與Ce~(3+)→Pr~(3+)能量傳遞過程對熒光膜發(fā)光特性的影響,YAG:Ce~(3+)/Eu~(3+)與YAG:Ce~(3+)/Pr~(3+)熒光膜在紅光區(qū)的發(fā)光性能均得到了提高,分別在610 nm與611 nm出現(xiàn)了尖銳的發(fā)光峰。Eu~(3+)的共摻雜會引起母體中的Ce~(3+)離子發(fā)生熒光猝滅,因此,雖然其在紅光區(qū)的發(fā)光得到了提高,但熒光膜的整體發(fā)光強度大幅度的下降;在YAG:Ce~(3+)/Pr~(3+)熒光膜中,當Pr~(3+)的摻雜濃度小于0.75%時,發(fā)光光譜的強度仍可保持在95%以上。首次制備的Y0.7Gd0.3AG:3.3%Ce~(3+),0.5%Pr~(3+)熒光膜的發(fā)光峰紅移到550 nm,在611 nm的尖銳的紅光發(fā)射峰,其發(fā)光光譜強度相對YAG:3.3%Ce~(3+)也得到了提高,對封裝的白光LED性能得到了改善,發(fā)光效率為84 lm/W,顯色指數(shù)為83.4,色溫為4327 K。6.論文以共摻雜能量傳遞敏化劑來增強熒光膜對激發(fā)光的吸收能力而提高了所制備熒光膜的發(fā)光特性。由于母體中含有高濃度的激發(fā)躍遷為4f→5d的Tb~(3+)離子,所制備的YTb AG:5%Eu~(3+)與YTb AG:3.3%Ce~(3+)在紫外區(qū)有著超強吸收峰,因此在275 nm激發(fā)條件下,在能量傳遞的作用下增強了所制備熒光膜的發(fā)光光譜強度。所制備的YTb AG:3.3%Ce~(3+)熒光膜在275 nm激發(fā)下有著明亮的黃綠光發(fā)射;YTb AG:x%Eu~(3+)熒光膜有可調(diào)控的發(fā)光性能,隨著Eu~(3+)熒濃度從0%增大5%,發(fā)光可從綠光向黃綠光、黃光、橙黃光、橙紅光、紅光轉(zhuǎn)變。
[Abstract]:YAG:Ce~ (3+) phosphor conversion white light LED has the advantages of high luminous efficiency, low energy consumption, long life and safety and so on. It is a new generation of all solid state lighting source, which occupies an incomparable position in the lighting market. However, commercial YAG:Ce~ (3+) phosphor particles are large and irregular in irregular distribution, inevitably producing back reflection and Back scattering results in a decrease in the efficiency of energy conversion; in addition, the differential thermal conductivity of the phosphor / epoxy layer causes the quenching of the temperature of the fluorescent material. The epoxy resin layer will be yellowed or fall off for a long time, reducing the stability and life of the white LED. The transparent YAG:Ce~ (3+) fluorescent film has smaller and more uniform particle sizes, and more Strong adhesion and better thermal conductivity, especially with small back reflection and backscattering effect, are considered to be a good fluorescent conversion layer of white LED, which is concerned by many researchers. The starting point of this paper is the preparation of rare earth doped YAG fluorescent films which can be applied to white light LED with high luminescence performance. The results obtained are as follows: 1 The effect of the sputtering power, oxygen content and annealing process on the deposition rate and properties of the YAG:3.3%Ce~ (3+) fluorescent film on a quartz substrate was systematically studied by using a powder target on a quartz substrate. The deposition rate of the film was increased by 1.2 Mu as the surface binding energy of the powder target atom was lower than the traditional high temperature sintered ceramic target. M/h. sputtering 2H under the optimum process conditions, the thickness of the deposited film is 2.92 u m, and is sintered at 1100 C in H2/Ar reduction atmosphere for 10 h, and the film is pure phase YAG film. Under the excitation of 450 nm, the luminescent quantum yield reaches 23%.2. using high solubility glycol as sol-gel solvent, and the preparation of YAG:3.3%Ce~ (3+) fluorescent film under high concentration sols is achieved. The film is 40 layers, and the prepared YAG:Ce~ (3+) fluorescent film is packed closely with 80 nm particles. The YAG:Ce~ (3+) fluorescent film with a thickness of 4.3 M. has good transmittance in the visible region, while the blue light region has a strong absorption peak and a quantum yield of 47%, which can be used as the raw material for the fluorescent conversion layer.3. in the white light LED, with nitrate as raw material, urea. The YAG:3.3%Ce~ (3+) fluorescent film was prepared by the sol combustion method with the amino acetic acid at a lower temperature. The 40 layer of the film was repeated on the 40 layer. The film layer was close to 50 nm particles, and the YAG:3.3%Ce~ (3+) fluorescent film prepared by the film thickness reached a strong absorption peak in the blue light region, and the wavelength was more than 500 nm with a good penetration. Photoluminescence, luminescence quantum yield up to 56%. YAG:3.3%Ce~ (3+) fluorescent film can be applied to the encapsulation of white light LED. Under 8V voltage and 100 m A current, the luminous efficiency is 82 lm/W, color temperature is 4536K, and the color index is 75.6.4. study on the effect of garnet matrix structure on Ce~ (3+) luminescence specificity. (3+) the position of the 12 sides will increase the crystal field splitting energy and the lattice distortion effect. Therefore, the half peak width and peak wavelength of the luminescence spectrum of Ce~ (3+) show broadening and red shift. The half peak width of the luminescence spectrum is broadened with scandium ions instead of aluminum ions, but the red shift does not occur. The proper increase of the cell volume of garnet can reduce the Ce~ (3+) hair. The probability of fluorescence quenching can improve the luminescence intensity of Ce~ (3+); the widening and redshift of the Ce~ (3+) luminescence peak effectively improve the luminescence of the white light LED. The luminous efficiency of the white light LED encapsulated by TAG:3.3%Ce~ (3+) fluorescent film is 72 lm/W, the color temperature is 4888 K, the color index is 79.2, and the (Y0.7Gd0.3) 3Al5O12:3.3%Ce~ (Y0.7Gd0.3) fluorescent membrane is encapsulated in white. The luminous efficiency of the light LED is 88 lm/W, the color temperature is 4356 K, the color index is 78.3, and the white light LED encapsulated with the (Y0.25Gd0.75) 3Al5O12:3.3%Ce~ (3+) fluorescent film has a higher color rendering index 81.2.5.. The effect of Ce~ (3+), Eu~ (3+) and energy transfer process on the luminescence properties of the fluorescent membrane in the YAG matrix is studied. (3 The luminescence properties of /Eu~ (3+) and YAG:Ce~ (3+) /Pr~ (3+) fluorescent films in the red light region have been improved, and the co doping of the sharp luminescence peak.Eu~ (3+) at 610 nm and 611 nm, respectively, will cause the fluorescence quenching of Ce~ (3+) ions in the parent body, therefore, although the luminescence in the red region is improved, the overall luminescence intensity of the fluorescent film is obtained. In the YAG:Ce~ (3+) /Pr~ (3+) fluorescence film, when the doping concentration of Pr~ (3+) is less than 0.75%, the intensity of the luminescence spectrum can still remain above 95%. The first prepared Y0.7Gd0.3AG:3.3%Ce~ (3+), the 0.5%Pr~ (3+) fluorescent film red shift to the 550 nm, the sharp red emission peak in the 611 nm, its luminescence spectral intensity relative to Ce~ (3+) has also been improved. The performance of the encapsulated white light LED is improved, the luminescence efficiency is 84 lm/W, the color rendering index is 83.4, the color temperature is 4327 K.6., and the Co doped energy transfer sensitizer is used to enhance the absorption ability of the fluorescence film to the stimulated luminescence. The transition is 4f to 5D Tb~ (3+), and the prepared YTb AG:5%Eu~ (3+) and YTb AG:3.3%Ce~ (3+) have a super absorption peak in the ultraviolet region. Therefore, under the condition of 275 nm excitation, the luminescent spectral intensity of the prepared fluorescent film is enhanced under the action of energy transfer. Green light emission; YTb AG:x%Eu~ (3+) fluorescence film has a controllable luminescence performance. With the increase of 5% of Eu~ (3+) concentration from 0%, the luminescence can change from green light to Huang Lvguang, yellow, orange, orange, red and red light.
【學位授予單位】：電子科技大學
【學位級別】：博士
【學位授予年份】：2016
【分類號】：TN104.3;TN312.8

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