Green BaSi2O2N2:0.02Eu2+ phosphor is synthesized through a two-step solid state reaction method. The first firing is for crystallization, and the second firing is for reduction of Eu3+ into Eu2+ and growth of crystal grains. By thermal analysis, the three-time endothermic reaction is confirmed: pyrolysis reaction of BaCO3 at 900 oC and phase transitions at 1,300 oC and 1,400 oC. By structural analysis, it is confirmed that single phase [BaSi2O2N2] is obtained with Cmcm space group of orthorhombic structure. After the first firing the morphology is rod-like type and, after the second firing, the morphology becomes round. Our phosphor shows a green emission with a peak position of 495 nm and a peak width of 32 nm due to the 4f65d1→4f7 transition of Eu2+ ion. An LED package (chip size 5.6 x 3.0 mm) is fabricated with a mixture of our green BaSi2O2N2, and yellow Y3Al5O12 and red Sr2Si5N8 phosphors. The color rendering index (90) is higher than that of the mixture without our green phosphor (82), which indicates that this is an excellent green candidate for white LEDs with a deluxe color rendering index.
We have synthesized bluish-green, highly-efficient BaSi2O2N2:Eu2+ and (Ba,Sr)Si2O2N2:Eu2+ phosphors through aconventional solid state reaction method using metal carbonate, Si3N4, and Eu2O3 as raw materials. The X-ray diffraction (XRD)pattern of these phosphors revealed that a BaSi2O2N2 single phase was obtained. The excitation and emission spectra showedtypical broadband excitation and emission resulting from the 5d to 4f transition of Eu2+. These phosphors absorb blue light ataround 450nm and emit bluish-green luminescence, with a peak wavelength at around 495 nm. From the results of anexperiment involving Eu concentration quenching, the relative PL intensity was reduced dramatically for Eu=0.033. A smallsubstitution of Sr in place of Ba increased the relative emission intensity of the phosphor. We prepared several white LEDsthrough a combination of BaSi2O2N2:Eu2+, YAG:Ce3+, and silicone resin with a blue InGaN-based LED. In the case of onlythe YAG:Ce3+-converted LED, the color rendering index was 73.4 and the efficiency was 127lm/W. In contrast, in theYAG:Ce3+ and BaSi2O2N2:Eu2+-converted LED, two distinct emission bands from InGaN (450nm) and the two phosphors (475-750nm) are observed, and combine to give a spectrum that appears white to the naked eye. The range of the color renderingindex and the efficiency were 79.7-81.2 and 117-128 lm/W, respectively. The increased values of the color rendering indexindicate that the two phosphor-converted LEDs have improved bluish-green emission compared to the YAG:Ce-converted LED.As such, the BaSi2O2N2:Eu2+ phosphor is applicable to white high-rendered LEDs for solid state lighting.