A modified structure Ca(MgAl)(SiAl)O (denoted as CMASO) from the evolution of CaMgSiO (denoted as CMSO) codoped with Ce and Tb ions was designed successfully by solid reaction method for application in phosphor-converted white-light-emitting diode (pc-wLED). The Rietveld refinement of these two structures verified the changes derived from the replacement of some of the Mg and Si ions by Al ions. The band gaps were calculated by density-functional theory (DFT) calculation method to verify the change of Al ions replacing further, and the diffuse reflectance spectra (DRS) proved the veracity of the calculation result. The phosphors CMASO:Ce showed blue emission excited by a wider excitation wavelength from 280 nm to 370 nm. The change of structure lead to the absorbable range broaden and the emission peak shifted to longer wavelength, compared with CMSO:Ce, although the amount of emitting center was the same. The reason for these phenomena was discussed in detail. The codoped phosphors CMASO:Ce,Tb exhibited different emission colors from blue to green as the concentration of Tb ions increased. Combined with commercial red phosphor CaAlSiN:Eu and ultraviolet LED (UV-LED) chips, the selected appropriate samples achieved white emission. The correlated color temperature (CCT) was 6137 K and the color rendering index (Ra) was 80.5, indicating that they could act as potential phosphors for possible applications in pc-wLED.
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