Engineering of K3YSi2O7 To Tune Photoluminescence with Selected Activators and Site Occupancy

Qiao, Jianwei; Amachraa, Mahdi; Molokeev, Maxim; Chuang, Yu-Chun; Ong, Shyue Ping; Zhang, Qinyuan; Xia, Zhiguo Source: CHEMISTRY OF MATERIALS, 31 (18):7770-7778; 10.1021/acs.chemmater.9b02990 SEP 24 2019

The luminescence of rare earth ions (Eu2+, Ce3+, and Eu3+)-doped inorganic solids is attractive for the screening of phosphors applied in solid-state lighting and displays and significant to probe the occupied crystallographic sites in the lattice also offering new routes to photoluminescence tuning. Here, we report on the discovery of the Eu- and Ce-activated K3YSi2O7 phosphors. K3YSi2O7:Eu is effectively excited by 450 nm InGaN blue light-emitting diodes (LEDs) and displays an orange-red emission originated from characteristic transitions of both Eu2+ and Eu3+, while K3YSi2O7:Ce3+ shows green emission upon 394 nm near-ultraviolet (NUV) light excitation. Rietveld refinement verifies the successful doping of the activators, and density functional theory (DFT) calculations further support that Eu2+ occupies both K1 and Y2 crystallographic sites, while Ce3+ and Eu3+ only occupy the Y2 site; hence, the broad-band red emission of Eu2+ are attributed to a small DFT band gap (3.69 eV) of K3YSi2O7 host and a selective occupancy of Eu2+ in a highly distorted K1 site and a high crystal field splitting around Y2 sites. The white LEDs device utilizing orange-red-emitting K3YSi2O7:Eu and green-emitting K3YSi2O7:Ce3+ exhibits an excellent CRI of 90.1 at a correlated color temperature of 4523 K. Our work aims at bridging multivalent Eu2+/Eu3+ and Ce3+ site occupancy in the same host to realize photoluminescence tuning and especially exposes new ways to explore new phosphors with multicolor emission pumped by blue and NUV light for white LEDs.


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