Trivalent terbium (Tb 3+ )‐activated luminescence materials usually show highly efficient green emission with the full width at half maximum of merely 10 nm, but suffer from the unsatisfactory excitable wavelength (<380 nm) as well as the inefficient light absorption. Here, the realization of efficient visible light excitation of Tb 3+ is demonstrated in terbium‐concentrated garnet Ca 2 TbHf 2 Al 3 O 12 (CTHA) by introducing Ce 3+ as the sensitizer. Owing to highly efficient energy transfer from Ce 3+ to Tb 3+ , CTHA:Ce 3+ combines advantages of the extra narrow green emission of Tb 3+ peaking at 544 nm and the efficient broad excitation of Ce 3+ covering the short‐wavelength visible light from 380 to 450 nm. The color gamut of the prototype white light‐emitting diode (LED) by using CTHA:Ce 3+ as the green emitter can reach 95% (coverage ratio) of National Television Standards Committee (NTSC) space in Commission Internationale de L'Eclairage (CIE) 1931, indicating its great potential for LED (or laser diode)‐based applications.
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