Strategic Tuning of Photophysical Response in the Polyhedral Framework of the Garnet Structure toward White Light-Emitting Devices with Enhanced Color Rendering.

Designing a single-phase phosphor with high quantum efficiency and full spectrum emission is inevitable for today's scientific world. Herein, an optimal strategy for realizing white emission in a single component matrix is envisaged based on the structure-property-design-device policy. Cationic substitution corresponding to polyhedral expansion and contraction in AA'BVO confirms the existence of strong and intricate linkage in the garnet structure. The dodecahedral expansion causes compression of VO tetrahedra and a blue shift. The direct correlation of V-O bond distance with red shift validates the distortion of the VO tetrahedra. The interdependence of photophysical properties via cationic substitution and subsequent correlation of the V-O bond distance with emission bands enabled the tailoring of phosphor-CaSrNaMgVO with a high quantum efficiency of 52% and excellent thermal stability of 0.39 eV. Bright warm white light-emitting diode (WLED) devices are fabricated based on Eu and Sm-activators. A high quantum efficiency-74% is obtained for the designed Eu phosphor. CIE coordinates near the achromatic point (0.329, 0.366), low CCT-5623 K, and high color rendering index (CRI)-87 are obtained for the single-phase WLED device. This work puts forth a new direction for designing and engineering promising WLEDs with enhanced color rendering based on single-phase phosphors with full spectrum emission.