“…Over the past several decades, due to the great demand for broad applications of trivalent rare earth (RE)-doped inorganic crystals, − research has focused on the effect of material structure on energy transfer (ET) and the resultant photoluminescence (PL) of RE ions, from theory to technology, such as Judd–Ofelt theory, Dexter theory, crystallinity, size, morphology, absorption, lattice relaxation, and radiative and nonradiative relaxation (NR) processes. − However, this enormous scope of research also means that there is a need for new perspectives in the in-depth study of RE-doped materials; otherwise, fundamental breakthroughs in material structure design and PL control cannot be achieved. In this work, we find for the first time the ET inhibition of RE ions via efficient vertical photocarrier separation, triggered by a highly anisotropic layered semiconductor.…”