A Synergy Approach to Enhance Upconversion Luminescence Emission of Rare Earth Nanophosphors with Million-Fold Enhancement Factor

Lanthanide (Ln(3+))-doped upconversion nanoparticles (UCNPs) offer an ennormous future for a broad range of biological applications over the conventional downconversion fluorescent probes such as organic dyes or quantum dots. Unfortunately, the efficiency of the anti-Stokes upconversion luminescence (UCL) process is typically much weaker than that of the Stokes downconversion emission. Albeit recent development in the synthesis of UCNPs, it is still a major challenge to produce a high-efficiency UCL, meeting the urgent need for practical applications of enhanced markers in biology. The poor quantum yield efficiency of UCL of UCNPs is mainly due to the fol-lowing reasons: (i) the low absorption coefficient of Ln(3+) dopants, the specific Ln(3+) used here being ytterbium (Yb3+), (ii) UCL quenching by high-energy oscillators due to surface defects, impurities, ligands, and solvent molecules, and (iii) the insufficient local excitation intensity in broad-field il-lumination to generate a highly efficient UCL. In order to tackle the problem of low absorption cross-section of Ln3+ ions, we first incorporate a new type of neodymium (Nd3+) sensitizer into UCNPs to promote their absorption cross-section at 793 nm. To minimize the UCL quenching induced by surface defects and surface ligands, the Nd3+-sensitized UCNPs are then coated with an inactive shell of NaYF4. Finally, the excitation light intensity in the vicinity of UCNPs can be greatly enhanced using a waveguide grating structure thanks to the guided mode resonance. Through the synergy of these three approaches, we show that the UCL intensity of UCNPs can be boosted by a million-fold compared with conventional Yb3+-doped UCNPs.