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NaYbF4 upconverting nanoparticles (UCNPs) have enhanced optical properties compared to the NaYF4 UCNPs. However, synthesis of monodisperse NaYbF4 with controllable size and optical properties poses challenges, and the mechanism of phase transformation remains to be understood. Here, they report on the effect of Na+/Yb3+ molar ratio on the morphological and optical properties of upconverting NaYbF4: 2% Er3+ nanoparticles. Controllable transformation of cubic phase nanoparticles produced with [Na+]/[Yb3+] = 1 to hexagonal phase is achieved by increasing Na+ content. The hexagonal UCNPs produced with [Na+]/[Yb3+] = 4 have significantly enhanced intensity of optical emission of ≈600 times compared with the pure cubic phase crystal. The work reveals that the increasing dislocation of sodium and ytterbium distribution cause the accumulation of the lattice strain with increasing Na+ content, and triggers the lattice strain‐mediated phase transformation in cubic cell, as confirmed by the Density Function Theory simulations. These results provide new insights into the growth of UCNPs and pave the way for developing controlled synthesis of UCNPs for applications as bio‐probes and for energy harvesting. [ABSTRACT FROM AUTHOR]

NaYbF4 upconverting nanoparticles (UCNPs) have enhanced optical properties compared to the NaYF4 UCNPs. However, synthesis of monodisperse NaYbF4 with controllable size and optical properties poses challenges, and the mechanism of phase transformation remains to be understood. Here, they report on the effect of Na+/Yb3+ molar ratio on the morphological and optical properties of upconverting NaYbF4: 2% Er3+ nanoparticles. Controllable transformation of cubic phase nanoparticles produced with [Na+]/[Yb3+] = 1 to hexagonal phase is achieved by increasing Na+ content. The hexagonal UCNPs produced with [Na+]/[Yb3+] = 4 have significantly enhanced intensity of optical emission of ≈600 times compared with the pure cubic phase crystal. The work reveals that the increasing dislocation of sodium and ytterbium distribution cause the accumulation of the lattice strain with increasing Na+ content, and triggers the lattice strain‐mediated phase transformation in cubic cell, as confirmed by the Density Function Theory simulations. These results provide new insights into the growth of UCNPs and pave the way for developing controlled synthesis of UCNPs for applications as bio‐probes and for energy harvesting. [ABSTRACT FROM AUTHOR]