Power-dependent upconversion quantum yield of NaYF 4 :Yb 3+ ,Er 3+ nano- and micrometer-sized particles - measurements and simulations

Photophysical studies of nonlinear lanthanide-doped photon upconverting nanoparticles (UCNPs) increasingly used in biophotonics and photovoltaics require absolute measurements of the excitation power density (P)-dependent upconversion luminescence (UCL) and luminescence quantum yields (Φ ) for quantifying the material performance, UCL deactivation pathways, and possible enhancement factors. We present here the P-dependence of the UCL spectra, Φ , and slope factors of the different emission bands of representative 25 nm-sized oleate-capped β-NaYF :17% Yb , 3% Er UCNPs dispersed in toluene and as powder as well as Φ of 3 μm-sized upconversion particles (UCμP), all measured with a newly designed integrating sphere setup, enabling controlled variation of P over four orders of magnitude. This includes quantifying the influence of the beam shape on the measured Φ and comparison of experimental Φ with simulations utilizing the balancing power density model of the Andersson-Engels group and the simulated Φ of UCμP from the Berry group, underpinned by closely matching decay kinetics of our UC material. We obtained a maximum Φ of 10.5% for UCμP and a Φ of 0.6% and 2.1% for solid and dispersed UCNPs, respectively. Our results suggest an overestimation of the contribution of the purple and an underestimation of that of the red emission of β-NaYF :Yb ,Er : microparticles by the simulations of the Berry group. Moreover, our measurements can be used as a guideline to the absolute determination of UCL and Φ .