We assessed the influence of Yb^3+ and Er34 dopant concentration on the relative spectral distribution, quantum yield (Фuc), and decay kinetics of the upconversion luminescence (UCL) and particle brightness (BUC) for...We assessed the influence of Yb^3+ and Er34 dopant concentration on the relative spectral distribution, quantum yield (Фuc), and decay kinetics of the upconversion luminescence (UCL) and particle brightness (BUC) for similarly sized (33 nm) oleate-capped p-NaYF4:Yb3t,Er^3+ upconversion (UC) nanoparticles (UCNPs) in toluene at broadly varied excitation power densities (F). This included an Yb^3+ series where the Yb^3+ concentration was varied between 11%—21% for a constant Er^3+ concentration of 3%, and an Er^3+ series, where the Er^3+ concentration was varied between 1%-4% for a constant Yb^3+ concentration of 14%. The results were fitted with a coupled rate equation model utilizing the UCL data and decay kinetics of the green and red Er34 emission and the Yb34 luminescence at 980 nm. An increasing Yb34 concentration favors a pronounced triphotonic population of 4F9/2 at high P by an enhanced back energy transfer (BET) from the 4G11/2 level. Simultaneously, the Yb^3+-controlled UCNPs absorption cross section overcompensates for the reduction in Фuc with increasing Yb^3+ concentration at high P, resulting in an increase in Sue. Additionally, our results show that an increase in Yb34 and a decrease in Er^3+ concentration enhance the color tuning range by P. These findings will pave the road to a deeper understanding of the energy transfer processes and their contribution to efficient UCL, as well as still debated trends in green-to-red intensity ratios of UCNPs at different P.展开更多
文摘We assessed the influence of Yb^3+ and Er34 dopant concentration on the relative spectral distribution, quantum yield (Фuc), and decay kinetics of the upconversion luminescence (UCL) and particle brightness (BUC) for similarly sized (33 nm) oleate-capped p-NaYF4:Yb3t,Er^3+ upconversion (UC) nanoparticles (UCNPs) in toluene at broadly varied excitation power densities (F). This included an Yb^3+ series where the Yb^3+ concentration was varied between 11%—21% for a constant Er^3+ concentration of 3%, and an Er^3+ series, where the Er^3+ concentration was varied between 1%-4% for a constant Yb^3+ concentration of 14%. The results were fitted with a coupled rate equation model utilizing the UCL data and decay kinetics of the green and red Er34 emission and the Yb34 luminescence at 980 nm. An increasing Yb34 concentration favors a pronounced triphotonic population of 4F9/2 at high P by an enhanced back energy transfer (BET) from the 4G11/2 level. Simultaneously, the Yb^3+-controlled UCNPs absorption cross section overcompensates for the reduction in Фuc with increasing Yb^3+ concentration at high P, resulting in an increase in Sue. Additionally, our results show that an increase in Yb34 and a decrease in Er^3+ concentration enhance the color tuning range by P. These findings will pave the road to a deeper understanding of the energy transfer processes and their contribution to efficient UCL, as well as still debated trends in green-to-red intensity ratios of UCNPs at different P.
