期刊
NANOSCALE
卷 9, 期 12, 页码 4283-4294出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7nr00092h
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- Federal Ministry of Economics and Technology [BMWI-13/09, BMWI-11/12]
- German Research Council (German Research Foundation (DFG) [WO 669/12-1, RE 1203/18-1]
The rational design of brighter upconversion nanoparticles (UCNPs) requires a better understanding of the radiationless deactivation pathways in these materials. Here, we demonstrate the potential of excitation power density (P)-dependent studies of upconversion (UC) luminescence intensities, slope factors, and absolute quantum yields (Phi(UC)) of popular beta-NaYF4: 20% Yb3+, 2% Er3+ UCNPs of different surface chemistries in organic solvents, D2O, and water as a tool to gain deeper insight into the UC mechanism including population and deactivation pathways particularly of the red emission. Our measurements, covering a P regime of three orders of magnitude, reveal a strong difference of the P-dependence of the ratio of the green and red luminescence bands (I-g/(r)) in water and organic solvents and P-dependent population pathways of the different emissive energy levels of Er3+. In summary, we provide experimental evidence for three photon processes in UCNPs, particularly for the red emission. Moreover, we demonstrate changes in the excited population dynamics via bi- and triphotonic processes dependent on the environment, surface chemistry, and P, and validate our findings theoretically.
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