Abstract
Ensemble and single particle studies of the excitation power density (P)-dependent upconversion luminescence (UCL) of core and core-shell β-NaYF4:Yb,Er upconversion nanoparticles (UCNPs) doped with 20% Yb3+ and 1% or 3% Er3+ performed over a P regime of 6 orders of magnitude reveal an increasing contribution of the emission from high energy Er3+ levels at P > 1 kW/cm2. This changes the overall emission color from initially green over yellow to white. While initially the green and with increasing P the red emission dominate in ensemble measurements at P < 1 kW/cm2, the increasing population of higher Er3+ energy levels by multiphotonic processes at higher P in single particle studies results in a multitude of emission bands in the ultraviolet/visible/near infrared (UV/vis/NIR) accompanied by a decreased contribution of the red luminescence. Based upon a thorough analysis of the P-dependence of UCL, the emission bands activated at high P were grouped and assigned to 2–3, 3–4, and 4 photonic processes involving energy transfer (ET), excited-state absorption (ESA), cross-relaxation (CR), back energy transfer (BET), and non-radiative relaxation processes (nRP). This underlines the P-tunability of UCNP brightness and color and highlights the potential of P-dependent measurements for mechanistic studies required to manifest the population pathways of the different Er3+ levels.
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Acknowledgements
The authors thank the European Upconversion Network (EUN) for financial support of a research exchange program (COST-CM1403). U. R.-G., F. F. and C. W. acknowledge financial support by research grants RE 1203/20-1 (project NANOHYPE; DFG and M-Eranet). Y. M. is grateful to the Institut Universitaire de France (IUF) for support and providing additional time to be dedicated to research.
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Multiband emission from single β-NaYF4(Yb,Er) nanoparticles at high excitation power densities and comparison to ensemble studies
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Frenzel, F., Würth, C., Dukhno, O. et al. Multiband emission from single β-NaYF4(Yb,Er) nanoparticles at high excitation power densities and comparison to ensemble studies. Nano Res. 14, 4107–4115 (2021). https://doi.org/10.1007/s12274-021-3350-y
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DOI: https://doi.org/10.1007/s12274-021-3350-y