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• W3128299118 endingPage "117953" @default.
• W3128299118 startingPage "117953" @default.
• W3128299118 abstract "Fundamental studies of light-matter interactions are important for basic knowledge and in applications. Thanks to advances in experimental and theoretical methods, nowadays it is possible to perform such studies in a broad dynamic range, covering timescales from that of elementary interactions to real time. In the present work, we perform an experimental-theoretical study of light intensity-dependent femtosecond and CW-laser induced frequency upconversion in hierarchically structured core-multishell nanoparticles co-doped with Nd III , Yb III , and Er III . Upconversion spectra recorded with CW and femtosecond excitation are qualitatively similar whereas the intensity dependence of upconversion depends on excitation mode (CW or femtosecond). To further assess the observed intensity dependence, we perform light-matter interaction simulations in the dynamic range from 100 fs to 3 ms for 18-level system describing the UCNPs, including nine levels of the Nd III , two of the Yb III , and seven of the Er III ions and a classical model for the excitation source. The calculated time- and intensity-dependent energy level population are compared with measured spectra to understand CW vs femtosecond laser-induced upconversion. To further discuss the differences between CW and femtosecond laser-induced light-matter interactions for the systems studied here, we perform semi-classical pulse propagation simulations and ultrafast pump-probe measurements to study how the light source bandwidth, relative to the absorption linewidth, influence light absorption and transmission and further connect these results with the intensity dependence. Overall, we report our progress toward mechanistic studies of light-matter interaction and photophysical pathways following femtosecond excitation and UCNPs. • Core@shell UCNP upconversion was investigated with CW and femtosecond laser. • For same average power, different upconversion mechanism with CW vs. femtosecond. • 18-level system modeling of Nd III Yb III Er III to understand experimental results. • CW/femtosecond power-dependent upconversion can be treated on the same footing. • Excitation bandwidth of CW/femtosecond source also affects UCNP photophysics." @default.
• W3128299118 created "2021-02-15" @default.
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• W3128299118 date "2021-06-01" @default.
• W3128299118 modified "2023-10-14" @default.
• W3128299118 title "Femtosecond laser induced luminescence in hierarchically structured NdIII, YbIII, ErIII co-doped upconversion nanoparticles: Light-matter interaction mechanisms from experiments and simulations" @default.
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• W3128299118 doi "https://doi.org/10.1016/j.jlumin.2021.117953" @default.
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