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Femtosecond Laser Induced Luminescence in Hierarchically Structured Nd3+,Yb3+,Er3+ Co-Doped Upconversion Nanoparticles: Light-Matter Interaction Mechanisms from Experiments and Simulations

Guilherme Oliveira, Flávia de Sousa Ferreira, Guilherme Ferreira Ferbonink, Marcos Paulo Belançon, Fernando Aparecido Sigoli, Rene Alfonso Nome

Published Sep 14, 2020• 0 citations
Publisher

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 NdIII, YbIII, and ErIII. 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 9 NdIII levels, 2 YbIII, and 7 ErIII levels 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.

DOI
10.26434/chemrxiv.12949310

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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 NdIII, YbIII, and ErIII. 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 9 NdIII levels, 2 YbIII, and 7 ErIII levels 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.
Abstract Controlling the up-conversion luminescence of rare-earth ions in real-time, in a dynamical and reversible manner, is very important for their application in laser sources, fiber-optic communications, light-emitting diodes, color displays and biological systems. In previous studies, the up-conversion luminescence control mainly focused on the weak femtosecond laser field. Here, we further extend this control behavior from weak to intermediate femtosecond laser fields. In this work, we experimentally and theoretically demonstrate that the up-conversion luminescence in Dy 3+ ion doped glass can be artificially controlled by a π phase step modulation, but the up-conversion luminescence control behavior will be affected by the femtosecond laser intensity, and the up-conversion luminescence is suppressed by lower laser intensity while enhanced by higher laser intensity. We establish a new theoretical model (i.e. the fourth-order perturbation theory) to explain the physical control mechanism by considering the two- and four-photon absorption processes, and the theoretical results show that the relative weight of four-photon absorption in the whole excitation process will increase with the increase in laser intensity, and the interference between two- and four-photon absorptions results in up-conversion luminescence control modulation under different laser intensities. These theoretical and experimental works can provide a new method to control and understand up-conversion luminescence in rare-earth ions, and also may open a new opportunity to the related application areas of rare-earth ions.
Continuous-wave lasers in which the emitted photon energy may be up to three times greater than that of the incident pump light by virtue of cooperative (coupled atom) upconversion processes are reported for the first time in this thesis. Cw upconversion laser action was obtained at wavelengths of 0.55μ\muμm, 0.70μ\muμm, 0.85μ\muμm and 2.8μ\muμm using infrared excitation in the range λ\lambdaλ = 1.48-1.70μ\muμm in concentrated crystals of Er:CaF$\sb2$ and Er:LiYF$\sb4$. Detailed aspects of the behavior and internal dynamics of these systems have been considered both experimentally and theoretically in this work. Two limiting approaches were applied to gain theoretical insight into possible unique features of cooperative upconversion lasers. These corresponded to strong and weak coupling theories. A density matrix approach describing the strong coupling limit predicted several new results of cooperative interactions, including enhanced quantum efficiency, enhanced energy transfer, and cooperative instabilities. A rate equation analysis appropriate to weaker coupling was used to confirm that cooperative upconversion lasers can operate continuously on self-terminating transitions and established threshold conditions for pair- and trio-pumped lasers. Time dependent upconversion fluorescence measurements were performed to investigate the pumping mechanism of the new lasers experimentally. These observations and measurement of the intensity dependence of upconversion emission established that the inversion mechanism was exclusively cooperative in nature. Upconversion laser instabilities were also studied and related to nonlinear, cooperative dynamics. Unique features of cooperative upconversion lasers were identified, compared with other upconversion pumping schemes, and exploited to demonstrate the first cw mode-locked solid state laser operating in the visible spectral range. On the basis of this work, it may be concluded that cooperative upconversion provides a practical means of generating coherent radiation in new spectral regions, even on self-terminating transitions.
Upconversion luminescence (UCL) of lanthanide-doped nanomaterials is usually a low-efficiency nonlinear process, involving multi-step, multi-channel transitions in a multi-level system. Here, we demonstrate quantum control and enhancement of multi-color (e.g., red and green) UCLs of NaYF4:Yb3+/Er3+ nanoparticles with metallic Fabry-Perot micro-cavities. Besides realization of controlled single-color UCLs, their internal quantum efficiencies are strongly enhanced, up to 3–4 orders of times. Experimental results indicate that the controlled single-color UCLs and enhancements are caused not only by modifications of the spontaneous radiation rates for the red- and green-color transitions but also by influencing the intermediate transitions to result in modified distributions of electrons in each of the multiple Er3+ levels, facilitating emission of either red- or green-color light. This work suggests a way to control photon emissions in systems with multi-channel transitions and/or multi-step excitations.
Abstract Photon upconversion through lanthanide-doped nanoparticles is of great significance for various applications. However, the current development of upconversion nanoparticles is hindered by the low quantum efficiency and long radiative lifetimes of lanthanide ions, restricting their applications in time-dependent nanophotonics. Herein, we report ultrafast upconversion superfluorescence with a lifetime of sub-2.5 ns in lanthanide-doped nanoparticles at room temperature. Upon excitation with an 800-nm fs-pulsed laser, we achieve a large number ( N = 912) of correlated dipoles in Nd 3+ -concentrated nanoparticles, resulting in collective coherent emission with two orders of magnitude amplification in intensity and more than three orders of magnitude improvement in the radiative decay rate. Furthermore, we demonstrate that the control of excitation power and emitting sample length enables the lifetime manipulation of upconversion emission in a wide range from μs to sub-ns, accompanied by the typical superfluorescence signature of Burnham-Chiao ringing. These findings may benefit applications in many advanced technologies such as quantum counting and high-speed super-resolution bioimaging.
In this work, we have investigated experimentally and theoretically the process of frequency upconversion at low temperatures in rare earth doped vitreous samples. A sample of chalcogenide glass doped with erbium ions (Er3+) was pumped with a laser source at 1.54 μm. We have observed, at room temperature, three different emission bands around 530 nm, 555 nm and 670 nm, originating from the excited state erbium levels 2H11/2, 4S3/2 and 4F9/2 to the 4I15/2 ground-state, respectively. A cryogenic system cooled the sample down to 4 K, and we have recorded many spectra in this range of temperature. We have observed relative increase in the intensity of the green fluorescence, which comes from the level 4S3/2, and also the vanishing emission of the 530 nm line around 210 K. For all emission lines, the frequency upconversion process has been accounted for with three photons absorbed from the pumping source, but saturation effects were observed above 10 mW of incident power. We have made a theoretical treatment of the experimental data and a numeric simulation, which has revealed that the observed behaviors are related to processes that involve step-wise photon absorption and phonon assisted nonradiative decay, both dependent on the temperature and phonon energy of the sample. We also present, in the third chapter, an analytic treatment of pulse propagation in nonlinear media. We have used a variational approach to predict the behavior of an optical pulse propagating in the vicinity of a two-photon resonance, where the third order nonlinearities may be enhanced and limits optical devices development. A possible solution for the problem is the propagation of a pulse with suitable profile and frequency chirp resulting in a balancing of the nonlinear effects.