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Journal of Applied Spectroscopy

The influence of reverse excitation transfer on donor and acceptor fluorescence decay: Monte Carlo simulations

Leszek Kułak, R. Twardowski, Czeslaw Bojarski

Published Jul 1, 1995• 0 citations
Publisher
DOI
10.1007/bf02606527

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We investigate homogeneous upconversion (HUC) assisted decay of the population inversion in Er-doped silica after delta-pulse excitations by means of Monte Carlo simulations. We derive an analytic expression for this decay when energy migration among Er is negligible and show that it is essentially an extension of the Fo/spl uml/rster-type donor-acceptor quenching decay for the case when donor and acceptor ions are the same species. We compare HUC during the decay to HUC while pumping CW and show that they considerably differ at the low and moderate Er concentrations. Based on Monte Carlo (MC) simulations, we construct a heuristic approximation to the HUC assisted decay, which makes our MC results readily available for the future experimental and theoretical studies and provides simple means for determination of HUC parameters by fitting to experimental data.
We have investigated the process of quenching of fluorescence from the 3P0^{3}P_{0}3P0​ state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in La0.72{\mathrm{La}}_{0.72}La0.72​Pr0.25{\mathrm{Pr}}_{0.25}Pr0.25​Nd0.03{\mathrm{Nd}}_{0.03}Nd0.03​F3{\mathrm{F}}_{3}F3​ due to cross relaxation to Pr and Nd ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature in the (2-70)-K region. Cross relaxation occurs either directly or through a donor-donor transfer within the inhom-geneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from previous fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint according to models for fluorescence decay in the presence of traps. In general the decay is consistent with an electric dipole-dipole transfer mechanism. At 2 K the decay can be well described by a direct transfer to Pr and Nd traps without donor-donor transfer. The temperature dependence of the decay at long times can be described for 35<T<7035<T<7035<T<70 K by the hopping model. The agreement with theory is much better if the cross relaxation to Nd ions is assumed to occur mainly via the lowest Stark level of the 4I92^{4}I_{\frac{9}{2}}4I29​​ manifold.
In this paper, we study quantum dynamics of entanglement and single excitation transfer (SET) in an LH1-RC-type trimer which can describe a basic unit cell in the LH1-RC complex in the photosynthetic process. It is shown that there exists a sudden change of entanglement at the critic point of quantum phase transition (QPT) of the system at low temperatures, the entanglement sudden change caused by the QPT is suppressed at higher temperatures. We investigate the influence of environment on entanglement and SET. We show the generation of the dephasing-assisted entanglement between a donor and an acceptor and the existence of the steady-state entanglement, and demonstrate the entanglement transfer from donor-donor entanglement to donor-acceptor entanglement in the dynamic evolution. We reveal the close relation between the SET probability and donor-acceptor entanglement. Especially, we find that the SET probability is proportional to the amount of donor-acceptor entanglement under certain conditions.