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Nonradiative excitation energy transport in one-component disordered systems

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Abstract

High-accuracy Monte Carlo simulations of the time-dependent excitation probabilityG s (t) and steady-state emission anisotropyr M /r 0M for one-component three-dimensional systems were performed. It was found that the values ofr M /r 0M obtained for the averaged orientation factor\(\overline {\kappa ^2 } \) only slightly overrate those obtained for the real values of the orientation factor κ 2ik . This result is essentially different from that previously reported. Simulation results were compared with the probability coursesG s (t) andR(t) obtained within the frameworks of diagrammatic and two-particle Huber models, respectively. The results turned out to be in good agreement withR(t) but deviated visibly fromG s (t) at long times and/or high concentrations. Emission anisotropy measurements on glycerolic solutions of Na-fluorescein and rhodamine 6G were carried out at different excitation wavelengths. Very good agreement between the experimental data and the theory was found, with λex≈λ0-0 for concentrations not exceeding 3.5·10−2 and 7.5·10−3 M in the case of Na-fluorescein and rhodamine 6G, respectively. Up to these concentrations, the solutions investigated can be treated as one-component systems. The discrepancies observed at higher concentrations are caused by the presence of dimers. It was found that forλ ex <λ0-0 (Stokes excitation) the experimental emission anisotropies are lower than predicted by the theory. However, upon anti-Stokes excitation (λex>λ0-0), they lie higher than the respective theoretical values. Such a dispersive character of the energy migration can be explained qualitatively by the presence of fluorescent centers with 0-0 transitions differing from the “mean” at λ0-0.

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Authors and Affiliations

  1. Institute of Experimental Physics, University of Gdańsk, 80-952, Gdańsk, Wita Stwosza 57, Poland

    Piotr Bojarski & Alfons Kawski

  2. Department of Applied Mathematics and Technical Physics, Technical University of Gdańsk, 80-952, Gdańsk, Majkowskiego 11/12, Poland

    Leszek Kulak & Czeslaw Bojarski

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  1. Piotr Bojarski
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  2. Leszek Kulak
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  3. Czeslaw Bojarski
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  4. Alfons Kawski
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Bojarski, P., Kulak, L., Bojarski, C. et al. Nonradiative excitation energy transport in one-component disordered systems. J Fluoresc 5, 307–319 (1995). https://doi.org/10.1007/BF01152557

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