On the Förster model: Computational and ultrafast studies of electronic energy transport

摘要: Abstract The Forster model was used to study the transport of electronic energy in condensed, spatially disordered systems. Several analytical theories were compared a computation benchmark over an expansive domain parameters (reduced concentration C, distance R0, and chromophore diameter rmin) for systems consisting up 5000 chromophores. first-order cumulant approximation (FCA) is found be most consistent predicting survival probability P0(t), observable which differ most. Its range applicability usually P0(t) > 0.05, yet never better than 0.01. In addition, nondiffusive 0.001. computations combined with experiments further test model. Femtosecond polarization grating methods determine high spatial resolution population gratings determined long-time diffusion coefficient D concentrated dye solutions. FCA satisfactorily describe on femtosecond time scale C ⩽ 41 within its accuracy; whereas limit good agreement theory Loring, Franchi Mukamel (LFM). For 10, scales as 4 3 prefactor, 0.20 ± 0.03, that agreess LFM (0.212).At higher concentrations, there decrease from behavior sooner predicts discussed context long-range correlations distribution due electrostatic or aggregation effects. experiments, conjunction computations, identify accurate theoretical models different regimes, illustrate details are understood at quantitative level relatively concentrations.