Simulations of fluorescence quenching using theoretical models of energy and electron transfer in random arrays

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Abstract
A master equation is solved numerically for investigating energy transfer and trapping in two-dimensional disordered systems of chlorophylls and quinones. Quenching of the excitation occurs both by electron transfer from a chlorophyll to a neighbouring quinone and by energy transfer to self-quenching traps consisting of statistical pairs of chlorophyll molecules closer than a critical distance. The quinone concentration dependence of the average lifetime of the calculated fluorescence decay is determined for different values of the Förster transfer radius 0 and A, the microscopic electron transfer rate at ‘zero distance’. Quasi-Stern-Volmer behaviour is obtained. The half-quenching concentration and the quenching rate kQ depend strongly on A; they increase little with faster energy transfer because of competing self-quenching and slow electron transfer. Our results are compared to recent fluorescence quenching data that Chauvet and Patterson obtained from real-time measurements in monolayers of chlorophyll a and vitamin K1 diluted in dioleylphosphatidylcholine (DOL). Our convoluted decays fit the experimental data if A = 50–100 ns-1 and = 60–70 Å. Accordingly, kQ = 3–5 × 10-5 cm2/molecules·s. These values are in close agreement with those reported in the literature.

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