Paillotin G, Swenberg C E, Breton J, Geacintov N E
Biophys J. 1979 Mar;25(3):513-33. doi: 10.1016/S0006-3495(79)85320-5.
A Pauli master equation is formulated and solved to describe the fluorescence quantum yield, phi, and the fluorescence temporal decay curves. F(t), obtained in picosecond laser excitation experiments of photosynthetic systems. It is assumed that the lowering of phi with increasing pulse intensity is due to bimolecular singlet exciton annihilation processes which compete with the monomolecular exciton decay processes; Poisson statistics are taken into account. Calculated curves of phi as a function of the number of photon hits per domain are compared with experimental data, and it is concluded that these domains contain at least two to four connected photosynthetic units (depending on the temperature), where each photosynthetic unit is assumed to contain approximately 300 pigment molecules. It is shown that under conditions of high excitation intensities, the fluorescence decays approximately according to the (time)1/2 law.
推导并求解了一个泡利主方程，以描述光合系统皮秒激光激发实验中获得的荧光量子产率φ和荧光时间衰减曲线F(t)。假设随着脉冲强度增加，φ降低是由于双分子单重态激子湮灭过程与单分子激子衰减过程相互竞争所致；考虑了泊松统计。将φ作为每个区域光子撞击数函数的计算曲线与实验数据进行了比较，得出这些区域至少包含两到四个相连的光合单元（取决于温度），其中每个光合单元假定包含约300个色素分子。结果表明，在高激发强度条件下，荧光近似按照（时间）1/2规律衰减。
