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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Photophysics of Soret-Excited Tetrapyrroles in Solution. II. Effects of Perdeuteration, Substituent Nature and Position, and Macrocycle Structure and Conformation in Zinc(II) Porphyrins
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Photophysics of Soret-Excited Tetrapyrroles in Solution. II. Effects of Perdeuteration, Substituent Nature and Position, and Macrocycle Structure and Conformation in Zinc(II) Porphyrins

机译：溶液中Soret激发的四吡咯的光物理。二。氘化，取代基的性质和位置以及卟啉锌（II）大环结构和构象的影响

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摘要

The steady-state absorption, fluorescence, and excitation spectra and upper excited-state temporal fluorescence decay profiles of 11 tetrapyrroles in several fluid solvents are presented and analyzed to ascertain the factors that control their S2 population decay times. The S2 lifetimes, which vary by more than 2 orders of magnitude, are controlled exclusively by their rates of radiationless decay. The only important electronic relaxation path is S2-S1 internal conversion, the efficiency of which is near 1.0 in all compounds studied (except CdTPP where it is 0.69). The rate of S1 population rise equals the rate of S2 population decay in all cases. Among the compounds studied, only MgTPP exhibits S2-S1 decay behavior that corresponds to the weak coupling limit of radiationless transition theory; all zinc metalloporphyrins exhibit intermediate to strong coupling. Perdeuteration of ZnTPP produces no significant change in the rate of S2 decay or in the quantum yield of S2-S0 fluorescence, indicating that in-plane C-C and C-N vibrations are the accepting modes in S1 with the largest Franck-Condon factors. The initial vibrational energy content of the S2 states (0
机译：提出并分析了11种四吡咯在几种流体溶剂中的稳态吸收光谱，荧光光谱和激发光谱以及上激发态时间荧光衰减曲线，以确定控制其S2种群衰减时间的因素。 S2的寿命变化超过2个数量级，仅受其无辐射衰减率控制。唯一重要的电子弛豫路径是S2-S1内部转换，在所有研究的化合物中其转换效率均接近1.0（CdTPP除外，其为0.69）。在所有情况下，S1人口上升的速度等于S2人口下降的速度。在研究的化合物中，只有MgTPP表现出S2-S1衰减行为，这与无辐射跃迁理论的弱耦合极限相对应。所有的金属卟啉锌均表现出中等至强的偶联作用。 ZnTPP的氘代化不会对S2衰减速率或S2-S0荧光的量子产率产生显着变化，表明平面C-C和C-N振动是S1中具有最大Franck-Condon因子的接受模式。 S2状态的初始振动能含量（在化合物范围内为0

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