首页> 外文期刊>The Journal of Chemical Physics >Exciton exciton annihilation dynamics in chromophore complexes. I. Multiexciton density matrix formulation
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Exciton exciton annihilation dynamics in chromophore complexes. I. Multiexciton density matrix formulation

机译:发色团配合物中的激子激子an灭动力学。一,多激子密度矩阵公式

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摘要

The multiexciton (MX) description of excitation energy transfer in chromophore complexes and biological light harvesting antenna systems is extended to the incorporation of exciton exciton annihilation (EEA) processes. To achieve a complete microscopic description the approach is baed on intrachromophore internal conversion processes leading to nonradiative transitions from higher to lower lying exciton manifolds. Besides an inclusion of EEA the MX density matrix theory which has been utilized for a description of excitation energy transfer also accounts for a coupling to low-frequency vibrational modes and the radiation field. Concentrading on transitions from the two to the single-excition manifold exact and approximate expression for the EEA rate are derived. In part II of this paper the approach is applied to the LH2 antenna putting emphasis on the EEA induced change of transient absorption spectra.
机译:发色团配合物和生物光收集天线系统中激发能转移的多激子(MX)描述扩展到了激子exc灭(EEA)过程的结合。为了获得完整的微观描述,该方法基于发色团内部转化过程,该过程导致了从高位激子到低位激子歧管的非辐射跃迁。除了包含EEA之外,已用于描述激发能传递的MX密度矩阵理论还考虑了与低频振动模式和辐射场的耦合。集中讨论了从两个过渡到单重流形的转变,EEA速率的精确表达式和近似表达式。在本文的第二部分中,该方法应用于LH2天线,重点在于EEA引起的瞬态吸收光谱变化。

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