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利用量子化学DFT从头计算方法,计算经过突变的细菌光合反应中心HM202L原初电子给体和其他色素分子的电子结构,然后对其原初电子转移机理进行探讨.结果表明:1)超分子D-2A的HOMO主要是由定域在其组成单元BChl_L分子上的原子轨道组成,而它的LUMO主要是由定域在其组成单元MBPheo_M分子上的原子轨道组成.这表明它在基态和激发态时分别存在超分子内的电荷分离态[BChl_L~--MBPheo_M~+]和[BChl_L~+-MBPheo_M~-].同时也说明了D-2A阳离子态的正电荷完全分布在组成单元细菌叶绿素分子BChl_L上,与实验事实相符.2)HM202L细菌光合反应中心原初电子转移反应存在由ABCh a_L~h(?)驱动的电子转移反应.
The electronic structure of HM202L primary electron donor and other pigment molecules that pass through the mutated bacterial photosynthetic reaction center was calculated by ab initio quantum chemistry method and the primary electron transfer mechanism was discussed.The results showed that: 1) the molecular structure of supramolecular D-2A HOMO consists mainly of atomic orbitals localized on the BChl_L molecule of its constituent unit, while its LUMO consists mainly of atomic orbitals localized on the MBPheo_M molecule of its constituent unit, indicating that it exists separately in the ground and excited states Supramolecular charge separated state [BChl_L ~ --MBPheo_M ~ +] and [BChl_L ~ + -MBPheo_M ~ -] also shows that the D-2A cationic state of the positive charge is completely distributed in the constituent unit of bacterial chlorophyll molecule BChl_L, Which is consistent with the experimental fact.2) There is an electron transfer reaction driven by ABCh a_L ~ h (?) In the primary electron transfer reaction of HM202L bacterial photosynthetic reaction center.