Charge-transfer excited states in aqueous DNA: Insights from many-body Green's function theory.
Charge-transfer excited states in aqueous DNA: Insights from many-body Green's function theory.
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DOI：
10.1103/physrevlett.112.228301
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发表时间：
2014-06
影响因子：
8.6
通讯作者：
Huabing Yin;Yuchen Ma;J. Mu;Chengbu Liu;M. Rohlfing
中科院分区：
文献类型：
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作者：
Huabing Yin;Yuchen Ma;J. Mu;Chengbu Liu;M. Rohlfing
电荷转移（CT）激发态在水溶液中DNA的激发态动力学中起着重要的作用。然而，关于它们的能量仍然存在很大争议。通过从头算多体绿色函数理论，结合经典分子动力学模拟，我们证实了实验中观察到的DNA水溶液在光吸收最大值的低能侧存在CT态.我们发现，水化壳层可以通过偶极电场对DNA分子的电子结构和CT态产生强烈的影响（约1eV）。在这种情况下，溶剂不能像通常那样简单地被视为宏观筛选介质。讨论了碱基堆积和碱基配对对CT态的影响。
Charge-transfer (CT) excited states play an important role in the excited-state dynamics of DNA in aqueous solution. However, there is still much controversy on their energies. By ab initio many-body Green's function theory, together with classical molecular dynamics simulations, we confirm the existence of CT states at the lower energy side of the optical absorption maximum in aqueous DNA as observed in experiments. We find that the hydration shell can exert strong effects (∼1 eV) on both the electronic structure and CT states of DNA molecules through dipole electric fields. In this case, the solvent cannot be simply regarded as a macroscopic screening medium as usual. The influence of base stacking and base pairing on the CT states is also discussed.