多发色团天线的电子结构和电荷转移激发态
Electronic structure and charge transfer excited states of a multichromophoric antenna
摘要：
用密度泛函理论研究了一个由两个硼二吡咯甲烷染料、锌四苯基卟啉、二苯基蒽和富勒烯组成的多发色分子配合物的电子结构。雪花状分子表现得像天线，以不同的频率捕获光子，并将光子能量转移到卟啉，其中发生电子从卟啉转移到富勒烯。这个大的复杂的分子结构首先优化使用平面波投影增强波方法。随后的电子结构的计算使用的实空间方法，使用所有电子赝势基组包含总共12478个基函数。结果表明，HOMO和低于HOMO的一个态主要位于其中一个卟啉上，而LUMO主要位于配合物的富勒烯组分上。的HOMO和LUMO状态的能量在复杂的，判断的电离势和电子亲和势的值，显示出显着的差异，相对于它们的值在参与的亚基隔离。我们系统地研究了结构应变和配体的存在对电离能和电子亲和势的影响。最后，我们已经计算了几个最低的电荷转移能量涉及电子跃迁从卟啉组分的富勒烯亚基的复杂使用微扰的delta-SCF方法。我们的预测值的最低电荷转移激发态（1.67 eV）是一个类似的复杂的电荷转移能量的实验估计相媲美。
英文摘要：
The electronic structure of a multichromophoric molecular complex containing two of each borondipyrromethane dye, Zn-tetraphenyl-porphyrin, bisphenyl anthracene and a fullerene are studied using density functional theory. The snowflake shaped molecule behaves like an antenna capturing photon at different frequencies and transferring the photon energy to the porphyrin where electron transfer occurs from the porphyrin to the fullerene. Molecular structure of this large complex is first optimized using plane wave projector augmented wave methodology. Subsequent electronic structure calculations are performed using the real space methodology using an all electron pseudopotential basis set containing total of 12478 basis functions. The results show that the HOMO and a state below the HOMO are primarily localized on one of the porphyrins while the LUMO resides mainly on the fullerene component of the complex. The energies of the HOMO and LUMO states in the complex, as adjudged by the ionization potential and the electron affinity values, show significant differences with respect to their values in participating subunits in isolation. We have systematically examined the effect of structural strain and the presence of ligands on the ionization energy and the electron affinity. Finally, we have calculated a few lowest charge transfer energies involving electronic transitions from a the porphyrin component to the fullerene subunit of the complex using the perturbative delta-SCF method. Our predicted value of the lowest charge transfer excited state (1.67 eV) is comparable to the experimental estimate of the charge transfer energy of a similar complex.
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