点击次数：

论文类型：期刊论文

发表时间：2012-03-01

发表刊物：DYES AND PIGMENTS

收录刊物：SCIE、EI

卷号：92

期号：3

页面范围：1344-1350

ISSN号：0143-7208

关键字：Fullerene derivatives; Real-space analysis; Excited state; Charge transfer

摘要：Quantum chemistry methods as well as two-dimensional (2D) and three-dimensional (3D) real-space analysis have been conducted to study the photo-induced intramolecular charge-transfer (ICT) and excited state properties of fullerene-phenylphenothiazine, which has recently been developed for solar cells. Firstly, we obtained the energy levels and spatial distributions of HOMO/LUMO, energy gap (Delta EH-L) and excitation energies on the basis of quantum chemistry study. Secondly, two-dimensional (2D) and three-dimensional (3D) real-space analysis were used to visualize the CT process and to reveal the nature of the excited states. In the above analyses, the 2D real-space analysis of the transition density matrix provided information about the electron-hole coherence, and the 3D real-space analysis of charge difference density enabled the visualization of the orientation and result of the ICT. The results of real-space analysis directly indicate that some states are ICT states, and others belong to locally excited states. Moreover, according to the generalized Mulliken Hush theory, we calculated the electronic coupling matrix elements and predict that electron transfer for some ICT states more easily takes place than that for some locally excited states. (C) 2011 Elsevier Ltd. All rights reserved.