A multiconfigurational time-dependent Hartree-Fock method for excited electronic states. II. Coulomb interaction effects in single conjugated polymer chains.
A multiconfigurational time-dependent Hartree-Fock method for excited electronic states. II. Coulomb interaction effects in single conjugated polymer chains.
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DOI：
10.1063/1.3600404
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发表时间：
2011-06
期刊：
影响因子：
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通讯作者：
R. Miranda;A. Fisher;L. Stella;A. Horsfield
中科院分区：
文献类型：
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作者：
R. Miranda;A. Fisher;L. Stella;A. Horsfield
共轭聚合物由于其潜在的光电应用前景，在过去的几十年里引起了人们的广泛关注。需要优化的关键步骤是光激发后的电荷载流子分离。为了更好地了解激子的动力学电荷分离之前，我们已经进行了模拟的形成和动力学的局部激发在单一的共轭聚合物链。我们使用非绝热分子动力学方法，该方法允许核自由度和多构型电子波函数的耦合演化。我们示出的电子-空穴对的弛豫形成激子和带相反电荷的极化子对，并讨论了修改的弛豫过程中预测的载子之间的库仑相互作用的列入。本文还讨论了共轭聚合物在稀溶液中的电荷光生问题。
Conjugated polymers have attracted considerable attention in the last few decades due to their potential for optoelectronic applications. A key step that needs optimisation is charge carrier separation following photoexcitation. To understand better the dynamics of the exciton prior to charge separation, we have performed simulations of the formation and dynamics of localised excitations in single conjugated polymer strands. We use a nonadiabatic molecular dynamics method which allows for the coupled evolution of the nuclear degrees of freedom and of multiconfigurational electronic wavefunctions. We show the relaxation of electron-hole pairs to form excitons and oppositely charged polaron pairs and discuss the modifications to the relaxation process predicted by the inclusion of the Coulomb interaction between the carriers. The issue of charge photogeneration in conjugated polymers in dilute solution is also addressed.