Ciencias de la Tierra y Física de la Materia Condensada, Universidad de Cantabria, Santander, Spain.
J Chem Phys. 2013 Nov 7;139(17):174101. doi: 10.1063/1.4827398.
The interplay of excitonic and vibronic coupling in coupled chromophores determines the efficiency of exciton localization vs delocalization, or in other words, coherent excitation energy transfer vs exciton hopping. For the investigation of exciton localization in large coupled dimers, a model Hamiltonian approach is derived, the ingredients of which can all be obtained from monomer ab initio calculations alone avoiding costly ab initio computation of the full dimer. The accuracy and applicability of this model are exemplified for the benzene dimer by rigorous comparison to ab initio results.
激子和振子耦合的相互作用决定了激子局域化与去局域化的效率，换句话说，决定了相干激发能量转移与激子跳跃的效率。为了研究大耦合二聚体中的激子局域化，推导了一个模型哈密顿量方法，其中的成分都可以仅从单体从头计算中获得，而无需对整个二聚体进行昂贵的从头计算。通过与从头计算结果的严格比较，该模型的准确性和适用性在苯二聚体上得到了例证。
