Study of the exciton dynamics in perylene bisimide (PBI) aggregates with symmetrical quasiclassical dynamics based on the Meyer–Miller mapping Hamiltonian

Abstract

The exciton dynamics in one-dimensional stacked PBI (Perylene Bisimide) aggregates was studied with SQC-MM dynamics (Symmetrical Quasiclassical Dynamics based on the Meyer-Miller mapping Hamiltonian). Based on linear vibronic coupling models, one-dimensional PBI aggregates with different lengths were investigated. Based on an investigation of short PBI aggregates (10 sites and 80-140 modes) using both the SQC-MM and ML-MCTDH (multilayer multiconfigurational time-dependent Hartree) methods, we showed that SQC-MM dynamics give a reasonable description of the exciton dynamics for organic PBI aggregates composed of 101 sites and 808 modes. This allows us to employ SQC-MM dynamics in the explicit study of exciton diffusion for long one-dimensional PBI aggregates based on models with different site-site coupling strengths with/without static disorder by including all the involved electronic and vibrational degrees of freedom.