Exciton-Vibration Dynamics in J-Aggregates of a Perylene Bisimide from Real-Time Path Integral Calculations

Sohang Kundu, Nancy Makri

Research output: Contribution to journalArticlepeer-review


We use the modular path integral (MPI) and the small matrix path integral (SMatPI) methods to obtain numerically exact, fully quantum mechanical results for the excitation energy-transfer (EET) dynamics of perylene bisimide (PBI) J-aggregates containing 2, 3, 5, or 25 PBI-1 molecular units at zero and room temperature. Our calculations are based on a parameterized Frenkel exciton Hamiltonian and treat explicitly 28 intramolecular vibrations in each molecule that have been found to have nonzero Huang-Rhys factors. We find that the vibrational modes cause significant changes to the dynamics, smearing electronic recurrence peaks and introducing a substantial temperature dependence to the time evolution of the electronic populations. We also identify a high-frequency vibronic mode which is primarily responsible for additional oscillatory features that exhibit variable temperature sensitivity dependent on aggregate length. These results provide a quantitative picture and useful insights into the complex interplay of exciton-vibration interactions in the EET dynamics of PBI aggregates.

Original languageEnglish (US)
Pages (from-to)201-210
Number of pages10
JournalJournal of Physical Chemistry C
Issue number1
StatePublished - Jan 14 2021

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • General Energy
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films


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