Nonadiabatic Excited-State Dynamics in Perylene Diimides

ORAL

Abstract

Perylene diimides (PDI) are promising materials for optoelectronics. We study the photo-induced excited-state dynamics of a PDI derivative using the NEXMD software that goes beyond the Born-Oppenheimer description of electron-nuclear interactions. By comparing the internal conversion processes of the monomer and dimer, we determine the role of inter-molecular interactions on the time-scales associated with energy transfer and exciton localization dynamics. We predict that energy conversion in the dimer happens significantly faster than in the monomer. For the dimer, analysis of the electronic transition density during photo-dynamics reveals the transient trapping of the exciton, suggesting that the strength of thermal fluctuations exceeds electronic coupling between the two molecules. Lastly, vibrational normal mode analysis during the dynamics allows us to identify the intra- and iner-molecular modes that assist the electronic relaxation.

*We acknowledge financial support from the National Science Foundation (DMR-1847774). This work was partially supported by CONICET, UNQ, ANPCyT (PICT-2018-2360). The work at LANL was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy Office of Science.

Presenters

  • Aliya Mukazhanova

    • Boston University

Authors

  • Aliya Mukazhanova

    • Boston University
  • Walter Malone

    • Theoretical Division and Center for Integrated Nanotechnologies, Los Alamos National Laboratory
  • Hassiel Negrin-Yuvero

    • Universidad Nacional de Quilmes
  • Sebastian Fernandez-Alberti

    • Universidad Nacional de Quilmes
  • Sergei Tretiak

    • Los Alamos National Laboratory
    • Theoretical Division and Center for Integrated Nanotechnologies, Los Alamos National Laboratory
    • CINT, Los Alamos National Lab
  • Sahar Sharifzadeh

    • Department of Electrical and Computer Engineering, Boston University
    • Boston University