Testing new chromophores for singlet fission: A computational protocol applied to 2,3-diamino-1,4-benzoquinone

Davide Accomasso, Giovanni Granucci, Remco W. A. Havenith, Maurizio Persico*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

2 Citations (Scopus)

Abstract

We present a computational protocol devised to test the suitability of newly proposed chromophores for singlet fission. The protocol includes two main steps: testing the basic energetic requirements by ab initio calculations and simulating the photodynamics to determine singlet fission quantum yields. We applied this protocol to 2,3-diamino-1,4-benzoquinone (DAPBQ), recently proposed as a possible chromophore for singlet fission. We determined the excitation energies of DAPBQ by second order perturbation CASPT2 and NEVPT2 calculations. Then, we optimized a possible crystal structure of DAPBQ, we identified the most favourable pair of molecules within it and we ran a simulation of the excited state dynamics for that dimer embedded in the crystal at a semiempirical QM/MM level. The results indicate that DAPBQ in the crystalline phase does not undergo singlet fission and the initially prepared singlet excited state rapidly decays to the ground state.

Original languageEnglish
Pages (from-to)635-642
Number of pages8
JournalChemical Physics
Volume515
DOIs
Publication statusPublished - 14-Nov-2018

Keywords

  • MOLECULAR WAVE-FUNCTIONS
  • ANO BASIS-SETS
  • PERTURBATION-THEORY
  • EXCITON FISSION
  • DENSITY
  • GENERATION

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