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.

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

ACCOMASSO, DAVIDE;Granucci, Giovanni;Persico, Maurizio
2018

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.
Accomasso, Davide; Granucci, Giovanni; Havenith, Remco W. A.; Persico, Maurizio
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/11568/939618
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