2013/01/30 by Ivan Duchemin, Xavier Blase
Chemistry · Engineering · Materials Science · Physics and Astronomy · #Acceptor #Atomic physics #Charge (physics) #Chemical physics #Chemistry #Condensed matter physics #Excitation #Excited state #Exciton #Fullerene #Intramolecular force #Materials science #Molecular Junctions and Nanostructures #Molecular physics #Photochemistry and Electron Transfer Studies #Physics #Porphyrin and Phthalocyanine Chemistry #Quantum mechanics #cond-mat.mtrl-sci
paper · pdf · doi:10.1103/physrevb.87.245412
9 pages, 4 figures
openalex publication_date 2013/01/30 · arxiv created 2013/05/29 · arxiv updated 2015/06/12 · openalex created_date 2022/10/03 · openalex updated_date 2026/08/05
We study within the many-body Green's function GW and Bethe-Salpeter approaches the neutral singlet excitations of the zinctetraphenylporphyrin and C70 fullerene donor-acceptor complex. The lowest transition is a charge-transfer excitation between the donor and the acceptor with an energy in excellent agreement with recent constrained density functional theory calculations. Beyond the lowest charge-transfer state, of which the energy can be determined with simple electrostatic models that we validate, the Bethe-Salpeter approach provides the full excitation spectrum. We evidence the existence of hot electron-hole states which are resonant in energy with the lowest donor intramolecular excitation and show an hybrid intramolecular and charge-transfer character, favouring the transition towards charge separation. These findings support the recently proposed scenario for charge separation at donor-acceptor interfaces through delocalized hot charge-transfer states.