Theory of interfacial charge-transfer complex photophysics in $π$-conjugated polymer-fullerene blends

Details Theory of interfacial charge-transfer complex photophysics in $π$-conjugated polymer-fullerene blends Theory of interfacial charge-transfer complex photophysics in $π$-conjugated polymer-fullerene blends

2009-08-03

arxiv.org/abs/0908.0366v2

Phys. Rev. B 81, 085407 (2010)

Physics

Condensed Matter

Strongly Correlated Electrons

9 pages, 8 figures

Scientific paper

We present a theory of the electronic structure and photophysics of 1:1 blends of derivatives of polyparaphenylenevinylene and fullerenes. Within the same Coulomb-correlated Hamiltonian applied previously to interacting chains of single-component $\pi$-conjugated polymers, we find an exciplex state that occurs below the polymer's optical exciton. Weak absorption from the ground state occurs to the exciplex. We explain transient photoinduced absorptions in the blend, observed for both above-gap and below-gap photoexcitations, within our theory. Photoinduced absorptions for above-gap photoexcitation are from the optical exciton as well as the exciplex, while for below-gap photoexcitation induced absorptions are from the exciplex alone. In neither case are free polarons generated in the time scale of the experiment. Importantly, the photophysics of films of single-component $\pi$-conjugated polymers and blends can both be understood by extending Mulliken's theory of ground-state charge transfer to the case of excited-state charge transfer.

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