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Role of coherence and delocalization in photo-induced electron transfer at organic interfaces.

ABSTRACT: Photo-induced charge transfer at molecular heterojunctions has gained particular interest due to the development of organic solar cells (OSC) based on blends of electron donating and accepting materials. While charge transfer between donor and acceptor molecules can be described by Marcus theory, additional carrier delocalization and coherent propagation might play the dominant role. Here, we describe ultrafast charge separation at the interface of a conjugated polymer and an aggregate of the fullerene derivative PCBM using the stochastic Schrödinger equation (SSE) and reveal the complex time evolution of electron transfer, mediated by electronic coherence and delocalization. By fitting the model to ultrafast charge separation experiments, we estimate the extent of electron delocalization and establish the transition from coherent electron propagation to incoherent hopping. Our results indicate that even a relatively weak coupling between PCBM molecules is sufficient to facilitate electron delocalization and efficient charge separation at organic interfaces.

SUBMITTER: Abramavicius V

PROVIDER: S-EPMC5015064 | biostudies-literature | 2016 Sep

REPOSITORIES: biostudies-literature

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Role of coherence and delocalization in photo-induced electron transfer at organic interfaces.

Abramavicius V V Pranculis V V Melianas A A Inganäs O O Gulbinas V V Abramavicius D D

Scientific reports 20160908

Photo-induced charge transfer at molecular heterojunctions has gained particular interest due to the development of organic solar cells (OSC) based on blends of electron donating and accepting materials. While charge transfer between donor and acceptor molecules can be described by Marcus theory, additional carrier delocalization and coherent propagation might play the dominant role. Here, we describe ultrafast charge separation at the interface of a conjugated polymer and an aggregate of the fu ...[more]

PMID: 27605035

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Project description:We describe the electronic structure and the origin of ferromagnetic exchange coupling in two new metal complexes, NN-SQ-Co(III)(py)(2)Cat-NN (1) and NN-Ph-SQ-Co(III)(py)(2)Cat-Ph-NN (2) (NN = nitronylnitroxide radical, Ph = 1,4-phenylene, SQ = S = (1)/(2) semiquinone radical, Cat = S = 0 catecholate, and py = pyridine). Near-IR electronic absorption spectroscopy for 1 and 2 reveals a low-energy optical band that has been assigned as a Psi(u) --> Psi(g) transition involving bonding and antibonding linear combinations of delocalized dioxolene (SQ/Cat) valence frontier molecular orbitals. The ferromagnetic exchange interaction in 1 is so strong that only the high-spin quartet state (S(T) = (3)/(2)) is thermally populated at temperatures up to 300 K. The temperature-dependent magnetic susceptibility data for 2 reveals that an excited state spin doublet (S(T) = (1)/(2)) is populated at higher temperatures, indicating that the phenylene spacer modulates the magnitude of the magnetic exchange. The valence delocalization within the dioxolene dyad of 2 results in ferromagnetic alignment of two localized NN radicals separated by over 22 A. The ferromagnetic exchange in 1 and 2 results from a spin-dependent delocalization (double exchange type) process and the origin of this strong electron correlation has been understood in terms of a valence bond configuration interaction (VBCI) model. We show that ferromagnetic coupling promoted by organic mixed-valency provides keen insight into the ability of single molecules to communicate spin information over nanoscale distances. Furthermore, the strong interaction between the itinerant dioxolene electron and localized NN electron spins impacts our ability to understand the exchange interaction between delocalized electrons and pinned magnetic impurities in technologically important dilute magnetic semiconductor materials. The long correlation length (22 A) of the itinerant electron that mediates this coupling indicates that high-spin pi-delocalized organic molecules could find applications as nanoscale spin-polarized electron injectors and molecular wires.

Dataset Information

Role of coherence and delocalization in photo-induced electron transfer at organic interfaces.

Publications

Role of coherence and delocalization in photo-induced electron transfer at organic interfaces.

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