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Study on the Intermolecular Carrier Recombination Dynamics in Organic Solar Cells
Chong LI, Meijiao WANG, Lin GE, Lianzhen CAO
Chinese Journal of Computational Physics    2024, 41 (2): 182-192.   DOI: 10.19596/j.cnki.1001-246x.8704
Abstract209)   HTML4)    PDF (9428KB)(569)      

Based on the important effect of carrier recombination on the photovoltaic efficiency of organic solar cells, the intermolecular carrier recombination dynamics in organic solar cells is studied theoretically by using an extended Su-Schrieffer-Heeger tight binding model combined with the non-adiabatic quantum dynamical method in this article. Firstly, intermolecular charge recombination dynamics of the positive and negative carriers at the donor/acceptor interface is simulated and revealed, and it is found that the intermolecular carrier recombination exhibits fractional charge recombination along with energy loss. Subsequently, influence of the system energy offset Δ, electric field, thermal effect and aggregation of acceptor molecules on intermolecular carrier recombination dynamics is studied. The results show that the system energy offset Δ exhibits the carrier recombination barrier, and the larger the energy offset Δ, the more favorable it is to suppress the recombination of carriers. The electric field can inhibit the recombination of carriers by inducing spatial delocalization of positive and negative charges. Especially, as the electric field is strong enough, it can dissociate the recombined charge transfer state into free carriers. Thermal effects can cause random fluctuations of the potential energy of the donor/acceptor material, which can reduce the recombination barrier of carriers, and further to aggravate the carrier recombination. The aggregation of acceptor molecules will induce the expansion of electrons between acceptor molecules, increasing the distance between positive and negative charge centers at the interface, thereby inhibiting the recombination of carriers.

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