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تسجيل مستخدم جديدEffect of Disorder on Free Energy and Open-Circuit Voltage of Organic Photovoltaic Systems
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Organic Photovoltaic devices (OPVs) are becoming adequately cost and energy efficient to be considered a good investment and it is, therefore, especially important to have a concrete understanding of their operation. We compute energies of charge-transfer (CT) states of the model donor-acceptor lattice system with varying degrees of structural disorder to investigate how fluctuations in the material properties affect electron-hole separation. We also demonstrate how proper statistical treatment of the CT energies recovers experimentally observed hot and cold exciton dissociation pathways. Using a quantum mechanical model for a model heterojunction interface, we recover experimental values for the open-circuit voltage at 50 and 100meV of site-energy disorder. We find that energetic and conformational disorder generally facilitates charge transfer; however, due to excess energy supplied by photoexcitation, highly energetic electron-hole pairs can dissociate in unfavorable directions, potentially never contributing to the photocurrent. We find that cold excitons follow the free energy curve defined at the operating temperature of the device. Our results provide a unifying picture linking various proposed mechanisms for charge separation.
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