Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.262
Publication date: 18th July 2019
The energetic offset between the initial photoexcited state and charge-transfer (CT) state in organic heterojunction solar cells influences both charge generation and open-circuit voltage (Voc). In this work, we use time-resolved spectroscopy and voltage loss measurements to analyse the effect of the exciton-CT state offset on charge transfer, separation and recombination processes in chemically similar blends of a low-bandgap isoindigoid polymer (INDT-S) with fullerenes derivatives of different electron affinity (PCBM and KL). The two blends possess large offsets for hole transfer, but different offsets for electron transfer: a very low offset for the INDT-S:PCBM blend and a higher one for the INDT-S:KL blend. In the case of the lower exciton-CT state offset (INDT-S:PCBM), the photocurrent generation is lower, Voc is higher and non-radiative voltage losses are lower than in INDT-S:KL. By characterising the dynamics of the devices after photoexcitation using both transient absorption spectroscopy (TAS) and pump push photocurrent (PPPC) , we find that the dynamics of the INDT-S:PCBM blend shows different excited state dynamics depending on whether the donor or acceptor is photoexcited. Interestingly, the charge recombination dynamics in INDT-S:PCBM are distinctly faster than in INDT-S:KL upon excitation of the donor. We reconcile these observations using a model for the dependence of Voc on radiative and non-radiative recombination. We also explain the effect of exciting donor or acceptor on charge transfer and recombination using a simple kinetic model. The results of the model show that hybridisation between the lowest excitonic and CT states can significantly reduce Voc losses whilst still allowing reasonable charge generation efficiency.