TY - JOUR
T1 - Hybridization of Local Exciton and Charge-Transfer States Reduces Nonradiative Voltage Losses in Organic Solar Cells
AU - Eisner, Flurin D.
AU - Azzouzi, Mohammed
AU - Fei, Zhuping
AU - Hou, Xueyan
AU - Anthopoulos, Thomas D.
AU - Dennis, T. John S.
AU - Heeney, Martin
AU - Nelson, Jenny
N1 - KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: F.D.E. and M.A. thank the Engineering and Physical Sciences Research Council (EPSRC) for support via doctoral studentships. J.N. is grateful for funding from EPSRC (Grant Nos. EP/P005543/1 and EP/M025020/1) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Grant Agreement No. 742708). M.H. and Z.F. thank the British Council (337323) for support. X.H. thanks the Chinese Scholarship council for support via a PhD studentship. F.D.E., M.A., and J.N. thank Artem Bakulin, Nathaniel Gallop, Shawn Zheng, and Thomas Kirchartz for helpful discussions.
PY - 2019/3/18
Y1 - 2019/3/18
N2 - A number of recent studies have shown that the nonradiative voltage losses in organic solar cells can be suppressed in systems with low energetic offsets between donor and acceptor molecular states, but the physical reasons underpinning this remain unclear. Here, we present a systematic study of 18 different donor/acceptor blends to determine the effect that energetic offset has on both radiative and nonradiative recombination of the charge-transfer (CT) state. We find that, for certain blends, low offsets result in hybridization between charge-transfer and lowest donor or acceptor exciton states, which leads to a strong suppression in the nonradiative voltage loss to values as low as 0.23 V associated with an increase in the luminescence of the CT state. Further, we extend a two-state CT-state recombination model to include the interaction between CT and first excited states, which allows us to explain the low nonradiative voltage losses as an increase in the effective CT to ground state oscillator strength due to the intensity borrowing mechanism. We show that low nonradiative voltage losses can be achieved in material combinations with a strong electronic coupling between CT and first excited states and where the lower band gap material has a high oscillator strength for transitions from the excited state to the ground state. Finally, from our model we propose that achieving very low nonradiative voltage losses may come at a cost of higher overall recombination rates, which may help to explain the generally lower FF and EQE of highly hybridized systems.
AB - A number of recent studies have shown that the nonradiative voltage losses in organic solar cells can be suppressed in systems with low energetic offsets between donor and acceptor molecular states, but the physical reasons underpinning this remain unclear. Here, we present a systematic study of 18 different donor/acceptor blends to determine the effect that energetic offset has on both radiative and nonradiative recombination of the charge-transfer (CT) state. We find that, for certain blends, low offsets result in hybridization between charge-transfer and lowest donor or acceptor exciton states, which leads to a strong suppression in the nonradiative voltage loss to values as low as 0.23 V associated with an increase in the luminescence of the CT state. Further, we extend a two-state CT-state recombination model to include the interaction between CT and first excited states, which allows us to explain the low nonradiative voltage losses as an increase in the effective CT to ground state oscillator strength due to the intensity borrowing mechanism. We show that low nonradiative voltage losses can be achieved in material combinations with a strong electronic coupling between CT and first excited states and where the lower band gap material has a high oscillator strength for transitions from the excited state to the ground state. Finally, from our model we propose that achieving very low nonradiative voltage losses may come at a cost of higher overall recombination rates, which may help to explain the generally lower FF and EQE of highly hybridized systems.
UR - http://hdl.handle.net/10754/652458
UR - https://pubs.acs.org/doi/10.1021/jacs.9b01465
UR - http://www.scopus.com/inward/record.url?scp=85064575803&partnerID=8YFLogxK
U2 - 10.1021/jacs.9b01465
DO - 10.1021/jacs.9b01465
M3 - Article
C2 - 30882218
SN - 0002-7863
VL - 141
SP - 6362
EP - 6374
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 15
ER -