Solution-processable small molecule (SM) donors are promising alternatives to their polymer counterparts in bulk-heterojunction (BHJ) solar cells. While SM donors with favorable spectral absorption, self-assembly patterns, optimum thin-film morphologies, and high carrier mobilities in optimized donor–acceptor blends are required to further BHJ device efficiencies, material structure governs each one of those attributes. As a result, the rational design of SM donors with gradually improved BHJ solar cell efficiencies must concurrently address: (i) bandgap tuning and optimization of spectral absorption (inherent to the SM main chain) and (ii) pendant-group substitution promoting structural order and mediating morphological effects. In this paper, the rational pendant-group substitution in benzo[1,2-b:4,5-b′]dithiophene–6,7-difluoroquinoxaline SMs is shown to be an effective approach to narrowing the optical gap (Eopt) of the SM donors (SM1 and SM2), without altering their propensity to order and form favorable thin-film BHJ morphologies with PC71BM. Systematic device examinations show that power conversion efficiencies >8% and open-circuit voltages (VOC) nearing 1 V can be achieved with the narrow-gap SM donor analog (SM2, Eopt = 1.6 eV) and that charge transport in optimized BHJ solar cells proceeds with minimal, nearly trap-free recombination. Detailed device simulations, light intensity dependence, and transient photocurrent analyses emphasize how carrier recombination impacts BHJ device performance upon optimization of active layer thickness and morphology.
Bibliographical noteKAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): CRG_R2_13_BEAU_KAUST_1
Acknowledgements: R.-Z.L. and K.W. contributed equally to this work. This publication is based upon work supported by the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under Award No. CRG_R2_13_BEAU_KAUST_1. The authors acknowledge concurrent support under Baseline Research Funding from KAUST. The authors thank KAUST ACL for technical support in the mass spectrometry analyses.