Enhancing performance and scalability of HTL-free organic solar cells with keggin polyoxometalates-type additive

Interfacial layers play a crucial role in enhancing the performances and stabilities of organic solar cells (OSCs). Despite achieving high efficiencies from OSCs, the challenges associated with large-area manufacturing and the need for nanoscale uniformity during coating have hindered the large-scale production of these devices. To address these issues, we propose the concept of hole transport layer (HTL)-free OSCs to simplify the fabrication processes and improve the efficiency of production. In this study, we explore the potential of phosphotungstic acid (PTA), a Keggin polyoxometalate, both as a promising HTL and as an additive in HTL-free OSCs to enhance device performances and scalabilities in cell-to-module OSCs. Remarkably, incorporating PTA as an annealing-free HTL and as an additive in the photoactive layer (PM6:Y6:PC71BM) significantly increases power conversion efficiency (PCE) up to 17.28 % and 16.33 %, respectively, with respect to that of the reference device with PEDOT:PSS (15.88 %). We successfully fabricate a large-area OSC module, exhibiting an impressive PCE of 15.18 % and an active area of 54 cm2, achieving approximately 85 % of the effectiveness of small-area OSCs. The improved performance is attributed to the enhanced transmittance, excellent carrier-dynamic capacity, suppressed carrier recombination, and reduced trap-states in the ternary bulk-heterojunction OSCs. This study demonstrates the promising versatility of PTA for application in OSCs, offering potential enhancements in device performance and scalability for future applications.