Raising the open circuit voltage (Voc) of organic photovoltaic (OPV) devices is one of the key parameters to enhance the performance and increase utility. We report an active layer composed...
Herein, we investigate the role of processing solvent additives on the formation of polymer−perylene diimide bulk-heterojunction active layers for organic photovoltaics using both spin-coating and slot-die coating methods. We compare the effect of 1,8-diiodooctane (DIO) and diphenyl ether (DPE) as solvent additives on the aggregation behavior of the non-fullerene acceptor, N-annulated perylene diimide dimer (tPDI 2 N-EH), in neat films and blended films with the benzodithiophene-quinoxaline (BDT-QX, QX-3) donor polymer, processed from toluene in air. DIO processing crystallizes the tPDI 2 N-EH acceptor and leads to the decreased solar cell performance. DPE processing has a more subtle effect on the bulk-heterojunction morphology and leads to an improved solar cell performance. A comparison of the spin-coating vs slot-die coating methods shows that the effect of DPE is prominent for the slot-die coated active layers. While similar device power conversion efficiencies are achieved with active layers coated with both methods (ca. 7.3% vs 6.5%), the use of DPE improves the film quality when the slot-die coating method is employed.
Efficient organic photovoltaics (OPVs) based on slot-die-coated (SD) ternary blends were developed for lowintensity indoor light harvesting. For active layers processed in air and from eco-friendly solvents, our device performances (under 1 sun and low light intensity) are the highest reported values for fluoro-dithiophenyl-benzothiadiazole donor polymer-based OPVs. The N-annulated perylene diimide dimer acceptor was incorporated into a blend of donor polymer (FBT) and fullerene acceptor (PC 61 BM) to give ternary bulk heterojunction blends. SD ternarybased devices under 1 sun illumination showed enhanced power conversion efficiency (PCE) from 6.8 to 7.7%. We observed enhancement in the short-circuit current density and open-circuit voltage of the devices. Under low light intensity light-emitting device illumination (ca. 2000 lux), the ternary-based devices achieved a PCE of 14.0% and a maximum power density of 79 μW/cm 2 compared to a PCE of 12.0% and a maximum power density of 68 μW/cm 2 for binary-based devices. Under the same illumination conditions, the spin-coated (SC) devices showed a PCE of 15.5% and a maximum power density of 88 μW/cm 2 . Collectively, these results demonstrate the exceptional promise of a SD ternary blend system for indoor light harvesting and the need to optimize active layers based on industry-relevant coating approaches toward mini modules.
Most high-performance OPV devices, however, use fabrication methods that are only suitable for small-scale laboratory experiments, such as spin-coating, alongside controlled atmospheric conditions in gloveboxes for both fabrication and testing. [1][2][3][4]10] In addition, the halogenated and volatile solvent chloroform is commonly used, despite it not being industrially viable. This is due to adverse health and environmental effects, as well as poor compatibility with printing methods due to the low boiling point and high volatility. Thermal procedures such as hot casting and thermal annealing are also used to process and cure the photoactive layer, respectively, of such OPVs devices, [12] which introduces energy-intensive steps during the fabrication process. To facilitate the lab-to-fab transition, it is necessary to move high-performance systems to industry-compatible processing. Slot-Die Coating (SDC) has been identified as a viable coating technique due to its inherent scalability, compatibility with roll-to-roll manufacturing, and a much reduced material waste compared to spin-coating. [13] It is estimated that 95-98% of material is wasted using spin-coating methods. [14] In addition, SDC is effective for high throughput film formation on flexible substrates, while maintaining control over film thickness. [15] SDC has challenges in controlling drying rates which impact film morphology, [16] but offers opportunities for efficient layer-by-layer coating. [17] Increased effort has been put towards the construction of OPV devices using industrially compatible conditions, that is, OPV at scale. This is encouraging for commercialization, but performance gaps exist between engineered lab-scale devices and roll-processed modules. [13,[18][19][20] It is critical that when developing roll-to-roll compatible coated OPV devices, all layers must be considered in the stack, not just the organic photoactive layer, which is most often only investigated. Although reported by some, the SDC of all three critical OPV layers (hole transport layer HTL, electron transport ETL, photoactive layer) remains largely unexplored in the academic literature using NFAs. This has been presented by Baran and co-workers, [13] and it remains a challenge to prepare multilayer SDC OPVs with high efficiency. [21,22] Encouraging, Destouesse et al., have demonstrated roll-to-roll processed, ITO-free OPVs based on NFAs, in air, with 5% PCE. [23] For single-layer SDC OPVs we have reported PCEs upwards of 6%, [24][25][26] while PCEs upwards of 12% have been reached. [12,27,28] For two-and three-layer SDC
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