Organic solar cells (OSCs) containing non‐fullerene acceptors have realized high power conversion efficiency (PCE) up to 14%. However, most of these high‐performance non‐fullerene OSCs have been reported with optimal active layer thickness of about 100 nm, mainly due to the low electron mobility (≈10−4–10−5 cm2 V−1 s−1) of non‐fullerene acceptors, which are not suitable for roll‐to‐roll large‐scale processing. In this work, an efficient non‐fullerene OSC based on poly[(5,6‐difluoro‐2,1,3‐benzothiadiazol‐4,7‐diyl)‐alt‐(3,3′″‐di(2‐octyldodecyl)‐2,2′;5′,2″;5″,2′″‐quaterthiophen‐5,5′′′‐diyl)] (PffBT4T‐2OD):EH‐IDTBR (consists of electron‐rich indaceno[1,2‐b:5,6‐b′]dithiophene as the central unit and an electron‐deficient 5,6‐benzo[c][1,2,5]thiadiazole unit flanked with rhodanine as the peripheral group) with thickness‐independent PCE (maintaining a PCE of 9.1% with an active layer thickness of 300 nm) is presented by optimizing device architectures to overcome the space‐charge effects. Optical modeling reveals that most of the incident light is absorbed near the transparent electrode side in thick‐film devices. The transport distance of electrons with lower mobility will therefore be shortened when using inverted device architecture, in which most of the excitons are generated close to the cathode side and therefore substantially reduces the accumulation of electrons in the device. As a result, an efficient thick‐film non‐fullerene OSC is realized. These results provide important guidelines for the development of more efficient thick‐film non‐fullerene OSCs.

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Embedding nanostructures in organic solar cells (OSCs) is a well-known method to improve the absorption efficiency of the device by introducing the plasma resonance and scattering effects without increasing the active layer thickness. The introduction of nanostructures imposes greater demands on the optical analysis method for OSCs. In this paper, the generalized rigorous coupled-wave analysis (GRCWA) is presented to analyze and optimize the performance of coherent-incoherent hybrid organic solar cells (OSCs) with nanostructures. Considering the multiple reflections of light scattered within the glass substrate by the device, the correction vector g is derived, then the modified expressions for the field and absorption distribution in OSCs are provided. The proposed method is validated by comparing the simulated results of various structures with results obtained by the generalized transfer matrix method (GTMM) and the “equispaced thickness method” (ETM). The results demonstrate that the proposed method can reduce the number of simulations by at least half compared to the ETM while maintaining accuracy. With the proposed method, we discussed the device performance depending on the geometrical parameters of nanostructures, and the optimization and analysis are accomplished for single and tandem OSCs. After optimization based on the proposed method, the performance of OSCs are significantly improved, which further demonstrates the practicality of the method.

Tandem organic solar cells (OSCs) show great potential due to advantages such as the utilization of wide-spectrum light and low thermalization loss. The current mismatch between sub-cells is one of the major issues reducing the final output efficiency of a tandem device. In this paper, we focus on the current mismatch of tandem OSCs at oblique incidence and aim to reduce its adverse effect on the performances of realistic devices working at varying incident angle. Firstly, we propose an optical analysis method based on the 4×4 matrix formalism to analyze and optimize the performance of tandem solar cells at arbitrary incident angles. Compared with those optimal designs via matching the currents of sub-cells only at normal incidence, the proposed method chooses the optimal structure of the tandem device by maximizing the generated energy density per day with considering the current match at different incident angles during daytime. With the proposed method, a typical tandem organic solar cell is optimized as an example, and the optimized tandem device has a balanced current match at all incident angles during a whole day. Experimental results demonstrate that the generated energy density per day of the optimized tandem device has increased by 4.9% compared to the conventional device optimized only at normal incidence. The proposed method and results are expected to provide some new insights for the performance analysis and optimization of tandem or multi-junction solar cells, especially those devices exhibiting serious current mismatch between sub-cells at varying incident angles in practical applications.