Single layered organic solar cells (OSCs) using non-fullerene acceptors have This article is protected by copyright. All rights reserved. 35A power conversion efficiency of 16.88% (certified as 16.4%) is achieved based on PM6:Y6 by morphology optimization, which is the top efficient for organic solar cells. Through the study of single structure and film morphology, a well ordered 2D crystal was found, which helps to enhance ultrafast hole and electron transfer, thus improving performance.

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resulting in inefficient charge separation and collection. [7][8][9] However, recent progresses show quite steep climbing of power conversion efficiency (PCE) for all-PSCs, reaching a value over 10%, [10][11][12] under systematic optimization, leaving a large gap to be filled in understanding the mechanism of morphology evolution. Polymer blends that reach nanoscaled phase separation in organic photovoltaic (OPV) application have distinctive advantages. They are more suitable for printing fabrication because of their good filmforming ability and mechanical flexibility, prominent device stability, and readily tunable ink viscosity. [13][14][15][16][17] Such benefits make all-PSC unique in scalable OPV fabrication, which also leads to boosted interest in understanding and manipulating the morphology. Initiative efforts on all-PSC printing have been surveyed, showing PCEs way below device made by spin-coating. [16,18] The mystery lies in morphology control, of which BHJ thin film is typical nonequilibrium nature that film-drying kinetics dictates the final nanostructure composed of crystalline networks and mixed and phase-separated domains. [19][20][21] It has been shown that solar cells using polymer:non-fullerene acceptor blends processed by slot die printing have exceed 11% in PCE, [22][23][24][25][26][27][28] from which we think that fine-tuning of morphology in all-PSCs could reach a similar level once a All-polymer solar cells (all-PSCs) exhibit excellent stability and readily tunable ink viscosity, and are therefore especially suitable for printing preparation of large-scale devices. At present, the efficiency of state-of-the-art all-PSCs fabricated by the spin-coating method has exceeded 11%, laying the foundation for the preparation and practical utilization of printed devices.A high power conversion efficiency (PCE) of 11.76% is achieved based on PTzBI-Si:N2200 all-PSCs processing with 2-methyltetrahydrofuran (MTHF, an environmentally friendly solvent) and preparation of active layers by slot die printing, which is the top efficient for all-PSCs. Conversely, the PCE of devices processed by high-boiling point chlorobenzene is less than 2%. Through the study of film formation kinetics, volatile solvents can freeze the morphology in a short time, and a more rigid conformation with strong intermolecular interaction combined with the solubility limit of PTzBI-Si and N2200 in MTHF results in the formation of a fibril network in the bulk heterojunction. The multilength scaled morphology ensures fast transfer of carriers and facilitates exciton separation, which boosts carrier mobility and current density, thus improving the device performance. These results are of great significance for large-scale printing fabrication of high-efficiency all-PSCs in the future. Polymer Solar Cells