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
Revealing the nanostructure of bulk‐heterojunction (BHJ) photovoltaic blends is a critical task in the field of organic photovoltaics. The complicated morphology, ranging from binary blends to ternary mixtures, shows quite varied structural details that need to be fully characterized in terms of correlating them with device performance. The nonequilibrium nature of the BHJ thin‐film morphology makes the structure optimization difficult, and fundamental principles that relate to chemical structure, processing methods, and device performances have not yet been fully understood. On the other hand, various high‐powered techniques ranging from in‐house instrumentation to synchrotron techniques have been applied to this tremendously difficult research topic. More structural details, including length scale of phase separation, structural ordering, chain/molecular orientation, surface topology, etc., can be obtained in a quantitative manner, which finally allows the structure–property relationships to be determined. Here, the most important characterization techniques in understanding the morphology of BHJ solar cells are summarized, targeting chemists and materials scientists.
2D Ruddlesden–Popper perovskites (RPPs) are emerging as potential challengers to their 3D counterpart due to superior stability and competitive efficiency. However, the fundamental questions on energetics of the 2D RPPs are not well understood. Here, the energetics at (PEA)2(MA)n−1PbnI3n+1/[6,6]‐phenyl‐C61‐butyric acid methyl ester (PCBM) interfaces with varying n values of 1, 3, 5, 40, and ∞ are systematically investigated. It is found that n–n junctions form at the 2D RPP interfaces (n = 3, 5, and 40), instead of p–n junctions in the pure 2D and 3D scenarios (n = 1 and ∞). The potential gradient across phenethylammonium iodide ligands that significantly decreases surface work function, promotes separation of the photogenerated charge carriers with electron transferring from perovskite crystal to ligand at the interface, reducing charge recombination, which contributes to the smallest energy loss and the highest open‐circuit voltage (Voc) in the perovskite solar cells (PSCs) based on the 2D RPP (n = 5)/PCBM. The mechanism is further verified by inserting a thin 2D RPP capping layer between pure 3D perovskite and PCBM in PSCs, causing the Voc to evidently increase by 94 mV. Capacitance–voltage measurements with Mott–Schottky analysis demonstrate that such Voc improvement is attributed to the enhanced potential at the interface.
2D perovskite solar cells with high stability and high efficiency have attracted significant attention. A systematical static and dynamic structure investigation is carried out to show the details of 2D morphology evolution. A dual additive approach is used, where the synergy between an alkali metal cation and a polar solvent leads to high‐quality 2D perovskite films with sandwich‐type structures and vertical phase segregation. Such novel structure can induce high‐quality 2D slab growth and reduce internal and surface defects, resulting in a high device efficiency of 16.48% with enhanced continuous illumination stability and improved moisture (55–60%) and thermal (85 °C) tolerances. Transient absorption spectra reveal the carrier migration from low n to high n species with different kinetics. An [PbI6]4− octagon coalescence transformation mechanism coupled with metal and organic cations wrapped is proposed. By solvent vapor annealing, a recrystallization and reorientation of the 2D perovskite slabs occurs to form an ideal structure with improved device performance and stability.
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