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The rapid advance of fused‐ring electron acceptors (FREAs) has greatly promoted the leap‐forward development of organic solar cells (OSCs). However, the synthetic complexity of FREAs may be detrimental for future commercial applications. Recently, nonfused‐ring electron acceptors (NREAs) have been developed to be a promising candidate to maintain a rational balance between cost and performance, of which the cores are composed of simple fused rings (NREAs‐I) or nonfused rings (NREAs‐II). Moreover, "noncovalently conformational locks", are used as an effective strategy to enhance the rigidity and planarity of NREAs and improve device performance. Herein, a novel series of NREAs‐II (PhO4T‐1, PhO4T‐2, and PhO4T‐3) is constructed as a valuable platform for exploring the impact of the end group engineering on optoelectronic properties, intermolecular packing behaviors, and device performance. As a result, a high power conversion efficiency of 13.76% is achieved for PhO4T‐3 based OSCs, which is much higher than those of the PhO4T‐1 and PhO4T‐2‐based devices. Compared with several representative FREAs, PhO4T‐3 possesses the highest figure‐of‐merit value of 133.45 based on a cost‐efficiency evaluation. This work demonstrates that the simple‐structured NREAs‐II are promising candidates for low‐cost and high‐performance OSCs. [ABSTRACT FROM AUTHOR]

Solid-state refrigeration based on the caloric effect is viewed as a promising efficient and clean refrigeration technology. Barocaloric materials were developed rapidly but have since encountered a general obstacle: the prominent caloric effect cannot be utilized reversibly under moderate pressure. Here, we report a mechanism of an emergent large, reversible barocaloric effect (BCE) under low pressure in the hybrid organic–inorganic layered perovskite (CH3–(CH2)n−1–NH3)2MnCl4 (n = 9,10), which show the reversible barocaloric entropy change as high as ΔSr ∼ 218, 230 J kg−1 K−1 at 0.08 GPa around the transition temperature (Ts ∼ 294, 311.5 K). To reveal the mechanism, single-crystal (CH3–(CH2)n−1–NH3)2MnCl4 (n = 10) was successfully synthesized, and high-resolution single-crystal X-ray diffraction (SC-XRD) was carried out. Then, the underlying mechanism was determined by combining infrared (IR) spectroscopy and density function theory (DFT) calculations. The colossal reversible BCE and the very small hysteresis of 2.6 K (0.1 K/min) and 4.0 K (1 K/min) are closely related to the specific hybrid organic–inorganic structure and single-crystal nature. The drastic transformation of organic chains confined to the metallic frame from ordered rigidity to disordered flexibility is responsible for the large phase-transition entropy comparable to the melting entropy of organic chains. This study provides new insights into the design of novel barocaloric materials by utilizing the advantages of specific organic–inorganic hybrid characteristics.Solid-state coolants: Hybrid crystals deliver big chills at low pressures Materials that can absorb and release heat under low mechanical pressure hold promise for high-efficiency refrigeration technology. Recent studies have shown that significant compression-induced cooling effects at low pressures can be achieved using crystals known as perovskites containing layers of organic chains and metal cations. Yihong Gao from the Chinese Academy of Sciences in Beijing and colleagues have now uncovered the mechanism underlying the thermal response of layered perovskites. Using a combination of x-rays, spectroscopy and theoretical calculations, the team discovered how the crystal structure changes at different temperatures. Their experiments revealed a low-energy phase transition where organic chains transform from rigid states to highly flexible conformations held in place by metallic layers. The large entropy change associated with this transition and its reversible nature could aid in the design of other organic–inorganic solid-state coolants.For the emergent colossal, reversible barocaloric effect in organic–inorganic perovskite hybrids (CH3–(CH2)n−1–NH3)2MnCl4 (n = 9, 10), we successfully grew a single crystal, and the underlying mechanism was determined by high-resolution SC-XRD, IR spectroscopy and DFT calculations. The drastic transformation of organic chains confined to the metallic frame from ordered rigidity to disordered flexibility is responsible for the large phase-transition entropy, which is comparable to the melting entropy of organic chains. The result provides new insights into designing novel barocaloric materials by utilizing the disordering of organic chains of organic–inorganic hybrid materials. [ABSTRACT FROM AUTHOR]

Noncovalently fused-ring electron acceptors (NFREAs) have attracted much attention in recent years owing to their advantages of simple synthetic routes, high yields and low costs. However, the efficiencies of NFREAs based organic solar cells (OSCs) are still far behind those of fused-ring electron acceptors (FREAs). Herein, a series of NFREAs with S⋅⋅⋅O noncovalent intramolecular interactions were designed and synthesized with a two-step synthetic route. Upon introducing π-extended end-groups into the backbones, the electronic properties, charge transport, film morphology, and energy loss were precisely tuned by fine-tuning the degree of multi-fluorination. As a result, a record PCE of 14.53 % in labs and a certified PCE of 13.8 % for NFREAs based devices were obtained. This contribution demonstrated that combining the strategies of noncovalent conformational locks and π-extended end-group engineering is a simple and effective way to explore high-performance NFREAs., (© 2021 Wiley-VCH GmbH.)