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• W3169372242 abstract "Understanding the fundamental origin of morphological degradation in non-fullerene acceptor-based organic solar cells is challenging. In the April 2021 issue of Nature Materials, Ghasemi et al. reveal that the most thermodynamically unstable and low-miscibility systems with high Flory-Huggins interaction parameter (χ) exhibit the most kinetically stable (low diffusion) morphology for superior device operation stability under thermal stress. Understanding the fundamental origin of morphological degradation in non-fullerene acceptor-based organic solar cells is challenging. In the April 2021 issue of Nature Materials, Ghasemi et al. reveal that the most thermodynamically unstable and low-miscibility systems with high Flory-Huggins interaction parameter (χ) exhibit the most kinetically stable (low diffusion) morphology for superior device operation stability under thermal stress. Organic solar cells (OSCs) contain a blend of electron-donating and electron-accepting molecules to form a nanoscale interpenetrating network that provides a sufficient exciton separation with small pure phase and efficient charge transport and extraction with percolation pathways.1Yu G. Gao J. Hummelen J.C. Wudl F. Heeger A.J. Polymer photovoltaic cells: Enhanced efficiencies via a network of internal donor-acceptor heterojunctions.Science. 1995; 270: 1789-1791Crossref Scopus (9508) Google Scholar Although fullerene-based electron acceptors have been widely used due to their high electron affinity for charge separation and high electron mobility for efficient charge transport leading to high efficiency OSCs, their limited synthetic flexibility makes it difficult to alter their absorption range and energy levels. There are also concerns over their stability undergoing detrimental aggregation under thermal stress and showing of high sensitivity to light and oxygen.2Lee H.K.H. Telford A.M. Röhr J.A. Wyatt M.F. Rice B. Wu J. De Castro Maciel A. Tuladhar S.M. Speller E. McGettrick J. et al.The role of fullerenes in the environmental stability of polymer:fullerene solar cells.Energy Environ. Sci. 2018; 11: 417-428Crossref Google Scholar The development of non-fullerene acceptors (NFAs) to replace these fullerene acceptors has driven a rapid increase in the power conversion efficiency (PCE) of OSCs, exceeding 18% due to excellent tunability of electron affinity and bandgaps to increase open circuit voltage (VOC) and current density (JSC).3Liu Q. Jiang Y. Jin K. Qin J. Xu J. Li W. Xiong J. Liu J. Xiao Z. Sun K. et al.18% Efficiency organic solar cells.Sci. Bull. (Beijing). 2020; 65: 272-275Crossref Scopus (1678) Google Scholar However, while some NFA-based OSCs exhibit improved morphological stability with less degradation compared to fullerene-based OSCs,4Du X. Heumueller T. Gruber W. Classen A. Unruh T. Li N. Brabec C.J. Efficient Polymer Solar Cells Based on Non-fullerene Acceptors with Potential Device Lifetime Approaching 10 Years.Joule. 2019; 3: 215-226Abstract Full Text Full Text PDF Scopus (243) Google Scholar achieving long-term device stability remains a key challenge to overcome for their commercialization due to the lack of the design rules and understanding of their degradation mechanisms for enhancing their stability. The optimal morphology of OSCs is crucial to achieve the optimum trade-off in the bulk heterojunction morphology between a highly intermixed phase of electron-donating and electron-accepting molecules and the molecular packing and aggregation within pure donor and/or pure acceptor phases.5Wang Y. Lee J. Hou X. Labanti C. Yan J. Mazzolini E. Parhar A. Nelson J. Kim J.S. Li Z. Recent Progress and Challenges toward Highly Stable Nonfullerene Acceptor-Based Organic Solar Cells.Adv. Energy Mater. 2021; 11: 2003002Crossref Scopus (64) Google Scholar In addition, the morphological stability is an important issue to realize long-term device operation under illumination or thermal stress. While thermally induced aggregation, phase demixing, and vertical separation have been known as possible degradation pathways of fullerene-based OSCs, some NFA molecules have shown a lower tendency to diffuse and aggregate within the donor polymer matrix, reducing the formation of detrimental aggregates and improving their morphological stability.6Hu H. Ghasemi M. Peng Z. Zhang J. Rech J.J. You W. Yan H. Ade H. The Role of Demixing and Crystallization Kinetics on the Stability of Non-Fullerene Organic Solar Cells.Adv. Mater. 2020; 32: e2005348Crossref PubMed Scopus (29) Google Scholar Recently it has been reported that small pure NFA phase can give a high degree of thermal stability, fabricating with a reduced molecular packing time to suppress the multi-crystalline structure and enhance the face-on π–π stacking of NFAs.7Zhang Z. Liu X. Yu J. Wang H. Zhang M. Yang L. Geng R. Cao J. Du F. Liu F. et al.Enhancing phase separation with a conformation-locked nonfullerene acceptor for over 14.4% efficiency solar cells.J. Mater. Chem. C Mater. Opt. Electron. Devices. 2019; 7: 13279-13286Crossref Google Scholar However, the key factors determining the morphological stability of NFA-based solar cells remain unexplained. Therefore, to achieve highly stable, high-performance OSCs, a quantitative property-function relation is needed to predict morphological stability. Writing in the April 2021 issue of Nature Materials, Ghasemi et al.8Ghasemi M. Balar N. Peng Z. Hu H. Qin Y. Kim T. Rech J.J. Bidwell M. Mask W. McCulloch I. et al.A molecular interaction-diffusion framework for predicting organic solar cell stability.Nat. Mater. 2021; 20: 525-532Crossref PubMed Scopus (63) Google Scholar establish the molecular interaction-diffusion framework to predict OSC stability, studying the kinetic and thermodynamic factors governing the morphological stability of several NFA-based OSC systems. They revealed that the diffusion of the NFA molecules into donor polymer domains shows Arrhenius behavior, and the activation energy (Ea) exhibits linear relations with χHT, including the enthalpic interaction parameters (χH) between the polymer and the NFA molecules, and shows exponential relations with diffusion coefficient (D) (Figures 1A and 1B ). The D has linear relations with relatively easily measurable mechanical and thermal properties, such as glass transition temperature (Tg) of NFA and elastic modulus (EF) of the polymer (Figures 1C and 1D). In addition, the study in Nature Materials reveals that highly hypo-miscible systems with large χH, high Ea and low D exhibit the kinetically stable morphology. Therefore, the correlations between thermodynamic, diffusion, thermal, and mechanical properties of polymer:NFA blends provide a guideline to evaluate promising materials for their long-term stability of OSCs. Understanding the intrinsic stability of organic molecules is necessary toward superior stability, with various aspects to be taken into account such as NFA chemical structure, molecular conformation, structural rigidity, symmetry, and energetics. Although the high-performance NFA Y6 shows highly rigid molecular structure controlled by outer core alkyl chains conformational locking, they do not provide device stability.9Yang W. Luo Z. Sun R. Guo J. Wang T. Wu Y. Wang W. Guo J. Wu Q. Shi M. et al.Simultaneous enhanced efficiency and thermal stability in organic solar cells from a polymer acceptor additive.Nat. Commun. 2020; 11: 1218Crossref PubMed Scopus (111) Google Scholar This suggests that additionally altering of NFA molecular structure is needed to boost device efficiency and ensure long-term device stability. Owing to many researchers’ effort to develop synthetic strategies such as 3D design, the NFA-based OSCs show promising thermal stability. However, understanding the key factors determining long-term device operation stability under thermal stress is still challenging. Here, the work from Ghasemi et al.8Ghasemi M. Balar N. Peng Z. Hu H. Qin Y. Kim T. Rech J.J. Bidwell M. Mask W. McCulloch I. et al.A molecular interaction-diffusion framework for predicting organic solar cell stability.Nat. Mater. 2021; 20: 525-532Crossref PubMed Scopus (63) Google Scholar is based on aiming to kinetically hypo-miscible systems in a mixed phase with a sufficient electron-acceptor content to enable electron percolation in order to acquire morphological stability under thermal stress. Here, we note that the low-miscibility systems may bring low device performance due to insufficient exciton separation and diffusion. Therefore, the blend system should exhibit a good balance between a nanoscale interpenetrating network and hypo-miscibility to achieve high performance as well as high morphological stability for organic solar cells. Consequently, the important take-home messages from Ghasemi et al.’s8Ghasemi M. Balar N. Peng Z. Hu H. Qin Y. Kim T. Rech J.J. Bidwell M. Mask W. McCulloch I. et al.A molecular interaction-diffusion framework for predicting organic solar cell stability.Nat. Mater. 2021; 20: 525-532Crossref PubMed Scopus (63) Google Scholar research are (1) the diffusion of NFA molecules into the donor polymers exhibits Arrhenius behavior and that the Ea scales linearly with the χH, and (2) the most thermodynamically unstable and low-miscibility systems with high χH exhibit the most kinetically stable morphology for superior stable device operation under thermal stress. The study thus validates the differences in Ea to measured and selectively simulated molecular self-interaction properties of the constituent materials and develop quantitative property-function relations that link thermal and mechanical characteristics of the NFA and polymer to predict relative diffusion properties and morphological stability. It may also be interesting that this morphological stability issue is likely to be much less of an issue for some ternary or all polymer blends and perhaps one reason why such blends can show enhanced thermal stability compared to binary polymer:NFA blend solar cells. Recently, highly efficient, highly stable, ternary blend all-polymer solar cells have been highlighted by Sun et al.10Sun R. Wang W. Yu H. Sun R. Wang W. Yu H. Chen Z. Xia X. Shen H. Guo J. et al.Achieving over 17% efficiency of ternary all- polymer solar cells with two well-compatible polymer acceptors Achieving over 17% efficiency of ternary all-polymer solar cells with two well-compatible polymer acceptors.Joule. 2021; https://doi.org/10.1016/j.joule.2021.04.007Abstract Full Text Full Text PDF Scopus (112) Google Scholar in Joule. A ternary blend with the newly designed near-infrared polymer acceptors PY2F-T and polymer donor PM6 showed 17.2% with PYT as the third component achieving the complementary absorption spectra and finely tuned microstructures of the ternary blend. Interestingly, the ternary blend exhibited photo-thermal stability compared to binary blend and highlighted the ternary strategy—a promising approach to improve the stabilities of all polymers system. Analogous to the work of Ghasemi et al.,8Ghasemi M. Balar N. Peng Z. Hu H. Qin Y. Kim T. Rech J.J. Bidwell M. Mask W. McCulloch I. et al.A molecular interaction-diffusion framework for predicting organic solar cell stability.Nat. Mater. 2021; 20: 525-532Crossref PubMed Scopus (63) Google Scholar this study demonstrated that, for ternary blend all-polymer with polymeric NFA materials, the phase separated morphologies of binary system have been investigated by the Flory-Huggins theory in which the enthalpic and entropic contribution for mixing two types of polymer materials are considered quantitatively. Sun et al.10Sun R. Wang W. Yu H. Sun R. Wang W. Yu H. Chen Z. Xia X. Shen H. Guo J. et al.Achieving over 17% efficiency of ternary all- polymer solar cells with two well-compatible polymer acceptors Achieving over 17% efficiency of ternary all-polymer solar cells with two well-compatible polymer acceptors.Joule. 2021; https://doi.org/10.1016/j.joule.2021.04.007Abstract Full Text Full Text PDF Scopus (112) Google Scholar considered the interfacial surface energy and solubility of the polymeric NFA acceptor, resulting in suppressed phase separation and suitably fixed blend microstructure with the third component introduced to the binary blend. Going forward, it would be stimulating to understand the degradation mechanism of more complicated morphology such as all-polymer blends and ternary blends. Interestingly, morphological degradation in NFA-based OSCs, responsible for the thermal stability in NFA-based OSCs, relies on thermodynamic and kinetic behavior of NFA molecules governed by self-interaction energy (and cohesive energy density) of molecules. Consequently, the design strategies of NFA molecules need to follow a high activation energy and low diffusion coefficient with molecular self-interactions toward thermal stability. With greater thermodynamic understanding suggesting the key requirement of thermally stable morphology of photoactive layer, we envision that the landscape for NFA design will change in the coming years. The wider applicability of the proposed model to other newly synthesizing NFA and complicated morphological systems will be the focus of future studies. This work thus poses new and important insights into property-function relations for predicting morphological stability by evaluating thermodynamic and kinetic factors, which lie at the heart of future commercialized OSCs. This work was supported by a National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) ( NRF-2021R1C1C1009032 ). Both authors would like to thank James R. Durrant for proofreading the manuscript." @default.
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• W3169372242 title "Understanding what determines the organic solar cell stability" @default.
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