The solution aggregation structures of conjugated polymers are pivotal in determining their film morphology and optoelectronic properties,yet the relationship between solution aggregation and device performance remain...The solution aggregation structures of conjugated polymers are pivotal in determining their film morphology and optoelectronic properties,yet the relationship between solution aggregation and device performance remains elusive in organic photodiode(OPD)systems.Herein,we introduce the first examination of solution aggregation structures of all-polymer OPD blends,with a focus on how molecular entanglement modulates aggregation behavior and subsequent photodiode performance of low-cost poly(3-pentylthiophene).Using small-angle neutron scattering and freeze-dried imaging,we provide a comprehensive analysis of the solution-state aggregation behavior of poly(3-pentylthiophene)and its evolution in the blend,revealing profound impacts on film morphology and device performance.With finely optimized aggregation,the resulting all-polymer OPD achieves a record-high specific detectivity of ~4×10^(13) Jones at zero bias,outperforming all bulk heterojunction(BHJ)-type self-powered OPDs reported to date.This device also demonstrates remarkable thermal stability,with negligible performance degradation after over 800 h of thermal annealing at 85℃.Furthermore,the self-powered OPD exhibits excellent performance across a broad spectral range,enabling its application in both water quality monitoring and biosensing.This work offers new insights into the solution aggregation behavior of conjugated polymers in OPDs and highlights the importance of resolving solution aggregation in optimizing device function.展开更多
Halide perovskites are promising candidates for optoelectronic devices,but their solution-processed films frequently suffer from solute aggregation,crystalline disorder,and random orientation,that is,defects that sign...Halide perovskites are promising candidates for optoelectronic devices,but their solution-processed films frequently suffer from solute aggregation,crystalline disorder,and random orientation,that is,defects that significantly compromise device performance.These issues arise from complex multiscale interactions during film formation,where macroscopic mechanical forces could hypothetically influence atomic-scale assembly.This review elucidates the critical role of multiscale mechanical coupling(linking surface/interface mechanics,fluid dynamics,and crystallization kinetics)in governing perovskite film quality,which ultimately enhanced the uniformity of film thickness,photoelectric performance,and long-term stability.We first analyze how solvent evaporation,interfacial energy,and flow-induced shear shape the spatiotemporal evolution of solute distribution and crystal growth.Building on this understanding,we present mechanical regulation strategies aimed at directing film formation:modifying wettability through surfactants and surface energy modulators;manipulating flow behavior via Marangoni convection and shear stress;and mitigating interfacial stress through lattice and thermal expansion matching.To further enhance structural control,we highlight fabrication techniques that couple multiple external fields(e.g.,thermal,electrical,mechanical,and chemical fields)and leverage in situ characterization for real-time feedback.Finally,we explore machine learning-assisted multiscale modeling as a powerful tool to connect atomic interactions with macroscopic processing variables,enabling predictive optimization.By integrating these insights,this review establishes a unified framework for guiding high-quality,scalable perovskite film fabrication toward industrial deployment.展开更多
基金supported by the National Natural Science Foundation of China(22375143,52422313,52073207,and 52121002)the Science Fund for Distinguished Young Scholars of Tianjin Municipality(23JCJQJC00240)+2 种基金the Open Fund of Hubei Longzhong Laboratory(2022KF-01)Open Fund for Spallation Neutron Source in Songshan Lake Science City(KFKT2023B08)the Fundamental Research Funds for the Central Universities for their support in facilitating the characterization of small-angle neutron scattering。
文摘The solution aggregation structures of conjugated polymers are pivotal in determining their film morphology and optoelectronic properties,yet the relationship between solution aggregation and device performance remains elusive in organic photodiode(OPD)systems.Herein,we introduce the first examination of solution aggregation structures of all-polymer OPD blends,with a focus on how molecular entanglement modulates aggregation behavior and subsequent photodiode performance of low-cost poly(3-pentylthiophene).Using small-angle neutron scattering and freeze-dried imaging,we provide a comprehensive analysis of the solution-state aggregation behavior of poly(3-pentylthiophene)and its evolution in the blend,revealing profound impacts on film morphology and device performance.With finely optimized aggregation,the resulting all-polymer OPD achieves a record-high specific detectivity of ~4×10^(13) Jones at zero bias,outperforming all bulk heterojunction(BHJ)-type self-powered OPDs reported to date.This device also demonstrates remarkable thermal stability,with negligible performance degradation after over 800 h of thermal annealing at 85℃.Furthermore,the self-powered OPD exhibits excellent performance across a broad spectral range,enabling its application in both water quality monitoring and biosensing.This work offers new insights into the solution aggregation behavior of conjugated polymers in OPDs and highlights the importance of resolving solution aggregation in optimizing device function.
基金funded by the Zhejiang Provincial Natural Science Foundation of China(Grant LR25A020002,K.W.)the National Local Joint Laboratory for Advanced Textile Processing and Clean Production,Wuhan Textile University(Grant FX20240005,L.R.)the National Natural Science Foundation of China(Grant 12125205,J.Q.)。
文摘Halide perovskites are promising candidates for optoelectronic devices,but their solution-processed films frequently suffer from solute aggregation,crystalline disorder,and random orientation,that is,defects that significantly compromise device performance.These issues arise from complex multiscale interactions during film formation,where macroscopic mechanical forces could hypothetically influence atomic-scale assembly.This review elucidates the critical role of multiscale mechanical coupling(linking surface/interface mechanics,fluid dynamics,and crystallization kinetics)in governing perovskite film quality,which ultimately enhanced the uniformity of film thickness,photoelectric performance,and long-term stability.We first analyze how solvent evaporation,interfacial energy,and flow-induced shear shape the spatiotemporal evolution of solute distribution and crystal growth.Building on this understanding,we present mechanical regulation strategies aimed at directing film formation:modifying wettability through surfactants and surface energy modulators;manipulating flow behavior via Marangoni convection and shear stress;and mitigating interfacial stress through lattice and thermal expansion matching.To further enhance structural control,we highlight fabrication techniques that couple multiple external fields(e.g.,thermal,electrical,mechanical,and chemical fields)and leverage in situ characterization for real-time feedback.Finally,we explore machine learning-assisted multiscale modeling as a powerful tool to connect atomic interactions with macroscopic processing variables,enabling predictive optimization.By integrating these insights,this review establishes a unified framework for guiding high-quality,scalable perovskite film fabrication toward industrial deployment.
