Two-dimensional organic semiconductor single crystals(2D OSSCs)have great potential for use in highperformance optoelectronic devices.However,challenges associated with controlling complex fluid dynamics and molecular...Two-dimensional organic semiconductor single crystals(2D OSSCs)have great potential for use in highperformance optoelectronic devices.However,challenges associated with controlling complex fluid dynamics and molecular mass transfer during solution-based processes hinder large-scale high-quality production.To address this issue,we developed a nanoconfinement-driven approach for controlling molecular crystallization,improving isotropic molecular mass transfer in fluids,and regulating the morphology of the 2D molecular film.Using a dual-solvent strategy,we created a stable nanoscale extended evaporation meniscus that modulates molecular nucleation and growth dynamics,thereby facilitating the direct shift from one-dimensional to two-dimensional crystals.Dual solvents are essential for generating and maintaining nanoscale wet films during meniscal recession,which is crucial for 2D crystal engineering.Mechanistic studies revealed that adhesion in a dual-solvent system is vital for meniscus formation while disjoining pressure maintains its stability.We also systematically evaluated several[1]benzothieno[3,2-b][1]benzothiophenes(BTBTs)bearing various alkyl chains,which revealed how molecular interactions affect morphology during printing.Organic-field-effect transistors fabricated using 2D OSSCs have significantly higher carrier mobilities than those with striped structures.Moreover,the highly ordered 2D C8-BTBT single-crystal thin film exhibited high sensitivity to polarized ultraviolet light,boasting a dichroic ratio of 2.80 and demonstrating exceptional imaging capabilities for polarized ultraviolet light.展开更多
基金supported by the National Natural Science Foundation of China(22175185,52293470,52321006,T2394480,and T2394484)the National Key R&D Program of China(2018YFA0703200)+1 种基金the Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-202005)the CAS-VPST Silk Road Science Fund 2022(121111KYSB20210006).
文摘Two-dimensional organic semiconductor single crystals(2D OSSCs)have great potential for use in highperformance optoelectronic devices.However,challenges associated with controlling complex fluid dynamics and molecular mass transfer during solution-based processes hinder large-scale high-quality production.To address this issue,we developed a nanoconfinement-driven approach for controlling molecular crystallization,improving isotropic molecular mass transfer in fluids,and regulating the morphology of the 2D molecular film.Using a dual-solvent strategy,we created a stable nanoscale extended evaporation meniscus that modulates molecular nucleation and growth dynamics,thereby facilitating the direct shift from one-dimensional to two-dimensional crystals.Dual solvents are essential for generating and maintaining nanoscale wet films during meniscal recession,which is crucial for 2D crystal engineering.Mechanistic studies revealed that adhesion in a dual-solvent system is vital for meniscus formation while disjoining pressure maintains its stability.We also systematically evaluated several[1]benzothieno[3,2-b][1]benzothiophenes(BTBTs)bearing various alkyl chains,which revealed how molecular interactions affect morphology during printing.Organic-field-effect transistors fabricated using 2D OSSCs have significantly higher carrier mobilities than those with striped structures.Moreover,the highly ordered 2D C8-BTBT single-crystal thin film exhibited high sensitivity to polarized ultraviolet light,boasting a dichroic ratio of 2.80 and demonstrating exceptional imaging capabilities for polarized ultraviolet light.
