Owing to enhanced charge transport efficiency arising from the ultrathin nature,two-dimensional(2D)organic semiconductor single crystals(OSSCs)are emerging as a fascinating platform for high-performance organic field-...Owing to enhanced charge transport efficiency arising from the ultrathin nature,two-dimensional(2D)organic semiconductor single crystals(OSSCs)are emerging as a fascinating platform for high-performance organic field-effect transistors(OFETs).However,ucoffee-ring"effect induced by an evaporation-induced convective flow near the contact line hinders the large-area growth of 2D OSSCs through a solution process.Here,we develop a new strategy of suppressing the"coffee-ring"effect by using an organic semiconductor:polymer blend solution.With the high-viscosity polymer in the organic solution,the evaporation-induced flow is remarkably weakened,ensuring the uniform molecule spreading for the 2D growth of the OSSCs.As an example,wafer-scale growth of crystalline film consisting of few-layered 2,7-didecylbenzothienobenzothiophene(C10-BTBT)crystals was successfully accomplished via blade coating.OFETs based on the crystalline film exhibited a maximum hole mobility up to 12.6 cm^2·V^-1·s^-1,along with an average hole mobility as high as 8.2 cm^2·V^-1·s^-1.Our work provides a promising strategy for the large-area growth of 2D OSSCs toward high-performance organic electronics.展开更多
The rational molecular design of light-emitting conjugated polymers that inherently suppress the ubiquitous coffee-ring effect(CRE)is a great challenge and the critical bottleneck for printing displays.Herein,we descr...The rational molecular design of light-emitting conjugated polymers that inherently suppress the ubiquitous coffee-ring effect(CRE)is a great challenge and the critical bottleneck for printing displays.Herein,we describe a supramolecular route to construct an intrinsically viscoelastic rigid conjugated polymer(RCP)(PHDPF-Cz)toward avoiding the CRE without sacrificing optoelectronic properties.Theπ-πstacking interactions derived fromthe pendant carbazole(Cz)units enable PHDPF-Cz to self-assemble into criss-cross nanofibers and endow its solutionwith great viscosity.Consequently,a high-quality and continuous PHDPFCz film was obtained by impeding the transport of aggregates to the droplet edge due to outward capillary flow during evaporation,in sharp contrast to the random aggregate migration and rapid precipitation generated fromthe controlled poly[4-(6-(9H-diphenylaniline-9-yl)hexyloxy)-9,9-diphenylfluorene]-co-[5-(6-(9H-diphenylaniline-9-yl)hexyloxy)-9,9-diphenylfluorene]and poly(9,9-dioctylfluorene)solutions.Finally,an efficient random laser is also achieved based on these cross-linked films with ultrastable single-chain excitonic behavior,confirming the effectiveness of our design strategy.展开更多
In the process of spraying coating perovskite films,the"coffee ring"effect(CRE)leads to the problem of excessive organic ammonium salt accumulation in local areas that cannot be completely eliminated.We intr...In the process of spraying coating perovskite films,the"coffee ring"effect(CRE)leads to the problem of excessive organic ammonium salt accumulation in local areas that cannot be completely eliminated.We introduce an in-situ targeted defect-healing strategy by incorporating butylamine formate(BAFa)ionic liquid into the spray ink.Ionic liquids,due to their long carbon chain structure,tend to target flow towards the CRE region during the droplet evaporation process.The coordination between the lone pair electrons in the C=O group of BAFa and Pb^(2+)effectively reduces defects in perovskite and suppresses non-radiative recombination losses.Simultaneously,amine ligands,which are repelled to the film surface and grain boundaries,form a thin insulating monolayer in the CRE areas,forcing charge carriers to transport through areas of the perovskite with fewer defects.This approach enables the crystallization control and defect-heal over the Cs_(0.19)FA_(0.81)PbI_(3-x-y)Br_(x)Cl_(y)perovskite films.Consequently,the champion perovskite solar cell achieved a power conversion efficiency of 22.04%,while mini-modules with an effective area of 64.8 cm^(2)reached a peak power conversion efficiency of 18.35%,demonstrating the significant potential for commercializing large-area perovskite solar cells.展开更多
Metal oxide thin-films transistors(TFTs)produced from solution-based printing techniques can lead to large-area electronics with low cost.However,the performance of current printed devices is inferior to those from va...Metal oxide thin-films transistors(TFTs)produced from solution-based printing techniques can lead to large-area electronics with low cost.However,the performance of current printed devices is inferior to those from vacuum-based methods due to poor film uniformity induced by the“coffeering”effect.Here,we report a novel approach to print highperformance indium tin oxide(ITO)-based TFTs and logic inverters by taking advantage of such notorious effect.ITO has high electrical conductivity and is generally used as an electrode material.However,by reducing the film thickness down to nanometers scale,the carrier concentration of ITO can be effectively reduced to enable new applications as active channels in transistors.The ultrathin(~10-nm-thick)ITO film in the center of the coffee-ring worked as semiconducting channels,while the thick ITO ridges(>18-nm-thick)served as the contact electrodes.The fully inkjet-printed ITO TFTs exhibited a high saturation mobility of 34.9 cm2 V^(−1) s^(−1) and a low subthreshold swing of 105 mV dec^(−1).In addition,the devices exhibited excellent electrical stability under positive bias illumination stress(PBIS,ΔV_(th)=0.31 V)and negative bias illuminaiton stress(NBIS,ΔV_(th)=−0.29 V)after 10,000 s voltage bias tests.More remarkably,fully printed n-type metal–oxide–semiconductor(NMOS)inverter based on ITO TFTs exhibited an extremely high gain of 181 at a low-supply voltage of 3 V,promising for advanced electronics applications.展开更多
The formations of desiccation cracks and their pattems in drying droplets of protein solutions are studied experimentally. The solvent evaporation causes the dehydration self-organization phenomenon in colloidal dropl...The formations of desiccation cracks and their pattems in drying droplets of protein solutions are studied experimentally. The solvent evaporation causes the dehydration self-organization phenomenon in colloidal droplets, followed by the formations of desiccation cracks. Two categories of highly ordered crack patterns, which we name ＂daisy＂ and ＂wavy-ring＂, are identified in the drying droplets. We explore the shifting of crack patterns from the ＂daisy＂ to the ＂wavy-ring＂ by varying the concentration of protein droplets. The results show that the concentration correlates with the pattern of deposition film directly, and modulates the periodicity of the crack pattern. We investigate the formations and periodicities of these two kinds of crack patterns, and obtain the scaling law of periodicity of the ＂wavy-ring＂ crack pattern. The relationship between the deposition pattern and the highly ordered crack patterns is also examined. This study will help in understanding the formation mechanisms of crack patterns in drying droplets of protein solutions and assist the future design of crack patterns in practical applications.展开更多
基金This work was supported by the National Natural Science Foundation of China(Nos.51973147,61904117,51821002 and 51672180)the Natural Science Foundation of Jiangsu Province of China(No.BK20180845)+1 种基金the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD),the 111 Project,Joint International Research Laboratory of Carbon-Based Functional Materials and DevicesThe authors thank the Collaborative Innovation Center of Suzhou Nano Science and Technology(Nano-CIC),Soochow University and Beamline BLI4B1(Shanghai Synchrotron Radiation Facility)for providing beam time.
文摘Owing to enhanced charge transport efficiency arising from the ultrathin nature,two-dimensional(2D)organic semiconductor single crystals(OSSCs)are emerging as a fascinating platform for high-performance organic field-effect transistors(OFETs).However,ucoffee-ring"effect induced by an evaporation-induced convective flow near the contact line hinders the large-area growth of 2D OSSCs through a solution process.Here,we develop a new strategy of suppressing the"coffee-ring"effect by using an organic semiconductor:polymer blend solution.With the high-viscosity polymer in the organic solution,the evaporation-induced flow is remarkably weakened,ensuring the uniform molecule spreading for the 2D growth of the OSSCs.As an example,wafer-scale growth of crystalline film consisting of few-layered 2,7-didecylbenzothienobenzothiophene(C10-BTBT)crystals was successfully accomplished via blade coating.OFETs based on the crystalline film exhibited a maximum hole mobility up to 12.6 cm^2·V^-1·s^-1,along with an average hole mobility as high as 8.2 cm^2·V^-1·s^-1.Our work provides a promising strategy for the large-area growth of 2D OSSCs toward high-performance organic electronics.
基金The work was supported by the National Natural Science Foundation of China(nos.22075136 and 61874053)National Key Research and Development Program of China(no.2020YFA0709900)+5 种基金Natural Science Funds of the Education Committee of Jiangsu Province(no.18KJA430009)Natural Science Foundation of Jiangsu Province(no.BK20200700)“High-Level Talents in Six Industries”of Jiangsu Province(no.XYDXX-019)China Postdoctoral Science Foundation(no.2021M692623)the Open Research Fund from State Key Laboratory of Supramolecular Structure and Materials(no.sklssm202108)Anhui Province Key Laboratory of Environment-friendly Polymer Materials and Anhui Province Key Laboratory of Optoelectronic Materials Science and Technology,Research Innovation in University of Jiangsu Province(nos.KYCX21_0771,KYCX21_0772,and KYCX21_1097).
文摘The rational molecular design of light-emitting conjugated polymers that inherently suppress the ubiquitous coffee-ring effect(CRE)is a great challenge and the critical bottleneck for printing displays.Herein,we describe a supramolecular route to construct an intrinsically viscoelastic rigid conjugated polymer(RCP)(PHDPF-Cz)toward avoiding the CRE without sacrificing optoelectronic properties.Theπ-πstacking interactions derived fromthe pendant carbazole(Cz)units enable PHDPF-Cz to self-assemble into criss-cross nanofibers and endow its solutionwith great viscosity.Consequently,a high-quality and continuous PHDPFCz film was obtained by impeding the transport of aggregates to the droplet edge due to outward capillary flow during evaporation,in sharp contrast to the random aggregate migration and rapid precipitation generated fromthe controlled poly[4-(6-(9H-diphenylaniline-9-yl)hexyloxy)-9,9-diphenylfluorene]-co-[5-(6-(9H-diphenylaniline-9-yl)hexyloxy)-9,9-diphenylfluorene]and poly(9,9-dioctylfluorene)solutions.Finally,an efficient random laser is also achieved based on these cross-linked films with ultrastable single-chain excitonic behavior,confirming the effectiveness of our design strategy.
基金supported by the National Natural Science Foundation of China(U21A20171,U20A20245)Natural Scienceof Hubei Province(2023AFA010)Independent Innovation Projects of the Hubei Longzhong Laboratory。
文摘In the process of spraying coating perovskite films,the"coffee ring"effect(CRE)leads to the problem of excessive organic ammonium salt accumulation in local areas that cannot be completely eliminated.We introduce an in-situ targeted defect-healing strategy by incorporating butylamine formate(BAFa)ionic liquid into the spray ink.Ionic liquids,due to their long carbon chain structure,tend to target flow towards the CRE region during the droplet evaporation process.The coordination between the lone pair electrons in the C=O group of BAFa and Pb^(2+)effectively reduces defects in perovskite and suppresses non-radiative recombination losses.Simultaneously,amine ligands,which are repelled to the film surface and grain boundaries,form a thin insulating monolayer in the CRE areas,forcing charge carriers to transport through areas of the perovskite with fewer defects.This approach enables the crystallization control and defect-heal over the Cs_(0.19)FA_(0.81)PbI_(3-x-y)Br_(x)Cl_(y)perovskite films.Consequently,the champion perovskite solar cell achieved a power conversion efficiency of 22.04%,while mini-modules with an effective area of 64.8 cm^(2)reached a peak power conversion efficiency of 18.35%,demonstrating the significant potential for commercializing large-area perovskite solar cells.
基金This research was financially supported under the Westlake Multidisciplinary Research Initiative Center(MRIC)Seed Fund(Grant No.MRIC20200101).
文摘Metal oxide thin-films transistors(TFTs)produced from solution-based printing techniques can lead to large-area electronics with low cost.However,the performance of current printed devices is inferior to those from vacuum-based methods due to poor film uniformity induced by the“coffeering”effect.Here,we report a novel approach to print highperformance indium tin oxide(ITO)-based TFTs and logic inverters by taking advantage of such notorious effect.ITO has high electrical conductivity and is generally used as an electrode material.However,by reducing the film thickness down to nanometers scale,the carrier concentration of ITO can be effectively reduced to enable new applications as active channels in transistors.The ultrathin(~10-nm-thick)ITO film in the center of the coffee-ring worked as semiconducting channels,while the thick ITO ridges(>18-nm-thick)served as the contact electrodes.The fully inkjet-printed ITO TFTs exhibited a high saturation mobility of 34.9 cm2 V^(−1) s^(−1) and a low subthreshold swing of 105 mV dec^(−1).In addition,the devices exhibited excellent electrical stability under positive bias illumination stress(PBIS,ΔV_(th)=0.31 V)and negative bias illuminaiton stress(NBIS,ΔV_(th)=−0.29 V)after 10,000 s voltage bias tests.More remarkably,fully printed n-type metal–oxide–semiconductor(NMOS)inverter based on ITO TFTs exhibited an extremely high gain of 181 at a low-supply voltage of 3 V,promising for advanced electronics applications.
基金supported by the National Natural Science Foundation of China(Grant Nos.U1562105,11372313)the Chinese Academy of Sciences through CAS Interdisciplinary Innovation Team Project+1 种基金the Chinese Academy of Sciences Key Research Program of Frontier Sciences(Grant No.QYZDJ-SSW-JSC019)the Chinese Academy of Sciences Strategic Priority Research Program(Grant No.XDB22040401)
文摘The formations of desiccation cracks and their pattems in drying droplets of protein solutions are studied experimentally. The solvent evaporation causes the dehydration self-organization phenomenon in colloidal droplets, followed by the formations of desiccation cracks. Two categories of highly ordered crack patterns, which we name ＂daisy＂ and ＂wavy-ring＂, are identified in the drying droplets. We explore the shifting of crack patterns from the ＂daisy＂ to the ＂wavy-ring＂ by varying the concentration of protein droplets. The results show that the concentration correlates with the pattern of deposition film directly, and modulates the periodicity of the crack pattern. We investigate the formations and periodicities of these two kinds of crack patterns, and obtain the scaling law of periodicity of the ＂wavy-ring＂ crack pattern. The relationship between the deposition pattern and the highly ordered crack patterns is also examined. This study will help in understanding the formation mechanisms of crack patterns in drying droplets of protein solutions and assist the future design of crack patterns in practical applications.
