Incorporating organic bulky cations in the precursor or post-treatment to achieve two-dimensional/thr ee-dimensional(2D/3D)heterojunction is an effective strategy for enhancing the stability of perovskite materials.Ho...Incorporating organic bulky cations in the precursor or post-treatment to achieve two-dimensional/thr ee-dimensional(2D/3D)heterojunction is an effective strategy for enhancing the stability of perovskite materials.However,the issue of insufficient charge transport in 2D perovskites limits their development,and the fundamental mechanism of out-of-plane carrier transport remains unclear.This study designed and synthesized seven organic phenyl-core cations,differentiated at the 1-and 1,4-positions,and identified the impacts on the corresponding properties of the 2D crystalline perovskite.Shorter cations facilitated a more compact arrangement of adjacent inorganic layers,aligning to favor charge transport along the vertical direction.In addition,introducing high electronegativity led to increased intermolecular interactions,resulting in enhanced structural stability and improved phenyl ring π-orbital overlap and interlayer electron coupling,yielding efficient charge transport.Resilience to thermal stressing of the perovskite was strongly correlated with the carbon chain length of the spacer cations.The increase in cation length and the reduction in the rigidity of the amino-terminal both aided in the dispersion of thermal stress in the inorganic framework.Additional hydrogen bonding also contributed to mitigating structural disorder.展开更多
Organic-inorganic halide perovskite,as a low-cost,solution-processable material with remarkable optoelectronic properties,is ideal candidate to fabricate high-performance photodetectors and is expected to significantl...Organic-inorganic halide perovskite,as a low-cost,solution-processable material with remarkable optoelectronic properties,is ideal candidate to fabricate high-performance photodetectors and is expected to significantly reduce device costs.Compared to the common Dion-Jacobson and Ruddlesden-Popper two-dimensional(2D)layered hybrid perovskite compounds,the perovskites with alternating cations in the interlayer(ACI)phase show higher crystal symmetry and narrower optical bandgaps,which exhibit great potential for excellent photodetection performance.Herein,we report a high-performance photodetector based on the 2D bilayered hybrid lead halide perovskite single crystal with the ACI phase(GAMA_(2)Pb_(2)I_(7);GA=C(NH_(2))_(3)and MA=CH_(3)NH_(3)).The single-crystal photodetector exhibits high photoresponsivity of 1.56,2.54,and 2.60 A/W for incident light wavelengths of 405,532,and 635 nm under 9.82 nW,respectively,together with the correspondingly high detectivity values of 1.86×10^(12),3.04×10^(12),and 3.11×10^(12)Jones under the same operating conditions.Meanwhile,a high-resolution imaging sensor is built based on the GAMA_(2)Pb_(2)I_(7)single-crystal photodetector,confirming the high stability and photosensitivity of the imaging system.These results show that the 2D hybrid lead halide perovskites with alternating interlayer cations are promising for high-performance visible light photodetectors and imaging systems.展开更多
To analyze the water swelling characteristics of black cotton soil(BCS),X-ray fluorescence and X-ray diffraction characterizations were performed to investigate the chemical compositions and types of clay minerals in ...To analyze the water swelling characteristics of black cotton soil(BCS),X-ray fluorescence and X-ray diffraction characterizations were performed to investigate the chemical compositions and types of clay minerals in BCS.A montmorillonite crystal lattice was established to simulate the hydration of interlayer cations by applying the SPC/E potential energy model,universal force field,algorithm of charge balance,and periodic boundary.Results indicated that the main clay mineral found in the BCS was montmorillonite(32.6%)with small amounts of interstratified illite-montmorillonite(10.9%),illite(2.3%),and kaolinite(1.5%).The high expansive potential of BCS comes from the strong adsorption property of montmorillonite with a high content of magnesium and sodium ions to water molecules.The exchangeable cations of Na^(+)in BCS were only 3.73%,but they enhanced the adsorption capacity of clay to water molecules and accelerated the hydration of Mg^(2+)(47.1%)and Ca^(2+)(4.78%).The free swell index can be used as a classification index of the swelling potential of BCS.展开更多
As emerging semiconductor materials,Dion-Jacobson(DJ)phase two-dimensional(2D)perovskites exhibit remarkable stability and structural diversity.However,their limited charge transport capability hinders further advance...As emerging semiconductor materials,Dion-Jacobson(DJ)phase two-dimensional(2D)perovskites exhibit remarkable stability and structural diversity.However,their limited charge transport capability hinders further advancement,and the underlying carrier transport mechanisms require deeper investigation.In this work,six diammonium spacer cations and their corresponding DJ-phase 2D perovskite single crystals were rationally designed and synthesized to explore how spacer characteristics(such as heterocyclic type and amino group substitution position)affect the properties of 2D perovskites.Diammonium cations with meta-substituted amino groups tended to adopt a tilted configuration to balance the interactions between both ends of the cation and the inorganic layers.This orientation helped reduce the interlayer spacing,weakened hydrogen bonding between the cation and the inorganic framework,and lowered lattice distortion,promoting efficient carrier generation and transport.Beyond steric hindrance from branched side chains,the thermal stability of perovskites was also closely related to the nature of the heterocycle within the spacer.Diammonium cations bearing flexible aliphatic rings can buffer thermal deformation of the inorganic layers,dissipating internal thermal stress and enhancing overall thermal stability.展开更多
With the support by the National Natural Science Foundation of China,a collaborative study by the research groups led by Prof.Fang Haiping(方海平)from Shanghai Institute of Applied Physics,Chinese Academy of Sciences,...With the support by the National Natural Science Foundation of China,a collaborative study by the research groups led by Prof.Fang Haiping(方海平)from Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Prof.Wu Minghong(吴明红)from Shanghai Applied Radiation Institute。展开更多
基金financially supported by the Key Fund Project of Tianjin Natural Science Foundation(24JCZDJC00510)the Fundamental Research Funds for the Central Universitiespartially supported by the U.S.Department of Energy under Contract No.DE-AC3608GO28308 with Alliance for Sustainable Energy,Limited Liability Company(LLC),the Manager and Operator of the National Renewable Energy Laboratory,through Grant No.DE-SC0020718。
文摘Incorporating organic bulky cations in the precursor or post-treatment to achieve two-dimensional/thr ee-dimensional(2D/3D)heterojunction is an effective strategy for enhancing the stability of perovskite materials.However,the issue of insufficient charge transport in 2D perovskites limits their development,and the fundamental mechanism of out-of-plane carrier transport remains unclear.This study designed and synthesized seven organic phenyl-core cations,differentiated at the 1-and 1,4-positions,and identified the impacts on the corresponding properties of the 2D crystalline perovskite.Shorter cations facilitated a more compact arrangement of adjacent inorganic layers,aligning to favor charge transport along the vertical direction.In addition,introducing high electronegativity led to increased intermolecular interactions,resulting in enhanced structural stability and improved phenyl ring π-orbital overlap and interlayer electron coupling,yielding efficient charge transport.Resilience to thermal stressing of the perovskite was strongly correlated with the carbon chain length of the spacer cations.The increase in cation length and the reduction in the rigidity of the amino-terminal both aided in the dispersion of thermal stress in the inorganic framework.Additional hydrogen bonding also contributed to mitigating structural disorder.
基金the Research Grants Council of the Hong Kong Special Administrative Region,China(CityU RFS2021-1S04).
文摘Organic-inorganic halide perovskite,as a low-cost,solution-processable material with remarkable optoelectronic properties,is ideal candidate to fabricate high-performance photodetectors and is expected to significantly reduce device costs.Compared to the common Dion-Jacobson and Ruddlesden-Popper two-dimensional(2D)layered hybrid perovskite compounds,the perovskites with alternating cations in the interlayer(ACI)phase show higher crystal symmetry and narrower optical bandgaps,which exhibit great potential for excellent photodetection performance.Herein,we report a high-performance photodetector based on the 2D bilayered hybrid lead halide perovskite single crystal with the ACI phase(GAMA_(2)Pb_(2)I_(7);GA=C(NH_(2))_(3)and MA=CH_(3)NH_(3)).The single-crystal photodetector exhibits high photoresponsivity of 1.56,2.54,and 2.60 A/W for incident light wavelengths of 405,532,and 635 nm under 9.82 nW,respectively,together with the correspondingly high detectivity values of 1.86×10^(12),3.04×10^(12),and 3.11×10^(12)Jones under the same operating conditions.Meanwhile,a high-resolution imaging sensor is built based on the GAMA_(2)Pb_(2)I_(7)single-crystal photodetector,confirming the high stability and photosensitivity of the imaging system.These results show that the 2D hybrid lead halide perovskites with alternating interlayer cations are promising for high-performance visible light photodetectors and imaging systems.
基金The National Natural Science Foundation of China(No.51778139)Jiangsu Planned Projects for Postdoctoral Research Funds(No.2020Z422).
文摘To analyze the water swelling characteristics of black cotton soil(BCS),X-ray fluorescence and X-ray diffraction characterizations were performed to investigate the chemical compositions and types of clay minerals in BCS.A montmorillonite crystal lattice was established to simulate the hydration of interlayer cations by applying the SPC/E potential energy model,universal force field,algorithm of charge balance,and periodic boundary.Results indicated that the main clay mineral found in the BCS was montmorillonite(32.6%)with small amounts of interstratified illite-montmorillonite(10.9%),illite(2.3%),and kaolinite(1.5%).The high expansive potential of BCS comes from the strong adsorption property of montmorillonite with a high content of magnesium and sodium ions to water molecules.The exchangeable cations of Na^(+)in BCS were only 3.73%,but they enhanced the adsorption capacity of clay to water molecules and accelerated the hydration of Mg^(2+)(47.1%)and Ca^(2+)(4.78%).The free swell index can be used as a classification index of the swelling potential of BCS.
基金financially supported by the Key Fund Project of the Tianjin Natural Science Foundation(24JCZDJC00510)the Fundamental Research Funds for the Central Universities.
文摘As emerging semiconductor materials,Dion-Jacobson(DJ)phase two-dimensional(2D)perovskites exhibit remarkable stability and structural diversity.However,their limited charge transport capability hinders further advancement,and the underlying carrier transport mechanisms require deeper investigation.In this work,six diammonium spacer cations and their corresponding DJ-phase 2D perovskite single crystals were rationally designed and synthesized to explore how spacer characteristics(such as heterocyclic type and amino group substitution position)affect the properties of 2D perovskites.Diammonium cations with meta-substituted amino groups tended to adopt a tilted configuration to balance the interactions between both ends of the cation and the inorganic layers.This orientation helped reduce the interlayer spacing,weakened hydrogen bonding between the cation and the inorganic framework,and lowered lattice distortion,promoting efficient carrier generation and transport.Beyond steric hindrance from branched side chains,the thermal stability of perovskites was also closely related to the nature of the heterocycle within the spacer.Diammonium cations bearing flexible aliphatic rings can buffer thermal deformation of the inorganic layers,dissipating internal thermal stress and enhancing overall thermal stability.
文摘With the support by the National Natural Science Foundation of China,a collaborative study by the research groups led by Prof.Fang Haiping(方海平)from Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Prof.Wu Minghong(吴明红)from Shanghai Applied Radiation Institute。
