Without adding feedback to modulate light path system, the dissymmetrical 3×3 coupled optical accelerometer reduces the complexity of the design of light path system. Experiments prove that it can attain good dem...Without adding feedback to modulate light path system, the dissymmetrical 3×3 coupled optical accelerometer reduces the complexity of the design of light path system. Experiments prove that it can attain good demodulation effects. As carrier is not needed in this system, the frequency range of input signal is diminished so as to decrease the sampling frequency of accelerometer. This makes for the system on programmable chip(SOPC) design of digital demodulating system. The upper limit of accelerometer working frequency can reach 3 500 Hz. But affected by the inherent frequency of sensitive components, its working frequency is 10 Hz^1 000 Hz, and the sensitivity is 8.718 0 V/(m·s-2). This accelerometer can detect the dynamic range of acceleration signal real-timely, steadily and accurately, solving the dissymmetrical problem of light path caused by circumstances and the complexity of process.展开更多
Herein,we report on the guest-responsive hierarchical self-assembly of dissymmetric cage DC-1 with an intrinsic dipole along its C_(3)-symmetric axis.DC-1 molecules self-assemble into supramolecular columns with themo...Herein,we report on the guest-responsive hierarchical self-assembly of dissymmetric cage DC-1 with an intrinsic dipole along its C_(3)-symmetric axis.DC-1 molecules self-assemble into supramolecular columns with themolecular dipoles aligned along the columnar axis.Mediated by different host-guest interactions of ethyl acetate(EtOAc)and chloroform(CHCl_(3)),the columns are arranged in an antiparallel and parallel fashion,respectively,leading to a switch of the centrosym metric and noncentrosymmetric superstructures.The symmetry of themolecular packing of DC-1 molecules of the noncentrosymmetric crystalline phase is therefore broken,producing a supramolecular ferroelectric with second-harmonic generation and piezoelectric responses.We demonstrate that cages can serve as promising building blocks for the discovery of supramolecular materials with emergent functions and properties,including but not limited to,organic ferroelectrics and nonlinear optics.展开更多
Homobinuclear complex (HCuL)2 (1) (H3L: N-3-carboxylsalicylidene-N'-salicylaldehyde-1,2-diaminoethane) was obtained from self-organization of the reported complex HCuL, and its crystal structure was determined...Homobinuclear complex (HCuL)2 (1) (H3L: N-3-carboxylsalicylidene-N'-salicylaldehyde-1,2-diaminoethane) was obtained from self-organization of the reported complex HCuL, and its crystal structure was determined through X-ray diffraction at room temperature. The crystal of complex 1 belongs to monolinic system, the space group Cc, a=2.5326(5) nm, b=0.88861(18) nm, c=1.3738(3) nm, β=96.95(3)°, Z=4, R1=0.0520, wR2=0.1185. (HCuL)2 is a dimeric molecule and has extended phenolic oxygen-bridged structure. In addition, using mononuclear complex HCuL as building blocks, Cu(Ⅱ)-Mg(Ⅱ)-Cu(Ⅱ) heterotrinuclear complex 2 was synthesized, and its crystal structure also has been determined by X-ray analysis. The crystal of complex 2 is of monoclinic system, space group Pc, a=1.1816(2) nm, b=1.5599(3) nm, c=1.9642 (4) nm, β=98.22°, Z=2, R1=0.0701, wR2=0.1498. Each dissymmetricai cell unit of complex 2 contains two heterotrinucler neutral molecules: {[CuL(H2O)]Mg[CuL(CH3OH)]} and {[CuL]Mg[CuL(H2O)]}.展开更多
Chiral ligand (R)-N, N'-Bis(2-hydroxy-3,5-di- tert-butyl-aryl-methyl)-1, 1'-binaphthalene-2,2'-diamine derived from the reduction of Schiff base (R)-2,2'-bis (3,5-di-tert-butyl-2-hy-droxybenzylideneami...Chiral ligand (R)-N, N'-Bis(2-hydroxy-3,5-di- tert-butyl-aryl-methyl)-1, 1'-binaphthalene-2,2'-diamine derived from the reduction of Schiff base (R)-2,2'-bis (3,5-di-tert-butyl-2-hy-droxybenzylideneamino)-1, 1'-binaphthyl with LiAIH(4) is fairly effective in the asymmetric addition reaction of diethylzinc to aldehydes by which good yields (46%-94%) of the corresponding sec-alcohols can be obtained in moderate ee (51%-79%) with R configuration for a variety of aldehydes.展开更多
A series of heterogemini imidazolium surfactants with two-methylene spacer groups ([Cm- 2-Cnim]Br2, m, n=8, 10, 12, 14, 16; m≠n) have been synthesized and characterized by 1H NMR and ESI-MS spectroscopy. The effect...A series of heterogemini imidazolium surfactants with two-methylene spacer groups ([Cm- 2-Cnim]Br2, m, n=8, 10, 12, 14, 16; m≠n) have been synthesized and characterized by 1H NMR and ESI-MS spectroscopy. The effects of various reaction parameters, including stoichiometry, reaction temperature and time, were investigated. In addition, the surface activity study about heterogemini imidazolium surfactants was carried out and the influences of dissymmetric degree on the surface properties were also discussed.展开更多
After field survey and literature review, we found that software requirement development (SRD) is a knowledge creation process, and knowledge creation theory of Nonaka is appropriate for analyzing knowledge creating o...After field survey and literature review, we found that software requirement development (SRD) is a knowledge creation process, and knowledge creation theory of Nonaka is appropriate for analyzing knowledge creating of SRD. The characteristics of knowledge in requirement elicitation process are analyzed, and dissymmetric knowledge of SRD is discussed. Experts on requirement are introduced into SRD process as a third knowledge entity. In addition, a knowledge creation model of SRD is put forward and the knowledge flow and the relationship of entities of this model are illustrated. Case study findings are illustrated in the following: 1) The necessary diversity of the project team can facilitate the implementation of the SRD. 2) The introduction of experts on requirement can achieve the transformation of knowledge effectively, thus helping to carry out the SRD. 3) Methodology and related technologies are important for carrying out the SRD.展开更多
Chiral inorganic semiconductors with high dissymmetric factor are highly desirable,but it is generally difficult to induce chiral structure in inorganic semiconductors because of their structure rigidity and symmetry....Chiral inorganic semiconductors with high dissymmetric factor are highly desirable,but it is generally difficult to induce chiral structure in inorganic semiconductors because of their structure rigidity and symmetry.In this study,we introduced chiral ZnO film as hard template to transfer chirality to CsPbBr_(3) film and PbS quantum dots(QDs)for circularly polarized light(CPL)emission and detection,respectively.The prepared CsPbBr_(3)/ZnO thin film exhibited CPL emission at 520 nm and the PbS QDs/ZnO film realized CPL detection at 780 nm,featuring high dissymmetric factor up to around 0.4.The electron transition based mechanism is responsible for chirality transfer.展开更多
Multichromophoric architectures with wellorganized chromophoric arrangements are of vital importance to gain insights into interchromophoric interactions.Herein,we report a novel heteroleptic self-assembly strategy an...Multichromophoric architectures with wellorganized chromophoric arrangements are of vital importance to gain insights into interchromophoric interactions.Herein,we report a novel heteroleptic self-assembly strategy and construct three achiral and one chiral sandwich-like heterochromophore complexes(Zn_(4)L^(G)L^(A-C)_(2)and Zn_(4)L_(G)L^(D)_(2)).Possible dynamic products,including homoleptic oligomers and isomers,are eliminated,producing achiral complexes with exceptional purity.Isomers are observed in chiral complexes due to the flexible geometry of LD.Perfectly aligned chromophore arrangements with precise spacing and orientations are evidenced by single-crystal X-ray diffraction.The distinct segments in the ligands lead to different interchromophoric interactions.Impressively,energy transfer and tunable emission,including white-light emission,are achieved for Zn_(4)L^(G)L^(A)_(2)and Zn_(4)L^(G)L^(B)_(2).In addition,chirality transfer is observed for Zn_(4)L_(G)L^(D)_(2),due to conformational restriction from chiral LD,leading to chiral rotational conformations of tetraphenylethylene moiety in LG.展开更多
Self-assembly has been widely explored to improve the circularly polarized_(lum)inescence(CPL)activities of molecular chromophores,but it is hard to amplify CPL while maintaining strong emissions.Optically pure,planar...Self-assembly has been widely explored to improve the circularly polarized_(lum)inescence(CPL)activities of molecular chromophores,but it is hard to amplify CPL while maintaining strong emissions.Optically pure,planar-chiral[2.2]paracyclophane(pCp)is one of the most important sources of chirality for electronic and optoelectronic materials,but the photo_(lum)inescence of its derivatives is significantly quenched after forming aggregates.Here we demonstrate that reticulation of pCp chromophores into highly stable Zr(IV)metal-organic frameworks(MOFs)can simultaneously boost the dissymmetry factor(|g_(lum)|)and_(lum)inescence efficiency(Φ_(PL)).Functionalization of pCp enables the synthesis of two tetracarboxylate linkers with different side arms,which are assembled into two highly stable Zr-MOFswith different topological structures.Geometrical constraints and segregated arrangements of the pCp chromophores imposed by the framework inhibit the aggregation-caused quenching effect and boost their CPL behaviors.Both Zr-MOFs display strong CPL emissions,affording|g_(lum)|andΦ_(PL)values of up to 8.3×10^(-3)and 87%,respectively,which are amplified by∼18-and 52-fold compared to the corresponding free ligands.This work highlights the potential of optimizing CPL performances of chiral chromophores by using MOFs as support structures.展开更多
文摘Without adding feedback to modulate light path system, the dissymmetrical 3×3 coupled optical accelerometer reduces the complexity of the design of light path system. Experiments prove that it can attain good demodulation effects. As carrier is not needed in this system, the frequency range of input signal is diminished so as to decrease the sampling frequency of accelerometer. This makes for the system on programmable chip(SOPC) design of digital demodulating system. The upper limit of accelerometer working frequency can reach 3 500 Hz. But affected by the inherent frequency of sensitive components, its working frequency is 10 Hz^1 000 Hz, and the sensitivity is 8.718 0 V/(m·s-2). This accelerometer can detect the dynamic range of acceleration signal real-timely, steadily and accurately, solving the dissymmetrical problem of light path caused by circumstances and the complexity of process.
基金supported by the Shanghai Natural Science Foundation(no.18ZR1420800)National Natural Science Foundation of China(no.21890733,22071153).
文摘Herein,we report on the guest-responsive hierarchical self-assembly of dissymmetric cage DC-1 with an intrinsic dipole along its C_(3)-symmetric axis.DC-1 molecules self-assemble into supramolecular columns with themolecular dipoles aligned along the columnar axis.Mediated by different host-guest interactions of ethyl acetate(EtOAc)and chloroform(CHCl_(3)),the columns are arranged in an antiparallel and parallel fashion,respectively,leading to a switch of the centrosym metric and noncentrosymmetric superstructures.The symmetry of themolecular packing of DC-1 molecules of the noncentrosymmetric crystalline phase is therefore broken,producing a supramolecular ferroelectric with second-harmonic generation and piezoelectric responses.We demonstrate that cages can serve as promising building blocks for the discovery of supramolecular materials with emergent functions and properties,including but not limited to,organic ferroelectrics and nonlinear optics.
基金Project supported by the Natural Science Foundation of Henan Province (No. 0311020800).
文摘Homobinuclear complex (HCuL)2 (1) (H3L: N-3-carboxylsalicylidene-N'-salicylaldehyde-1,2-diaminoethane) was obtained from self-organization of the reported complex HCuL, and its crystal structure was determined through X-ray diffraction at room temperature. The crystal of complex 1 belongs to monolinic system, the space group Cc, a=2.5326(5) nm, b=0.88861(18) nm, c=1.3738(3) nm, β=96.95(3)°, Z=4, R1=0.0520, wR2=0.1185. (HCuL)2 is a dimeric molecule and has extended phenolic oxygen-bridged structure. In addition, using mononuclear complex HCuL as building blocks, Cu(Ⅱ)-Mg(Ⅱ)-Cu(Ⅱ) heterotrinuclear complex 2 was synthesized, and its crystal structure also has been determined by X-ray analysis. The crystal of complex 2 is of monoclinic system, space group Pc, a=1.1816(2) nm, b=1.5599(3) nm, c=1.9642 (4) nm, β=98.22°, Z=2, R1=0.0701, wR2=0.1498. Each dissymmetricai cell unit of complex 2 contains two heterotrinucler neutral molecules: {[CuL(H2O)]Mg[CuL(CH3OH)]} and {[CuL]Mg[CuL(H2O)]}.
基金theMajorStateBasicResearchDevelopmentProgram (No .G2 0 0 0 0 480 0 7)andtheNationalNaturalScienceFoundationofChina (No .2 0 0 2 5 2 0 6 )
文摘Chiral ligand (R)-N, N'-Bis(2-hydroxy-3,5-di- tert-butyl-aryl-methyl)-1, 1'-binaphthalene-2,2'-diamine derived from the reduction of Schiff base (R)-2,2'-bis (3,5-di-tert-butyl-2-hy-droxybenzylideneamino)-1, 1'-binaphthyl with LiAIH(4) is fairly effective in the asymmetric addition reaction of diethylzinc to aldehydes by which good yields (46%-94%) of the corresponding sec-alcohols can be obtained in moderate ee (51%-79%) with R configuration for a variety of aldehydes.
文摘A series of heterogemini imidazolium surfactants with two-methylene spacer groups ([Cm- 2-Cnim]Br2, m, n=8, 10, 12, 14, 16; m≠n) have been synthesized and characterized by 1H NMR and ESI-MS spectroscopy. The effects of various reaction parameters, including stoichiometry, reaction temperature and time, were investigated. In addition, the surface activity study about heterogemini imidazolium surfactants was carried out and the influences of dissymmetric degree on the surface properties were also discussed.
文摘After field survey and literature review, we found that software requirement development (SRD) is a knowledge creation process, and knowledge creation theory of Nonaka is appropriate for analyzing knowledge creating of SRD. The characteristics of knowledge in requirement elicitation process are analyzed, and dissymmetric knowledge of SRD is discussed. Experts on requirement are introduced into SRD process as a third knowledge entity. In addition, a knowledge creation model of SRD is put forward and the knowledge flow and the relationship of entities of this model are illustrated. Case study findings are illustrated in the following: 1) The necessary diversity of the project team can facilitate the implementation of the SRD. 2) The introduction of experts on requirement can achieve the transformation of knowledge effectively, thus helping to carry out the SRD. 3) Methodology and related technologies are important for carrying out the SRD.
基金supported by the National Natural Science Foundation of China(Grant No.61904065)the National Key R&D Program of China(No.2016YFB070700702)the National Postdoctoral Program for Innovative Talent(No.BX20190127)。
文摘Chiral inorganic semiconductors with high dissymmetric factor are highly desirable,but it is generally difficult to induce chiral structure in inorganic semiconductors because of their structure rigidity and symmetry.In this study,we introduced chiral ZnO film as hard template to transfer chirality to CsPbBr_(3) film and PbS quantum dots(QDs)for circularly polarized light(CPL)emission and detection,respectively.The prepared CsPbBr_(3)/ZnO thin film exhibited CPL emission at 520 nm and the PbS QDs/ZnO film realized CPL detection at 780 nm,featuring high dissymmetric factor up to around 0.4.The electron transition based mechanism is responsible for chirality transfer.
基金the National Natural Science Foundation of China(22271116,22071079 for M.W.)the fellowship of the China Postdoctoral Science Foundation(2021M701383 for J.S.)+1 种基金the Natural Science Foundation of Jilin Province(20230101027JC)the staff at the BL17B1 beamline of the National Facility for Protein Science in Shanghai(NFPS),the Shanghai Advanced Research Institute,and CAS for providing technical support in X-ray diffraction data collection and analysis.
文摘Multichromophoric architectures with wellorganized chromophoric arrangements are of vital importance to gain insights into interchromophoric interactions.Herein,we report a novel heteroleptic self-assembly strategy and construct three achiral and one chiral sandwich-like heterochromophore complexes(Zn_(4)L^(G)L^(A-C)_(2)and Zn_(4)L_(G)L^(D)_(2)).Possible dynamic products,including homoleptic oligomers and isomers,are eliminated,producing achiral complexes with exceptional purity.Isomers are observed in chiral complexes due to the flexible geometry of LD.Perfectly aligned chromophore arrangements with precise spacing and orientations are evidenced by single-crystal X-ray diffraction.The distinct segments in the ligands lead to different interchromophoric interactions.Impressively,energy transfer and tunable emission,including white-light emission,are achieved for Zn_(4)L^(G)L^(A)_(2)and Zn_(4)L^(G)L^(B)_(2).In addition,chirality transfer is observed for Zn_(4)L_(G)L^(D)_(2),due to conformational restriction from chiral LD,leading to chiral rotational conformations of tetraphenylethylene moiety in LG.
基金This work was financially supported by the National Natural Science Foundation of China(grant nos.21620102001,91856204,91956124,and 21875136)Key Project of Basic Research of Shanghai(grant no.19JC1412600)Shanghai Rising-Star Program(grant no.19QA1404300),and the China Postdoctoral Science Foundation(grant no.2020M681280).
文摘Self-assembly has been widely explored to improve the circularly polarized_(lum)inescence(CPL)activities of molecular chromophores,but it is hard to amplify CPL while maintaining strong emissions.Optically pure,planar-chiral[2.2]paracyclophane(pCp)is one of the most important sources of chirality for electronic and optoelectronic materials,but the photo_(lum)inescence of its derivatives is significantly quenched after forming aggregates.Here we demonstrate that reticulation of pCp chromophores into highly stable Zr(IV)metal-organic frameworks(MOFs)can simultaneously boost the dissymmetry factor(|g_(lum)|)and_(lum)inescence efficiency(Φ_(PL)).Functionalization of pCp enables the synthesis of two tetracarboxylate linkers with different side arms,which are assembled into two highly stable Zr-MOFswith different topological structures.Geometrical constraints and segregated arrangements of the pCp chromophores imposed by the framework inhibit the aggregation-caused quenching effect and boost their CPL behaviors.Both Zr-MOFs display strong CPL emissions,affording|g_(lum)|andΦ_(PL)values of up to 8.3×10^(-3)and 87%,respectively,which are amplified by∼18-and 52-fold compared to the corresponding free ligands.This work highlights the potential of optimizing CPL performances of chiral chromophores by using MOFs as support structures.