Flexible molecules have great potential for constructing multicolor luminescent materials.Understanding the relationship between conformation and luminescence and exploring strategies to regulate emissions are crucial...Flexible molecules have great potential for constructing multicolor luminescent materials.Understanding the relationship between conformation and luminescence and exploring strategies to regulate emissions are crucial for the development of flexible molecules.In this work,we designed a molecule(HTP)with multiple flexibility and realized its color-tunable emissions via vip regulation.Interestingly,HTP can adjust its conformation and adopt different arrangements with vip water molecules.Two single crystals are obtained,which show green and yellow emissions with HTP:water ratios of 2:1 and 1:1,respectively.Meanwhile,the amorphous sample without water exhibits an orange emission.Notably,the tunable triplet excited state plays an important role in the luminescence of HTP,participating in thermally activated delayed fluorescence(TADF)and room temperature phosphorescence(RTP).Further combining theoretical calculations,the relationship between the multiple flexibility and excited-state energy levels is revealed.Different flexible structures show different dominant effects on the photophysical properties.Moreover,the multicolor and stimulus-responsive luminescence property of HTP is successfully applied in the application of anti-counterfeiting and information encryption.This work demonstrates a paradigm for designing and regulating the molecule with multiple flexibility,which may broaden the understanding of the conformation-luminescence relationship and enlarge the scope of flexible molecules.展开更多
Polymeric ultralong organic phosphorescence(UOP)with persistent emission is of great importance in practical applications.However,achieving good water-resistance for long-term environmental stability is a formidable c...Polymeric ultralong organic phosphorescence(UOP)with persistent emission is of great importance in practical applications.However,achieving good water-resistance for long-term environmental stability is a formidable challenge.In this contribution,through tailoring the alkyl-chain length of the hardeners and emitters,polymeric UOPs with varying crosslinking density and hydrophobic effect were obtained.Notably,all the polymers show no obvious decrease in UOP emission after high temperature-humidity test(85℃/85%relative humidity for 7 days).Detailed investigations demonstrate that the rigid covalent crosslinking networks suppress the quenching of triplet excitons while the hydrophobic microenvironment affords good water/moisture-resistance ability.Moreover,the polymers with superior processability are successfully applied as optical coatings,prepreg,and afterglow displays.With this work,we provide a new strategy to promote the long-term stability of polymeric UOP materials in high-temperature-humidity conditions.展开更多
Organic hole-transporting materials(HTMs)are an essential component in conventional perovskite solar cells(PSCs).In this work,two sulfonyldibenzene-based molecules,named CS-04 and CS-05,are synthesized and employed as...Organic hole-transporting materials(HTMs)are an essential component in conventional perovskite solar cells(PSCs).In this work,two sulfonyldibenzene-based molecules,named CS-04 and CS-05,are synthesized and employed as HTMs in n-i-p PSCs.In comparison with CS-04,the carbazole-substituted methoxytriphenylamine(Cz MOTPA)group in CS-05 exhibits an increased degree of molecular distortion,thus endowing CS-05 with excellent solvent solubility and film-formation ability.Moreover,CS-05 shows a high hole mobility,superior hole extraction and hole transporting properties.As a result,CS-05 yields impressive device performances with a high power conversion efficiency(PCE)of 20.15%,while that of CS-04 based device is 19.50%,which is comparable to that of the Spiro-OMe TAD based control device(19.59%).This finding illustrates the potential of sulfonyldibenzene-based molecules for the applications in PSCs,and also provides a novel avenue to improve the performances and stability of PSCs by tailoring the sulfonyldibenzene-based molecules.展开更多
Luminescent hydrogen-bonded organic frameworks(HOFs)have attracted increasing attention due to their corresponding luminescence that enables readily visualization of structural dynamics.HOFs with the mechanoluminescen...Luminescent hydrogen-bonded organic frameworks(HOFs)have attracted increasing attention due to their corresponding luminescence that enables readily visualization of structural dynamics.HOFs with the mechanoluminescence(ML)property can emit light without photon excitation and are greatly attractive for advanced applications,but research in this area has been limiting.Herein,we report the first example of an ML-active flexible HOF with permanent porosity,named 8PCOM,assembled from polar molecular rotors with an aggregation-induced emission property.When responding to different solvent vapors,reversible structural transformations between ML-active and-inactive 8PCOM frameworks occur,including a single-crystal-to-single-crystal(SCSC)transformation.Thus,vip-induced breathing behaviors are mainly attributed to phenyl rotations of polar molecular rotors induced by external stimuli.During reversible structural transformations of various 8PCOM frameworks with different pores,the significant ML property is achieved successfully through supramolecular dipole moment regulation.Upon mechanical force,bright emission of the ML-active 8PCOM framework is observed without UV irradiation,and the ML-active crystals can be easily prepared and regenerated.This work not only provides a valuable strategy for engineering future multifunctional HOFs but also enriches the types and applications of existing luminescent porous materials.展开更多
基金supported by the National Natural Science Foundation of China(52303250,52073316)the Guangdong Basic and Applied Basic Research Foundation(2022B1515020052)。
文摘Flexible molecules have great potential for constructing multicolor luminescent materials.Understanding the relationship between conformation and luminescence and exploring strategies to regulate emissions are crucial for the development of flexible molecules.In this work,we designed a molecule(HTP)with multiple flexibility and realized its color-tunable emissions via vip regulation.Interestingly,HTP can adjust its conformation and adopt different arrangements with vip water molecules.Two single crystals are obtained,which show green and yellow emissions with HTP:water ratios of 2:1 and 1:1,respectively.Meanwhile,the amorphous sample without water exhibits an orange emission.Notably,the tunable triplet excited state plays an important role in the luminescence of HTP,participating in thermally activated delayed fluorescence(TADF)and room temperature phosphorescence(RTP).Further combining theoretical calculations,the relationship between the multiple flexibility and excited-state energy levels is revealed.Different flexible structures show different dominant effects on the photophysical properties.Moreover,the multicolor and stimulus-responsive luminescence property of HTP is successfully applied in the application of anti-counterfeiting and information encryption.This work demonstrates a paradigm for designing and regulating the molecule with multiple flexibility,which may broaden the understanding of the conformation-luminescence relationship and enlarge the scope of flexible molecules.
基金Key-Area Research and Development Program of Guangdong Province,Grant/Award Number:2023B0101030002Shenzhen R&D Project,Grant/Award Number:JSGGZD20220822100001002Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2022A1515110927。
文摘Polymeric ultralong organic phosphorescence(UOP)with persistent emission is of great importance in practical applications.However,achieving good water-resistance for long-term environmental stability is a formidable challenge.In this contribution,through tailoring the alkyl-chain length of the hardeners and emitters,polymeric UOPs with varying crosslinking density and hydrophobic effect were obtained.Notably,all the polymers show no obvious decrease in UOP emission after high temperature-humidity test(85℃/85%relative humidity for 7 days).Detailed investigations demonstrate that the rigid covalent crosslinking networks suppress the quenching of triplet excitons while the hydrophobic microenvironment affords good water/moisture-resistance ability.Moreover,the polymers with superior processability are successfully applied as optical coatings,prepreg,and afterglow displays.With this work,we provide a new strategy to promote the long-term stability of polymeric UOP materials in high-temperature-humidity conditions.
基金the National Natural Science Foundation of China(51733010,21672267,51973239 and52073316)the Science and Technology Planning Project of Guangdong(2015B090913003)the Fundamental Research Funds for the Central Universities(19lgpy118,XDJK2019B065 and XDJK2020B002)。
文摘Organic hole-transporting materials(HTMs)are an essential component in conventional perovskite solar cells(PSCs).In this work,two sulfonyldibenzene-based molecules,named CS-04 and CS-05,are synthesized and employed as HTMs in n-i-p PSCs.In comparison with CS-04,the carbazole-substituted methoxytriphenylamine(Cz MOTPA)group in CS-05 exhibits an increased degree of molecular distortion,thus endowing CS-05 with excellent solvent solubility and film-formation ability.Moreover,CS-05 shows a high hole mobility,superior hole extraction and hole transporting properties.As a result,CS-05 yields impressive device performances with a high power conversion efficiency(PCE)of 20.15%,while that of CS-04 based device is 19.50%,which is comparable to that of the Spiro-OMe TAD based control device(19.59%).This finding illustrates the potential of sulfonyldibenzene-based molecules for the applications in PSCs,and also provides a novel avenue to improve the performances and stability of PSCs by tailoring the sulfonyldibenzene-based molecules.
基金the National Natural Science Foundation of China(grant nos.51733010,51973239,and 52073316)the Science and Technology Planning Project of Guangdong(grant nos.2015B090913003 and 2015B090915003).
文摘Luminescent hydrogen-bonded organic frameworks(HOFs)have attracted increasing attention due to their corresponding luminescence that enables readily visualization of structural dynamics.HOFs with the mechanoluminescence(ML)property can emit light without photon excitation and are greatly attractive for advanced applications,but research in this area has been limiting.Herein,we report the first example of an ML-active flexible HOF with permanent porosity,named 8PCOM,assembled from polar molecular rotors with an aggregation-induced emission property.When responding to different solvent vapors,reversible structural transformations between ML-active and-inactive 8PCOM frameworks occur,including a single-crystal-to-single-crystal(SCSC)transformation.Thus,vip-induced breathing behaviors are mainly attributed to phenyl rotations of polar molecular rotors induced by external stimuli.During reversible structural transformations of various 8PCOM frameworks with different pores,the significant ML property is achieved successfully through supramolecular dipole moment regulation.Upon mechanical force,bright emission of the ML-active 8PCOM framework is observed without UV irradiation,and the ML-active crystals can be easily prepared and regenerated.This work not only provides a valuable strategy for engineering future multifunctional HOFs but also enriches the types and applications of existing luminescent porous materials.
