Organic room-temperature phosphorescence(RTP)materials have attracted immense attention in bioimaging due to their long emission lifetime and large Stokes shift.RTP materials with long emission wavelength can improve ...Organic room-temperature phosphorescence(RTP)materials have attracted immense attention in bioimaging due to their long emission lifetime and large Stokes shift.RTP materials with long emission wavelength can improve the penetration depth for bioimaging.However,the design of red persistent RTP materials is still challenging.In this study,a fused-ring structure has been proposed to effectively decrease the triplet energy level,thus extending the emission wavelength of phosphorescence.In addition,the fused-ring structure exhibits a high molar extinction coefficient(ɛ)and high luminescence efficiency due to the rigid structure.A new class of crystalline hosts(iminodibenzyl,IDB)are developed to stabilize the triplet excitons that are generated from the fused-ring molecules.The maximum RTP wavelength of doping materials can reach 635 nm with a lifetime of 9.35 ms.Water-disperse nanoparticles are successfully prepared for in vivo time-resolved bioimaging,which eliminates the background fluorescence interference from biological tissues.These reveal a delicate design strategy for the construction of long-wavelength emissive RTP materials for high-resolution bioimaging.展开更多
Buckybowl structures as non-uniform electrostatic potential distributions of poly-cyclic aromatic materials show a unique photoelectric performance.In this work,OTC was utilized for dynamic modulation of triplet excit...Buckybowl structures as non-uniform electrostatic potential distributions of poly-cyclic aromatic materials show a unique photoelectric performance.In this work,OTC was utilized for dynamic modulation of triplet exciton transition processes.Five host molecules with different functional units were selected,thus providing dif-ferent intermolecular interactions in the host/guest systems.Therefore,the delayed emissions were regulated from 536 to 624 nm via the tuning of the triplet exciton transition processes of OTC in different hosts.Experimental data and theoretical calculations revealed that the varied triplet transition behaviors resulted from the competition between the intersystem crossing(ISC)process of OTC-monomer and the reverse intersystem crossing(RISC)process of OTC-aggregates.This work proves the superior structure of buckybowl-based luminophore for controlling triplet exciton transition processes and supplies a new perspective for persistent afterglow luminophore design.展开更多
Photothermal therapy(PTT)is emerging as an effective treatment for superficial carcinoma.A key challenge to the effectiveness of PTT is to develop photosensitizers with high photothermal conversion efficiency.Aiming t...Photothermal therapy(PTT)is emerging as an effective treatment for superficial carcinoma.A key challenge to the effectiveness of PTT is to develop photosensitizers with high photothermal conversion efficiency.Aiming to address this challenge,we develop a series of multi-arylpyrrole derivatives with different donors that contain different multi-rotor structures to explore highly efficient PTT photosensitizers.Among these multi-arylpyrrole derivatives,MAP4-FE nanoparticles with a small size of their donor groups and better-donating ability exhibit a high photothermal conversion efficiency(up to 72%)when they are encapsulated by an amphiphilic polymer.As a result,the MAP4-FE nanoparticles have shown satisfactory PTTeffects on in vivo tumor eradication under the guidance of photoacoustic signals.The findings of this study provide significant insights for the development of high-efficiency PTT photosensitizers for cancer treatment by making full use of the nonradiative decay of small size donors as rotors.展开更多
Organic room-temperature phosphorescence(RTP)materials have been used in high-resolution imaging.However,the development of long-wavelength-emis sion RTP materials in aqueous solution remains a challenge.Here,we repor...Organic room-temperature phosphorescence(RTP)materials have been used in high-resolution imaging.However,the development of long-wavelength-emis sion RTP materials in aqueous solution remains a challenge.Here,we report red-emissive RTP materials via integration of the ring-fusing effect and host–guest interaction.展开更多
Organic dyes with conformational sensitivity can be used to probe weak interactions at the molecular level.Here,three molecules based on tetraphenyl-1,3-butadienes(TPBs)were synthesized and studied with respect to the...Organic dyes with conformational sensitivity can be used to probe weak interactions at the molecular level.Here,three molecules based on tetraphenyl-1,3-butadienes(TPBs)were synthesized and studied with respect to their synthesis,structural characterization and potential application.All TPBs showed aggregation-induced emission(AIE)characteristics and sensitive conformational properties,in which the emission wavelengths could be changed in different states.The TPBs single crystals revealed that the phenyl groups at the 4-position of the 1,3-butadienes contributed to their conformational sensitivity.Furthermore,the potential application for monitoring the interactions among polyelectrolyte complexes and metal ions was explored,and the results showed that TPBs could be used for sensitively probing some weak interactions by changing the emission wavelengths due to their conformation-sensitive properties.TPBs may become a new star in AIE research fields.展开更多
In order to get an easy way to achieve the transformation from aggregation-caused quenching luminophores （ACQphores） to aggregation-induced emission luminogens （AIEgens）, we took aldehyde groups as the modifying g...In order to get an easy way to achieve the transformation from aggregation-caused quenching luminophores （ACQphores） to aggregation-induced emission luminogens （AIEgens）, we took aldehyde groups as the modifying group to decorate anthracene. The fluorescence performances of 9-anthraldehyde （AnA） and 9,10-anthracenedicarboxaldehyde （AnDA） in solution and aggregated state were studied. We found out that the aldehyde group can transform anthracene with aggregation-caused quenching properties to AIEgen. The single-crystal structures analy- sis of AnA and AnDA showed that their structure characteristics are responsible for the AIE properties of AnA and AnDA. On one hand, the aldehyde group can cause steric effects to lower intermolecular n-π packing style in aggregated state. On the other hand, intermolecular H-bonding interactions can restrict the intramolecular rotation and suppress internal charge transfer. These results may supply a new simple method for the transformation from ACQphores to AIEgens on the point of the molecular design.展开更多
Transition metal ions(Pb^(2+),Zn^(2+),Cd^(2+),Co^(2+),Mn^(2+),Cu^(2+),Ni^(2+),Hg^(2+),Ag^(+),Fe^(3+))in water are used to quench emission of 2-(6-oxido-6H-dibenz<c,e><1,2>oxaphosphorin-6-yl)-1,4-phenylene-...Transition metal ions(Pb^(2+),Zn^(2+),Cd^(2+),Co^(2+),Mn^(2+),Cu^(2+),Ni^(2+),Hg^(2+),Ag^(+),Fe^(3+))in water are used to quench emission of 2-(6-oxido-6H-dibenz<c,e><1,2>oxaphosphorin-6-yl)-1,4-phenylene-bis(p-pentyloxylbenzoate)s(MD5)with aggregation-induced emission enhancement(AIEE)in water-acetonitrile(AN)mixture(80:20 by volume).Among all metal ions,Fe^(3+)exhibits the highest quenching efficiency on AIEE of MD5 even when the concentration of Fe^(3+)is lower than 1×10^(-6) mol/L.The quenching efficiency of Hg^(2+)is lower than that of Fe^(3+)at the same concentration,though MD5 is used to detect Hg^(2+)efficiently,too.To other metal ions,low quenching efficiency has few relations with a wider concentration range.The UV absorbance spectra show only red shift of absorbance wavelength in the presence of Hg^(2+)and Fe^(3+),which indicates a salt-induced Jaggregation.SEM photos reveal larger aggregation and morphological change of nanoparticles of MD5 in water containing Hg^(2+)and Fe^(3+),which reduce the surface area of MD5 emission for further aggregation.The selective quenching effect of transition metal ions to emission of MD5 has a potential application in chemical sensors of some metal ions.展开更多
基金the National Natural Scientific Foundation of China(Grant Nos.22222501,21975021,21975020,21875019,22105019,and 22175023)supported by Beijing National Laboratory for Molecular Sciences(BNLMS202007)the BIT Research and Innovation Promoting Project(2022YCXZ035).
文摘Organic room-temperature phosphorescence(RTP)materials have attracted immense attention in bioimaging due to their long emission lifetime and large Stokes shift.RTP materials with long emission wavelength can improve the penetration depth for bioimaging.However,the design of red persistent RTP materials is still challenging.In this study,a fused-ring structure has been proposed to effectively decrease the triplet energy level,thus extending the emission wavelength of phosphorescence.In addition,the fused-ring structure exhibits a high molar extinction coefficient(ɛ)and high luminescence efficiency due to the rigid structure.A new class of crystalline hosts(iminodibenzyl,IDB)are developed to stabilize the triplet excitons that are generated from the fused-ring molecules.The maximum RTP wavelength of doping materials can reach 635 nm with a lifetime of 9.35 ms.Water-disperse nanoparticles are successfully prepared for in vivo time-resolved bioimaging,which eliminates the background fluorescence interference from biological tissues.These reveal a delicate design strategy for the construction of long-wavelength emissive RTP materials for high-resolution bioimaging.
基金National Natural Scientific Foundation of China,Grant/Award Numbers:21975021,21975020,21875019,21871119,22105019,22175023Beijing National Laboratory for Molecular Sciences,Grant/Award Number:BNLMS192007BIT Research and Innovation Promoting Project,Grant/Award Number:2022YCXZ035。
文摘Buckybowl structures as non-uniform electrostatic potential distributions of poly-cyclic aromatic materials show a unique photoelectric performance.In this work,OTC was utilized for dynamic modulation of triplet exciton transition processes.Five host molecules with different functional units were selected,thus providing dif-ferent intermolecular interactions in the host/guest systems.Therefore,the delayed emissions were regulated from 536 to 624 nm via the tuning of the triplet exciton transition processes of OTC in different hosts.Experimental data and theoretical calculations revealed that the varied triplet transition behaviors resulted from the competition between the intersystem crossing(ISC)process of OTC-monomer and the reverse intersystem crossing(RISC)process of OTC-aggregates.This work proves the superior structure of buckybowl-based luminophore for controlling triplet exciton transition processes and supplies a new perspective for persistent afterglow luminophore design.
基金This work was financially supported by the National Natural Science Foundation of China （Grant Nos. 21474009, 51328302, 51073026, 51061160500）, the National Basic Research Program of China （973 Program Grant No. 2013CB834704） and Basic Research Foundation of Beijing Institute of Technology （Grant No. 20130942007）.
基金financially supported by the National Natural Science Foundation of China(21875019,21803007,21975020,51803009)the National Key Research and Development Program of China(2018YFA0901800)+1 种基金the Department of Science and Technology of Guangdong Province(2019ZT08Y191)the Shenzhen Science and Technology Program(JSGG20200225151916021)。
文摘Photothermal therapy(PTT)is emerging as an effective treatment for superficial carcinoma.A key challenge to the effectiveness of PTT is to develop photosensitizers with high photothermal conversion efficiency.Aiming to address this challenge,we develop a series of multi-arylpyrrole derivatives with different donors that contain different multi-rotor structures to explore highly efficient PTT photosensitizers.Among these multi-arylpyrrole derivatives,MAP4-FE nanoparticles with a small size of their donor groups and better-donating ability exhibit a high photothermal conversion efficiency(up to 72%)when they are encapsulated by an amphiphilic polymer.As a result,the MAP4-FE nanoparticles have shown satisfactory PTTeffects on in vivo tumor eradication under the guidance of photoacoustic signals.The findings of this study provide significant insights for the development of high-efficiency PTT photosensitizers for cancer treatment by making full use of the nonradiative decay of small size donors as rotors.
基金supported by the National Natural Scientific Foundation of China(grant nos.21975021,51803009,21905021,51673024,21975020,and 21875019)supported by Beijing National Laboratory for Molecular Sciences(no.BNLMS202007),China Postdoctoral Science Foundation 2019TQ0034.
文摘Organic room-temperature phosphorescence(RTP)materials have been used in high-resolution imaging.However,the development of long-wavelength-emis sion RTP materials in aqueous solution remains a challenge.Here,we report red-emissive RTP materials via integration of the ring-fusing effect and host–guest interaction.
基金supported by the National Natural Science Foundation of China (51673024, 21875019, 21490574, 51803009)Beijing Institute of Technology Research Fund Program for Young Scholars
文摘Organic dyes with conformational sensitivity can be used to probe weak interactions at the molecular level.Here,three molecules based on tetraphenyl-1,3-butadienes(TPBs)were synthesized and studied with respect to their synthesis,structural characterization and potential application.All TPBs showed aggregation-induced emission(AIE)characteristics and sensitive conformational properties,in which the emission wavelengths could be changed in different states.The TPBs single crystals revealed that the phenyl groups at the 4-position of the 1,3-butadienes contributed to their conformational sensitivity.Furthermore,the potential application for monitoring the interactions among polyelectrolyte complexes and metal ions was explored,and the results showed that TPBs could be used for sensitively probing some weak interactions by changing the emission wavelengths due to their conformation-sensitive properties.TPBs may become a new star in AIE research fields.
基金We are grateful for the Basic Research Program 2013CB834704）, and the support from the National of China （973 Program, National Natural Science Foundation of China （Nos. 51328302, 21404010, 51073026, 51061160500）.
文摘In order to get an easy way to achieve the transformation from aggregation-caused quenching luminophores （ACQphores） to aggregation-induced emission luminogens （AIEgens）, we took aldehyde groups as the modifying group to decorate anthracene. The fluorescence performances of 9-anthraldehyde （AnA） and 9,10-anthracenedicarboxaldehyde （AnDA） in solution and aggregated state were studied. We found out that the aldehyde group can transform anthracene with aggregation-caused quenching properties to AIEgen. The single-crystal structures analy- sis of AnA and AnDA showed that their structure characteristics are responsible for the AIE properties of AnA and AnDA. On one hand, the aldehyde group can cause steric effects to lower intermolecular n-π packing style in aggregated state. On the other hand, intermolecular H-bonding interactions can restrict the intramolecular rotation and suppress internal charge transfer. These results may supply a new simple method for the transformation from ACQphores to AIEgens on the point of the molecular design.
基金This project was supported by the National Natural Science Foundation of China(No.20634020)the Basic Research Foundation of Beijing Institute of Technology(BIT-UBF-200504B4213,BIT-UBF-200504B4215).
文摘Transition metal ions(Pb^(2+),Zn^(2+),Cd^(2+),Co^(2+),Mn^(2+),Cu^(2+),Ni^(2+),Hg^(2+),Ag^(+),Fe^(3+))in water are used to quench emission of 2-(6-oxido-6H-dibenz<c,e><1,2>oxaphosphorin-6-yl)-1,4-phenylene-bis(p-pentyloxylbenzoate)s(MD5)with aggregation-induced emission enhancement(AIEE)in water-acetonitrile(AN)mixture(80:20 by volume).Among all metal ions,Fe^(3+)exhibits the highest quenching efficiency on AIEE of MD5 even when the concentration of Fe^(3+)is lower than 1×10^(-6) mol/L.The quenching efficiency of Hg^(2+)is lower than that of Fe^(3+)at the same concentration,though MD5 is used to detect Hg^(2+)efficiently,too.To other metal ions,low quenching efficiency has few relations with a wider concentration range.The UV absorbance spectra show only red shift of absorbance wavelength in the presence of Hg^(2+)and Fe^(3+),which indicates a salt-induced Jaggregation.SEM photos reveal larger aggregation and morphological change of nanoparticles of MD5 in water containing Hg^(2+)and Fe^(3+),which reduce the surface area of MD5 emission for further aggregation.The selective quenching effect of transition metal ions to emission of MD5 has a potential application in chemical sensors of some metal ions.
