Organic room-temperature phosphorescence(RTP)materials are promising for bioimaging applications due to their tunable structures,excellent biocompatibility,and long-lived luminescence.However,the development of highly...Organic room-temperature phosphorescence(RTP)materials are promising for bioimaging applications due to their tunable structures,excellent biocompatibility,and long-lived luminescence.However,the development of highly efficient organic RTP materials for aqueous systems remains challenging,as the organic phosphorescence is prone to being quenched by the dissolved oxygen in water.Herein,heteroaromatic carboxylic acids serve as ligand vips to construct a series of host-vip composites with nontoxic,dense EDTA-M(M=Ca,Mg,and Al)coordination polymer in water.These composites exhibit ultra-long pure RTP of vip molecules with phosphorescence quantum yield up to 53%,and lifetime up to 589.7 ms,due to the synergistic effect of dual-network structure:a coordinatively cross-linked network of EDTA-M,and a non-covalent bonded network formed by ligands and water molecules.The phosphorescence intensity is more than three times that of the composite with a single coordination network.Notably,the dual-network configuration can form a rigid and dense structure and block the intrusion of external H_(2)O and O_(2) molecules to avoid phosphorescence quenching in water.As a result,the RTP of the composites remains unchanged after 1 month in water.Furthermore,the nanoparticles fabricated from composites and anionic surfactants can be successfully applied in in vivo imaging of mice for the stable RTP in water.This work provides a novel strategy for the development of high-performance RTP materials in aqueous systems.展开更多
Internal rotation of conjugated organic backbone seriously impaired room temperature phosphorescence(RTP),leading to rare realization of ultra-long afterglows with RTP lifetimes over 2 s in non-bibulous polymers.Herei...Internal rotation of conjugated organic backbone seriously impaired room temperature phosphorescence(RTP),leading to rare realization of ultra-long afterglows with RTP lifetimes over 2 s in non-bibulous polymers.Herein,N-(bromophenyl)carbazoles are cyclized to lock up phenyl-carbazol internal rotation in advance and the fused nitrogen hetero-cyclic compounds are doped into poly(methyl methacrylate)(PMMA).The results show that locking up the molecular internal rotation can achieve ultra-long RTP polymers with lifetimes over 2 s,in contrast,the unlocked molecules hardly emit RTP in PMMA.The high-lying triplet excitons can transfer the energy to low-lying organic fluorescent dyes,and the persistent multicolor afterglows including white emission can be readily modulated.This work discloses an effective and extendable dopant molecular strategy for developing high-performance ultra-long organic RTP polymers.展开更多
As the cornerstone of future information security,quantum key distribution(QKD)is evolving towards large-scale hybrid discrete-variable/continuous-variable(DV/CV)multi-domain quantum networks.Meanwhile,multicast-orien...As the cornerstone of future information security,quantum key distribution(QKD)is evolving towards large-scale hybrid discrete-variable/continuous-variable(DV/CV)multi-domain quantum networks.Meanwhile,multicast-oriented multi-party key negotiation is attracting increasing attention in quantum networks.However,the efficient key provision for multicast services over hybrid DV/CV multi-domain quantum networks remains challenging,due to the limited probability of service success and the inefficient utilization of key resources.Targeting these challenges,this study proposes two key-resource-aware multicast-oriented key provision strategies,namely the link distance-resource balanced key provision strategy and the maximum shared link key provision strategy.The proposed strategies are applicable to hybrid DV/CV multi-domain quantum networks,which are typically implemented by GG02-based intra-domain connections and BB84-based inter-domain connections.Furthermore,the multicast-oriented key provision model is formulated,based on which two heuristic algorithms are designed,i.e.,the shared link distance-resource(SLDR)dependent and the maximum shared link distance-resource(MSLDR)dependent multicast-oriented key provision algorithms.Simulation results verify the applicability of the designed algorithms across different multi-domain quantum networks,and demonstrate their superiority over the benchmark algorithms in terms of the success probability of multicast service requests,the number of shared links,and the key resource utilization.展开更多
基金supported by the Startup Funds for Introduced Talents of Wuyi University(YJ202304)the National Natural Science Foundation of China(22375044).
文摘Organic room-temperature phosphorescence(RTP)materials are promising for bioimaging applications due to their tunable structures,excellent biocompatibility,and long-lived luminescence.However,the development of highly efficient organic RTP materials for aqueous systems remains challenging,as the organic phosphorescence is prone to being quenched by the dissolved oxygen in water.Herein,heteroaromatic carboxylic acids serve as ligand vips to construct a series of host-vip composites with nontoxic,dense EDTA-M(M=Ca,Mg,and Al)coordination polymer in water.These composites exhibit ultra-long pure RTP of vip molecules with phosphorescence quantum yield up to 53%,and lifetime up to 589.7 ms,due to the synergistic effect of dual-network structure:a coordinatively cross-linked network of EDTA-M,and a non-covalent bonded network formed by ligands and water molecules.The phosphorescence intensity is more than three times that of the composite with a single coordination network.Notably,the dual-network configuration can form a rigid and dense structure and block the intrusion of external H_(2)O and O_(2) molecules to avoid phosphorescence quenching in water.As a result,the RTP of the composites remains unchanged after 1 month in water.Furthermore,the nanoparticles fabricated from composites and anionic surfactants can be successfully applied in in vivo imaging of mice for the stable RTP in water.This work provides a novel strategy for the development of high-performance RTP materials in aqueous systems.
文摘Internal rotation of conjugated organic backbone seriously impaired room temperature phosphorescence(RTP),leading to rare realization of ultra-long afterglows with RTP lifetimes over 2 s in non-bibulous polymers.Herein,N-(bromophenyl)carbazoles are cyclized to lock up phenyl-carbazol internal rotation in advance and the fused nitrogen hetero-cyclic compounds are doped into poly(methyl methacrylate)(PMMA).The results show that locking up the molecular internal rotation can achieve ultra-long RTP polymers with lifetimes over 2 s,in contrast,the unlocked molecules hardly emit RTP in PMMA.The high-lying triplet excitons can transfer the energy to low-lying organic fluorescent dyes,and the persistent multicolor afterglows including white emission can be readily modulated.This work discloses an effective and extendable dopant molecular strategy for developing high-performance ultra-long organic RTP polymers.
基金supported by the National Natural Science Foundation of China(Grant Nos.62201276,62350001,U22B2026,and 62425105)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0300701)the Key R&D Program(Industry Foresight and Key Core Technologies)of Jiangsu Province(Grant No.BE2022071)。
文摘As the cornerstone of future information security,quantum key distribution(QKD)is evolving towards large-scale hybrid discrete-variable/continuous-variable(DV/CV)multi-domain quantum networks.Meanwhile,multicast-oriented multi-party key negotiation is attracting increasing attention in quantum networks.However,the efficient key provision for multicast services over hybrid DV/CV multi-domain quantum networks remains challenging,due to the limited probability of service success and the inefficient utilization of key resources.Targeting these challenges,this study proposes two key-resource-aware multicast-oriented key provision strategies,namely the link distance-resource balanced key provision strategy and the maximum shared link key provision strategy.The proposed strategies are applicable to hybrid DV/CV multi-domain quantum networks,which are typically implemented by GG02-based intra-domain connections and BB84-based inter-domain connections.Furthermore,the multicast-oriented key provision model is formulated,based on which two heuristic algorithms are designed,i.e.,the shared link distance-resource(SLDR)dependent and the maximum shared link distance-resource(MSLDR)dependent multicast-oriented key provision algorithms.Simulation results verify the applicability of the designed algorithms across different multi-domain quantum networks,and demonstrate their superiority over the benchmark algorithms in terms of the success probability of multicast service requests,the number of shared links,and the key resource utilization.
