Stimulating and harnessing circularly polarized luminescence(CPL)is not only a sine qua non for fundamentally unveiling chirogenesis in physical chemistry,but also a pivotal prerequisite for implementation of such phe...Stimulating and harnessing circularly polarized luminescence(CPL)is not only a sine qua non for fundamentally unveiling chirogenesis in physical chemistry,but also a pivotal prerequisite for implementation of such phenomenon in research fields including chiral optoelectronics and theranostics.Herein,red-emissive carbonized polymer dots(CPDs)-based helical structures were synthesized in this work via biomolecule-tailored organic–inorganic co-assembly strategy.The surface statesrelated chirality exhibits enhanced circular dichroism(CD)and CPL activities with anisotropic factors as high as gCD,max=5.4×10^(−3) and glum,max=1.5×10^(−2),respectively.The obtained CPL signals can be further manipulated in an excitationdependent manner,indicating that a synergistic-competition phenomenon exists between configurational chirality and intermolecular energy-transfer dynamics,which is further supported by simulations based on density function theory(DFT).Such tunable CPL behavior triggers revolutionary designs and applications of these chiral CPDs into the realm of chirality-related biological issues and next-generation chiral optoelectronics.展开更多
Chiral ligand conjugated transition metal oxide nanoparticles(NPs) are a promising platform for chiral recognition, biochemical sensing, and chiroptics. Herein, we present chirality-based strategy for effective sensin...Chiral ligand conjugated transition metal oxide nanoparticles(NPs) are a promising platform for chiral recognition, biochemical sensing, and chiroptics. Herein, we present chirality-based strategy for effective sensing of mercury ions via ligand-induced chirality derived from metal-to-ligand charge transfer(MLCT) effects. The ligand competition effect between molybdenum and heavy metal ions such as mercury is designated to be essential for MLCT chirality. With this know-how, mercury ions, which have a larger stability constant(Kf) than molybdenum, can be selectively identified and quantified with a limit of detection(LOD) of 0.08 and 0.12 nmol/L for D-cysteine and L-cysteine(Cys) capped Mo O2 NPs. Such chiral chemical sensing nanosystems would be an ideal prototype for biochemical sensing with a significant impact on the field of biosensing, biological systems,and water research-based nanotoxicology.展开更多
基金National Natural Science Foundation of China,Grant/Award Number:22075240Shenzhen Fundamental Research Foundation,Grant/Award Number:JCYJ20180508162801893+3 种基金National Natural Science Foundation of Hubei Province,Grant/Award Numbers:2020CFB200,2021CFB018Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2019A1515012094Project of Department of Education of Guangdong Province,Grant/Award Number:2018KTSCX198Shenzhen Basic Research Project of Science and Technology,Grant/Award Number:JCYJ20210324094414039。
文摘Stimulating and harnessing circularly polarized luminescence(CPL)is not only a sine qua non for fundamentally unveiling chirogenesis in physical chemistry,but also a pivotal prerequisite for implementation of such phenomenon in research fields including chiral optoelectronics and theranostics.Herein,red-emissive carbonized polymer dots(CPDs)-based helical structures were synthesized in this work via biomolecule-tailored organic–inorganic co-assembly strategy.The surface statesrelated chirality exhibits enhanced circular dichroism(CD)and CPL activities with anisotropic factors as high as gCD,max=5.4×10^(−3) and glum,max=1.5×10^(−2),respectively.The obtained CPL signals can be further manipulated in an excitationdependent manner,indicating that a synergistic-competition phenomenon exists between configurational chirality and intermolecular energy-transfer dynamics,which is further supported by simulations based on density function theory(DFT).Such tunable CPL behavior triggers revolutionary designs and applications of these chiral CPDs into the realm of chirality-related biological issues and next-generation chiral optoelectronics.
基金Science,Technology and Innovation Commission of Shenzhen Municipality(JCYJ20180305180553701,KQTD2015071710313656)Guangdong Basic and Applied Basic Research Foundation(2019A1515012094)+4 种基金Natural Science Foundation of Hubei Province(2020CFB200)Shenzhen Fundamental Research Foundation(JCYJ20180508162801893)National Natural Science Foundation of China(21805234,22075240)Guangdong Introducing Innovative and Enterpreneurial Teams(2019ZT08L101)Shenzhen Institute of Artificial Intelligence and Robotics for Society(AIRS)。
文摘Chiral ligand conjugated transition metal oxide nanoparticles(NPs) are a promising platform for chiral recognition, biochemical sensing, and chiroptics. Herein, we present chirality-based strategy for effective sensing of mercury ions via ligand-induced chirality derived from metal-to-ligand charge transfer(MLCT) effects. The ligand competition effect between molybdenum and heavy metal ions such as mercury is designated to be essential for MLCT chirality. With this know-how, mercury ions, which have a larger stability constant(Kf) than molybdenum, can be selectively identified and quantified with a limit of detection(LOD) of 0.08 and 0.12 nmol/L for D-cysteine and L-cysteine(Cys) capped Mo O2 NPs. Such chiral chemical sensing nanosystems would be an ideal prototype for biochemical sensing with a significant impact on the field of biosensing, biological systems,and water research-based nanotoxicology.
