Circularly polarized luminescence(CPL)materials have received widespread attention due to their remarkable performance and broad applications.However,current CPL material research primarily focuses on tunable color,in...Circularly polarized luminescence(CPL)materials have received widespread attention due to their remarkable performance and broad applications.However,current CPL material research primarily focuses on tunable color,intensity,and reversibility.Constructing CPL with adjustable lifetime remains a significant challenge.Herein,a series of CPL polymeric materials with tunable lifetime were obtained by employing phosphorescent terephthalic acid and chiral organic small molecule R/S-BNAF(a luminescent binaphthol derivative)to copolymerize with acrylamide in different ratios.It was verified that this performance results from the different energy transfer efficiency between luminophores with varying ratios of the monomers for copolymerization.This strategy to realize CPL with tunable lifetime by modulating the energy transfer efficiency will provide a new perspective to broaden the applications of CPL materials.展开更多
次硝酸(Nitroxyl,HNO)由一氧化氮(NO)经单电子还原和质子化作用产生,在生理和病理过程中都有着重要作用.本工作构建了一种基于发光共振能量转移(Luminescence resonance energy transfer,LRET)的比率型上转换纳米探针用于检测生物体系中...次硝酸(Nitroxyl,HNO)由一氧化氮(NO)经单电子还原和质子化作用产生,在生理和病理过程中都有着重要作用.本工作构建了一种基于发光共振能量转移(Luminescence resonance energy transfer,LRET)的比率型上转换纳米探针用于检测生物体系中HNO含量.该探针以上转换纳米颗粒(Upconversion nanoparticles,UCNPs)为能量供体,有机染料Fl-TP为能量受体构建.Fl-TP能特异性识别HNO并与之反应生成Fl-HNO,Fl-HNO在400~500 nm处具有明显的吸收峰,与UCNPs的蓝色发射光谱重叠,从而发生LRET过程.随着HNO浓度增加,Fl-HNO的荧光强度(F525 nm)逐渐增强,UCNPs的荧光强度(F480nm)逐渐下降,比率信号(F525nm/F480nm)逐渐增加,并与HNO浓度对数呈良好的线性关系,该探针的线性检测范围为3~100μmol·L^-1,检出限23.4nmol·L^-1.实验结果表明该比率探针特异性强,灵敏度高,并可成功实现在活细胞和生物组织中HNO的检测.展开更多
Eu3+ions embedded in silica thin films codoped with SnO2 nanocrystals were fabricated by sol–gel and spin-coating methods.SnO2 nanocrystals with controllable sizes were synthesized through precisely controlling the S...Eu3+ions embedded in silica thin films codoped with SnO2 nanocrystals were fabricated by sol–gel and spin-coating methods.SnO2 nanocrystals with controllable sizes were synthesized through precisely controlling the Sn concentrations.The influences of doping and annealing conditions on the photoluminescence intensity from SnO2 nanocrystals are systematically investigated.The effective energy transfer from the defect states of SnO2nanocrystals to nearby Eu3+ions has revealed by the selective photoluminescence excitation spectra.The efficiency of the Forster resonance energy transfer is evaluated by the time-resolved photoluminescence measurements,which is about 29.1%based on the lifetime tests of the SnO2emission.展开更多
Although upconversion nanoparticle(UCNP)-based luminescence resonance energy transfer(LRET)has attracted intensive attention,its application in sensing strategies for biomacromolecule detection is still limited due to...Although upconversion nanoparticle(UCNP)-based luminescence resonance energy transfer(LRET)has attracted intensive attention,its application in sensing strategies for biomacromolecule detection is still limited due to the low energy-transfer efficiency.Here,we develop an energy pumping strategy to enhance the upconversion LRET efficiency of UCNP from 3.6% to 70.3%.Surface collector dye cyanine-3(Cy3)is modified on the UCNP surface to concentrate the scattered emission energy from interior UCNP to particle surface and then further pumped to the surface extended acceptor.Using caspase-3 as a target,its recognition and cleavage of QSY7-labeled peptide co-assembled on UCNP-Cy3 leads to the release of QSY7 to recover Cy3 fluorescence.Owing to the multiple emissions of UCNP,this system can be integrated with another surface collector to enhance reactive oxygen species(ROS)generation for photodynamic therapy(PDT).Caspase-3,as a PDT product,is imaged in situ with an internal standard to self-evaluate the PDT effect.展开更多
We report the rational design of a dual stimulus-activated quaternary chiral emission nematic liquid crystals(Q-N*-LCs)containing light-driven chiral dopant R-S-R-1,a static chiral dopant S-2 and an achiral Nile Red(N...We report the rational design of a dual stimulus-activated quaternary chiral emission nematic liquid crystals(Q-N*-LCs)containing light-driven chiral dopant R-S-R-1,a static chiral dopant S-2 and an achiral Nile Red(NR)in a nematic liquid crystal(SLC1717).The dopant R-S-R-1 acts as a dynamic chiral donor and an energy donor,and the achiral NR serves as a circularly polarized luminescence(CPL)emitter and energy acceptor.Interestingly,this kind of Q-N*-LCs appears reversal CPL emission direction(L-CPL)using 365 nm UV light irradiation compared with the initial state(R-CPL).Most importantly,the“On-Off”CPL switch behavior of Q-N*-LCs can be repeatedly driven by revoking or rearranging the applied direct current(DC)electric field.An OR chiral information logic gate demonstrates that this dual driven Q-N*-LCs can be potentially used for chiral information storage and coding.展开更多
Excessive reactive oxygen species(ROS)would attack living cells and cause a series of oxidative stress related diseases,such as liver damage.Hydroxyl radicals(·OH)are currently known as one of the most toxic and ...Excessive reactive oxygen species(ROS)would attack living cells and cause a series of oxidative stress related diseases,such as liver damage.Hydroxyl radicals(·OH)are currently known as one of the most toxic and harmful free radicals to organisms.Therefore,studies involving hydroxyl radicals have become important research topics in the fields of biology,biochemistry,and biomedicine.In addition,imaging of analytes using upconversion nanoparticles(UCNPs)possesses significant advantages over that using general fluorescent dyes or nanoparticles due to its high spatial resolution,reduced photodamage,and deep tissue penetration properties.Herein,we designed a highly selective and sensitive hydroxyl radical nanoprobe based on the luminescence resonance energy transfer between upconversion nanoparticles and methylene blue(MB).The concentration of·OH could be determined by the fluorescence recovery of the UCNPs due to the oxidative damage of MB.Using this nanoprobe,the·OH in living cells or in liver tissues could be monitored with high sensitivity and selectivity.展开更多
β-NaYF4:Yb,Er nanoparticles (NPs) are one of the most efficient upconversion materials, which can convert near-infrared light to higher-energy light through multiple photon absorptions or energy transfer. In addition...β-NaYF4:Yb,Er nanoparticles (NPs) are one of the most efficient upconversion materials, which can convert near-infrared light to higher-energy light through multiple photon absorptions or energy transfer. In addition, they may be attractive alternative donors for luminescence resonance energy transfer (LRET) studies, because of their sharp absorption and emission profiles, high quantum yields, large anti-stokes shifts, long lifetime, low toxicity, and superior photo-stability. In principle, many problems of fluorescence resonance energy transfer (FRET), such as excitation of acceptors, emission overlaps between donors and acceptors, high background noise, potential toxicity, and instability, can be overcome using β-NaYF4:Yb,Er NPs as energy donors. Because the organic coating induced separation can significantly reduce the energy transfer efficiency and aqueous FRET system is difficult to be applied in devices, we demonstrate a novel NP-dye LRET system in solid state. The emission of the β-NaYF4:Yb,Er NPs at 539 nm overlaps with the absorption of the tetrametrylrhodarnine isothiocyante (TRITC), satisfying the requirement of LRET process. Since TRITC molecules are adsorbed on the β-NaYF4:Yb,Er NPs by an electrostatic interaction, the interaction distance is suitable for LRET without any further modulation. The resultant solid LRET system is ready for the further applications for devices.展开更多
基金supported by the National Key Research and Development Program of China(2022YFB3203500)the National Natural Science Foundation of China(22125803,22020102006)+2 种基金Shanghai Municipal Science and Technology Major Project(2018SHZDZX03)the Postdoctoral Fellowship Program of China Postdoctoral Science Foundationthe Fundamental Research Funds for the Central Universities。
文摘Circularly polarized luminescence(CPL)materials have received widespread attention due to their remarkable performance and broad applications.However,current CPL material research primarily focuses on tunable color,intensity,and reversibility.Constructing CPL with adjustable lifetime remains a significant challenge.Herein,a series of CPL polymeric materials with tunable lifetime were obtained by employing phosphorescent terephthalic acid and chiral organic small molecule R/S-BNAF(a luminescent binaphthol derivative)to copolymerize with acrylamide in different ratios.It was verified that this performance results from the different energy transfer efficiency between luminophores with varying ratios of the monomers for copolymerization.This strategy to realize CPL with tunable lifetime by modulating the energy transfer efficiency will provide a new perspective to broaden the applications of CPL materials.
基金supported by the National Basic Research Program of China(2013CB632101)the National Natural Science Foundation of China(11274155)
文摘Eu3+ions embedded in silica thin films codoped with SnO2 nanocrystals were fabricated by sol–gel and spin-coating methods.SnO2 nanocrystals with controllable sizes were synthesized through precisely controlling the Sn concentrations.The influences of doping and annealing conditions on the photoluminescence intensity from SnO2 nanocrystals are systematically investigated.The effective energy transfer from the defect states of SnO2nanocrystals to nearby Eu3+ions has revealed by the selective photoluminescence excitation spectra.The efficiency of the Forster resonance energy transfer is evaluated by the time-resolved photoluminescence measurements,which is about 29.1%based on the lifetime tests of the SnO2emission.
基金the National Natural Science Foundation of China(nos.21635005,21974064,22022405,21827812,21890741,22004062,and 22004068)Natural Science Foundation of Jiangsu Province for distinguished Young Scholars(no.BK20200010)+2 种基金Specially appointed Professor Foundation of Jiangsu ProvinceChina Postdoctoral Science Foundation(no.252986)Program for Innovative Talents and Entrepreneurs of Jiangsu Province.
文摘Although upconversion nanoparticle(UCNP)-based luminescence resonance energy transfer(LRET)has attracted intensive attention,its application in sensing strategies for biomacromolecule detection is still limited due to the low energy-transfer efficiency.Here,we develop an energy pumping strategy to enhance the upconversion LRET efficiency of UCNP from 3.6% to 70.3%.Surface collector dye cyanine-3(Cy3)is modified on the UCNP surface to concentrate the scattered emission energy from interior UCNP to particle surface and then further pumped to the surface extended acceptor.Using caspase-3 as a target,its recognition and cleavage of QSY7-labeled peptide co-assembled on UCNP-Cy3 leads to the release of QSY7 to recover Cy3 fluorescence.Owing to the multiple emissions of UCNP,this system can be integrated with another surface collector to enhance reactive oxygen species(ROS)generation for photodynamic therapy(PDT).Caspase-3,as a PDT product,is imaged in situ with an internal standard to self-evaluate the PDT effect.
基金supported by the National Natural Science Foundation of China (21975118,92156014)
文摘We report the rational design of a dual stimulus-activated quaternary chiral emission nematic liquid crystals(Q-N*-LCs)containing light-driven chiral dopant R-S-R-1,a static chiral dopant S-2 and an achiral Nile Red(NR)in a nematic liquid crystal(SLC1717).The dopant R-S-R-1 acts as a dynamic chiral donor and an energy donor,and the achiral NR serves as a circularly polarized luminescence(CPL)emitter and energy acceptor.Interestingly,this kind of Q-N*-LCs appears reversal CPL emission direction(L-CPL)using 365 nm UV light irradiation compared with the initial state(R-CPL).Most importantly,the“On-Off”CPL switch behavior of Q-N*-LCs can be repeatedly driven by revoking or rearranging the applied direct current(DC)electric field.An OR chiral information logic gate demonstrates that this dual driven Q-N*-LCs can be potentially used for chiral information storage and coding.
基金the support from the National Natural Science Foundation of China(21601046,31500812,and 21603051)the Natural Science Foundation of Hebei Province(B2016201169,B2017201226,B2018201221,and B2018201157)+2 种基金Key Projects of Education Department of Hebei Province(ZD2018036)the Foundation for Returned Overseas Chinese Scholars of Hebei Province(CY201703)Hebei Youth Top Talent Project.
文摘Excessive reactive oxygen species(ROS)would attack living cells and cause a series of oxidative stress related diseases,such as liver damage.Hydroxyl radicals(·OH)are currently known as one of the most toxic and harmful free radicals to organisms.Therefore,studies involving hydroxyl radicals have become important research topics in the fields of biology,biochemistry,and biomedicine.In addition,imaging of analytes using upconversion nanoparticles(UCNPs)possesses significant advantages over that using general fluorescent dyes or nanoparticles due to its high spatial resolution,reduced photodamage,and deep tissue penetration properties.Herein,we designed a highly selective and sensitive hydroxyl radical nanoprobe based on the luminescence resonance energy transfer between upconversion nanoparticles and methylene blue(MB).The concentration of·OH could be determined by the fluorescence recovery of the UCNPs due to the oxidative damage of MB.Using this nanoprobe,the·OH in living cells or in liver tissues could be monitored with high sensitivity and selectivity.
基金Supported by the National Natural Science Foundation of China (Grant Nos. 20821091 and 20671005)the National Natural Science Foundation of China & Research Grants Council (20731160001)the Ministry of Science and Technology of China (Grant No. 2006CB601104)
文摘β-NaYF4:Yb,Er nanoparticles (NPs) are one of the most efficient upconversion materials, which can convert near-infrared light to higher-energy light through multiple photon absorptions or energy transfer. In addition, they may be attractive alternative donors for luminescence resonance energy transfer (LRET) studies, because of their sharp absorption and emission profiles, high quantum yields, large anti-stokes shifts, long lifetime, low toxicity, and superior photo-stability. In principle, many problems of fluorescence resonance energy transfer (FRET), such as excitation of acceptors, emission overlaps between donors and acceptors, high background noise, potential toxicity, and instability, can be overcome using β-NaYF4:Yb,Er NPs as energy donors. Because the organic coating induced separation can significantly reduce the energy transfer efficiency and aqueous FRET system is difficult to be applied in devices, we demonstrate a novel NP-dye LRET system in solid state. The emission of the β-NaYF4:Yb,Er NPs at 539 nm overlaps with the absorption of the tetrametrylrhodarnine isothiocyante (TRITC), satisfying the requirement of LRET process. Since TRITC molecules are adsorbed on the β-NaYF4:Yb,Er NPs by an electrostatic interaction, the interaction distance is suitable for LRET without any further modulation. The resultant solid LRET system is ready for the further applications for devices.
