The synthesis and upconverted fluorescent properties of a series of organic compounds with the structure: donor/bridge/acceptor, and different side-chains are reported. The results show that the compounds with differe...The synthesis and upconverted fluorescent properties of a series of organic compounds with the structure: donor/bridge/acceptor, and different side-chains are reported. The results show that the compounds with different side-chains exhibit different two-photon induced fluorescent properties, although they have the same main donor/bridge/acceptor structure.展开更多
The combination of upconverting nanoparticles(UCNPs)and immunochromatography has become a widely used and promising new detection technique for point-of-care testing(POCT).However,their low luminescence efficiency,non...The combination of upconverting nanoparticles(UCNPs)and immunochromatography has become a widely used and promising new detection technique for point-of-care testing(POCT).However,their low luminescence efficiency,non-specific adsorption,and image noise have always limited their progress toward practical applications.Recently,artificial intelligence(AI)has demonstrated powerful representational learning and generalization capabilities in computer vision.We report for the first time a combination of AI and upconversion nanoparticle-based lateral flow assays(UCNP-LFAs)for the quantitative detection of commercial internet of things(IoT)devices.This universal UCNPs quantitative detection strategy combines high accuracy,sensitivity,and applicability in the field detection environment.By using transfer learning to train AI models in a small self-built database,we not only significantly improved the accuracy and robustness of quantitative detection,but also efficiently solved the actual problems of data scarcity and low computing power of POCT equipment.Then,the trained AI model was deployed in IoT devices,whereby the detection process does not require detailed data preprocessing to achieve real-time inference of quantitative results.We validated the quantitative detection of two detectors using eight transfer learning models on a small dataset.The AI quickly provided ultra-high accuracy prediction results(some models could reach 100%accuracy)even when strong noise was added.Simultaneously,the high flexibility of this strategy promises to be a general quantitative detection method for optical biosensors.We believe that this strategy and device have a scientific significance in revolutionizing the existing POCT technology landscape and providing excellent commercial value in the in vitro diagnostics(IVD)industry.展开更多
This paper describes the synthesis of new upconverting luminescent nanoparticles that consist of YF_(3):Yb^(3+)/Er^(3+)functionalized with poly(acrylic acid)(PAA).Unlike the upconverting nanocrystals previously report...This paper describes the synthesis of new upconverting luminescent nanoparticles that consist of YF_(3):Yb^(3+)/Er^(3+)functionalized with poly(acrylic acid)(PAA).Unlike the upconverting nanocrystals previously reported in the literature that emit visible(blue-green-red)upconversion fluorescence,these as-prepared nanoparticles emit strong near-infrared(NIR,831 nm)upconversion luminescence under 980 nm excitation.Scanning electron microscopy,transmission electron microscopy,and powder X-ray diffraction were used to characterize the size and composition of the luminescent nanocrystals.Their average diameter was about 50 nm.The presence of the PAA coating was confirmed by infrared spectroscopy.The particles are highly dispersible in aqueous solution due to the presence of carboxylate groups in the PAA coating.By carrying out the synthesis in the absence of PAA,YF_(3):Yb^(3+)/Er^(3+)nanorice materials were obtained.These nanorice particles are larger(~700 nm in length)than the PAA-functionalized nanoparticles and show strong typical visible red(668 nm),rather than NIR(831 nm),upconversion fluorescence.The new PAA-coated luminescent nanoparticles have the pottential be used in a variety of bioanalytical and medical assays involving luminescence detection and fluorescence imaging,especially in vivo fluorescence imaging,due to the deep penetration of NIR radiation.展开更多
Optical imaging plays an important role in biomedical research being extremely useful for early detection, screening and image-guided therapy. Lanthanide-doped up-converting nanoparticles were ideally suited for bioim...Optical imaging plays an important role in biomedical research being extremely useful for early detection, screening and image-guided therapy. Lanthanide-doped up-converting nanoparticles were ideally suited for bioimaging because they could be ex- cited in near infrared （NIR） and emit in NIR or visible （VIS）. Here, we compared lanthanide doped up-converting NaYF4 and organic fluorophores for application in deep-tissue imaging. For that purpose - tissue phantoms mimicking the natural properties of light scat- tering by living tissues were prepared. The studies allowed to quantitatively compare optical resolution of different fluorescent com- pounds, revealing that the NIR photoexcitation was favorable over conventional UV photoexcitation.展开更多
Rattle structure is a topic of great interest in design and application of nano- materials due to the unique core@void@shell architecture and the integration of functions. Herein, we developed a novel ＂ship-in-a-bot...Rattle structure is a topic of great interest in design and application of nano- materials due to the unique core@void@shell architecture and the integration of functions. Herein, we developed a novel ＂ship-in-a-bottle＂ method to fabricate upconverting （UC） luminescent nanorattles by incorporating lanthanide-doped fluorides into hollow mesoporous silica. The size of nanorattles and the filling amount of fluorides can be well controlled. In addition, the modification of silica shell （with phenylene and amine groups） and the variation of efficient UC fluorides （NaYF4：Yb, Er, NaLuF4：Yb, Er, NaGdF4：Yb, Er and LiYF4：Yb, Er） were readily achieved. The resulting nanorattles exhibited a high capacity and pH-dependent release of the anti-cancer drug doxorubicin （DOX）. Furthermore, we employed these nanorattles in proof-of-concept UC-monitoring drug release by utilizing the energy transfer process from UC fluorides to DOX, thus revealing the great potential of the nanorattles as efficient cancer theranostic agent.展开更多
Alkaline-earth dihalide nanocrystals(NCs) such as SrFCl, owing to their high chemical stability and low phonon energy, are excellent host materials for lanthanide(Ln3+) doping to achieve desirable optical properties f...Alkaline-earth dihalide nanocrystals(NCs) such as SrFCl, owing to their high chemical stability and low phonon energy, are excellent host materials for lanthanide(Ln3+) doping to achieve desirable optical properties for various bioapplications, Herein, we report a novel strategy for the synthesis of sub-10 nm Ln3+-doped SrFCl NCs with efficient upconverting and downshifting luminescence through a facile onestep hot-injection method. Utilizing the temperature-dependent upconverting luminescence(UCL) from the thermally coupled 2H11/2 and 4S3/2 levels of Er3+, we showed the potential of SrFCl:Yb,Er NCs as sensitive UCL nanoprobes for non-contact thermal sensing with a maximum detection sensitivity of 0.0066 K-1, which is among the highest values for thermal sensing based on Er3+-activated UCL nanoprobes. Furthermore, by employing the intense downshifting luminescence from Tb3+ and Eu3+, we demonstrated the successful use of biotinylated SrFCl:Ce,Tb and SrFCl:Eu3+ nanoprobes for biotin receptor-targeted cancer cell imaging, thus revealing the great promise of SrFCl:Ln3+ nanoprobes for versatile bioapplications.展开更多
Achieving large luminescence dissymmetry factors(pium)is challenging in the research field of circularly polarized luminescence(CPL).While various approaches have been developed to construct organic systems with CPL a...Achieving large luminescence dissymmetry factors(pium)is challenging in the research field of circularly polarized luminescence(CPL).While various approaches have been developed to construct organic systems with CPL activity,there is still a lack of effective methods for fabricating CPL active inorganic materials.Herein,we propose an approach for endowing upconversion nanoparticles(UCNPs)and perovskite nanocrystal(PKNC)hybrid nanomaterials with upconverted circularly polarized luminescence(UC-CPL)activity.Chiral cesium lead bromides(CsPbBr_(3))PKNCs were synthesized by a chiral-ligand-assistant method.Meanwhile,UCNP could be embedded into the chiral PKNC,enabling a photon upconvesion feature to the PKNC.The embedded UCNPs in PKNCs were confirmed by electron tomography.Consequently,various CPL activities,including prompt CPL,UC-CPL,and energy transfer enhanced circularly polarized luminescence(ET-CPL),were realized.The chiral perovskite nanocrystals could reabsorb the chiral energy generated from UCNPs,showing energy transfer enhanced CPL activity with four times magnification of the circular polarization.These findings provide a meaningful strategy for designing chiral photon upconversion inorganic nanomaterials with highly efficient UC-CPL activity.展开更多
Oxygen sensing,magnetic,and upconversion luminescence properties are combined in multi-functional composite particles prepared herein by a simple mixing,baking,and grinding procedure.Upconverting nanocrystals are used...Oxygen sensing,magnetic,and upconversion luminescence properties are combined in multi-functional composite particles prepared herein by a simple mixing,baking,and grinding procedure.Upconverting nanocrystals are used as an excitation source and an oxygen indicator with far-red emission.The composite particles are excited with near infrared(NIR)laser light(980 nm).The visible upconversion emission is converted into an oxygen concentration-dependent far-red emission(<750 nm)using an inert mediator dye and a platinated benzoporphyrin dye.This concept combines the advantages of NIR excitation and far-red emissive indicator dyes,offering minimized auto-fluorescence and enhanced membrane permeability.Additional functionality is obtained by incorporating magnetic nanoparticles into the composite particles,which enables easy manipulation and separation of the particles by the application of an external magnetic field.展开更多
基金This work was supported by thc grant for State Key Program of Chinaby the National Natural Science Foundation of China.
文摘The synthesis and upconverted fluorescent properties of a series of organic compounds with the structure: donor/bridge/acceptor, and different side-chains are reported. The results show that the compounds with different side-chains exhibit different two-photon induced fluorescent properties, although they have the same main donor/bridge/acceptor structure.
基金The authors thank the financial support from the National Natural Science Foundation of China(61905033 and 62122017).
文摘The combination of upconverting nanoparticles(UCNPs)and immunochromatography has become a widely used and promising new detection technique for point-of-care testing(POCT).However,their low luminescence efficiency,non-specific adsorption,and image noise have always limited their progress toward practical applications.Recently,artificial intelligence(AI)has demonstrated powerful representational learning and generalization capabilities in computer vision.We report for the first time a combination of AI and upconversion nanoparticle-based lateral flow assays(UCNP-LFAs)for the quantitative detection of commercial internet of things(IoT)devices.This universal UCNPs quantitative detection strategy combines high accuracy,sensitivity,and applicability in the field detection environment.By using transfer learning to train AI models in a small self-built database,we not only significantly improved the accuracy and robustness of quantitative detection,but also efficiently solved the actual problems of data scarcity and low computing power of POCT equipment.Then,the trained AI model was deployed in IoT devices,whereby the detection process does not require detailed data preprocessing to achieve real-time inference of quantitative results.We validated the quantitative detection of two detectors using eight transfer learning models on a small dataset.The AI quickly provided ultra-high accuracy prediction results(some models could reach 100%accuracy)even when strong noise was added.Simultaneously,the high flexibility of this strategy promises to be a general quantitative detection method for optical biosensors.We believe that this strategy and device have a scientific significance in revolutionizing the existing POCT technology landscape and providing excellent commercial value in the in vitro diagnostics(IVD)industry.
基金We acknowledge the financial support from the National Natural Science Foundation of China(Nos.20605001 and 20871004)and start-up funding of Beijing University of Chemical Technology.
文摘This paper describes the synthesis of new upconverting luminescent nanoparticles that consist of YF_(3):Yb^(3+)/Er^(3+)functionalized with poly(acrylic acid)(PAA).Unlike the upconverting nanocrystals previously reported in the literature that emit visible(blue-green-red)upconversion fluorescence,these as-prepared nanoparticles emit strong near-infrared(NIR,831 nm)upconversion luminescence under 980 nm excitation.Scanning electron microscopy,transmission electron microscopy,and powder X-ray diffraction were used to characterize the size and composition of the luminescent nanocrystals.Their average diameter was about 50 nm.The presence of the PAA coating was confirmed by infrared spectroscopy.The particles are highly dispersible in aqueous solution due to the presence of carboxylate groups in the PAA coating.By carrying out the synthesis in the absence of PAA,YF_(3):Yb^(3+)/Er^(3+)nanorice materials were obtained.These nanorice particles are larger(~700 nm in length)than the PAA-functionalized nanoparticles and show strong typical visible red(668 nm),rather than NIR(831 nm),upconversion fluorescence.The new PAA-coated luminescent nanoparticles have the pottential be used in a variety of bioanalytical and medical assays involving luminescence detection and fluorescence imaging,especially in vivo fluorescence imaging,due to the deep penetration of NIR radiation.
基金Project supported by Wroclaw Research Centre EIT+within the project"The Application of Nanotechnology in Advanced Materials"-NanoMat(POIG.01.01.02-02-002/08)financed by the European Regional Development Fund(Operational Programme Innovative Economy,1.1.2)
文摘Optical imaging plays an important role in biomedical research being extremely useful for early detection, screening and image-guided therapy. Lanthanide-doped up-converting nanoparticles were ideally suited for bioimaging because they could be ex- cited in near infrared （NIR） and emit in NIR or visible （VIS）. Here, we compared lanthanide doped up-converting NaYF4 and organic fluorophores for application in deep-tissue imaging. For that purpose - tissue phantoms mimicking the natural properties of light scat- tering by living tissues were prepared. The studies allowed to quantitatively compare optical resolution of different fluorescent com- pounds, revealing that the NIR photoexcitation was favorable over conventional UV photoexcitation.
基金This work is supported by the National Basic Research Program of China （No. 2014CB845605）, Special Project of National Major Scientific Equipment Development of China （No. 2012YQ120060）, the National Natural Science Foundation of China （Nos. 21201163, 21401196, U1305244, and 21325104）, the CAS/SAFEA International Partnership Program for Creative Research Teams, and Strategic Priority Research Program of the CAS （No. XDA09030307）.
文摘Rattle structure is a topic of great interest in design and application of nano- materials due to the unique core@void@shell architecture and the integration of functions. Herein, we developed a novel ＂ship-in-a-bottle＂ method to fabricate upconverting （UC） luminescent nanorattles by incorporating lanthanide-doped fluorides into hollow mesoporous silica. The size of nanorattles and the filling amount of fluorides can be well controlled. In addition, the modification of silica shell （with phenylene and amine groups） and the variation of efficient UC fluorides （NaYF4：Yb, Er, NaLuF4：Yb, Er, NaGdF4：Yb, Er and LiYF4：Yb, Er） were readily achieved. The resulting nanorattles exhibited a high capacity and pH-dependent release of the anti-cancer drug doxorubicin （DOX）. Furthermore, we employed these nanorattles in proof-of-concept UC-monitoring drug release by utilizing the energy transfer process from UC fluorides to DOX, thus revealing the great potential of the nanorattles as efficient cancer theranostic agent.
基金Project supported by the CAS/SAFEA International Partnership Program for Creative Research Teamsthe National Natural Science Foundation of China(21771185,11774345,21875250,21650110462)+2 种基金the CAS Youth Innovation Promotion Association(2016277)the Chunmiao Project of Haixi Institutes of the CAS(CMZX-2016-002)Natural Science Foundation of Fujian Province(201710018)
文摘Alkaline-earth dihalide nanocrystals(NCs) such as SrFCl, owing to their high chemical stability and low phonon energy, are excellent host materials for lanthanide(Ln3+) doping to achieve desirable optical properties for various bioapplications, Herein, we report a novel strategy for the synthesis of sub-10 nm Ln3+-doped SrFCl NCs with efficient upconverting and downshifting luminescence through a facile onestep hot-injection method. Utilizing the temperature-dependent upconverting luminescence(UCL) from the thermally coupled 2H11/2 and 4S3/2 levels of Er3+, we showed the potential of SrFCl:Yb,Er NCs as sensitive UCL nanoprobes for non-contact thermal sensing with a maximum detection sensitivity of 0.0066 K-1, which is among the highest values for thermal sensing based on Er3+-activated UCL nanoprobes. Furthermore, by employing the intense downshifting luminescence from Tb3+ and Eu3+, we demonstrated the successful use of biotinylated SrFCl:Ce,Tb and SrFCl:Eu3+ nanoprobes for biotin receptor-targeted cancer cell imaging, thus revealing the great promise of SrFCl:Ln3+ nanoprobes for versatile bioapplications.
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB36000000)the National Natural Science Foundation of China(Nos.21802027,21908161,51673050,and 91856115)+1 种基金the Ministry of Science and Technology of the Peoples Republic of China(No.2017YFA0206600,and 2016YFA0203400)Beijing Natural Science Foundation(No.2212023)。
文摘Achieving large luminescence dissymmetry factors(pium)is challenging in the research field of circularly polarized luminescence(CPL).While various approaches have been developed to construct organic systems with CPL activity,there is still a lack of effective methods for fabricating CPL active inorganic materials.Herein,we propose an approach for endowing upconversion nanoparticles(UCNPs)and perovskite nanocrystal(PKNC)hybrid nanomaterials with upconverted circularly polarized luminescence(UC-CPL)activity.Chiral cesium lead bromides(CsPbBr_(3))PKNCs were synthesized by a chiral-ligand-assistant method.Meanwhile,UCNP could be embedded into the chiral PKNC,enabling a photon upconvesion feature to the PKNC.The embedded UCNPs in PKNCs were confirmed by electron tomography.Consequently,various CPL activities,including prompt CPL,UC-CPL,and energy transfer enhanced circularly polarized luminescence(ET-CPL),were realized.The chiral perovskite nanocrystals could reabsorb the chiral energy generated from UCNPs,showing energy transfer enhanced CPL activity with four times magnification of the circular polarization.These findings provide a meaningful strategy for designing chiral photon upconversion inorganic nanomaterials with highly efficient UC-CPL activity.
基金This research was funded by Austrian Science Fund(FWF,I 442-N19)Deutsche Forschungsgemeinschaft(DFG,WO 669/12-1),both within the framework of an ERA Chemistry project.
文摘Oxygen sensing,magnetic,and upconversion luminescence properties are combined in multi-functional composite particles prepared herein by a simple mixing,baking,and grinding procedure.Upconverting nanocrystals are used as an excitation source and an oxygen indicator with far-red emission.The composite particles are excited with near infrared(NIR)laser light(980 nm).The visible upconversion emission is converted into an oxygen concentration-dependent far-red emission(<750 nm)using an inert mediator dye and a platinated benzoporphyrin dye.This concept combines the advantages of NIR excitation and far-red emissive indicator dyes,offering minimized auto-fluorescence and enhanced membrane permeability.Additional functionality is obtained by incorporating magnetic nanoparticles into the composite particles,which enables easy manipulation and separation of the particles by the application of an external magnetic field.
