Hexagonal-phase NaYF_(4)(β-NaYF_(4))has been acknowledged to be one of the most efficient doping hosts to prepare bright lanthanide-doped luminescent nano-bioprobes for various biomedical applications.However,to date...Hexagonal-phase NaYF_(4)(β-NaYF_(4))has been acknowledged to be one of the most efficient doping hosts to prepare bright lanthanide-doped luminescent nano-bioprobes for various biomedical applications.However,to date,it remains a great challenge to synthesize ultra-bright lanthanide-dopedβ-NaYF_(4)nano-bioprobes under a low reaction temperature by using conventional synthetic methods.Herein,we first develop an acetic acid(HAc)-mediated coprecipitation method for the preparation of ultrabright lanthanide-dopedβ-NaYF_(4)nanoprobes under a low reaction temperature at 200℃.Based on a series of comparative spectroscopic investigations,we show that the use of HAc in the reaction environment can not only promote the rapidα-βphase transformation of NaYF_(4)host at 200℃ within 1 h but also boost the absolute photoluminescence quantum yield(PLQY)of NaYF_(4)nanocrystals to 30.68%for near-infrared emission and to 3.79%for upconversion luminescence,both of which are amongst the highest values for diverse lanthanide-doped luminescent nanocrystals ever reported.By virtue of their superior nearinfrared luminescence,we achieve optical-guided dynamic vasculature imaging in vivo of the whole body at a high spatial resolution(23.8μm)under 980 nm excitation,indicating its potential for the diagnosis and treatment evaluation of vasculaturerelated diseases.展开更多
Trivalent lanthanide(Ln^(3+))-doped luminescent nanoparticles(NPs)have been extensively investigated as deep-tissue-penetration visual bioimaging agents owing to their exceptional upconversion and near-infrared(NIR)lu...Trivalent lanthanide(Ln^(3+))-doped luminescent nanoparticles(NPs)have been extensively investigated as deep-tissue-penetration visual bioimaging agents owing to their exceptional upconversion and near-infrared(NIR)luminescence upon irradiation of NIR light.However,in most cases,the power density of irradiation used for in vivo biological imaging is much higher than that of the reported maximum permissible exposure(MPE)value of NIR light,which inevitably does great damage to the living organisms under study and thus impedes the plausible clinical applications.Herein,by using a facile syringe pump-aided shell epitaxial growth method,we construct for the first time a new class of Ln^(3+)-doped KMgF_(3):Yb/Er@KMgF_(3)core-shell NPs that can be activated by utilizing a 980-nm xenon lamp or diode laser with an ultralow excitation power density down to 0.08 mW cm^(−2),a value that is approximately 4 orders of magnitude lower than the MPE value set by the American National Standards Institute(ANSI)for safe bioimaging in vivo.By combining the comparative spectroscopic investigations with atomic-resolved spherical aberration corrected transmission electron microscopy(AC-TEM)characterization,we find that the reduced crystallographic defects are the primary cause underlying such an ultralow-power-excitable feature of the KMgF_(3):Yb/Er@KMgF_(3)core-shell NPs.And,by the same token,the resultant KMgF_(3):Yb/Er@KMgF_(3)core-shell NPs also exhibit an anomalous thermo-enhanced photoluminescence(PL)behavior coupled with an excellent photothermal stability that cannot occur in other Ln^(3+)-doped core-shell NPs.These findings described here unambiguously pave a new way to prepare high-quality Ln^(3+)-doped luminescent NPs with desirable ultralow-power-excitable capability and photothermal stability for future biomedical applications.展开更多
A novel coordination polymer,formulated as Zn_(6)(TIB)_(4)(BPTC)_(3)(DMA)_(4)(H_(2)O)_(10)[TIB=1,3,5-tris(1-imidazolyl)-benzene,H_(4)BPTC=3,3',5,5'-biphenyltetracarboxylate],has been synthesized and structural...A novel coordination polymer,formulated as Zn_(6)(TIB)_(4)(BPTC)_(3)(DMA)_(4)(H_(2)O)_(10)[TIB=1,3,5-tris(1-imidazolyl)-benzene,H_(4)BPTC=3,3',5,5'-biphenyltetracarboxylate],has been synthesized and structurally characterized.Further investigations reveal that it presents a new topology(topological symbol{6^(2).8^(4)}{6^(3)}4{6^(5).8}6{6^(6)}2)based on self-penetration,and shows interesting fluorescent properties.展开更多
Lanthanide-doped ultrasmall nanoparticles(NPs)are attractive for diverse applications because of their unique optical properties compared with their bulk materials;their practical use,however,is greatly limited by ext...Lanthanide-doped ultrasmall nanoparticles(NPs)are attractive for diverse applications because of their unique optical properties compared with their bulk materials;their practical use,however,is greatly limited by extremely weak photoluminescence(PL)associated with severe surface quenching.Herein,we demonstrate an effective strategy to activate surface dark emitters of Eu3+in ultrasmall Sc_(2)O_(3).展开更多
基金This work was supported by the Fund of Fujian Science&Technology Innovation Laboratory for Optoelectronic Information(No.2020ZZ114)the Key Research Program of Frontier Science CAS(No.QYZDY-SSW-SLH025)+2 种基金the National Natural Science Foundation of China(Nos.21871256 and 12204481)the Natural Science Foundation of Fujian Province(No.2022J01211422)Fund of Advanced Energy Science and Technology Guangdong Laboratory(No.DJLTN0200/DJLTN0240).
文摘Hexagonal-phase NaYF_(4)(β-NaYF_(4))has been acknowledged to be one of the most efficient doping hosts to prepare bright lanthanide-doped luminescent nano-bioprobes for various biomedical applications.However,to date,it remains a great challenge to synthesize ultra-bright lanthanide-dopedβ-NaYF_(4)nano-bioprobes under a low reaction temperature by using conventional synthetic methods.Herein,we first develop an acetic acid(HAc)-mediated coprecipitation method for the preparation of ultrabright lanthanide-dopedβ-NaYF_(4)nanoprobes under a low reaction temperature at 200℃.Based on a series of comparative spectroscopic investigations,we show that the use of HAc in the reaction environment can not only promote the rapidα-βphase transformation of NaYF_(4)host at 200℃ within 1 h but also boost the absolute photoluminescence quantum yield(PLQY)of NaYF_(4)nanocrystals to 30.68%for near-infrared emission and to 3.79%for upconversion luminescence,both of which are amongst the highest values for diverse lanthanide-doped luminescent nanocrystals ever reported.By virtue of their superior nearinfrared luminescence,we achieve optical-guided dynamic vasculature imaging in vivo of the whole body at a high spatial resolution(23.8μm)under 980 nm excitation,indicating its potential for the diagnosis and treatment evaluation of vasculaturerelated diseases.
基金supported by the Fund of Fujian Science&Technology Innovation Laboratory for Optoelectronic Information(2020ZZ114)the Key Research Program of Frontier Science CAS(QYZDY-SSW-SLH025)+1 种基金the National Natural Science Foundation of China(21731006 and 21871256)the Fund of Advanced Energy Science and Technology Guangdong Laboratory(DJLTN0200/DJLTN0240)。
文摘Trivalent lanthanide(Ln^(3+))-doped luminescent nanoparticles(NPs)have been extensively investigated as deep-tissue-penetration visual bioimaging agents owing to their exceptional upconversion and near-infrared(NIR)luminescence upon irradiation of NIR light.However,in most cases,the power density of irradiation used for in vivo biological imaging is much higher than that of the reported maximum permissible exposure(MPE)value of NIR light,which inevitably does great damage to the living organisms under study and thus impedes the plausible clinical applications.Herein,by using a facile syringe pump-aided shell epitaxial growth method,we construct for the first time a new class of Ln^(3+)-doped KMgF_(3):Yb/Er@KMgF_(3)core-shell NPs that can be activated by utilizing a 980-nm xenon lamp or diode laser with an ultralow excitation power density down to 0.08 mW cm^(−2),a value that is approximately 4 orders of magnitude lower than the MPE value set by the American National Standards Institute(ANSI)for safe bioimaging in vivo.By combining the comparative spectroscopic investigations with atomic-resolved spherical aberration corrected transmission electron microscopy(AC-TEM)characterization,we find that the reduced crystallographic defects are the primary cause underlying such an ultralow-power-excitable feature of the KMgF_(3):Yb/Er@KMgF_(3)core-shell NPs.And,by the same token,the resultant KMgF_(3):Yb/Er@KMgF_(3)core-shell NPs also exhibit an anomalous thermo-enhanced photoluminescence(PL)behavior coupled with an excellent photothermal stability that cannot occur in other Ln^(3+)-doped core-shell NPs.These findings described here unambiguously pave a new way to prepare high-quality Ln^(3+)-doped luminescent NPs with desirable ultralow-power-excitable capability and photothermal stability for future biomedical applications.
基金We are thankful for financial support from the 973 Program(Nos.2014CB932101,2013CB933200)the National Natural Science Foundation of China(Nos.21471148,21141006)the Natural Science Foundation of Fujian Province(No.2011J05038).
文摘A novel coordination polymer,formulated as Zn_(6)(TIB)_(4)(BPTC)_(3)(DMA)_(4)(H_(2)O)_(10)[TIB=1,3,5-tris(1-imidazolyl)-benzene,H_(4)BPTC=3,3',5,5'-biphenyltetracarboxylate],has been synthesized and structurally characterized.Further investigations reveal that it presents a new topology(topological symbol{6^(2).8^(4)}{6^(3)}4{6^(5).8}6{6^(6)}2)based on self-penetration,and shows interesting fluorescent properties.
基金support by the Strategic Priority Research Program of the Chinese Academy of Sciences(no.XDB20000000)the National Natural Science Foundation of China(nos.21871256 and 21731006)+2 种基金the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(no.QYZDY-SSWSLH025)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(no.Y201747)the China Postdoctoral Science Foundation(no.2020T130652).
文摘Lanthanide-doped ultrasmall nanoparticles(NPs)are attractive for diverse applications because of their unique optical properties compared with their bulk materials;their practical use,however,is greatly limited by extremely weak photoluminescence(PL)associated with severe surface quenching.Herein,we demonstrate an effective strategy to activate surface dark emitters of Eu3+in ultrasmall Sc_(2)O_(3).