The aggregation-caused quenching(ACQ)rationale has been employed to improve the fluorescence imaging accuracy of nanocarriers by precluding free probe-derived interferences.However,its usefulness is undermined by limi...The aggregation-caused quenching(ACQ)rationale has been employed to improve the fluorescence imaging accuracy of nanocarriers by precluding free probe-derived interferences.However,its usefulness is undermined by limited penetration and low spatiotemporal resolution of NIR-Ⅰ(700-900 nm)bioimaging owing to absorption and diffraction by biological tissues and tissue-derived autofluorescence.This study aimed to develop ACQ-based NIR-Ⅱ(1000-1700 nm)probes to further improve the imaging resolution and accuracy.The strategy employed is to install highly planar and electron-rich julolidine into the 3,5-position of aza-BODIPY based on the larger substituent effects.The newly developed probes displayed remarkable photophysical properties,with intense absorption centered at approximately 850 nm and bright emission in the 950-1300 nm region.Compared with the NIR-Ⅰ counterpart P2,the NIR-Ⅱ probes demonstrated superior water sensitivity and quenching stability.ACQ1 and ACQ6 exhibited more promising ACQ effects with absolute fluorescence quenching at water fractions above 40% and higher quenching stability with less than 2.0% fluorescence reillumination in plasma after 24 h of incubation.Theoretical calculations verified that molecular planarity is more important than hydrophobicity for ACQ properties.Additionally,in vivo and ex vivo reillumination studies revealed less than 2.5% signal interference from prequenched ACQ1,in contrast to 15% for P2.展开更多
Lanthanide(Ln^(3+))-doped near infrared(NIR)-II luminescent nanoprobes have shown great promise in many technological fields,but are currently limited by the low absorption efficiency of Ln^(3+)due to the forbidden 4f...Lanthanide(Ln^(3+))-doped near infrared(NIR)-II luminescent nanoprobes have shown great promise in many technological fields,but are currently limited by the low absorption efficiency of Ln^(3+)due to the forbidden 4f→4f transition.Herein,we report a novel NIR-II luminescent nanoprobe based on efficient energy transfer from Ce^(3+)to Er^(3+)and Nd^(3+)in sub-10 nm SrS nanocrystals(NCs),which are excitable by using a commercial blue light-emitting diode(LED).Through sensitization by the allowed 4f→5d transition of Ce^(3+),the NCs exhibit strong NIR-II luminescence from Er^(3+)and Nd^(3+)with quantum yields of 2.9%and 2.3%,respectively.Furthermore,by utilizing the intense NIR-II luminescence of Er^(3+)from the thermally coupled Stark sublevels of ^(4)I_(13/2),we demonstrate the application of SrS:Ce^(3+)/Er^(3+)NCs as blue-LED-excitable NIR-II luminescent nanoprobes for ratiometric thermal sensing.These findings reveal the unique advantages of SrS:Ln^(3+)NCs in NIR-II luminescence,which may open up a new avenue for exploring novel and versatile luminescent nanoprobes based on Ln^(3+)-doped sulphide NCs.展开更多
Due to less interference in biological imaging,nanomaterials with second near-infrared(NIR-II)window(950–1700 nm)emission have received tremendous attention.However,no reports on NIR-Ⅱ electrochemiluminescence(ECL)i...Due to less interference in biological imaging,nanomaterials with second near-infrared(NIR-II)window(950–1700 nm)emission have received tremendous attention.However,no reports on NIR-Ⅱ electrochemiluminescence(ECL)imaging exist because of the lack of high-efficiency NIR-Ⅱ ECL luminophores.Herein,we designed and synthesized a NaYbF4@SiO_(2) core–shell nanoparticle for the first time.展开更多
Ovarian cancer is a global problem,and is typically diagnosed in the middle or late stages,with a mysterious abdominal mass or atypical abdominal metastases due to the lack of specific initial diagnostic methods.Dual-...Ovarian cancer is a global problem,and is typically diagnosed in the middle or late stages,with a mysterious abdominal mass or atypical abdominal metastases due to the lack of specific initial diagnostic methods.Dual-modal near-infrared Ⅱ(NIR-Ⅱ,1,000–1,700 nm)fluorescence/photoacoustic imaging has great potential in early ovarian cancer diagnosis and image-guided surgery due to its high sensitivity and deep penetration.Herein,we report a novel organic NIR-Ⅱ dye(H10)with excellent aggregation-induced-emission(AIE)characteristics(I/I0>1.6)utilizing a selenadiazolo-[3,4-f]benzo[c][1,2,5]thiadiazole(ST)-based building block.Then,water-soluble and biocompatible H10@follicle-stimulating hormone(H10@FSH)dots with superior optical/photoacoustic properties and a tenfold increase in ovarian-specific targeting ability were synthesized.Finally,for the first time,in vivo dual-mode NIR-Ⅱ fluorescent/photoacoustic(PA)imaging and image-guided surgery of patient-derived tumor xenograft(PDTX)and micro-metastatic abdominal ovarian cancer lesions were investigated.This novel strategy will establish a new method for early detection of ovarian cancer and significantly improve the prognosis of ovarian cancer patients.展开更多
基金supported by the National Natural Science Foundation of China(Nos.82273867 and 82030107)the Science and Technology Commission of Shanghai Municipality(No.21430760800,China).
文摘The aggregation-caused quenching(ACQ)rationale has been employed to improve the fluorescence imaging accuracy of nanocarriers by precluding free probe-derived interferences.However,its usefulness is undermined by limited penetration and low spatiotemporal resolution of NIR-Ⅰ(700-900 nm)bioimaging owing to absorption and diffraction by biological tissues and tissue-derived autofluorescence.This study aimed to develop ACQ-based NIR-Ⅱ(1000-1700 nm)probes to further improve the imaging resolution and accuracy.The strategy employed is to install highly planar and electron-rich julolidine into the 3,5-position of aza-BODIPY based on the larger substituent effects.The newly developed probes displayed remarkable photophysical properties,with intense absorption centered at approximately 850 nm and bright emission in the 950-1300 nm region.Compared with the NIR-Ⅰ counterpart P2,the NIR-Ⅱ probes demonstrated superior water sensitivity and quenching stability.ACQ1 and ACQ6 exhibited more promising ACQ effects with absolute fluorescence quenching at water fractions above 40% and higher quenching stability with less than 2.0% fluorescence reillumination in plasma after 24 h of incubation.Theoretical calculations verified that molecular planarity is more important than hydrophobicity for ACQ properties.Additionally,in vivo and ex vivo reillumination studies revealed less than 2.5% signal interference from prequenched ACQ1,in contrast to 15% for P2.
基金supported by the Science and Technology Cooperation Fund between Chinese and Australian Governments(2017YFE0132300)the National Natural Science Foundation of China(22135008,12074379,21875250,12004384)+1 种基金the Natural Science Foundation of Fujian Province(2020I0037,2021L3024)the Chinese Academy of Sciences/State Administration of Foreign Experts Affairs(CAS/SAFEA)International Partnership Program for Creative Research Teams,and Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZR125)。
文摘Lanthanide(Ln^(3+))-doped near infrared(NIR)-II luminescent nanoprobes have shown great promise in many technological fields,but are currently limited by the low absorption efficiency of Ln^(3+)due to the forbidden 4f→4f transition.Herein,we report a novel NIR-II luminescent nanoprobe based on efficient energy transfer from Ce^(3+)to Er^(3+)and Nd^(3+)in sub-10 nm SrS nanocrystals(NCs),which are excitable by using a commercial blue light-emitting diode(LED).Through sensitization by the allowed 4f→5d transition of Ce^(3+),the NCs exhibit strong NIR-II luminescence from Er^(3+)and Nd^(3+)with quantum yields of 2.9%and 2.3%,respectively.Furthermore,by utilizing the intense NIR-II luminescence of Er^(3+)from the thermally coupled Stark sublevels of ^(4)I_(13/2),we demonstrate the application of SrS:Ce^(3+)/Er^(3+)NCs as blue-LED-excitable NIR-II luminescent nanoprobes for ratiometric thermal sensing.These findings reveal the unique advantages of SrS:Ln^(3+)NCs in NIR-II luminescence,which may open up a new avenue for exploring novel and versatile luminescent nanoprobes based on Ln^(3+)-doped sulphide NCs.
基金the National Natural Science Foundation of China(grant no.22034003)the Excellent Research Program of Nanjing University(no.ZYJH004).
文摘Due to less interference in biological imaging,nanomaterials with second near-infrared(NIR-II)window(950–1700 nm)emission have received tremendous attention.However,no reports on NIR-Ⅱ electrochemiluminescence(ECL)imaging exist because of the lack of high-efficiency NIR-Ⅱ ECL luminophores.Herein,we designed and synthesized a NaYbF4@SiO_(2) core–shell nanoparticle for the first time.
基金supported by the National Natural Science Foundation of China (21971185 and 52173177)the Natural Science Foundation of Jiangsu Province (BK20230010 and BK20221362)+4 种基金the Science and Technology Support Program of Jiangsu Province (TJ-2022-002)funded by the Collaborative Innovation Center of Suzhou Nano Science&Technologythe 111 Projectthe Joint International Research Laboratory of Carbon-Based Functional Materials and DevicesSoochow University Tang Scholar。
基金supported by the National Natural Science Foundation of China(62175262)the Fundamental Research Funds for the Central Universities(2020CX021)the Key R&D plan of Hunan Province(2022SK2101)。
基金supported by the National Key Research and development Program of China(Nos.2020YFA0908800 and 2015DFA30440)the National Natural Science Foundation of China(Nos.82111530209,81773674,81573383,91959103,and 61971447)+4 种基金Hubei Province Scientific and Technical Innovation Key Project(No.2020BAB058)Beijing Natural Science Foundation(No.JQ18023)Shenzhen Science and Technology Research Grant(No.JCYJ20190808152019182)the Local Development Funds of Science and Technology Department of Tibet(Nos.XZ202102YD0033C and XZ202202YD0021C)the Fundamental Research Funds for the Central Universities.
文摘Ovarian cancer is a global problem,and is typically diagnosed in the middle or late stages,with a mysterious abdominal mass or atypical abdominal metastases due to the lack of specific initial diagnostic methods.Dual-modal near-infrared Ⅱ(NIR-Ⅱ,1,000–1,700 nm)fluorescence/photoacoustic imaging has great potential in early ovarian cancer diagnosis and image-guided surgery due to its high sensitivity and deep penetration.Herein,we report a novel organic NIR-Ⅱ dye(H10)with excellent aggregation-induced-emission(AIE)characteristics(I/I0>1.6)utilizing a selenadiazolo-[3,4-f]benzo[c][1,2,5]thiadiazole(ST)-based building block.Then,water-soluble and biocompatible H10@follicle-stimulating hormone(H10@FSH)dots with superior optical/photoacoustic properties and a tenfold increase in ovarian-specific targeting ability were synthesized.Finally,for the first time,in vivo dual-mode NIR-Ⅱ fluorescent/photoacoustic(PA)imaging and image-guided surgery of patient-derived tumor xenograft(PDTX)and micro-metastatic abdominal ovarian cancer lesions were investigated.This novel strategy will establish a new method for early detection of ovarian cancer and significantly improve the prognosis of ovarian cancer patients.
