Creation of new fluorophores is important for understanding the structure-property relationship,by which the required optical properties are likely to be attained.Herein,through theory calculation,it is found that fur...Creation of new fluorophores is important for understanding the structure-property relationship,by which the required optical properties are likely to be attained.Herein,through theory calculation,it is found that furan-modified thiadiazolo quinoxaline acting as an electron acceptor can endow donor-acceptor-donor(D-A-D)type second near-infrared(NIR-Ⅱ)fluorophores with longer emission wavelength than the other thiadiazolo quinoxaline-based acceptors containing pyridine,pyrrole,thiophene,and phenyl groups,respectively.On the basis of this theoretical prediction,a D-A-D type NIR-Ⅱ fluorophore with 6,7-di(furan-2-yl)-[1,2,5]thiadiazolo[3,4-g]quinoxaline(DFTQ)as the acceptor and dithieno[3,2-b:2′,3′-d]pyrrole(DTP)as the donor is designed and synthesized,and the aggregation-induced emission(AIE)function is further achieved by introducing the AIE units of tetraphenylethylene(TPE)and triphenylamine(TPA),respectively,totally forming three NIR-Ⅱ fluorophores DFTQ-DTP,DFTQ-DTPE,and DFTQ-DTPA.For biological applications,the fluorophores are encapsulated by amphiphilic DSPE-PEG2000 to generate water-dispersible nanoparticles(NPs).Almost the whole emission of each of the NPs falls into the NIR-Ⅱ spectral range,with part emission beyond 1300 nm.By using DFTQ-DTPA NPs as the contrast and photothermal therapy(PTT)agent,high-resolution in vivo fluorescence imaging is achieved in the greater than 1300 nm window,and their good performance in photoacoustic imaging and high tumor PTT efficacy in tumor-bearing mice are also demonstrated.Taken together,this work mainly provides a strong electron acceptor for constructing longemitting fluorophores,and by using the electron acceptor,a AIE fluorophore with desirable quantum yield(QY)and photothermal conversion efficienciy(PCE)is synthesized and demonstrated to be promising in fluorescence/photoacoustic imaging and PTT.展开更多
Combining resonant excitation with Purcell-enhanced single quantum dots(QDs)stands out as a prominent strategy for realizing high-performance solid-state single-photon sources.However,optimizing photon extraction effi...Combining resonant excitation with Purcell-enhanced single quantum dots(QDs)stands out as a prominent strategy for realizing high-performance solid-state single-photon sources.However,optimizing photon extraction efficiency requires addressing the challenge of effectively separating the excitation laser from the QDs’emission.Traditionally,this involves polarization filtering,limiting the achievable polarization directions and the scalability of polarized photonic states.In this study,we have successfully tackled this challenge by employing spatially orthogonal resonant excitation of QDs,deterministically coupled to monolithic Fabry–Perot microcavities.Leveraging the planar microcavity structure,we have achieved spectral filter-free single-photon resonant fluorescence.The resulting source produces single photons with a high extraction efficiency of 0.87 and an indistinguishability of 0.963(4).展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:523731405217312951973092,52103157China Postdoctoral Science Foundation,Grant/Award Numbers:2022M711544,2023T160301。
文摘Creation of new fluorophores is important for understanding the structure-property relationship,by which the required optical properties are likely to be attained.Herein,through theory calculation,it is found that furan-modified thiadiazolo quinoxaline acting as an electron acceptor can endow donor-acceptor-donor(D-A-D)type second near-infrared(NIR-Ⅱ)fluorophores with longer emission wavelength than the other thiadiazolo quinoxaline-based acceptors containing pyridine,pyrrole,thiophene,and phenyl groups,respectively.On the basis of this theoretical prediction,a D-A-D type NIR-Ⅱ fluorophore with 6,7-di(furan-2-yl)-[1,2,5]thiadiazolo[3,4-g]quinoxaline(DFTQ)as the acceptor and dithieno[3,2-b:2′,3′-d]pyrrole(DTP)as the donor is designed and synthesized,and the aggregation-induced emission(AIE)function is further achieved by introducing the AIE units of tetraphenylethylene(TPE)and triphenylamine(TPA),respectively,totally forming three NIR-Ⅱ fluorophores DFTQ-DTP,DFTQ-DTPE,and DFTQ-DTPA.For biological applications,the fluorophores are encapsulated by amphiphilic DSPE-PEG2000 to generate water-dispersible nanoparticles(NPs).Almost the whole emission of each of the NPs falls into the NIR-Ⅱ spectral range,with part emission beyond 1300 nm.By using DFTQ-DTPA NPs as the contrast and photothermal therapy(PTT)agent,high-resolution in vivo fluorescence imaging is achieved in the greater than 1300 nm window,and their good performance in photoacoustic imaging and high tumor PTT efficacy in tumor-bearing mice are also demonstrated.Taken together,this work mainly provides a strong electron acceptor for constructing longemitting fluorophores,and by using the electron acceptor,a AIE fluorophore with desirable quantum yield(QY)and photothermal conversion efficienciy(PCE)is synthesized and demonstrated to be promising in fluorescence/photoacoustic imaging and PTT.
基金Key R&D Program of Guangdong Province(2020B0303020001)National Natural Science Foundation of China(12074442)+1 种基金Innovation Program for Quantum Science and Technology(2021ZD0301400)Science and Technology Program of Guangzhou(202103030001)。
文摘Combining resonant excitation with Purcell-enhanced single quantum dots(QDs)stands out as a prominent strategy for realizing high-performance solid-state single-photon sources.However,optimizing photon extraction efficiency requires addressing the challenge of effectively separating the excitation laser from the QDs’emission.Traditionally,this involves polarization filtering,limiting the achievable polarization directions and the scalability of polarized photonic states.In this study,we have successfully tackled this challenge by employing spatially orthogonal resonant excitation of QDs,deterministically coupled to monolithic Fabry–Perot microcavities.Leveraging the planar microcavity structure,we have achieved spectral filter-free single-photon resonant fluorescence.The resulting source produces single photons with a high extraction efficiency of 0.87 and an indistinguishability of 0.963(4).