The demand for enhanced optical properties in advanced fluorescence technologies has driven research into the structure-property relationship of fluorophores.In this paper,we use naphthalene fluorophores Na DC-Aze and...The demand for enhanced optical properties in advanced fluorescence technologies has driven research into the structure-property relationship of fluorophores.In this paper,we use naphthalene fluorophores Na DC-Aze and PhDO-Aze as a case study to emphasize the pivotal role of cross conjugation in tuning the optical structure-property relationship.Na DC-Aze and PhDO-Aze,formed by hybridizing two distinct conjugated systems in a single naphthalene molecule,exhibit spectral characteristics from both conjugated systems.Experimental data and theoretical calculations demonstrate the coexistence of two electron-delocalization systems in a cross-conjugation manner in both Na DC-Aze and PhDO-Aze.The cross-conjugation fluorophores exhibit high brightness,large Stokes shift,and a broad absorption wavelength range by combining distinct spectral properties from its parent fluorophores.These spectral properties will be advantageous for certain applications(i.e.,panchromatic absorption in organic solar cells,and fluorophores compatible with a wide range of excitation wavelengths).展开更多
Cyclooctatetraene(COT)attachment to fluorophores(“self-healing”dyes)is known for quenching reac-tive triplet states via triplet-state energy transfer(TET),enhancing photostability.However,COT’s impact on singlet st...Cyclooctatetraene(COT)attachment to fluorophores(“self-healing”dyes)is known for quenching reac-tive triplet states via triplet-state energy transfer(TET),enhancing photostability.However,COT’s impact on singlet states remains unclear.Quantum calculations reveal that COT induces energy transfer to dark states in deep blue dyes while promoting photoinduced electron transfer(PET)and intersystem crossing(ISC)in visible dyes,potentially compromising brightness and/or photostability.To address this,we pro-pose the use of △E descriptor to optimize COT’s effects.Our findings uncover COT’s multifaceted impact.These insights will guide the development of superior triplet state quenchers and photostable dyes.展开更多
Energy transfer and electron transfer are both fundamental mechanisms enabling numerous functional materials and applications.While most materials systems employ either energy transfer or electron transfer,the combine...Energy transfer and electron transfer are both fundamental mechanisms enabling numerous functional materials and applications.While most materials systems employ either energy transfer or electron transfer,the combined effect of energy and electron transfer processes in a single donor/acceptor system remains largely unexplored.Herein,we demonstrated the energy transfer followed by electron transfer(ETET)process in a molecular dyad TPE-NBD.Due to energy transfer,the fluorescence of TPE-NBD was greatly enhanced in non-polar solvents.In contrast,polar solvents activated subsequent electron transfer and markedly quenched the emission of TPE-NBD.Consequently,ETET endows TPE-NBD with significant polarity sensitivities.We expect that employing ETET could generate many functional materials with unprecedented properties,i.e.,for single laser powered multicolor fluorescence imaging and sensing.展开更多
The upregulation of 4-hydroxyphenylpyruvate dioxygenase(HPPD)can protect plants from adverse abiotic stress.Therefore,studying the changes of HPPD under abiotic stress is extremely valuable.In this study,we employed a...The upregulation of 4-hydroxyphenylpyruvate dioxygenase(HPPD)can protect plants from adverse abiotic stress.Therefore,studying the changes of HPPD under abiotic stress is extremely valuable.In this study,we employed a rational molecular design strategy to prepare an HPPD-responsive fluorescent probe consisting of a pyrene fluorophore,a linker and a benquitrione skeleton recognition moiety that functions via an aggregation–disaggregation sensing mechanism.As predicted,this probe exhibited an obvious turn-on fluorescence response towards HPPD.In addition,in vivo imaging demonstrated the excellent capability of this probe to track HPPD in Arabidopsis thaliana,and the dynamic changes in HPPD were monitored under different stress degrees of high temperature and Cadmium(II)ion(Cd^(2+))stress.This work provides an efficient design strategy for acquiring a noninvasive HPPD fluorescence probe,which could evaluate the degree of stress and be further employed for exploring the stress resistance mechanism in plants.展开更多
Cascading reactions in fluorophores accompanied by the replacement of different fluorescence wavelengths can be used to develop luminescent materials and reactive fluorescent probes.Based on multiple signal channels,t...Cascading reactions in fluorophores accompanied by the replacement of different fluorescence wavelengths can be used to develop luminescent materials and reactive fluorescent probes.Based on multiple signal channels,the selectivity of probes can be improved and the range of response to vip molecule recognition can be expanded.By regulating the position,number,and activity of active sites in fluorophores,fluorescent probes that successively react with thiol and amino groups in cysteine(Cys),homocysteine(Hcy)have been developed,which can only react with the thiol group of GSH,In this paper,we report the first probe capable of cascading nucleophilic substitution reaction with the thiol group and amino group of GSH at a single reaction site,and showed the dual-color recognition of GSH,which improved the selectivity of GSH also was an extension of GSH probes.The probe Rho-DEA was based on a TICS fluorophore,and the intramolecular cascade nucleophilic substitution reaction occurs with Cys/Hcy.The thiol substitution of the first step reaction with Cys/Hcy was quenched due to intersystem crossing to triplet state,so GSH can be selectively recognized from the fluorescence signal.Rho-DEA has the ability of mitochondrial localization,and finally realized in situ dual-color fluorescence recognition of GSH in mitochondria.展开更多
Understanding relationships between molecular structures and fluorescent properties is critical to enable rational deployment of fluorophores. 1-Acetyl pyrene is an important pyrene-derivative, used extensively as an ...Understanding relationships between molecular structures and fluorescent properties is critical to enable rational deployment of fluorophores. 1-Acetyl pyrene is an important pyrene-derivative, used extensively as an environment-sensitive probe. In the past, the fluorescence of 1-acetylpyrene was considered to be polarity-sensitive with a large positive solvatochromism, and its monomer emissions were believed in the range of 410-470 nm. In this paper, our experimental and theoretical studies showed that the monomer fluorescence of 1-acetylpyrene is centered at ～390 nm,which is similar to that of pyrene dyes and not polarity-sensitive. Previously observed "monomer emission" has been re-assigned to that of dimers, which represent the dominant existence form of 1-acetylpyrene in the solution phase,as a result of strong intermolecular π-π stacking interactions.展开更多
The widespread applications of aggregation-induced emission luminogens(AIEgens)inspire the creation of AIEgens with novel structures and functionalities.In this work,we focused on the direct and efficient synthesis of...The widespread applications of aggregation-induced emission luminogens(AIEgens)inspire the creation of AIEgens with novel structures and functionalities.In this work,we focused on the direct and efficient synthesis of a new type of AIEgens,imidazo[1,5-a]pyridicne derivatives,via iodine mediated cascade oxidative Csp^(2)–H or Csp–H amination route from phenylacetylene or styrenes under mild conditions.The resulted compounds showed excellent AIE characteristics with tunable maximum emissions,attractive bioimaging performance,and potential anti-inflammatory activity,which exert broad application prospects in material,biology,medicine,and other relevant areas.展开更多
Salt stress remains a significant challenge for crop growth and food security.The development of effective analytical tools for salt stress-related studies is of great importance.Recently,Yang and Yin et al.have devel...Salt stress remains a significant challenge for crop growth and food security.The development of effective analytical tools for salt stress-related studies is of great importance.Recently,Yang and Yin et al.have developed a novel biosensor that effectively traces salt stress in plants,based on salt-induced molecular J-aggregation and the corresponding changes in fluorescence signals.展开更多
Fluorophores that exhibit superior photostability have vast applications,ranging from long-term in vivo tracking to cellular super-resolution imaging.Herein,we showcased a promising buffering strategy that significant...Fluorophores that exhibit superior photostability have vast applications,ranging from long-term in vivo tracking to cellular super-resolution imaging.Herein,we showcased a promising buffering strategy that significantly enhanced the photostability of the near-infrared(NIR)emissive heptamethine cyanine(Cy7)by simply employing a water-responsive oxazolidine(Ox)switch to cage the Cy7 scaffold.This switch established an equilibrium between nonfluorescent closed form(CF)and fluorescent open form(OF)isomers that effectively compensated for the loss of OF due to photobleaching.Proven effective in both in vitro and in vivo contexts,this strategy markedly improved the durability and utility of Cy7 for sophisticated imaging techniques,including stable NIR tumor imaging in live mice and mitochondrial super-resolution imaging,thereby paving the way for enhanced bioimaging capabilities even under intense laser irradiation.展开更多
Heptamethine cyanine dyes,typified by indocyanine green,have been extensively employed as bioimaging indicators and theranostic agents.Significant efforts have been made to develop functional heptamethine cyanine dyes...Heptamethine cyanine dyes,typified by indocyanine green,have been extensively employed as bioimaging indicators and theranostic agents.Significant efforts have been made to develop functional heptamethine cyanine dyes with outstanding bioimaging and theranostic utilities.In this work,we rationally designed and successfully developed a novel indolium-like heptamethine cyanine dye by installing indolium-derived polycyclic aromatic hydrocarbons on the terminal ends of a conjugated polyene backbone.This dye showed excellent photostability and showed bright fluorescent emission in the second near-infrared(NIR-Ⅱ)window with a peak at approximately 1120 nm.Such long wavelength emission prompted a superior bioimaging resolution in vivo.In particular,this NIR-Ⅱ dye had the remarkable capability of marking the blood vessels of the hindlimbs,abdomens,and brains of mice.More significantly,this dye involved a typical indolium-like heptamethine skeleton and exhibited two strong absorption bands in the 700–1300 nm NIR range,which endowed it with an intrinsic tumor-targeting capability and a high photothermal conversion efficiency(up to 68.2%),serving for the photothermal therapy of tumors under the guidance of NIR-Ⅱ fluorescence imaging.This work provides an efficient design strategy for achieving indolium-like heptamethine cyanine dyes with further NIR-Ⅱ emission.展开更多
Nitric oxide(NO)participates in various pathways and revealing its dynamics is critical for resolving its pathophysiology.While there are methods available for detecting biological NO,few are capable of tracking NO dy...Nitric oxide(NO)participates in various pathways and revealing its dynamics is critical for resolving its pathophysiology.While there are methods available for detecting biological NO,few are capable of tracking NO dynamics.Herein,inspired by the cellular machinery of reversible thiol modification by NO,we have successfully designed a family of cysteine analogues tagged with fluorophores for visualizing cellular NO dynamics.展开更多
The combination of super-resolution microscopy and synthetic fluorescence probes has emerged as a universal tool to monitor dynamic biological events at the nanometer scale.However,the limited site-specificity and flu...The combination of super-resolution microscopy and synthetic fluorescence probes has emerged as a universal tool to monitor dynamic biological events at the nanometer scale.However,the limited site-specificity and fluorogenicity of synthetic fluorescent probes make it still difficult to realize long-term super-resolution imaging.Herein,we introduce a dynamic aggregation mediated SNAP-tag fluorogenic probe,BGAN-Aze,which can specifically bind to various SNAP-tag fusion proteins with 41-fold fluorescence enhancement.The equilibrium between the non-fluorescent aggregate/dimer(A–D)and the fluorescent monomer(M)of BGAN-Aze acts as an effective method to reduce the fluorescence background and endow BGAN-Aze with the capability of conducting washing-free super-resolution imaging of various intracellular and extracellular proteins.Using this probe,we monitored multiple dynamic biological events,such as MMC,mitophagy,the fusion of nucleolus,and the growth and contact of filopodia.We expect that BGAN-Aze will become a widely used SNAP-tag for super-resolution imaging of dynamic biological events and the A-D-M equilibrium can be a general strategy for designing fluorogenic probes.展开更多
Lipid droplets(LDs)are dynamic organelles interacting with a variety of intracellular organelles.Tracking intracellular LD dynamics employing synthetic small molecules is crucial for biological studies.Fluorescence im...Lipid droplets(LDs)are dynamic organelles interacting with a variety of intracellular organelles.Tracking intracellular LD dynamics employing synthetic small molecules is crucial for biological studies.Fluorescence imaging in the red and near infrared(NIR)region is more suitable for biological imaging due to its low phototoxicity and high signal-to-noise ratio.However,available LD-dyes in the red region with remarkable environmental sensitivity,selectivity for LDs staining are limited.Here,we constructed a red-emission D-π-A-π type LDdye LD 688P with higher environmental sensitivity and suitable“calculated log P”(Clog P)for LDs dynamic imaging.LD 688P was proved to be highly selective and photostable for tracing LD fusion including multiple consecutive fusions and fusions in a centrosymmetric manner by super-resolution microscopy.We believe that the D-π-A-π skeleton would be an efficient strategy to construct red and even NIR-emission dyes.展开更多
Photoinduced electron transfer(PET)is a critical process in many functional materials,underpinning various technological applications(i.e.,fluorescent probes and photocatalysts).Despite its signifi-cance,the detailed ...Photoinduced electron transfer(PET)is a critical process in many functional materials,underpinning various technological applications(i.e.,fluorescent probes and photocatalysts).Despite its signifi-cance,the detailed structural dynamics of PET,particularly during the excited state,remain poorly understood.This study investigates the mechanisms of conformational folding and their implications for activating PET in molecular systems characterized by a fluorophore-spacer-receptor configuration.We demonstrate that traditional computational models,primarily based on frontier molecular orbitals,often fall short in capturing these conformational dynamics,leading to inadequate explanations of PET phenomena.With the incorporation of conformational folding,our computational model has achieved excellent agreement with experimental data,thereby resolving several long-standing debates on PET mechanisms.This mechanistic advancement not only deepens our understanding of PET but also opens new avenues for designing advanced functional materials.We have thus successfully demonstrated the imaging of lysosomes in live cells using a PET probe.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22225806,22078314,21908216,22378385)Dalian Institute of Chemical Physics(Nos.DICPI202142,DICPI202436)+1 种基金Agency for Science,Technology and Research(No.A*STAR,Singapore)under its Advanced Manufacturing and Engineering Program(No.A2083c0051)SUTD Kickstarter Initiative(No.SKI 2021_03_10)。
文摘The demand for enhanced optical properties in advanced fluorescence technologies has driven research into the structure-property relationship of fluorophores.In this paper,we use naphthalene fluorophores Na DC-Aze and PhDO-Aze as a case study to emphasize the pivotal role of cross conjugation in tuning the optical structure-property relationship.Na DC-Aze and PhDO-Aze,formed by hybridizing two distinct conjugated systems in a single naphthalene molecule,exhibit spectral characteristics from both conjugated systems.Experimental data and theoretical calculations demonstrate the coexistence of two electron-delocalization systems in a cross-conjugation manner in both Na DC-Aze and PhDO-Aze.The cross-conjugation fluorophores exhibit high brightness,large Stokes shift,and a broad absorption wavelength range by combining distinct spectral properties from its parent fluorophores.These spectral properties will be advantageous for certain applications(i.e.,panchromatic absorption in organic solar cells,and fluorophores compatible with a wide range of excitation wavelengths).
基金the support from the Ministry of EducationSingapore (MOE,No.MOET2EP10120-0007)+4 种基金A^(*)STAR under its Advanced Manufacturing and Engineering Program (No.A2083c0051)the SUTD Kickstarter Initiative (No.SKI 2021_01_01)supported by QMUL Research-IT for computational resources,and the ARCHER UK National Supercomputing Service (No.EP/X035859/1) via the Materials Chemistry Consortiumthe Molecular Modelling Hub for computational resources,MMM Hub,which is partially funded by EPSRC (No.EP/T022213/1)Leverhulme Trust (No.RPG-2019-122) for funding
文摘Cyclooctatetraene(COT)attachment to fluorophores(“self-healing”dyes)is known for quenching reac-tive triplet states via triplet-state energy transfer(TET),enhancing photostability.However,COT’s impact on singlet states remains unclear.Quantum calculations reveal that COT induces energy transfer to dark states in deep blue dyes while promoting photoinduced electron transfer(PET)and intersystem crossing(ISC)in visible dyes,potentially compromising brightness and/or photostability.To address this,we pro-pose the use of △E descriptor to optimize COT’s effects.Our findings uncover COT’s multifaceted impact.These insights will guide the development of superior triplet state quenchers and photostable dyes.
基金supported by Singapore University of Technology and Design(No.T1SRCI17126)A*STAR under its Advanced Manufacturing and Engineering Program(No.A2083c0051)+1 种基金the National Natural Science Foundation of China(Nos.21878286,21908216)Dalian Institute of Chemical Physics(Nos.DMTO201603,TMSR201601)。
文摘Energy transfer and electron transfer are both fundamental mechanisms enabling numerous functional materials and applications.While most materials systems employ either energy transfer or electron transfer,the combined effect of energy and electron transfer processes in a single donor/acceptor system remains largely unexplored.Herein,we demonstrated the energy transfer followed by electron transfer(ETET)process in a molecular dyad TPE-NBD.Due to energy transfer,the fluorescence of TPE-NBD was greatly enhanced in non-polar solvents.In contrast,polar solvents activated subsequent electron transfer and markedly quenched the emission of TPE-NBD.Consequently,ETET endows TPE-NBD with significant polarity sensitivities.We expect that employing ETET could generate many functional materials with unprecedented properties,i.e.,for single laser powered multicolor fluorescence imaging and sensing.
基金supported by the National Key R&D Program of China(No.2021YFD1700103)National Natural Science Foundation of China(21837001,21676113,21772054,22007035)+1 种基金the 111 Project B17019,the Scholar support program of CCNU(0900–31101090002)Hubei Province Natural Science Foundation(No.2020CFB487).
文摘The upregulation of 4-hydroxyphenylpyruvate dioxygenase(HPPD)can protect plants from adverse abiotic stress.Therefore,studying the changes of HPPD under abiotic stress is extremely valuable.In this study,we employed a rational molecular design strategy to prepare an HPPD-responsive fluorescent probe consisting of a pyrene fluorophore,a linker and a benquitrione skeleton recognition moiety that functions via an aggregation–disaggregation sensing mechanism.As predicted,this probe exhibited an obvious turn-on fluorescence response towards HPPD.In addition,in vivo imaging demonstrated the excellent capability of this probe to track HPPD in Arabidopsis thaliana,and the dynamic changes in HPPD were monitored under different stress degrees of high temperature and Cadmium(II)ion(Cd^(2+))stress.This work provides an efficient design strategy for acquiring a noninvasive HPPD fluorescence probe,which could evaluate the degree of stress and be further employed for exploring the stress resistance mechanism in plants.
基金supported by the National Natural Science Foundation of China(Nos.22078314,21878286,21908216)。
文摘Cascading reactions in fluorophores accompanied by the replacement of different fluorescence wavelengths can be used to develop luminescent materials and reactive fluorescent probes.Based on multiple signal channels,the selectivity of probes can be improved and the range of response to vip molecule recognition can be expanded.By regulating the position,number,and activity of active sites in fluorophores,fluorescent probes that successively react with thiol and amino groups in cysteine(Cys),homocysteine(Hcy)have been developed,which can only react with the thiol group of GSH,In this paper,we report the first probe capable of cascading nucleophilic substitution reaction with the thiol group and amino group of GSH at a single reaction site,and showed the dual-color recognition of GSH,which improved the selectivity of GSH also was an extension of GSH probes.The probe Rho-DEA was based on a TICS fluorophore,and the intramolecular cascade nucleophilic substitution reaction occurs with Cys/Hcy.The thiol substitution of the first step reaction with Cys/Hcy was quenched due to intersystem crossing to triplet state,so GSH can be selectively recognized from the fluorescence signal.Rho-DEA has the ability of mitochondrial localization,and finally realized in situ dual-color fluorescence recognition of GSH in mitochondria.
基金financially supported by the National Natural Science Foundation of China(Nos. 21878286, 21502189)DICP (Nos. DMT0201603, TMSR201601)+1 种基金the financial support from Singapore University of Technology and Design (SUTD)the SUTD-MIT International Design Centre (Nos. T1SRCI17126, IDD21700101, IDG31800104)
文摘Understanding relationships between molecular structures and fluorescent properties is critical to enable rational deployment of fluorophores. 1-Acetyl pyrene is an important pyrene-derivative, used extensively as an environment-sensitive probe. In the past, the fluorescence of 1-acetylpyrene was considered to be polarity-sensitive with a large positive solvatochromism, and its monomer emissions were believed in the range of 410-470 nm. In this paper, our experimental and theoretical studies showed that the monomer fluorescence of 1-acetylpyrene is centered at ～390 nm,which is similar to that of pyrene dyes and not polarity-sensitive. Previously observed "monomer emission" has been re-assigned to that of dimers, which represent the dominant existence form of 1-acetylpyrene in the solution phase,as a result of strong intermolecular π-π stacking interactions.
基金financially supported by the National Natural Science Foundation of China(Nos.22077099,21807087and 21673173)Key Research and Development Plan in Shaanxi Province of China(No.2019KWZ-07)+2 种基金the Technology Innovation Leading Program of Shaanxi(No.2020TG-031)the Xi’an CityScience and Technology Project(Nos.2019218214GXRC018CG019-GXYD18.4 and 2020KJRC0115)the support from COVID-19 Prophylaxis and Treatment Emergency Research Special Projects of Northwest University。
文摘The widespread applications of aggregation-induced emission luminogens(AIEgens)inspire the creation of AIEgens with novel structures and functionalities.In this work,we focused on the direct and efficient synthesis of a new type of AIEgens,imidazo[1,5-a]pyridicne derivatives,via iodine mediated cascade oxidative Csp^(2)–H or Csp–H amination route from phenylacetylene or styrenes under mild conditions.The resulted compounds showed excellent AIE characteristics with tunable maximum emissions,attractive bioimaging performance,and potential anti-inflammatory activity,which exert broad application prospects in material,biology,medicine,and other relevant areas.
基金support from A*STAR under its Advanced Manufacturing and Engineering Program(A2083c0051).
文摘Salt stress remains a significant challenge for crop growth and food security.The development of effective analytical tools for salt stress-related studies is of great importance.Recently,Yang and Yin et al.have developed a novel biosensor that effectively traces salt stress in plants,based on salt-induced molecular J-aggregation and the corresponding changes in fluorescence signals.
基金supported by the National Natural Science Foundation of China(grant nos.22225806,22078314,22278394,and 22378385)the Dalian Institute of Chemical Physics,China(grant no.DICPI202142 and DICPI202436)+1 种基金the Ministry of Education,Singapore(grant no.MOE-T2EP10222-0001)Jiangsu Specially Appointed Professorship and the Startup Funding from Nanjing Normal University,China.
文摘Fluorophores that exhibit superior photostability have vast applications,ranging from long-term in vivo tracking to cellular super-resolution imaging.Herein,we showcased a promising buffering strategy that significantly enhanced the photostability of the near-infrared(NIR)emissive heptamethine cyanine(Cy7)by simply employing a water-responsive oxazolidine(Ox)switch to cage the Cy7 scaffold.This switch established an equilibrium between nonfluorescent closed form(CF)and fluorescent open form(OF)isomers that effectively compensated for the loss of OF due to photobleaching.Proven effective in both in vitro and in vivo contexts,this strategy markedly improved the durability and utility of Cy7 for sophisticated imaging techniques,including stable NIR tumor imaging in live mice and mitochondrial super-resolution imaging,thereby paving the way for enhanced bioimaging capabilities even under intense laser irradiation.
基金supported by the National Basic Research Foundation of China(no.2017YFA0505202)financial support from the National Natural Science Foundation of China(nos.21676113 and 21772054)+6 种基金the Distinguished Young Scholar of Hubei Province(no.2018CFA079)the 111 Project B17019the Scholar Support Program of CCNU(no.0900-31101090002)financial support from A*STAR under its Advanced Manufacturing and Engineering Program(no.A2083c0051)the Ministry of Education,Singapore(no.MOE-MOET2EP10120-0007)supported by grants from the 619 National Creative Research Initiative programs of the 620 National Research Foundation of Koreafunded by 621 the Korean government(no.2021R1A6A1A10039823).
文摘Heptamethine cyanine dyes,typified by indocyanine green,have been extensively employed as bioimaging indicators and theranostic agents.Significant efforts have been made to develop functional heptamethine cyanine dyes with outstanding bioimaging and theranostic utilities.In this work,we rationally designed and successfully developed a novel indolium-like heptamethine cyanine dye by installing indolium-derived polycyclic aromatic hydrocarbons on the terminal ends of a conjugated polyene backbone.This dye showed excellent photostability and showed bright fluorescent emission in the second near-infrared(NIR-Ⅱ)window with a peak at approximately 1120 nm.Such long wavelength emission prompted a superior bioimaging resolution in vivo.In particular,this NIR-Ⅱ dye had the remarkable capability of marking the blood vessels of the hindlimbs,abdomens,and brains of mice.More significantly,this dye involved a typical indolium-like heptamethine skeleton and exhibited two strong absorption bands in the 700–1300 nm NIR range,which endowed it with an intrinsic tumor-targeting capability and a high photothermal conversion efficiency(up to 68.2%),serving for the photothermal therapy of tumors under the guidance of NIR-Ⅱ fluorescence imaging.This work provides an efficient design strategy for achieving indolium-like heptamethine cyanine dyes with further NIR-Ⅱ emission.
基金supported by the National Natural Science Foundations of China(nos.22077112,21778048,81673489,31871414,and 81125023)Natural Science Foundation of Zhejiang Province,China(no.LR18H300001)National Science and Technology Major Project“Key New Drug Creation and Manufacturing Program”(nos.2018ZX09711002-010-004,2018ZX09711002-007-002,2019ZX09201001-003-009,2019ZX09201001-003-010,and 2019ZX09201001-004-010),K.C.Wong Education Foundation,and Singapore University of Technology and Design(SUTD)[SUTD-ZJU IDEA grant nos.T1SRCI17126 and SUTD-ZJU(VP)201905].
文摘Nitric oxide(NO)participates in various pathways and revealing its dynamics is critical for resolving its pathophysiology.While there are methods available for detecting biological NO,few are capable of tracking NO dynamics.Herein,inspired by the cellular machinery of reversible thiol modification by NO,we have successfully designed a family of cysteine analogues tagged with fluorophores for visualizing cellular NO dynamics.
基金National Natural Science Foundation of China,Grant/Award Numbers:22078314,21878286,21908216Dalian Institute of Chemical Physics,Grant/Award Numbers:DICPI202142,DICPI201938,DICPZZBS201805+1 种基金Advanced Manufacturing and Engineering Program,Grant/Award Number:A2083c0051Ministry of Education,Singapore,Grant/Award Number:MOE-MOET2EP10120-0007。
文摘The combination of super-resolution microscopy and synthetic fluorescence probes has emerged as a universal tool to monitor dynamic biological events at the nanometer scale.However,the limited site-specificity and fluorogenicity of synthetic fluorescent probes make it still difficult to realize long-term super-resolution imaging.Herein,we introduce a dynamic aggregation mediated SNAP-tag fluorogenic probe,BGAN-Aze,which can specifically bind to various SNAP-tag fusion proteins with 41-fold fluorescence enhancement.The equilibrium between the non-fluorescent aggregate/dimer(A–D)and the fluorescent monomer(M)of BGAN-Aze acts as an effective method to reduce the fluorescence background and endow BGAN-Aze with the capability of conducting washing-free super-resolution imaging of various intracellular and extracellular proteins.Using this probe,we monitored multiple dynamic biological events,such as MMC,mitophagy,the fusion of nucleolus,and the growth and contact of filopodia.We expect that BGAN-Aze will become a widely used SNAP-tag for super-resolution imaging of dynamic biological events and the A-D-M equilibrium can be a general strategy for designing fluorogenic probes.
基金supported by the National Natural Science Foundation of China(22078314,21878286,and 21908216)Dalian Institute of Chemical Physics(DICPI202142,DICPI201938,and DICPZZBS201805)+1 种基金the support from A^(*)STAR under its Advanced Manufacturing and Engineering Program(A2083c0051)the Ministry of Education,Singapore(MOE-MOET2EP10120-0007)
文摘Lipid droplets(LDs)are dynamic organelles interacting with a variety of intracellular organelles.Tracking intracellular LD dynamics employing synthetic small molecules is crucial for biological studies.Fluorescence imaging in the red and near infrared(NIR)region is more suitable for biological imaging due to its low phototoxicity and high signal-to-noise ratio.However,available LD-dyes in the red region with remarkable environmental sensitivity,selectivity for LDs staining are limited.Here,we constructed a red-emission D-π-A-π type LDdye LD 688P with higher environmental sensitivity and suitable“calculated log P”(Clog P)for LDs dynamic imaging.LD 688P was proved to be highly selective and photostable for tracing LD fusion including multiple consecutive fusions and fusions in a centrosymmetric manner by super-resolution microscopy.We believe that the D-π-A-π skeleton would be an efficient strategy to construct red and even NIR-emission dyes.
基金supported by the Ministry of Education,Singapore(MOE-T2EP10222-0001)the Singapore University of Technology and Design(SUTD)Kickstarter Initiative(No.SKI 2021_04_09)+1 种基金the National Natural Science Foundation of China(22225806,22078314,22278394,and 22378385)the Dalian Institute of Chemical Physics(DICPI202142 and DICPI202436).
文摘Photoinduced electron transfer(PET)is a critical process in many functional materials,underpinning various technological applications(i.e.,fluorescent probes and photocatalysts).Despite its signifi-cance,the detailed structural dynamics of PET,particularly during the excited state,remain poorly understood.This study investigates the mechanisms of conformational folding and their implications for activating PET in molecular systems characterized by a fluorophore-spacer-receptor configuration.We demonstrate that traditional computational models,primarily based on frontier molecular orbitals,often fall short in capturing these conformational dynamics,leading to inadequate explanations of PET phenomena.With the incorporation of conformational folding,our computational model has achieved excellent agreement with experimental data,thereby resolving several long-standing debates on PET mechanisms.This mechanistic advancement not only deepens our understanding of PET but also opens new avenues for designing advanced functional materials.We have thus successfully demonstrated the imaging of lysosomes in live cells using a PET probe.
