The structure-property characteristics of a series of newly synthesized intramolecular charge- transfer (ICT) compounds, single-branch monomer with triphenylmethane as electron donor and 2,1,3-benzothiadiazole as ac...The structure-property characteristics of a series of newly synthesized intramolecular charge- transfer (ICT) compounds, single-branch monomer with triphenylmethane as electron donor and 2,1,3-benzothiadiazole as acceptor, the corresponding two-branch dimer and three- branch trimer, have been investigated by means of steady-state and femtosecond time- resolved stimulated emission fluorescence depletion (FS TR-SEP FD) techniques in different polar solvents. The TD-DFT calculations are further performed to explain the observed ICT properties. The interpretation of the experimental results is based on the comparative studies of the series of compounds which have increased amount of identical branch moiety. The similarity of the absorption and fluorescence spectra as well as strong solvent-dependence of the spectral properties for the three compounds reveal that the excited state of the dimer and trimer are nearly the same with that of the monomer, which may localize on one branch. It is found that polar excited state emerged through multidimensional intramolecular charge transfer from the donating moiety to the acceptor upon excitation, and quickly relaxed to one branch before emission. Even so, the red-shift in the absorption and emission spectra and decreased fluorescence radiative lifetime with respect to their monomer counterpart still suggest some extent delocalization of excited state in the dimer and trimer upon excitation. The similar behavior of their excited ICT state is demonstrated by FS TR-SEP FD measurements, and shows that the trimer has the largest charge-separate extent in all studied three samples. Finally, steady-state excitation anisotropy measurements has further been carried out to estimate the nature of the optical excitation and the mechanism of energy redistribution among the branches, where no plateau through the ICT band suggests the intramolecular excitation transfer process between the branches in dimer and trimer.展开更多
The significant role of telomeres in cells has attracted much attention since they were discovered.Fluorescence imaging is an effective method to study subcellular structures like telomeres.However,the diffraction lim...The significant role of telomeres in cells has attracted much attention since they were discovered.Fluorescence imaging is an effective method to study subcellular structures like telomeres.However,the diffraction limit of traditional optical microscope hampers further investigation on them.Recent progress on superresolution fluorescence microscopy has broken this limit.In this work,we used stimulated emission depletion(STED) microscope to observe fluorescence-labeled telomeres in interphase cell nuclei.The results showed that the size of fluorescent puncta representing telomeres under the STED microscope was much smaller than that under the confocal microscope.Two adjacent telomeres were clearly separated via STED imaging,which could hardly be discriminated by confocal microscopy due to the diffraction limit.We conclude that STED microscope is a more powerful tool that enable us to obtain detailed information about telomeres.展开更多
Stimulated emission depletion(STED) microscope is one of the most prominent super-resolution bio-imaging instruments, which holds great promise for ultrahigh-resolution imaging of cells. To construct a STED microscope...Stimulated emission depletion(STED) microscope is one of the most prominent super-resolution bio-imaging instruments, which holds great promise for ultrahigh-resolution imaging of cells. To construct a STED microscope, it is challenging to realize temporal synchronization between the excitation pulses and the depletion pulses. In this study, we present a simple and low-cost method to achieve pulse synchronization by using a condensed fluorescent dye as a depletion indicator. By using this method, almost all the confocal microscopes can be upgraded to a STED system without losing its original functions. After the pulse synchronization,our STED system achieved sub-100-nm resolution for fluorescent nanospheres and single-cell imaging.展开更多
基金We sincerely thank Prof. Yong-fang Li for providing the samples. S. Vdovi5 thanks CAS for support through a CAS Research Fellowship for International Young Researchers. This work was supported by National Natural Science Foundation of China, the Chinese Academy of Sciences, and the State Key Project for Fundamental Research.
文摘The structure-property characteristics of a series of newly synthesized intramolecular charge- transfer (ICT) compounds, single-branch monomer with triphenylmethane as electron donor and 2,1,3-benzothiadiazole as acceptor, the corresponding two-branch dimer and three- branch trimer, have been investigated by means of steady-state and femtosecond time- resolved stimulated emission fluorescence depletion (FS TR-SEP FD) techniques in different polar solvents. The TD-DFT calculations are further performed to explain the observed ICT properties. The interpretation of the experimental results is based on the comparative studies of the series of compounds which have increased amount of identical branch moiety. The similarity of the absorption and fluorescence spectra as well as strong solvent-dependence of the spectral properties for the three compounds reveal that the excited state of the dimer and trimer are nearly the same with that of the monomer, which may localize on one branch. It is found that polar excited state emerged through multidimensional intramolecular charge transfer from the donating moiety to the acceptor upon excitation, and quickly relaxed to one branch before emission. Even so, the red-shift in the absorption and emission spectra and decreased fluorescence radiative lifetime with respect to their monomer counterpart still suggest some extent delocalization of excited state in the dimer and trimer upon excitation. The similar behavior of their excited ICT state is demonstrated by FS TR-SEP FD measurements, and shows that the trimer has the largest charge-separate extent in all studied three samples. Finally, steady-state excitation anisotropy measurements has further been carried out to estimate the nature of the optical excitation and the mechanism of energy redistribution among the branches, where no plateau through the ICT band suggests the intramolecular excitation transfer process between the branches in dimer and trimer.
基金supported by the National Natural Science Foundation of China(61378062,21227804,21390414,61475181)the National Basic ResearchProgram of China(2012CB825805)the Shanghai Municipal Commission for Science and Technology(14ZR1448000)
文摘The significant role of telomeres in cells has attracted much attention since they were discovered.Fluorescence imaging is an effective method to study subcellular structures like telomeres.However,the diffraction limit of traditional optical microscope hampers further investigation on them.Recent progress on superresolution fluorescence microscopy has broken this limit.In this work,we used stimulated emission depletion(STED) microscope to observe fluorescence-labeled telomeres in interphase cell nuclei.The results showed that the size of fluorescent puncta representing telomeres under the STED microscope was much smaller than that under the confocal microscope.Two adjacent telomeres were clearly separated via STED imaging,which could hardly be discriminated by confocal microscopy due to the diffraction limit.We conclude that STED microscope is a more powerful tool that enable us to obtain detailed information about telomeres.
基金supported by the National Natural Science Foundation of China (21227804, 21390414, 61378062, 21505148)National Key Research and Development Program (2016YFA0400902)the Natural Science Foundation of Shanghai (15ZR1448400, 14ZR1448000)
文摘Stimulated emission depletion(STED) microscope is one of the most prominent super-resolution bio-imaging instruments, which holds great promise for ultrahigh-resolution imaging of cells. To construct a STED microscope, it is challenging to realize temporal synchronization between the excitation pulses and the depletion pulses. In this study, we present a simple and low-cost method to achieve pulse synchronization by using a condensed fluorescent dye as a depletion indicator. By using this method, almost all the confocal microscopes can be upgraded to a STED system without losing its original functions. After the pulse synchronization,our STED system achieved sub-100-nm resolution for fluorescent nanospheres and single-cell imaging.