Femtosecond time-resolved fluorescence depletion spectroscopy was used in the study of the orientation relaxation of Rhodamine 700(LD700) and Oxazine 750(OX750) in DMSO. The anisotropy functions of the dye molecules w...Femtosecond time-resolved fluorescence depletion spectroscopy was used in the study of the orientation relaxation of Rhodamine 700(LD700) and Oxazine 750(OX750) in DMSO. The anisotropy functions of the dye molecules were obtained from the fluorescence depletion spectra, as the polarization of probe pulse is parallel and perpendicular respectively. The results show that the transition dipole moment of the pump and the probe of LD700 and OX750 are parallel. The time constants of the orientation relaxation of these dye molecules in DMSO are 1.8 and 1.9 ps for LD700 and OX750, respectively.展开更多
The internal conversion （IC） processes of chlorophyll a （chl-a） in solvents are studied based on the reduced density matrix theory. The IC times can be obtained by simulating the experimental fluorescence depletio...The internal conversion （IC） processes of chlorophyll a （chl-a） in solvents are studied based on the reduced density matrix theory. The IC times can be obtained by simulating the experimental fluorescence depletion spectra （FDS）. The calculated IC times of chl-a in ethyl acetate, tetrahydrofuran and dimethyl formamide are 141, 147, and 241 fs, respectively. The oscillation feature of the FDS results from the forward and backward transfer of the population between coupled electronic states. The effects of diabatic coupling between two electronic states on the IC time and the FDS are described. The influence of molecule-reservoir coupling on the IC time is also investigated.展开更多
文摘Femtosecond time-resolved fluorescence depletion spectroscopy was used in the study of the orientation relaxation of Rhodamine 700(LD700) and Oxazine 750(OX750) in DMSO. The anisotropy functions of the dye molecules were obtained from the fluorescence depletion spectra, as the polarization of probe pulse is parallel and perpendicular respectively. The results show that the transition dipole moment of the pump and the probe of LD700 and OX750 are parallel. The time constants of the orientation relaxation of these dye molecules in DMSO are 1.8 and 1.9 ps for LD700 and OX750, respectively.
基金We would like to thank Dr. Y. Shi and Professor K. L. Han for providing the FDS data and useful discussions. K. Niu is grateful to Professor V. May for enlightening suggestions. This work was supported by the National Natural Science Foundation of China （No. 10674022 and No.20633070）.
文摘The internal conversion （IC） processes of chlorophyll a （chl-a） in solvents are studied based on the reduced density matrix theory. The IC times can be obtained by simulating the experimental fluorescence depletion spectra （FDS）. The calculated IC times of chl-a in ethyl acetate, tetrahydrofuran and dimethyl formamide are 141, 147, and 241 fs, respectively. The oscillation feature of the FDS results from the forward and backward transfer of the population between coupled electronic states. The effects of diabatic coupling between two electronic states on the IC time and the FDS are described. The influence of molecule-reservoir coupling on the IC time is also investigated.
