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Ultrafast Excited State Dynamics of Biliverdin Dimethyl Ester Coordinate with Zinc Ions
Zhuang Chen1, Yang-yi Liu1, Xiao-xiao He*1, Jin-quan Chen*1,2
1.State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200241, China;2.Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan 030006, China
Abstract:
As one of the biological endogenous pigments, biliverdin (BV) and its dimethyl ester (BVE) have extremely weak fluorescence in solution with quantum yield less than 0.01%. However, the situation reverses with the addition of zinc ions. The strength for fluorescence of BVE-Zn2+ complex is greatly enhanced and fluorescence quantum yield can increase to ∽5%. Herein, we studied ultrafast excited state dynamics of BVE-Zn2+ complex in ethanol, n-propanol, and DMSO solutions in order to reveal the mechanism of fluorescence quantum yield enhancement. The results show that BVE can form a stable coordination complex with zinc with 1:1 stoichiometry in solution. BVE is structurally and energetically more stable in the complex. Using picosecond time-resolve fluorescence and femtosecond transient absorption spectroscopy, we show that smaller non-radiative rate constant of BVE-Zn2+ complex in DMSO is the key to increasing its fluorescence quantum yield and the excited state decay mechanism is also revealed. These results provide valuable information about the fluorescence property change after BVE binding to metal ions and may provide a guidance for the study of phytochromes or other fluorescence proteins in which BV/BVE acts as chromophores.
Key words:  Biliverdin, Zinc, Fluorescence, Quantum yield, Femtosecond transient absorption, Excited state dynamics
FundProject:
胆绿素二甲酯金属锌配合物超快激发态动力学研究
陈 壮1, 刘阳依1, 和晓晓*1, 陈缙泉*1,2
1.华东师范大学精密光谱科学与技术国家重点实验室,上海 200241;2.山西大学极端光学协同创新中心,太原 030006
摘要:
胆绿素(BV)及其二甲酯(BVE)是一种生物内源色素,他们在溶液中具有极弱的荧光,量子产率小于0.01%。然而,随着锌离子的加入,情况发生了变化. BVE-Zn2+配合物的荧光强度大大增强,荧光QY可提高到∽5%. 本文研究了BVE-Zn2+络合物在乙醇、正丙醇和二甲基亚砜溶液中的超快激发态动力学,以揭示其荧光增强的机理. 结果表明,BVE能与锌离子在溶液中形成1:1的稳定配合物,BVE分子结构在复合物中较为刚性,能量上更稳定. 利用皮秒时间分辨荧光光谱和飞秒瞬态吸收光谱技术,发现BVE-Zn2+配合物在二甲基亚砜中具有较小的非辐射速率常数,这是其高荧光量子产率关键原因.
关键词:  胆绿素,锌离子,荧光,量子产率,飞秒瞬态吸收,激发态动力学
DOI:10.1063/1674-0068/cjcp1911193
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