Femtosecond Stimulated Raman Spectroscopy of Linear Carotenoids,The Journal of Physical Chemistry Letters

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Femtosecond Stimulated Raman Spectroscopy of Linear Carotenoids
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-07-15 , DOI: 10.1021/acs.jpclett.4c01272
Ivana Šímová ₁ , Petra Chrupková _{1,

2} , Alastair T Gardiner ₃ , Michal Koblížek ₃ , Miroslav Kloz ₂ , Tomáš Polívka ₁

Affiliation

Femtosecond stimulated Raman spectroscopy (FSRS) and transient absorption data measured in a single experiment are used to determine the vibronic properties of the S₁ state of linear carotenoids with different conjugation lengths. The Raman band corresponding to the C═C stretching mode in the S₁ state peaks at 1799 cm^–1 (neurosporene), 1802 cm^–1 (spheroidene), and 1791 cm^–1 (lycopene). Contrary to the ground state C═C mode, variation of the C═C stretching mode in the S₁ state is small and does not follow a linear dependence on N. The lifetime of the Raman band matches the S₁ decays obtained from transient absorption, confirming its S₁ state origin. Direct comparison of transient absorption and FSRS signals allowed us to assign Raman signatures of nonrelaxed S₁ and S₀ states. For lycopene, FSRS data identified a component associated with a downshifted ground state C═C mode, which matches the dynamics of the S* signal observed in transient absorption data.

中文翻译：

线性类胡萝卜素的飞秒受激拉曼光谱

飞秒受激拉曼光谱 (FSRS) 和在单个实验中测量的瞬态吸收数据用于确定具有不同共轭长度的线性类胡萝卜素的 S ₁ 态的振动特性。对应于S ₁态C=C拉伸模式的拉曼谱带峰值位于1799 cm ^–1 （神经孢子烯）、1802 cm ^–1 （球状烯）和1791 cm ^–1 （番茄红素）。与基态C=C模式相反，S ₁态下C=C伸缩模式的变化很小并且不遵循与N的线性相关性。拉曼带的寿命与瞬态吸收获得的S ₁衰变相匹配，证实了其S ₁态起源。瞬态吸收和 FSRS 信号的直接比较使我们能够分配非松弛 S ₁和 S ₀态的拉曼特征。对于番茄红素，FSRS 数据确定了与下移基态 C=C 模式相关的成分，该成分与瞬态吸收数据中观察到的 S* 信号的动态相匹配。

更新日期：2024-07-15

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