Pump-probe and pump-deplete-probe spectroscopies on carotenoids with N=9-15 conjugated bonds
Pump-probe and pump-deplete-probe spectroscopies on carotenoids with N=9-15 conjugated bonds
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DOI：
10.1063/1.2388274
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发表时间：
2006-11-21
影响因子：
4.4
通讯作者：
Motzkus, Marcus
中科院分区：
文献类型：
--
作者：
Buckup, Tiago;Savolainen, Janne;Motzkus, Marcus
用抽运-探测和抽运-耗尽-探测光谱研究了一系列N=9，13和15共轭键的全反式类胡萝卜素，系统地分析了不同电子态之间的能量流动。类胡萝卜素中的超快动力学通过激发到S-2状态来初始化，随后通过在近红外光谱范围内的额外耗尽脉冲来操纵。激发态粒子数耗尽后的动力学变化使得激发态吸收分为两个分量，一个主要的分量对应于众所周知的S-1态，另一个小的分量对S-0-S-2吸收带的红翼有贡献，该吸收带来自热基态。我们没有发现额外的电子激发态的证据，通常称为S-*。相反，一个失活机制，包括热基态支持观察到的结果很好地在一个简单的三态模型（S-2，S-1和S-0）的框架。(c)2006年，美国物理学会。
A series of all-trans-carotenoids with N=9, 13, and 15 conjugated bonds has been studied by pump-probe and pump-deplete-probe spectroscopies to obtain a systematic analysis of the energy flow between the different electronic states. The ultrafast dynamics in the carotenoids are initialized by excitation to the S-2 state and subsequently manipulated by an additional depletion pulse in the near-IR spectral range. The changes in the dynamics after depletion of the excited state population allowed differentiation of the excited state absorption into two components, a major one corresponding to the well known S-1 state and the small contribution on the red wing of the S-0-S-2 absorption band originating from the hot ground state. We found no evidence for an additional electronically excited state, usually called S-*. Instead, a deactivation mechanism that includes the hot ground state supports the observed results nicely in the framework of a simple three state model (S-2, S-1, and S-0). (c) 2006 American Institute of Physics.