Ultrafast internal conversion and vibrational relaxation in singlet excited-state all-trans-β-carotene as revealed by femtosecond time-resolved stimulated Raman spectroscopy

Zhao Xiao-Hui; Ma Fei; Wu Yi-Shi; Ai Xi-Cheng; Zhang Jian-Ping

doi:10.7498/aps.57.298

Abstract
A femtosecond time-resolved stimulated Raman scattering (FSRS) apparatus was built, and was used to study the ultrafast internal conversion and vibrational relaxation processes between the singlet excited states of all-trans-β-carotene in solution. The FSRS apparatus, constructed on the basis of a three-pulse pump-probe scheme, achieved a time resolution of 150fs, a spectral resolution of 23.7cm-1, and a detection spectral window of 300—4000cm-1. The FSRS results are interpreted in terms of a serial internal-conversion scheme between the low-lying singlet excited states, i.e. S2→SX→S1→S0. Spectral dynamics analysis and kinetics analysis proved that the intra-molecular vibrational relaxation in the S1 state proceeds on a time scale of 0.3—0.6ps, while the ‘hot’ S1 state decays with a time constant similar to the lifetime of this state (～11ps). Furthermore, the time scale of intra-molecular vibrational relaxation and vibrational cooling processes in the S0 state are shown to be ～0.3 and ～15ps, respectively. These results are useful for a deeper insight into the light-harvesting function of carotenoids in photosynthetic organisms.

Keywords:
femtosecond time-resolved Raman spectroscopy /

all-trans-β-carotene /

excited-state internal conversion /

vibrational relaxation
Authors and contacts
Zhao Xiao-Hui¹,

Ma Fei²,

Wu Yi-Shi²,

Ai Xi-Cheng³,

Zhang Jian-Ping²

(1)北京分子科学国家实验室,中国科学院化学研究所分子动态与稳态结构国家重点实验室,北京 100080；河北大学物理科学与技术学院,保定 071002；中国人民大学理学院化学系,北京 100872; (2)北京分子科学国家实验室,中国科学院化学研究所分子动态与稳态结构国家重点实验室,北京 100080；中国人民大学理学院化学系,北京 100872; (3)中国人民大学理学院化学系,北京 100872
References

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Vol. 57, Issue 1 - 2008-01-05

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Ultrafast internal conversion and vibrational relaxation in singlet excited-state all-trans-β-carotene as revealed by femtosecond time-resolved stimulated Raman spectroscopy

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Ultrafast internal conversion and vibrational relaxation in singlet excited-state all-trans-β-carotene as revealed by femtosecond time-resolved stimulated Raman spectroscopy

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