Theory of femtosecond coherent double-pump single-molecule spectroscopy : application to light harvesting complexes
We develop a first principles theoretical description of femtosecond double-pump single-molecule signals of molecular aggregates. We incorporate all singly-excited electronic states and vibrational modes with significant electron-vibrational coupling into a system Hamiltonian and treat the ensuing s...
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| Main Authors: | , , , |
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| 其他作者: | |
| 格式: | Article |
| 語言: | English |
| 出版: |
2015
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| 主題: | |
| 在線閱讀: | https://hdl.handle.net/10356/107369 http://hdl.handle.net/10220/25478 |
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| 機構: | Nanyang Technological University |
| 語言: | English |
| 總結: | We develop a first principles theoretical description of femtosecond double-pump single-molecule signals of molecular aggregates. We incorporate all singly-excited electronic states and vibrational modes with significant electron-vibrational coupling into a system Hamiltonian and treat the ensuing system dynamics within the Davydov D1 Ansatz. The remaining intra- and inter-molecular vibrational modes are treated as a heat bath and their effect is accounted for through lineshape functions. We apply our theory to simulate single-molecule signals of the light harvesting complex II. The calculated signals exhibit pronounced oscillations of mixed electron-vibrational (vibronic) origin. Their period decreases with decreasing electron-vibrational couplings. |
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