Theory of femtosecond coherent double-pump single-molecule spectroscopy : application to light harvesting complexes

• المؤلفون الرئيسيون: Chen, Lipeng, Gelin, Maxim F., Domcke, Wolfgang, Zhao, Yang
• مؤلفون آخرون: School of Materials Science & Engineering
• التنسيق: مقال
• اللغة: English
• منشور في: 2015
• الموضوعات: DRNTU::Science::Chemistry::Physical chemistry
• الوصول للمادة أونلاين: https://hdl.handle.net/10356/107369; http://hdl.handle.net/10220/25478
• المؤسسة: Nanyang Technological University

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.