Optical Stark spectroscopy of molecular aggregates
Effects of static disorder and interaction with phonons on the dynamics of Frenkel excitons in molecular aggregates are studied by calculating the absorption of a weak probe in the presence of a strong resonant and off-resonant pump field. To second order in the pump amplitude, the self-energy which...
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Veröffentlicht in: | The Journal of chemical physics 1996-04, Vol.104 (14), p.5415-5423 |
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Hauptverfasser: | , , |
Format: | Artikel |
Sprache: | eng |
Online-Zugang: | Volltext |
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Zusammenfassung: | Effects of static disorder and interaction with phonons on the dynamics of Frenkel excitons in molecular aggregates are studied by calculating the absorption of a weak probe in the presence of a strong resonant and off-resonant pump field. To second order in the pump amplitude, the self-energy which determines the Stark shift and dynamical broadening of the probe absorption is expressed in terms of the single exciton Green function and the two-exciton scattering matrix. For stronger pump intensities the self-energy is calculated using higher-order optical response functions of the system. |
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ISSN: | 0021-9606 1089-7690 |
DOI: | 10.1063/1.471781 |