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
Hauptverfasser: Mukamel, Shaul, Rott, Pavel, Chernyak, Vladimir
Format: Artikel
Sprache:eng
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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.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.471781