Journal of Chemical Physics, Vol.104, No.14, 5415-5423, 1996
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 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.