Abstract

The multimode Brownian oscillator (MBO) model has been at the forefront in interpreting the subsystem−bath interaction manifestations in optical spectroscopy for probing homogeneous structure of chromophores in crystals and amorphous solids. The spectroscopic consequences of employing the underdamped MBO model with Ohmic dissipation in linear absorption, photon-echo, and hole-burning data of chromophores in solid hosts at low temperatures are investigated. The zero-phonon line (ZPL) in homogeneous linear absorption spectrum, the slow-decay component (due to ZPL) in photon-echo signal, and the zero-phonon hole (ZPH) in hole-burned spectra in host molecular solids at low temperatures are usually resolved from the multiphonon-transitions structure. In the MBO model, the harmonic vibrations (Brownian oscillators) are linearly coupled to bath modes. This coupling, with Ohmic dissipation, results in a maximum contribution of the bath modes to the ZPL region. This contribution affects the width of the ZPL profil...

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