Phase modulation of ultrashort pulses in a saturable absorber under vibronic relaxation conditions

Changes in the modulus and phase of a slowly varying envelope of an ultrashort pulse are calculated for the case of propagation across a saturable absorber. Vibronic relaxation of the optical transition in the absorber is allowed for. A study is made of the dependences of the duration of a pulse transmitted by a nonlinear absorber on the vibrational relaxation time of dye molecules and on the detuning of the carrier frequency of a pulse relative to the maximum of the equilibrium absorption spectrum. It is shown that a chirp appears even in the absence of such detuning provided the energy of lf quanta of optically active vibrations is comparable with the thermal excitation energy. This chirp originates from partial completion of the vibrational relaxation process during a pulse, so that absorption and refraction occur in a system which is not in a vibrational equilibrium.