Journal of the Optical Society of America B
Resonant inhomogeneous molecular absorption of ultrashort laser pulses: role of the pulse spectrum
Pritish Mukherjee, Hoi Sing Kwok
Abstract
A model molecular system composed of an inhomogeneous distribution of homogeneous wave packets is presented in analogy with gain saturation in atomic systems. The numerically computed optical free-induction-decay pulse spectrum (as a representative picosecond-pulsed laser system) and other idealized pulse spectra are used as inputs to the molecular system to probe its absorption characteristics in the inhomogeneous limit. Various aspects of pulse spectral structure and their relative significance to the observed nonlinearity of the numerically computed 1/σ2-versus-I plot is discussed in detail. The relevance of such behavior in interpreting experimental data is also indicated.