Master Equation Calculations of the Multiphoton Absorption Process of CDF3

BEATRIZ M. TOSELLI; JUAN CARLOS FERRERO; STARICCO EDUARDO

AMER CHEMICAL SOC

Año: 1985 p. 1982 - 1982

he applicability of the master equation formulation to small molecules was explored by using the available data on CDF3.A good reproduction of the experimental dependence of the absorption cross section and reaction probabilities on fluencewas obtained in a broad range of fluences. Calculations show that only a fraction of the total population is able to absorbthe laser radiation. This fraction also varies with the intensity, according to the Rabi frequency. The anharmonicity ofthe pumped vibrational mode had to be considered to explain the increase in uL with fluences higher than 2 J/cm2. Thesimple master equation, without fractionation and anharmonicity, reproduces well the behavior of CDF, with added Ar,which is interpreted as a total rotational relaxation during the pulse, but is unable to explain simultaneously the dependenceof the laser absorption cross section and reaction probabilities with fluence under collisionless conditions.