Abstract
The rate of absorption and emission of radiation is calculated for two laser fields interacting with a homogeneously broadened, three-level molecular system. The time-dependent Schrodinger equation is used in the density matrix formalism and the laser fields are treated classically. The laser fields, at frequencies ω p and ω s , are off resonance by δ p and δ s , respectively, such that |\delta_{p}|, |\delta_{s}| \ll \omega_{p}, \omega_{s} . Analytic expressions are derived for the imaginary part of the electric susceptibility, \chi(\omega_{p}) and \chi(\omega_{s}) . The present work differs from previous calculations in that the laser fields may have arbitrary values of field strength and each field may be on or off resonance. A discussion is presented of the properties of the solutions for \chi(\omega_{p}) and \chi(\omega_{s}) , for both strong and weak laser fields, based on computer evaluation of the general analytic expressions. It is shown that the solutions may be divided into single-photon and two-photon, or Raman, contributions. Conditions for optimizing dI(\omega_{s})/dz and the photon conversion efficiency are derived. These results may be applied to analyzing the pulsed, optically pumped submillimeter laser and to studying two-photon absorption in a gas.
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