We develop an analytical approach to the dynamics of band populations of reverse saturable absorbers modeled by the three-level approximation of the five-level rate equations. We find high-accuracy approximate solutions to these rate equations, taking into account the temporal shape of the incident laser pulse for different regimes of excitation. The results obtained are confirmed by direct numerical integration of the rate equations and are verified by solution of the full system of the rate and the propagation equations. The validity ranges of the approximations are determined. We also prove that for input pulses that are much longer than the lifetime of the first excited state the ground-state depletion obeys the same functional dependence on the input fluence as in the case of rectangular input pulses. The dynamics of the excited states, however, explicitly depends on the pulse shape. We quantitatively estimate the effect of various parameters on the nonlinear absorption coefficient and discuss implementation of the approach by a beam propagation method to reduce the computational time.
Resonantly enhanced sum-frequency generation of pulsed laser radiation is treated theoretically for the case of a three-level system. The density-matrix equations of motion are solved using second-order, time-dependent perturbation theory with the inclusion of transient effects. The energy and spectrum of the generated radiation are calculated as functions of laser detunings, laser pulse lengths, and temporal overlap of the laser pulses. The tuning characteristics and output pulse characteristics are found to differ qualitatively depending on whether or not the excitation pulses satisfy the adiabatic following criteria generalized for the case of a three-level atom.
To search after for the dependence of the emission fluorescence on the excitation rate and the spontaneous-radiation rate, the rate equation of the upper level population for two-level system was derived and it was solved on certain. conditions. The variation regularities of the aforementioned population and the photon-number of the emission fluorescence were presented. The fluorescence photon-number is proportional to the excitation rate while the spontaneous-radiation rate has an optimum decided by a trigonometric equation.
The excitation of a two-level system by a chirped laser pulse is analyzed using an analytical approach (in the perturbation-theory limit) that involves the modified rotating-wave approximation and the numerical solution to the Bloch equation. The dependence of the population of the upper energy level on the chirp is studied for various radiation intensities and pulse durations. An exact solution is compared with the result obtained using the modified rotating-wave approximation and the perturbation theory. It is demonstrated that, for a certain range of parameters, the excitation probability of a two-level system can be effectively controlled via a variation in the chirp.
We present a formalism to analyze the effects of collisions and intramolecular energy transfer and dephasing processes (
T1 and
T2 relaxation) on level-population dynamics and unimolecular decay of laser-driven gas molecules. Utilizing a Boltzmann or optical Bloch equation for the density matrix to describe laser excitation of a relaxing multilevel absorber, we develop a generalized master equation (GME) to describe the dynamics of level population evolution for multilevel absorbers having arbitrary numbers of quantum levels
N. Because the resulting level-population equations explicitly retain phase memory, the effect of complete or partial phase-coherent driving or incoherent driving by the laser field are all included within the GME solutions. The formalism provides straightforward means to calculate time-dependent solutions for arbitrary
N, where a single expression is valid on transient, post transient, approach to steady state, and steady-state time scales. We illustrate the behavior of these solutions for the special case of three- and eight-level systems, but the method is not restricted with regard to number of levels. In both this and the following paper, we use specific examples and general arguments to show that an ordinary master equation (OME) is invalid even under apparently favorable conditions including saturating field strengths. We demonstrate that, for an
N-level absorber with given coupling elements, there are
2N [or
2(N+1)] independent saturation solutions and that special conditions on the relaxation times are required to produce the ordinary equal-population solution. Explicit forms for the steady-state radiative-transition matrix $W(\ensuremath{\lambda}=0)$ are derived for arbitrary
N, and general arguments are given to show that the correct description of the dynamics given by the GME results from matrix singularities in $W(\ensuremath{\lambda}=0)$ which can never occur in an OME or similar rate equations.