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Physical Review A

Transient sum-frequency generation in resonant three-level media

John A. Benda, Daniel J. Gauthier, Robert W. Boyd

Published Dec 1, 1985• 5 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.32.3461

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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.
The perturbative density matrix formalism is used to study the time-dependent resonance Raman scattering (RRS) and resonance hot luminescence (RHL) components of the light-induced spontaneous emission process that has been called resonance secondary radiation (RSR). A three-level system coupled in a stochastic way to a bath is used to study the RSR emission driven by a coherent laser pulse with a variable Gaussian width in time. The spectral filter in a light detection system is explicitly included in the detection step of the problem. Observable time and frequency resolved RSR spectra are then calculated numerically. The spectral and temporal properties of the time-dependent RSR spectrum are very sensitive to the width of the driving pulse when the pulse width is of the same order of magnitude as the important system dephasing constants. In this domain the RRS contribution to the RSR spectrum weakens relative to the RHL as the light pulse is shortened. In the limit that the laser pulse becomes ‘‘delta function-like’’ the RSR spectrum consists essentially of RHL. When appropriate, the numerical results are compared to the stationary RSR problem as well as to the case where the RSR emission is driven by an exponential pulse. The analytical solutions to both of these cases are presented.
The time-dependent theory of the three-step absorption of three different light pulses in the electronic four-level systems is considered using the time-dependent perturbation theory. The first, the second, and the third pulse are in resonance with transitions from level 0 to level 1, from level 1 to level 2, and from level 2 to level 3, respectively. The spectral and temporal behaviour of the probability that the fourth level is excited at the moment of time t depends on the energy relaxation constants of the excited electronic levels, the frequencies of the maxima, the spectral widths (and so the durations) of the light pulses, and the time delays between the pulses. To conclude, there are 12 parameters that affect the spectra in the simple model used. We calculate and analyse the case where the frequencies of the maxima of the first and the second pulse are fixed and the frequency of the maximum of the third pulse varies. On the whole, three lines may exist, one of which corresponds to the coherent contribution and the others do not.
Rate equations for the population dynamics of multilevel systems in laser-induced fluorescence spectroscopy are solved by the aid of perturbation theory. This leads to a general expression for the population of the level pumped by the laser radiation. Arbitrary laser pulse shapes as well as collisional processes are admitted. In the first-order approximation three functions depending on time and the properties of the laser pulse remain. These functions have been tabulated for a bell-shaped laser pulse. The results are used in several characteristic situations and are compared with the numerical solutions of the rate equations.
For the interaction of coherent radiation with a nondegenerate, homogeneously broadened multilevel system the nonlinear susceptibilities and excitations and their time dependence are evaluated using a perturbation approach to the density matrix up to fourth order. This is done for the "off-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\gg}\frac{1}{\ensuremath{\tau}}$, as well as for the "on-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\ll}\frac{1}{\ensuremath{\tau}}$, with $\ensuremath{\tau}$ being the pulse duration, by taking into account the temporal change of the electric field amplitude and the phase and energy relaxation times, T2{T}_{2}T2​ and T1{T}_{1}T1​. It is shown that the transient one-photon excitation known as adiabatic following, is not only important for a pulse duration $\ensuremath{\tau}<{T}_{2}$, but may also be important for ${T}_{2}\ensuremath{\lesssim}\ensuremath{\tau}<{T}_{1}$. In addition, expressions for the transient two-photon excitation in a multilevel system are derived. Finally, the two-level limit is evaluated to all orders of the perturbation including damping effects, which gives results valid also for large incident light intensities. For the "off-resonance" case an expression is obtained which describes not only the transient adiabatic following process, but also the usual one-photon absorption including saturation effects giving rise to power broadening.
A theory is developed of resonant second harmonic generation in a medium consisting of three-level atoms (molecules). Reduced equations for wave propagation are solved without expanding a nonlinear polarization as a series in powers of the field intensities, so that the theory is applicable also to strong resonances. The case of a strong two-photon resonance is investigated and it is shown how the results differ from those obtained using the conventional theory which applies to the nonresonance cases. It is shown that the proposed theory can be generalized to the processes of generation of sum and difference frequencies.