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Laser Physics

Signal dynamics of the photothermal response in three-level media

М. Г. Кучеренко, A. P. Rusinov

Published Aug 30, 2006• 0 citations
Publisher

Abstract

In this paper, we consider the process of optical recording and decay of transient spatial structures in a system with a nonlinear response caused by incoherent saturation of three-level centers. The main attention is devoted to the thermal mechanism of phase recording in media with a temperature-independent heat conductivity. The relaxation of an inhomogeneous temperature field and the diffraction of a probe beam from the transient structure are studied. The designed theoretical model satisfactorily describes the obtained experimental results and allows the evolution of a temperature field to be viewed.

DOI
10.1134/s1054660x06090052

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In this paper, we consider the process of optical recording and decay of transient spatial structures in a system with a nonlinear response caused by incoherent saturation of three-level centers. The main attention is devoted to the thermal mechanism of phase recording in media with a temperature-independent heat conductivity. The relaxation of an inhomogeneous temperature field and the diffraction of a probe beam from the transient structure are studied. The designed theoretical model satisfactorily describes the obtained experimental results and allows the evolution of a temperature field to be viewed.
The increasing interest in the study of the interaction of several resonant fields with multilevel quantum systems is due to a wide range of possible applications of various effects observed in the multi-frequency excitation of quantum objects. Among them, we can note color echo holography, information compression in three-level environments, copying of quantum information, and multi-level quantum gates that perform logical operations. In addition, the recording and reproduction of echo holograms in multi-level systems leads to the possibility, along with logical operations, to perform a change in the real-time scale and the sequence of events in the echo-hologram response, the data on which were embedded into the temporal structure of the object laser pulse. The formation of optical transient processes in multilevel systems occurs when the short laser pulses separated in time and resonant of different frequency transitions at the substance have an effect on the system, so that their interaction with each other becomes possible only through the medium and only if the medium has a sufficiently long phase memory. In this situation, each laser pulse transmits information about its wave characteristics to the medium, and this information is retained here until the arrival of the next laser pulses. The formation of optical transient processes in a multilevel system in a solid depends essentially on the degree of correlation of the inhomogeneous broadening on different frequency transitions and different time intervals, in connection with the possible destruction of the reversible phase memory of the system due to a partial mutual fixation energies of transitions. The influence of external spatially inhomogeneous electric fields on the resonant medium can lead to an additional artificially created inhomogeneous broadening. In this case, it is possible to control the phase memory of the system by changing the parameters of external spatially inhomogeneous electric fields, and the most pronounced effect on phase memory is the case of laser excitation of narrow frequency regions of inhomogeneously broadened lines of the resonance transitions. Moreover, the artificially created inhomogeneous broadening by external spatially inhomogeneous electric fields due to the Stark effect can be comparable with the spread of frequencies due to a partial mutual fixation of the transition energies, which leads to a partial restoration of the coherence of the multilevel system. This effect can lead to an increase in the intensity of the response of the stimulated photon echo (SPE) in the three-level system, which is the opposite effect of photon echo locking.
A systematic theoretical and computational investigation of the microscopic factors which determine the phase of the signal field in time-resolved quasidegenerate three-pulse scattering experiments is presented. The third-order phase-matched response is obtained by density-matrix perturbation theory using a Green-function formalism for a system composed of two well-separated sets of closely spaced energy levels. Equations for calculating the electric field of four-wave-mixing signals generated by path-length delayed pulses are given. It is found that the phase of the signal field is determined by the excitation pulse phases, the dynamics of the nonlinear polarization decay, the product of four transition dipole matrix elements, and by a pulse-delay-dependent phase modulation at the frequency of the first dipole oscillation in the four-wave-mixing process. Analytic results for a two-level Bloch model show the phase shift from rapid nonlinear polarization decay. The product of dipole matrix elements is real and positive for three-level processes (bleached ground-state absorption and excited-state emission), but can be real and negative for some four-level Raman processes. The pulse-delay-dependent phase modulation treated here is closely related to the interferometric pulse-delay-dependent amplitude modulation observed in some collinear experiments, and plays a role in producing photon echos in inhomogeneously broadened samples. Numerical calculations of phase-resolved electric fields for finite duration pulses using a Brownian oscillator model appropriate for condensed-phase dynamics are presented. The ability of pulse-delay-dependent phase modulation to encode the frequency of the initially excited dipole onto the phase of the signal field can be exploited to examine energy-level connectivity, reveal correlations hidden under the inhomogeneous lineshape, and probe relaxation pathways in multilevel systems.
It is demonstrated theoretically and experimentally that, in four-wave phase conjugation of a spatially incoherent speckle signal, the reflection coefficient and the phase conjugation fidelity fall on increase in the rate of change of the spatial structure of the speckle beam. The law of decay of both these parameters is the same for media with an exponential grating erasure rate, but in the case of double-exponential relaxation the conjugated fraction of the signal decreases much more slowly than the reflection coefficient. Experimental results show that the standard model of deep trapping levels can describe the kinetics of formation of dynamic gratings in a nominally pure crystal of strontium barium niobate, but the presence of shallow trapping levels has to be taken into account for doped crystals.