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Journal of the Optical Society of America B

Three-dimensional view of signal propagation in femtosecond four-wave mixing with application to the boxcars geometry

Nadia Belabas, David M. Jonas

Published Mar 1, 2005• 59 citations
Publisher

Abstract

Maxwell's equations for the apparently complicated generation and propagation of femtosecond four-wave-mixing signals in optically thick samples can be solved by triple Fourier transformation into the three-dimensional (3D) frequency domain. Given the linear absorption and refractive-index spectra, the propagation problem can be solved in three dimensions under the assumption that nonlinear distortions of the excitation pulses can be neglected. A propagation function exactly incorporates the linear evolution of the excitation pulses, the nonlinear generation of the signal, and the linear propagation of the signal. A quantitative treatment of the directional filtering of the 3D susceptibility that arises from excitation with noncollinear pulses and selective interference detection of signal in one phase-matched direction is developed. This 3D treatment is used to examine the influence of phase-matching bandwidth, directional filtering, and sample absorption on femtosecond four-wave-mixing signals in the rectangular and square boxcars phase-matching geometries.

DOI
10.1364/josab.22.000655

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Maxwell's equations for the apparently complicated generation and propagation of femtosecond four-wave-mixing signals in optically thick samples can be solved by triple Fourier transformation into the three-dimensional (3D) frequency domain. Given the linear absorption and refractive-index spectra, the propagation problem can be solved in three dimensions under the assumption that nonlinear distortions of the excitation pulses can be neglected. A propagation function exactly incorporates the linear evolution of the excitation pulses, the nonlinear generation of the signal, and the linear propagation of the signal. A quantitative treatment of the directional filtering of the 3D susceptibility that arises from excitation with noncollinear pulses and selective interference detection of signal in one phase-matched direction is developed. This 3D treatment is used to examine the influence of phase-matching bandwidth, directional filtering, and sample absorption on femtosecond four-wave-mixing signals in the rectangular and square boxcars phase-matching geometries.
We study the temporal and spatial evolution of a pump, test, and signal field generated in a four-wave-mixing process for resonant excitation of a nonlinear medium by nanosecond pulses. The propagation effects for the pulses are taken into account beyond the usual mean-field approximation. The model is then applied to a three-level system, describing CuCl at low temperatures. A great deal of new information concerning the temporal and spatial structures of the different fields propagating through the sample is obtained. We show, for instance, that the temporal shapes of the interacting fields are well established after propagation through the first few micrometers of the sample. Beyond this, they propagate with a diminishing amplitude. We also show that these structures are due to the dephasing of the fields throughout their propagation as well as to the temporal evolution of the absorption and generation function of the sample.
The optical density of a resonant medium significantly affects the output signal in time resolved nonlinear optical interactions. The resonant interaction with a medium reshapes any propagating short pulse, and the mutual interaction of several such pulses, as in four-wave mixing, must be treated self-consistently. We present a theoretical framework for the proper handling of the propagation of all pulses, input as well as generated, in the small area limit. For optically thick resonant absorbers, negative time delay signals are observed, and the apparent decay rate of the induced polarization is faster than the rate observed for thin samples. We experimentally measure degenerate four-wave mixing in an atomic medium as an example, and demonstrate the quality of the theoretical model by the excellent fit to measured signals over several orders of magnitude. The improved understanding enables us to provide a simple, but surprisingly accurate, estimate for the apparent decay rate in homogeneously broadened optically thick media: If the absorption is given by \ensuremath{\alpha}, the propagation length is L, and the transverse relaxation time is T2{\mathit{T}}_{2}T2​, the apparent decay rate 2/Ta{\mathit{T}}_{\mathit{a}}Ta​ of a time resolved four-wave mixing signal is given by 2/Ta{\mathit{T}}_{\mathit{a}}Ta​=(2/T2{\mathit{T}}_{2}T2​)(1+\ensuremath{\alpha}L/2).
The four-wave mixing produced with two ultrashort phase-locked w-3w laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5w anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques.
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.
Propagation of single- and two-color hyperbolic secant femtosecond laser pulses in a three-level $\ensuremath{\Lambda}$-type quantum system is investigated by solving the Maxwell and density matrix equations with the finite-difference time-domain and Runge-Kutta methods. As a first study of our modeling, we simulate pulse self-induced transparency (SIT) in two-level systems and see how this phenomenon can be controlled by manipulating the initial relative phase between the SIT pulse and a second control pulse, provided the ratio between both pulse frequencies obeys the relation ${\ensuremath{\omega}}_{1}∕{\ensuremath{\omega}}_{2}=3$. We then examine frequency down-conversion processes that are observed with single- and two-color pulses the envelope area of which is equal to or a multiple of $2\ensuremath{\pi}$, for pulse frequencies close to resonance with the transitions of a three-level $\ensuremath{\Lambda}$ medium. Also, phase-sensitive phenomena are discussed in the case of two-color $\ensuremath{\omega}\text{\ensuremath{-}}3\ensuremath{\omega}$ pulses propagating resonantly in the three-level system. In particular, possibilities for such coherent control are found for frequency down-conversion processes when the ratio of the frequencies of optical transitions is ${\ensuremath{\omega}}_{13}∕{\ensuremath{\omega}}_{12}=3$. The conditions for quantum control of four-wave mixing processes are also examined when the pulse frequencies of two-color $\ensuremath{\omega}\text{\ensuremath{-}}3\ensuremath{\omega}$ pulses are far from any resonance of the three-level system. We demonstrate the possibility to cancel the phase sensitivity of the four-wave coupling in a $\ensuremath{\Lambda}$-type system by competition effects between optical transitions.