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Physical Review A

Nonlinear interaction of propagating short pulses in optically dense media

Opher Kinrot, Yehiam Prior

Published Jun 1, 1995• 24 citations
Publisher

Abstract

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 ${\mathit{T}}_{2}$, the apparent decay rate 2/${\mathit{T}}_{\mathit{a}}$ of a time resolved four-wave mixing signal is given by 2/${\mathit{T}}_{\mathit{a}}$=(2/${\mathit{T}}_{2}$)(1+\ensuremath{\alpha}L/2).

DOI
10.1103/physreva.51.4996

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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).
We show that four-wave mixing in optically dense media is very different than in an optically thin medium. In time-resolved degenerate four-wave mixing we experimentally observe ``negative'' time delay response, fast decay rates at short delay times, and broad shoulders at long delays. The observations are explained very well in terms of pulse propagation effects, and a theoretical framework is presented for the analysis of the nonlinear interaction. We treat both the incident and generated fields self-consistently, and solve for the interaction of short pulses with a resonantly absorbing medium. The implications for the extraction of relaxation rates from four-wave-mixing experiments involving ultrashort pulses in optically dense matter are discussed.
We show, both experimentally and theoretically, that short-pulse reshaping clue to propagation leads to the formation of negative-time-delay signals in four-wave mixing (FWM) and to apparent signal decay that is not given by the dephasing or the population-decay rates. Recently, pulse reshaping due to coherent propagation was used to estimate dephasing times in CD, and ZnP·. (Ref. 1), and negative time-delay response in FWM in quantum wells was reported and was explained in terms of higher-order susceptibilities interfering with the third-order FWM process.2
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 shown that the absorbtion of a weak field in a thick resonant absorber is a reversible process even in the case of the homogeneous broadening of the absorption line. As an example, the propagation of a long rectangular pulse with sharp edges in an optically dense resonant medium is studied theoretically in the linear response approximation. Transient nutation (TN), free induction decay (FID), and transients, induced by the phase switch of the incident pulse, are considered. It is shown that in exact resonance the amplitude of FID increases with the length of the medium. FID arises due to the scattered radiation field (dipoles ringing). In a thick medium the scattered field is almost of the same amplitude but opposite in phase with the incident radiation field. Both fields interfere destructively to produce what is seen as radiation damping at the output of the medium. The scattered field needs time to develop. Therefore, the leading edge of the pulse is not absorbed, demonstrating temporal transparency followed by TN. Phase shift (180${}^{\ensuremath{\circ}}$) of the pulse brings the incident pulse in phase with the scattered radiation. Constructive interference of the pulse with the scattered radiation field produces a short pulse with an amplitude that is two times larger than the amplitude of the incident pulse. If the input pulse is detuned from resonance, for a particular detuning and optical thickness of the medium the amplitude of the transient pulse, induced by the phase shift, is nearly three times larger than the amplitude of the incident pulse. This is explained by the interference of the scattered field, the phase-shifted input field, and the slowly propagating part of the pulse, developed before the phase shift.
An investigation of the propagation properties of a short pulse in a resonant absorber with a homogeneously broadened transition is presented with two main questions in mind: 1) the influence of the input pulse area on the transitory regime and on the steady-state propagation; 2) the effects of atomic coherence on the pulse shaping and the time delay of the leading edge of the pulse. The transitory regime of a propagating pulse is investigated and the stability of some asymptotic wave form confirmed. As expected, the transversal relaxation mechanism affects critically the major features of the coherent interaction. A detailed analysis of this problem is also presented.