Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Optics Letters

Fourier algorithm for four-wave-mixing signals from optically dense systems with memory

Nadia Belabas, David M. Jonas

Published Aug 1, 2004• 17 citations
Publisher

Abstract

A triple Fourier-transform algorithm for generating and propagating femtosecond four-wave-mixing signals in optically thick samples is demonstrated. The algorithm has a dynamic range that is useful for tests of theory and simulations of experiments with an arbitrary nonlinear response. Although two-pulse echoes decay faster as optical density increases for a Bloch model, we find that systems with memory exhibit the opposite trend.

DOI
10.1364/ol.29.001811

Related papers

Nonlinear interaction of propagating short pulses in optically dense media

Opher Kinrot, Yehiam Prior

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).

Physical Review A•Jun 1, 1995•24 citations

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

Nadia Belabas, David M. Jonas

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.

Journal of the Optical Society of America B•Mar 1, 2005•59 citations

Four-wave mixing in optically dense media

Opher Kinrot, Yehiam Prior

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.

Physical Review A•Sep 1, 1994•27 citations

Dynamics of triple quantum beats retrieved from coupled four-wave mixing signals

Changjun Zhu, Bei Xu, Qing Chu +2 more

A theoretical model of coupled four-wave mixing (FWM) processes comprising five atomic energy levels was proposed to investigate the coherent characteristics of atomic wave packets using perturbation theory. As several states in atoms are coherently excited by a two-photon transition, triple coupled FWM can be produced, and triple quantum beats associated with the atomic energy levels are embedded in the FWM signals. Triple coupled FWM processes were achieved experimentally in Rb vapor by two-photon excitation using broadband optical pulses. A pump–probe scheme was utilized to record the time-varying FWM signals, and Fourier transform was applied to retrieve the quantum beats. Furthermore, short-time Fourier transform was implemented to investigate the dynamics of quantum beats. The results show that the coherent characteristics of atomic wave packets, which are intimately related to the dynamics of quantum beats, can be probed by coupled nonlinear optical wave mixing.

Journal of the Optical Society of America B•Feb 25, 2016•0 citations

FWM in optically dense medía

Opher Kinrol, Yehiam Prior

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

•May 8, 1994•0 citations

Phase-resolved time-domain nonlinear optical signals

Sarah M. Gallagher Faeder, David M. Jonas

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.

Physical Review A•Aug 18, 2000•41 citations
A triple Fourier-transform algorithm for generating and propagating femtosecond four-wave-mixing signals in optically thick samples is demonstrated. The algorithm has a dynamic range that is useful for tests of theory and simulations of experiments with an arbitrary nonlinear response. Although two-pulse echoes decay faster as optical density increases for a Bloch model, we find that systems with memory exhibit the opposite trend.
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).
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 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.
A theoretical model of coupled four-wave mixing (FWM) processes comprising five atomic energy levels was proposed to investigate the coherent characteristics of atomic wave packets using perturbation theory. As several states in atoms are coherently excited by a two-photon transition, triple coupled FWM can be produced, and triple quantum beats associated with the atomic energy levels are embedded in the FWM signals. Triple coupled FWM processes were achieved experimentally in Rb vapor by two-photon excitation using broadband optical pulses. A pump–probe scheme was utilized to record the time-varying FWM signals, and Fourier transform was applied to retrieve the quantum beats. Furthermore, short-time Fourier transform was implemented to investigate the dynamics of quantum beats. The results show that the coherent characteristics of atomic wave packets, which are intimately related to the dynamics of quantum beats, can be probed by coupled nonlinear optical wave mixing.
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.