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

Journal of Physics Conference Series

On the non-linear spectroscopy including saturated absorption and four-wave mixing in two and multi-level atoms: a computational study

M Patel, Gerhard De Jager, Z Nkosi, A.T. Wyngaard, Kessie Govender

Published Oct 1, 2017• 0 citations
Publisher

Abstract

In this paper we report on the study of two and multi-level atoms interacting with multiple laser beams. The semi-classical approach is used to describe the system in which the atoms are treated quantum mechanically via the density matrix operator, while the laser beams are treated classically using Maxwells equations. We present results of a two level atom interacting with single and multiple laser beams and demonstrate Rabi oscillations between the levels. The effects of laser modulation on the dynamics of the atom (atomic populations and coherences) are examined by solving the optical Bloch equations. Plots of the density matrix elements as a function of time are presented for various parameters such as laser intensity, detuning, modulation etc. In addition, phase-space plots and Fourier analysis of the density matrix elements are provided. The atomic polarization, estimated from the coherence terms of the density matrix elements, is used in the numerical solution of Maxwells equations to determine the behaviour of the laser beams as they propagate through the atomic ensemble. The effects of saturation and hole-burning are demonstrated in the case of two counter propagating beams with one being a strong beam and the other being very weak. The above work is extended to include four-wave mixing in four level atoms in a diamond configuration. Two co-propagating beams of different wavelengths drive the atoms from a ground state |1〉 to an excited state |3〉 via an intermediate state |2〉. The atoms then move back to the ground state via another intermediate state |4〉, resulting in the generation of two additional correlated photon beams. The characteristics of these additional photons are studied.

DOI
10.1088/1742-6596/905/1/012005

Related papers

Optical hole-burnings and slow light in atoms vapors with laser interaction

李东康 Li Dongkang, 刘玉娟 Liu Yujuan

Five coherent hole-burning can be simultaneously observed in the absorption spectra of four-level N-style atoms vapors. In this system they adopt a saturated laser co-propagates and two coupling lasers counter-propagate with a probe laser, and the saturated laser can not be in the destructive Doppler state with the probe light. The positions of the coherent hole-burning can be explained by Dressed-state theory. The middle narrow deep hole-burning is induced by the superposition of two coherent hole-burnings. The depth of the coherent hole-burning can be changed by adjusting the reference parameters and the Rabi frequency of the saturated laser. The positions of the coherent hole-burning can be changed by modulating the Rabi frequency of the probe light. By numerical simulation it is found that Rabi frequency of the saturated light plays an important role in slowing the propagating speed. These results may be useful in optical quantum memory and optical quantum information.

Infrared and Laser Engineering•Jan 1, 2016•0 citations

Resonant multiwave-mixing spectra of gas-phase sodium: Nonperturbative calculations

Robert P. Lucht, Rick P. Trebino, Larry A. Rahn

We perform nonperturbative calculations of resonant multiwave mixing of two high-intensity laser beams of different frequencies both for a general three-level system and for the 3 $^{2}$${\mathit{S}}_{1/2}$--3 $^{2}$${\mathit{P}}_{1/2}$ electronic resonance of the sodium atom. Our calculations proceed by direct numerical integration of the density-matrix equations and subsequent Fourier analysis of the calculated time-dependent density-matrix elements. We examine the case where two nearly degenerate input beams are each detuned many collisional linewidths from electronic resonance, and the frequency difference between the input beams is tuned through a ground-state resonance. Unlike previous high-intensity analyses, each input beam can be resonant with numerous transitions simultaneously; for a three-level system, we refer to this as an ``M-type'' system, in analogy with \ensuremath{\Lambda}- and V-type systems. Calculated four-, six-, and eight-wave-mixing spectra exhibit subharmonic resonances of the type observed experimentally by Trebino and Rahn [Opt. Lett. 12, 912 (1987)]. The three-level system is studied to gain insight into the physics of these subharmonic resonances. For more quantitative comparison with experiment, we use a model that includes the 16 Zeeman and hyperfine states in the 3 $^{2}$${\mathit{S}}_{1/2}$ and the 3 $^{2}$${\mathit{P}}_{1/2}$ levels, and accounts for arbitrary linear polarization of the input laser radiation. The relative intensities of the resonance features in the calculated multiwave-mixing spectra show good agreement with experiment. These resonance features broaden and shift as laser intensity increases, as predicted for four-wave-mixing processes in previous, less general high-intensity analyses. Both theory and experiment also show additional resonant features in the eight-wave-mixing spectra that appear at very high intensity.

Physical Review A•Jun 1, 1992•23 citations

Limits on the atomic description of four-wave mixing

Irvin F. Ángeles-Aguillón, Nieves Arias-Téllez, Pablo Yanes-Thomas +2 more

The limits of the well-established single-atom model for describing photon-pair generation via four-wave mixing in a diamond configuration in atomic ensembles are experimentally tested. Using a cold-atom source, biphotons are generated and detected through polarization analyzers that resolve the emitted light into horizontal and vertical components in the laboratory frame. The pump lasers driving the first and second excitation transitions are horizontally and vertically polarized, respectively. To predict single-photon counts and coincidence rates in all polarization channels, the first- and second-order correlation functions are calculated directly using a comprehensive model that accounts for all Zeeman sublevels of the relevant hyperfine states. Furthermore, the population dynamics with and without the re-pump laser of the magneto-optical trap are compared, revealing substantial differences in the populations of the Zeeman sublevels. This motivates the inclusion of two additional hyperfine levels and their corresponding Zeeman sublevels in the final model. The resulting density matrix is used to calculate expectation values of the far-field electric-field operators and compare them with experimental measurements over a range of pump-laser powers. Excellent agreement with the measured photon counts is obtained over most of this range. For the coincidence measurements, good agreement is found when the polarization of the photon generated by the first (second) decay is parallel to that of the first (second) pump beam. In contrast, the model consistently underestimates the experimental coincidence rates for the opposite polarization configuration. These findings indicate that effects beyond the internal level dynamics of individual atoms, most notably collective phenomena, are required to fully account for photon coincidences generated by four-wave mixing in atomic ensembles.

quant-pharXiv:2609.15843•Sep 15, 2026•0 citations

Coherent Interactions of Fields with Atoms

Stephen Colby Rand

Chapter 5 begins the systematic application of the density matrix to describe optical interactions. Stationary two-and three-level atoms interacting with a traveling wave are compared to show that the presence of additional levels changes the saturation behavior of atoms. Then motion of the atoms is introduced and the phenomena of spatial and frequency-domain hole-burning are analyzed. Special effects due to standing waves, such as the light shift, are covered in this section. Next, tri-level coherence is considered, to extend the concept of coherences to two-photon transitions or Zeeman interactions in folded 3- or Λ-systems. Higher order interactions are also analyzed. This includes four-wave mixing and pump–probe techniques which form the basis of common nonlinear laser spectroscopies. Quantum interference is covered as a prelude to the topic of electromagnetically induced transparency. Higher order coherent interactions are also treated using a diagrammatic calculation technique based on Feynman diagrams.

Oxford University Press eBooks•Jun 9, 2016•0 citations

Collective coupling of driven multilevel atoms and its effect on four-wave mixing

P. Yanes-Thomas, R. Gutiérrez-Jáuregui, Pablo Barberis-Blostein +3 more

Microscopic models based on multilevel atoms are central to optimizing nonlinear optical responses and the coherent control of light. These models are traditionally based on single-atom effects that are parametrically extrapolated to include collective effects, such as an enhanced response or propagation within atomic media. In this work, we present a systematic analysis of the cooperative effects arising in driven systems composed of multilevel atoms coupled via a common electromagnetic environment. The analysis is based on an interplay between dressed states induced by the driving field and photon exchanges, and collective decay channels. This theory is applied to the case of four-wave mixing induced by a pair of lasers acting on an atomic pair with internal levels in the diamond configuration. The effect of interatomic correlations and collective decay over the photons created in this nonlinear process is then explored. We identify three regions of operation: (i) laser-dominated, (ii) intermediate, and (iii) dipole-dominated. The dependence of single- and two-photon correlations is studied in detail for each region by varying atomic orientations and laser parameters consistent with current experiments involving atomic gases. Photonic correlation functions are shown to exhibit a transition from a Lorentz-like dependence on the two-photon detuning—with general features that can be obtained in an isolated atom scheme—to a two-peaked distribution when the dipole-dipole interactions become relevant. For weak Rabi frequencies whose value is smaller than the highest collective decay rate, the atoms are trapped inside their ground state as they approach each other. It is found that the anisotropy of the dipole-dipole interaction and its wave nature are essential to understand the behavior of the photon correlations. Signatures of these processes are identified for existing experimental realizations. The intuition obtained from this connection helps to uncover relevant parameters that could be exploited for quantum control protocols based on dispersive and dissipative cooperative effects in multilevel systems.

arXiv:2404.03615•Physical Review Research•Jan 8, 2025•3 citations

Resonant degenerate four-wave mixing spectroscopy of transitions with degenerate energy levels: Saturation and polarization effects

Thomas A. Reichardt, Robert P. Lucht

The physics of the degenerate four-wave mixing process for resonant transitions between two degenerate energy levels is investigated by direct numerical integration of the time-dependent density matrix equations. The Zeeman structure of the upper and lower energy levels is included in a multistate formulation of the density matrix equations. The inclusion of the Zeeman structure enables the investigation of the degenerate four-wave mixing process for different polarization configurations of the forward pump, backward pump, and probe beams. Saturation curves and lineshapes are calculated for different polarization configurations and for numerous low-J transitions. At low laser intensity, the results of our calculations are in excellent agreement with perturbation theory in terms of the relative intensities of the degenerate four-wave mixing signal for linear polarization configurations. As the laser intensity increases and the resonance starts to saturate, we find in general that the relative degenerate four-wave mixing reflectivity increases for the crossed polarization configurations compared to the parallel polarization configuration because the saturation intensity is higher. However, for some resonance transitions, some of the crossed polarization configurations saturate at lower laser intensities than the parallel polarization configuration, even though the reflectivity for these crossed polarization configurations is much lower than for the parallel polarization configuration in the perturbative intensity limit. This result is explained in terms of the coupling of the various Zeeman states during the degenerate four-wave mixing interaction for specific polarization configurations. The effect of saturation on the resonance line shapes for the different polarization configurations is also investigated. Finally, a limited number of calculations are performed for resonances that are Doppler broadened as well as collision broadened. The effect of saturation on the reflectivity of the crossed polarization configurations compared to the parallel polarization configuration is even more significant for resonances with comparable Doppler and collisional broadening.

The Journal of Chemical Physics•Dec 8, 1999•22 citations
In this paper we report on the study of two and multi-level atoms interacting with multiple laser beams. The semi-classical approach is used to describe the system in which the atoms are treated quantum mechanically via the density matrix operator, while the laser beams are treated classically using Maxwells equations. We present results of a two level atom interacting with single and multiple laser beams and demonstrate Rabi oscillations between the levels. The effects of laser modulation on the dynamics of the atom (atomic populations and coherences) are examined by solving the optical Bloch equations. Plots of the density matrix elements as a function of time are presented for various parameters such as laser intensity, detuning, modulation etc. In addition, phase-space plots and Fourier analysis of the density matrix elements are provided. The atomic polarization, estimated from the coherence terms of the density matrix elements, is used in the numerical solution of Maxwells equations to determine the behaviour of the laser beams as they propagate through the atomic ensemble. The effects of saturation and hole-burning are demonstrated in the case of two counter propagating beams with one being a strong beam and the other being very weak. The above work is extended to include four-wave mixing in four level atoms in a diamond configuration. Two co-propagating beams of different wavelengths drive the atoms from a ground state |1〉 to an excited state |3〉 via an intermediate state |2〉. The atoms then move back to the ground state via another intermediate state |4〉, resulting in the generation of two additional correlated photon beams. The characteristics of these additional photons are studied.
Five coherent hole-burning can be simultaneously observed in the absorption spectra of four-level N-style atoms vapors. In this system they adopt a saturated laser co-propagates and two coupling lasers counter-propagate with a probe laser, and the saturated laser can not be in the destructive Doppler state with the probe light. The positions of the coherent hole-burning can be explained by Dressed-state theory. The middle narrow deep hole-burning is induced by the superposition of two coherent hole-burnings. The depth of the coherent hole-burning can be changed by adjusting the reference parameters and the Rabi frequency of the saturated laser. The positions of the coherent hole-burning can be changed by modulating the Rabi frequency of the probe light. By numerical simulation it is found that Rabi frequency of the saturated light plays an important role in slowing the propagating speed. These results may be useful in optical quantum memory and optical quantum information.
We perform nonperturbative calculations of resonant multiwave mixing of two high-intensity laser beams of different frequencies both for a general three-level system and for the 3 2^{2}2S1/2{\mathit{S}}_{1/2}S1/2​--3 2^{2}2P1/2{\mathit{P}}_{1/2}P1/2​ electronic resonance of the sodium atom. Our calculations proceed by direct numerical integration of the density-matrix equations and subsequent Fourier analysis of the calculated time-dependent density-matrix elements. We examine the case where two nearly degenerate input beams are each detuned many collisional linewidths from electronic resonance, and the frequency difference between the input beams is tuned through a ground-state resonance. Unlike previous high-intensity analyses, each input beam can be resonant with numerous transitions simultaneously; for a three-level system, we refer to this as an ``M-type'' system, in analogy with \ensuremath{\Lambda}- and V-type systems. Calculated four-, six-, and eight-wave-mixing spectra exhibit subharmonic resonances of the type observed experimentally by Trebino and Rahn [Opt. Lett. 12, 912 (1987)]. The three-level system is studied to gain insight into the physics of these subharmonic resonances. For more quantitative comparison with experiment, we use a model that includes the 16 Zeeman and hyperfine states in the 3 2^{2}2S1/2{\mathit{S}}_{1/2}S1/2​ and the 3 2^{2}2P1/2{\mathit{P}}_{1/2}P1/2​ levels, and accounts for arbitrary linear polarization of the input laser radiation. The relative intensities of the resonance features in the calculated multiwave-mixing spectra show good agreement with experiment. These resonance features broaden and shift as laser intensity increases, as predicted for four-wave-mixing processes in previous, less general high-intensity analyses. Both theory and experiment also show additional resonant features in the eight-wave-mixing spectra that appear at very high intensity.
The limits of the well-established single-atom model for describing photon-pair generation via four-wave mixing in a diamond configuration in atomic ensembles are experimentally tested. Using a cold-atom source, biphotons are generated and detected through polarization analyzers that resolve the emitted light into horizontal and vertical components in the laboratory frame. The pump lasers driving the first and second excitation transitions are horizontally and vertically polarized, respectively. To predict single-photon counts and coincidence rates in all polarization channels, the first- and second-order correlation functions are calculated directly using a comprehensive model that accounts for all Zeeman sublevels of the relevant hyperfine states. Furthermore, the population dynamics with and without the re-pump laser of the magneto-optical trap are compared, revealing substantial differences in the populations of the Zeeman sublevels. This motivates the inclusion of two additional hyperfine levels and their corresponding Zeeman sublevels in the final model. The resulting density matrix is used to calculate expectation values of the far-field electric-field operators and compare them with experimental measurements over a range of pump-laser powers. Excellent agreement with the measured photon counts is obtained over most of this range. For the coincidence measurements, good agreement is found when the polarization of the photon generated by the first (second) decay is parallel to that of the first (second) pump beam. In contrast, the model consistently underestimates the experimental coincidence rates for the opposite polarization configuration. These findings indicate that effects beyond the internal level dynamics of individual atoms, most notably collective phenomena, are required to fully account for photon coincidences generated by four-wave mixing in atomic ensembles.
Chapter 5 begins the systematic application of the density matrix to describe optical interactions. Stationary two-and three-level atoms interacting with a traveling wave are compared to show that the presence of additional levels changes the saturation behavior of atoms. Then motion of the atoms is introduced and the phenomena of spatial and frequency-domain hole-burning are analyzed. Special effects due to standing waves, such as the light shift, are covered in this section. Next, tri-level coherence is considered, to extend the concept of coherences to two-photon transitions or Zeeman interactions in folded 3- or Λ-systems. Higher order interactions are also analyzed. This includes four-wave mixing and pump–probe techniques which form the basis of common nonlinear laser spectroscopies. Quantum interference is covered as a prelude to the topic of electromagnetically induced transparency. Higher order coherent interactions are also treated using a diagrammatic calculation technique based on Feynman diagrams.
Microscopic models based on multilevel atoms are central to optimizing nonlinear optical responses and the coherent control of light. These models are traditionally based on single-atom effects that are parametrically extrapolated to include collective effects, such as an enhanced response or propagation within atomic media. In this work, we present a systematic analysis of the cooperative effects arising in driven systems composed of multilevel atoms coupled via a common electromagnetic environment. The analysis is based on an interplay between dressed states induced by the driving field and photon exchanges, and collective decay channels. This theory is applied to the case of four-wave mixing induced by a pair of lasers acting on an atomic pair with internal levels in the diamond configuration. The effect of interatomic correlations and collective decay over the photons created in this nonlinear process is then explored. We identify three regions of operation: (i) laser-dominated, (ii) intermediate, and (iii) dipole-dominated. The dependence of single- and two-photon correlations is studied in detail for each region by varying atomic orientations and laser parameters consistent with current experiments involving atomic gases. Photonic correlation functions are shown to exhibit a transition from a Lorentz-like dependence on the two-photon detuning—with general features that can be obtained in an isolated atom scheme—to a two-peaked distribution when the dipole-dipole interactions become relevant. For weak Rabi frequencies whose value is smaller than the highest collective decay rate, the atoms are trapped inside their ground state as they approach each other. It is found that the anisotropy of the dipole-dipole interaction and its wave nature are essential to understand the behavior of the photon correlations. Signatures of these processes are identified for existing experimental realizations. The intuition obtained from this connection helps to uncover relevant parameters that could be exploited for quantum control protocols based on dispersive and dissipative cooperative effects in multilevel systems.
The physics of the degenerate four-wave mixing process for resonant transitions between two degenerate energy levels is investigated by direct numerical integration of the time-dependent density matrix equations. The Zeeman structure of the upper and lower energy levels is included in a multistate formulation of the density matrix equations. The inclusion of the Zeeman structure enables the investigation of the degenerate four-wave mixing process for different polarization configurations of the forward pump, backward pump, and probe beams. Saturation curves and lineshapes are calculated for different polarization configurations and for numerous low-J transitions. At low laser intensity, the results of our calculations are in excellent agreement with perturbation theory in terms of the relative intensities of the degenerate four-wave mixing signal for linear polarization configurations. As the laser intensity increases and the resonance starts to saturate, we find in general that the relative degenerate four-wave mixing reflectivity increases for the crossed polarization configurations compared to the parallel polarization configuration because the saturation intensity is higher. However, for some resonance transitions, some of the crossed polarization configurations saturate at lower laser intensities than the parallel polarization configuration, even though the reflectivity for these crossed polarization configurations is much lower than for the parallel polarization configuration in the perturbative intensity limit. This result is explained in terms of the coupling of the various Zeeman states during the degenerate four-wave mixing interaction for specific polarization configurations. The effect of saturation on the resonance line shapes for the different polarization configurations is also investigated. Finally, a limited number of calculations are performed for resonances that are Doppler broadened as well as collision broadened. The effect of saturation on the reflectivity of the crossed polarization configurations compared to the parallel polarization configuration is even more significant for resonances with comparable Doppler and collisional broadening.