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

Physical Review A

Adiabatic following model for two-photon transitions: Nonlinear mixing and pulse propagation

D. Grischkowsky, M. M. T. Loy, P. F. Liao

Published Dec 1, 1975• 302 citations
Publisher

Abstract

Two-photon resonantly enhanced parametric generation processes have generally been described using time-dependent perturbation theory. In this paper we show that a theory of two-photon coherent effects can be used to derive and explain these nonlinear mixing processes. Our technique makes use of the adiabatic following (AF) approximation to obtain solutions to a vector model describing the two-photon resonance. We show that the usual results for the nonlinear susceptibilities correspond to the $\stackrel{\ensuremath{\rightarrow}}{\mathrm{r}}$ vector of Feynman, Vernon, and Hellwarth adiabatically following the $\stackrel{\ensuremath{\rightarrow}}{\mathrm{\ensuremath{\gamma}}}$ vector in the small-angle limit. Consequently, the theory allows a natural extension to large angles, and power-dependent nonlinear susceptibilities are obtained. We then use these AF results for the polarization to study the propagation of pulses nearly resonant with a two-photon transition, and we demonstrate that the pulse reshaping is due to the two related effects of a nonlinear pulse velocity and self-phase modulation.

DOI
10.1103/physreva.12.2514

Related papers

Coherent propagation of two-photon quasi-resonant pulses in a medium of multi-level atoms

Farhad H. M. Faisal

Coherent propagation of a circularly polarized pulse which is two-photon quasi-resonant with a medium of multi-level atoms is considered in the adiabatic following limit. The relevant pair of non-linear coupled partial differential equations are solved exactly for arbitrary pulse shapes. The development of the envelope and the phase of the pulse as it propagates through the medium is described analytically. Perturbation theoretical results are shown to apply only for small intensity or small distance of propagation or both. Qualitatively different results apply for higher intensities and longer distances of propagation. These include strong self-phase-modulation effects as well as reshaping of the pulse envelope.

Journal of Physics B Atomic and Molecular Physics•Jul 11, 1977•3 citations

A THREE-PHOTON VECTOR MODEL

Peixian Ye, 中国科学院物理研究所

It is shown that the optical Eabi precession model developed by Feynman, Vernon and Hellwarth for two-level systems can be extended not only to discuss the two-photon resonant coherent interaction, but also to the case of three photons. Using this model and the adiabatic following approximation, the third-order polarization expression in an intense and (or) resonant optical field is obtained, which differs from that obtained by perturbation theory. The saturation phenomena in the third-order resonant non-linear effects are also discussed.

Acta Physica Sinica•Jan 1, 1979•0 citations

Coherent excitation, incoherent excitation, and adiabatic states

D. Grischkowsky

Coherent excitation of an atomic excited state occurs during the propagation of near-resonant light pulses and is responsible for the induced polarization. Simultaneously, incoherent excitation occurs due to the relaxation processes described by the absorption coefficient. Here, the theory for the coherent and incoherent excitation is initially presented in terms of the traditional vector model. While a complete understanding of the two-level system is provided by the vector model, it is shown to be incomplete when the problem of directly monitoring the coherent and incoherent excitation is considered. This is because this latter problem involves more than two levels. For this more complicated multilevel problem, adiabatic states are introduced to gain further understanding. The adiabatic states are the stationary states of the atom in the presence of the near-resonant laser field; they help to explain the intimate connection between the coherent excitation and the two-photon resonance. Experimental measurements of the coherent and incoherent excitation associated with near-resonant pulse propagation in Rb vapor are presented. The double-resonance technique used a relatively strong pulsed dye laser tuned near the $5{S}_{\frac{1}{2}}\ensuremath{\leftrightarrow}5{P}_{\frac{1}{2}}$ transition (7948 \AA{}A) of Rb to produce the coherent and incoherent excitation, and a weak, tunable cw dye laser tuned in the region of the $5{P}_{\frac{1}{2}}\ensuremath{\leftrightarrow}6{D}_{\frac{3}{2}}$ transition (6206 \AA{}A) to monitor this excitation. In agreement with theory, the experimental results demonstrate that coherent excitation is responsible for two-photon absorption, while the incoherent excitation corresponds to one-photon absorption to the $5{P}_{\frac{1}{2}}$ state.

Physical Review A•Aug 1, 1976•80 citations

Four-photon coherent resonant propagation and transient wave mixing: Application to the mercury atom

Nandini Mukherjee, Arindum Mukherjee, J.-C. Diels

Density-matrix formalism is applied to construct a model for third- and fifth-harmonic generation in a four-photon resonant medium. The transition rates and coherent superposition of states associated with the resonant levels are treated rigorously, while the adiabatic following approximation is used to calculate the contribution of all nonresonant levels to the interaction. Expressions for the quadratic and quartic Stark shift and multiphoton ionization emerge naturally from the theory. At the power level required for appreciable four-photon absorption, the intensity-dependent Stark shift and ionization become overwhelming and limit the efficiency of harmonic generation. Because of the Stark shift, an intense pulse suffers a ``self-detuning'' effect and propagates through the resonant medium with minimal absorption. The interference of the phase-dependent Raman scattering with the multiphoton transition is found to be responsible for the vanishing of ionization in the presence of the generated third-harmonic field, an effect which was observed in earlier experiments.

Physical Review A•Aug 1, 1988•4 citations

Nonlinear polarizations and excitations and their time dependence in discrete multilevel systems

H. B. Puell, C. R. Vidal

For the interaction of coherent radiation with a nondegenerate, homogeneously broadened multilevel system the nonlinear susceptibilities and excitations and their time dependence are evaluated using a perturbation approach to the density matrix up to fourth order. This is done for the "off-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\gg}\frac{1}{\ensuremath{\tau}}$, as well as for the "on-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\ll}\frac{1}{\ensuremath{\tau}}$, with $\ensuremath{\tau}$ being the pulse duration, by taking into account the temporal change of the electric field amplitude and the phase and energy relaxation times, ${T}_{2}$ and ${T}_{1}$. It is shown that the transient one-photon excitation known as adiabatic following, is not only important for a pulse duration $\ensuremath{\tau}<{T}_{2}$, but may also be important for ${T}_{2}\ensuremath{\lesssim}\ensuremath{\tau}<{T}_{1}$. In addition, expressions for the transient two-photon excitation in a multilevel system are derived. Finally, the two-level limit is evaluated to all orders of the perturbation including damping effects, which gives results valid also for large incident light intensities. For the "off-resonance" case an expression is obtained which describes not only the transient adiabatic following process, but also the usual one-photon absorption including saturation effects giving rise to power broadening.

Physical Review A•Dec 1, 1976•32 citations

Dynamical model of coherent circularly polarized optical pulse interactions with two-level quantum systems

Gabriela M. Slavcheva, Ortwin G. Hess

We propose and develop a method for theoretical description of circularly (elliptically) polarized optical pulse resonant coherent interactions with two-level atoms. The method is based on the time-evolution equations of a two-level quantum system in the presence of a time-dependent dipole perturbation for electric dipole transitions between states with total angular-momentum projection difference $(\ensuremath{\Delta}{J}_{z}=\ifmmode\pm\else\textpm\fi{}1)$ excited by a circularly polarized electromagnetic field [Feynman et al., J. Appl. Phys. 28, 49 (1957)]. The adopted real-vector representation approach allows for coupling with the vectorial Maxwell's equations for the optical wave propagation and thus the resulting Maxwell pseudospin equations can be numerically solved in the time domain without any approximations. The model permits a more exact study of the ultrafast coherent pulse propagation effects taking into account the vector nature of the electromagnetic field and hence the polarization state of the optical excitation. We demonstrate self-induced transparency effects and formation of polarized solitons. The model represents a qualitative extension of the well-known optical Maxwell-Bloch equations valid for linearly polarized light and a tool for studying coherent quantum control mechanisms.

Physical Review A•Nov 3, 2005•19 citations
Two-photon resonantly enhanced parametric generation processes have generally been described using time-dependent perturbation theory. In this paper we show that a theory of two-photon coherent effects can be used to derive and explain these nonlinear mixing processes. Our technique makes use of the adiabatic following (AF) approximation to obtain solutions to a vector model describing the two-photon resonance. We show that the usual results for the nonlinear susceptibilities correspond to the r\ensuremath→\stackrel{\ensuremath{\rightarrow}}{\mathrm{r}}r\ensuremath→ vector of Feynman, Vernon, and Hellwarth adiabatically following the \ensuremathγ\ensuremath→\stackrel{\ensuremath{\rightarrow}}{\mathrm{\ensuremath{\gamma}}}\ensuremathγ\ensuremath→​ vector in the small-angle limit. Consequently, the theory allows a natural extension to large angles, and power-dependent nonlinear susceptibilities are obtained. We then use these AF results for the polarization to study the propagation of pulses nearly resonant with a two-photon transition, and we demonstrate that the pulse reshaping is due to the two related effects of a nonlinear pulse velocity and self-phase modulation.
Coherent propagation of a circularly polarized pulse which is two-photon quasi-resonant with a medium of multi-level atoms is considered in the adiabatic following limit. The relevant pair of non-linear coupled partial differential equations are solved exactly for arbitrary pulse shapes. The development of the envelope and the phase of the pulse as it propagates through the medium is described analytically. Perturbation theoretical results are shown to apply only for small intensity or small distance of propagation or both. Qualitatively different results apply for higher intensities and longer distances of propagation. These include strong self-phase-modulation effects as well as reshaping of the pulse envelope.
It is shown that the optical Eabi precession model developed by Feynman, Vernon and Hellwarth for two-level systems can be extended not only to discuss the two-photon resonant coherent interaction, but also to the case of three photons. Using this model and the adiabatic following approximation, the third-order polarization expression in an intense and (or) resonant optical field is obtained, which differs from that obtained by perturbation theory. The saturation phenomena in the third-order resonant non-linear effects are also discussed.
Coherent excitation of an atomic excited state occurs during the propagation of near-resonant light pulses and is responsible for the induced polarization. Simultaneously, incoherent excitation occurs due to the relaxation processes described by the absorption coefficient. Here, the theory for the coherent and incoherent excitation is initially presented in terms of the traditional vector model. While a complete understanding of the two-level system is provided by the vector model, it is shown to be incomplete when the problem of directly monitoring the coherent and incoherent excitation is considered. This is because this latter problem involves more than two levels. For this more complicated multilevel problem, adiabatic states are introduced to gain further understanding. The adiabatic states are the stationary states of the atom in the presence of the near-resonant laser field; they help to explain the intimate connection between the coherent excitation and the two-photon resonance. Experimental measurements of the coherent and incoherent excitation associated with near-resonant pulse propagation in Rb vapor are presented. The double-resonance technique used a relatively strong pulsed dye laser tuned near the $5{S}_{\frac{1}{2}}\ensuremath{\leftrightarrow}5{P}_{\frac{1}{2}}$ transition (7948 \AA{}A) of Rb to produce the coherent and incoherent excitation, and a weak, tunable cw dye laser tuned in the region of the $5{P}_{\frac{1}{2}}\ensuremath{\leftrightarrow}6{D}_{\frac{3}{2}}$ transition (6206 \AA{}A) to monitor this excitation. In agreement with theory, the experimental results demonstrate that coherent excitation is responsible for two-photon absorption, while the incoherent excitation corresponds to one-photon absorption to the 5P125{P}_{\frac{1}{2}}5P21​​ state.
Density-matrix formalism is applied to construct a model for third- and fifth-harmonic generation in a four-photon resonant medium. The transition rates and coherent superposition of states associated with the resonant levels are treated rigorously, while the adiabatic following approximation is used to calculate the contribution of all nonresonant levels to the interaction. Expressions for the quadratic and quartic Stark shift and multiphoton ionization emerge naturally from the theory. At the power level required for appreciable four-photon absorption, the intensity-dependent Stark shift and ionization become overwhelming and limit the efficiency of harmonic generation. Because of the Stark shift, an intense pulse suffers a ``self-detuning'' effect and propagates through the resonant medium with minimal absorption. The interference of the phase-dependent Raman scattering with the multiphoton transition is found to be responsible for the vanishing of ionization in the presence of the generated third-harmonic field, an effect which was observed in earlier experiments.
For the interaction of coherent radiation with a nondegenerate, homogeneously broadened multilevel system the nonlinear susceptibilities and excitations and their time dependence are evaluated using a perturbation approach to the density matrix up to fourth order. This is done for the "off-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\gg}\frac{1}{\ensuremath{\tau}}$, as well as for the "on-resonance" case, ${(\ensuremath{\Delta}{\ensuremath{\omega}}^{2}+{\ensuremath{\Gamma}}^{2})}^{\frac{1}{2}}\ensuremath{\ll}\frac{1}{\ensuremath{\tau}}$, with $\ensuremath{\tau}$ being the pulse duration, by taking into account the temporal change of the electric field amplitude and the phase and energy relaxation times, T2{T}_{2}T2​ and T1{T}_{1}T1​. It is shown that the transient one-photon excitation known as adiabatic following, is not only important for a pulse duration $\ensuremath{\tau}<{T}_{2}$, but may also be important for ${T}_{2}\ensuremath{\lesssim}\ensuremath{\tau}<{T}_{1}$. In addition, expressions for the transient two-photon excitation in a multilevel system are derived. Finally, the two-level limit is evaluated to all orders of the perturbation including damping effects, which gives results valid also for large incident light intensities. For the "off-resonance" case an expression is obtained which describes not only the transient adiabatic following process, but also the usual one-photon absorption including saturation effects giving rise to power broadening.
We propose and develop a method for theoretical description of circularly (elliptically) polarized optical pulse resonant coherent interactions with two-level atoms. The method is based on the time-evolution equations of a two-level quantum system in the presence of a time-dependent dipole perturbation for electric dipole transitions between states with total angular-momentum projection difference $(\ensuremath{\Delta}{J}_{z}=\ifmmode\pm\else\textpm\fi{}1)$ excited by a circularly polarized electromagnetic field [Feynman et al., J. Appl. Phys. 28, 49 (1957)]. The adopted real-vector representation approach allows for coupling with the vectorial Maxwell's equations for the optical wave propagation and thus the resulting Maxwell pseudospin equations can be numerically solved in the time domain without any approximations. The model permits a more exact study of the ultrafast coherent pulse propagation effects taking into account the vector nature of the electromagnetic field and hence the polarization state of the optical excitation. We demonstrate self-induced transparency effects and formation of polarized solitons. The model represents a qualitative extension of the well-known optical Maxwell-Bloch equations valid for linearly polarized light and a tool for studying coherent quantum control mechanisms.