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

International Journal of Quantum Chemistry

Coherent multiphoton absorption: Dependency on the relative phase of two successive pulses

Sylvette Besnaïnou, James P. Stone, Jean‐Claude Diels

Published Nov 1, 1982• 3 citations
Publisher

Abstract

Abstract When a multilevel system excited by a laser pulse absorbs a cascade of photons, a second pulse of same frequency, equal duration but dephased by π takes it back to its initial state. This property can be inferred by studying the laser field system interaction matrix, using the rotating wave approximation.
DOI
10.1002/qua.560220511

Related papers

Molecular multiphoton excitation by phase coherent pulse pairs

Sylvette Besnaïnou, J.-C. Diels, James P. Stone

We theoretically analyze the absorption of media excited by a pair of coherent pulses, as a function of their relative phase, in conditions of multiphoton resonance and negligible dephasing. It is shown that, the periodicity of transmission vs delay and phase, is characteristic of the nature and order of the process. Also a multilevel system may evolve from pure multiphoton resonance to cascade resonance under specific conditions depending on the detunings of the levels involved.

The Journal of Chemical Physics•Jul 1, 1984•14 citations

Temporal coherence in multiphoton absorption. Far off-resonance intermediate states

Peter W. Milonni, Joseph H. Eberly

We develop a consistent formalism for the treatment of temporal atomic or molecular coherence in multiphoton absorption. The formalism is fully quantum mechanical under the assumption that the exciting laser fields are well described by coherent states. We make use of the language and methodology of resonance physics to the extent possible, but deliberately avoid the rotating-wave approximation, and do not restrict the allowed atomic states to be finite in number or the electric field strengths to be small in magnitude. For compactness in the presentation only electric dipole transitions are considered. As all of the transitions, both stimulated and spontaneous, are due to the activation of quantum mechanical dipoles, it is most efficient to construct the formalism so that it emphasizes the role of dipole operators, and we do this. The one strong restriction imposed here, but avoided in a following paper, is to consider only multiphoton transitions that have one resonance between initial and final states and no intermediate resonance. We describe, in effect, the time dependences associated with the early multiphoton absorption calculations of Bebb and Gold.

The Journal of Chemical Physics•Feb 15, 1978•62 citations

Multiphoton coherent excitation of molecules

J.-C. Diels, Sylvette Besnaïnou

Two different approaches to multiphoton excitation of an anharmonic multilevel system are presented. Both methods result in nearly complete population of the upper state. The first approach involving phase shifting portions of the coherent excitation is treated analytically with square pulses. The second approach uses sequences of several pulses with selected relative phase and delays. Some numerical examples are presented for three- and four-photon excitation of the vibrational level structure of CH3F. This particular molecule is again taken as model to demonstrate four-photon excitation with a five pulse sequence, taking into account the rotational line structure. The rotational line distribution in the upper state is seen to correspond to a lower temperature than in the ground state.

The Journal of Chemical Physics•Dec 1, 1986•51 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

Coherent control of ultrafast optical four-wave mixing with two-color ω−3ω laser pulses

Carles Serrat

A theoretical investigation on the coherent control of optical transient four-wave mixing interactions in two-level systems with two intense few-cycle propagating laser pulses of central angular frequencies $\ensuremath{\omega}$ and $3\ensuremath{\omega}$ is reported. By numerically solving the full Maxwell-Bloch equations beyond the slowly varying envelope and rotating-wave approximations in the time domain, the nonlinear coupling to the optical field at frequency $5\ensuremath{\omega}$ is found to depend critically on the initial relative phase $\ensuremath{\phi}$ of the propagating pulses: the coupling is enhanced when the pulses interfere constructively in the center $(\ensuremath{\phi}=0)$, while it is nearly suppressed when they are out of phase $(\ensuremath{\phi}=\ensuremath{\pi})$.

arXiv:physics/0410192•Physical Review A•Aug 9, 2005•17 citations

Reverse-engineering control of the population and phase dynamics of strongly driven open systems

András Csehi

We apply reverse engineering to design laser pulse shapes for controlling the time evolution of strong-field transitions under environmental effects. Our effective two-state representation of the full quantum system involves dynamic Stark shifts and multiphoton Rabi frequency. Furthermore, the environment is modeled with dephasing and dissipative terms. Solving the master equation of the two-level density matrix inversely for the field, we obtain quasianalytic laser pulse shapes that simultaneously drive the populations and relative phase according to user-defined quantum pathways. The validity of the proposed scheme is demonstrated with the example of the $3s\ensuremath{\rightarrow}\ensuremath{\rightarrow}4s$ two-photon transition of atomic sodium by solving the master equation of the multilevel system that incorporates effects beyond the adiabatic elimination and the rotating wave approximation. Due to the open character of the system, the proposed control is not always possible. We explore these situations and point out the conditions for creating steady states with large coherence.

Physical Review A•Sep 26, 2025•1 citation
We develop a consistent formalism for the treatment of temporal atomic or molecular coherence in multiphoton absorption. The formalism is fully quantum mechanical under the assumption that the exciting laser fields are well described by coherent states. We make use of the language and methodology of resonance physics to the extent possible, but deliberately avoid the rotating-wave approximation, and do not restrict the allowed atomic states to be finite in number or the electric field strengths to be small in magnitude. For compactness in the presentation only electric dipole transitions are considered. As all of the transitions, both stimulated and spontaneous, are due to the activation of quantum mechanical dipoles, it is most efficient to construct the formalism so that it emphasizes the role of dipole operators, and we do this. The one strong restriction imposed here, but avoided in a following paper, is to consider only multiphoton transitions that have one resonance between initial and final states and no intermediate resonance. We describe, in effect, the time dependences associated with the early multiphoton absorption calculations of Bebb and Gold.
Two different approaches to multiphoton excitation of an anharmonic multilevel system are presented. Both methods result in nearly complete population of the upper state. The first approach involving phase shifting portions of the coherent excitation is treated analytically with square pulses. The second approach uses sequences of several pulses with selected relative phase and delays. Some numerical examples are presented for three- and four-photon excitation of the vibrational level structure of CH3F. This particular molecule is again taken as model to demonstrate four-photon excitation with a five pulse sequence, taking into account the rotational line structure. The rotational line distribution in the upper state is seen to correspond to a lower temperature than in the ground state.
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.
A theoretical investigation on the coherent control of optical transient four-wave mixing interactions in two-level systems with two intense few-cycle propagating laser pulses of central angular frequencies $\ensuremath{\omega}$ and $3\ensuremath{\omega}$ is reported. By numerically solving the full Maxwell-Bloch equations beyond the slowly varying envelope and rotating-wave approximations in the time domain, the nonlinear coupling to the optical field at frequency $5\ensuremath{\omega}$ is found to depend critically on the initial relative phase $\ensuremath{\phi}$ of the propagating pulses: the coupling is enhanced when the pulses interfere constructively in the center $(\ensuremath{\phi}=0)$, while it is nearly suppressed when they are out of phase $(\ensuremath{\phi}=\ensuremath{\pi})$.
We apply reverse engineering to design laser pulse shapes for controlling the time evolution of strong-field transitions under environmental effects. Our effective two-state representation of the full quantum system involves dynamic Stark shifts and multiphoton Rabi frequency. Furthermore, the environment is modeled with dephasing and dissipative terms. Solving the master equation of the two-level density matrix inversely for the field, we obtain quasianalytic laser pulse shapes that simultaneously drive the populations and relative phase according to user-defined quantum pathways. The validity of the proposed scheme is demonstrated with the example of the $3s\ensuremath{\rightarrow}\ensuremath{\rightarrow}4s$ two-photon transition of atomic sodium by solving the master equation of the multilevel system that incorporates effects beyond the adiabatic elimination and the rotating wave approximation. Due to the open character of the system, the proposed control is not always possible. We explore these situations and point out the conditions for creating steady states with large coherence.