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

Coherence versus incoherence in stepwise laser excitation of atoms and molecules

Jay R. Ackerhalt, Joseph H. Eberly

Published Nov 1, 1976• 107 citations
Publisher

Abstract

We discuss multistep resonant photoionization of atoms and photodissociation of molecules. We derive a condition under which induced atomic or molecular coherence can always be neglected, allowing accurate analysis of the multiphoton process by simple rate equations. The condition is realizable in practice, and consistent with large ionization and dissociation rates.

DOI
10.1103/physreva.14.1705

Related papers

Coherence vs incoherence in stepwise laser excitation

Bruce W. Shore, Michael Austin Johnson

We demonstrate the manner in which solutions of the (coherent) Schrödinger equation for multistep excitation approach those of an (incoherent) rate equation. For a two-level system, coherence produces oscillations about the mean rate-equation values. In more general N-level sequences the two types of solutions agree in the limit described by Ackerhalt and Eberly. We point out instances in which a simple rate equation cannot duplicate results of the Schrödinger equation.

The Journal of Chemical Physics•Jun 15, 1978•27 citations

Laser-Induced multiphoton transitions

Stig Stenholm

Laser induced multiphoton processes are reviewed. The effects of strong fields on atoms are discussed. The perturbation treatment is presented and also its generalization to treat intermediate resonances. Atomic ionization experiments are reviewed and the present understanding of multiphoton dissociation of molecules is explained. Finally some prospects for the future are discussed.

Contemporary Physics•Jan 1, 1979•10 citations

Laser photoselective ionization of atoms

Vladilen S Letokhov

Abstract In this and subsequent chapters, we consider are other laser methods for controlling atoms and molecules that, in contrast to all the methods discussed above in Chapters 2–8, are destructive. They result in the ionization of the atoms or molecules being controlled and the dissociation and fragmentation of molecules. All these methods are united by the capability of the particles to be ionized or dissociated in a photo selective manner, which makes it possible to detect and separate atoms or molecules of certain species. They are based on the fact that all the structural details of atoms and molecules manifest themselves in their spectra, for example, some details manifest in the spectra of atoms are the atomic weight (the number of nucleons), the number of protons (the nuclear charge and the type of element), the number of neutrons (the isotopic state), and even the excitation energy of the nucleus (the isomeric composition). This enables one to excite, and, in some cases, ionize atoms and molecules in a photo selective way and thus accomplish their photo selective excitation and separation. Figure 9.1 lists all types of photo selectivity. All of them have been successfully realized by the method of resonance multistep ionization of atoms that is considered in the present chapter. Our primary attention here is concentrated on the realization of laser control of the photo selectivity of ionization. A detailed description of this method can be found in the monographs by Letokhov (1987) and Hurst and Payne (1988).

•Feb 15, 2007•0 citations

ATOMS INTERACTING WITH ELECTROMAGNETIC FIELDS, MULTIPHOTON IONIZATION

G. Mainfray

The non linear interaction between an intense laser radiation and atoms leads to ionization through the absorption of N photons from the laser radiation via laser-induced virtual states. The multiphoton ionization rate varies as a function of the laser intensity I as IN. We discuss the two most important effects which govern multiphoton ionization processes : resonance effects and laser-coherence effects. In a moderate laser intensity range (107 - 109 W cm-2) corresponding to the two, three or four-photon ionization of atoms, resonance effects play a dominant role while the photon statistics of the laser radiation are relatively unimportant. On the contrary, in the very high intensity range (1012 - 1013 W cm-2) required to observe large Nth - order ionization processes, coherence effects play a dominant role through N! enhancement in the N-photon ionization rate, while resonance effects are completely damped due to the high laser intensity. We conclude by reviewing the possible applications of multiphoton absorption processes in other fields.

Le Journal de Physique Colloques•Nov 1, 1982•1 citation

Scheme for multistep resonance photoionization of atoms

Bo Liu, Xi‐Jing Ning

Traditional schemes for multistep resonance photoionization of atoms let every employed laser beam interact with the atoms simultaneously. In such a situation, analyses via time-dependent Schr\"odinger equation show that high ionization probability requires all the laser beams must be intense enough. In order to decrease laser intensity, we proposed a scheme that the laser beam used to pump the excited atoms (in a higher bound state) into an autoionization state does not interact with the atoms until all the population is transferred by the other lasers from a ground state to the bound state. As an interesting example, we examined three-step photoionization of ${}^{235}\mathrm{U}$ with our scheme, showing that the intensity of two laser beams can be lowered by two orders of magnitude without losing high ionization probability.

Physical Review A•May 30, 2001•6 citations

Collisions and half-collisions with lasers

N. K. Rahman, Carla Guidotti

Merging two subfields, collisions and spectroscopy, this book presents the latest research proposals, innovative experiments and fresh ideas. Topics considered include radiative collision induced electron continuum-continuum scattering; models of laser-induced chemical reactions; experimental studies of laser-induced ionizing collisions; laser photodissociation of Na/sub 2/ + ions produced by laser resonant ionization of Na vapor; steady-state electron-atom collision in a laser field; conditions for the observation of the predicted splitting of the laser assisted electron impact of the differential cross section of atoms; transitions between resonances; some proposals for experiments; above-threshold multiphoton ionization; observability of optical collisions in the frequency and the time domain; laser switched collisions - a diagrammatical approach; polarization of atomic fluorescence excited by molecular photodissociation; multiphoton selective excitation; on the role of chaotic dynamics with many basins of attraction; predissociation in a strong electromagnetic field; theory of double resonance; and coherent excitation of polyatomic molecules up to highly excited vibrational states by laser light.

•Jan 1, 1984•42 citations
We discuss multistep resonant photoionization of atoms and photodissociation of molecules. We derive a condition under which induced atomic or molecular coherence can always be neglected, allowing accurate analysis of the multiphoton process by simple rate equations. The condition is realizable in practice, and consistent with large ionization and dissociation rates.
Abstract In this and subsequent chapters, we consider are other laser methods for controlling atoms and molecules that, in contrast to all the methods discussed above in Chapters 2–8, are destructive. They result in the ionization of the atoms or molecules being controlled and the dissociation and fragmentation of molecules. All these methods are united by the capability of the particles to be ionized or dissociated in a photo selective manner, which makes it possible to detect and separate atoms or molecules of certain species. They are based on the fact that all the structural details of atoms and molecules manifest themselves in their spectra, for example, some details manifest in the spectra of atoms are the atomic weight (the number of nucleons), the number of protons (the nuclear charge and the type of element), the number of neutrons (the isotopic state), and even the excitation energy of the nucleus (the isomeric composition). This enables one to excite, and, in some cases, ionize atoms and molecules in a photo selective way and thus accomplish their photo selective excitation and separation. Figure 9.1 lists all types of photo selectivity. All of them have been successfully realized by the method of resonance multistep ionization of atoms that is considered in the present chapter. Our primary attention here is concentrated on the realization of laser control of the photo selectivity of ionization. A detailed description of this method can be found in the monographs by Letokhov (1987) and Hurst and Payne (1988).
The non linear interaction between an intense laser radiation and atoms leads to ionization through the absorption of N photons from the laser radiation via laser-induced virtual states. The multiphoton ionization rate varies as a function of the laser intensity I as IN. We discuss the two most important effects which govern multiphoton ionization processes : resonance effects and laser-coherence effects. In a moderate laser intensity range (107 - 109 W cm-2) corresponding to the two, three or four-photon ionization of atoms, resonance effects play a dominant role while the photon statistics of the laser radiation are relatively unimportant. On the contrary, in the very high intensity range (1012 - 1013 W cm-2) required to observe large Nth - order ionization processes, coherence effects play a dominant role through N! enhancement in the N-photon ionization rate, while resonance effects are completely damped due to the high laser intensity. We conclude by reviewing the possible applications of multiphoton absorption processes in other fields.
Traditional schemes for multistep resonance photoionization of atoms let every employed laser beam interact with the atoms simultaneously. In such a situation, analyses via time-dependent Schr\"odinger equation show that high ionization probability requires all the laser beams must be intense enough. In order to decrease laser intensity, we proposed a scheme that the laser beam used to pump the excited atoms (in a higher bound state) into an autoionization state does not interact with the atoms until all the population is transferred by the other lasers from a ground state to the bound state. As an interesting example, we examined three-step photoionization of 235U{}^{235}\mathrm{U}235U with our scheme, showing that the intensity of two laser beams can be lowered by two orders of magnitude without losing high ionization probability.
Merging two subfields, collisions and spectroscopy, this book presents the latest research proposals, innovative experiments and fresh ideas. Topics considered include radiative collision induced electron continuum-continuum scattering; models of laser-induced chemical reactions; experimental studies of laser-induced ionizing collisions; laser photodissociation of Na/sub 2/ + ions produced by laser resonant ionization of Na vapor; steady-state electron-atom collision in a laser field; conditions for the observation of the predicted splitting of the laser assisted electron impact of the differential cross section of atoms; transitions between resonances; some proposals for experiments; above-threshold multiphoton ionization; observability of optical collisions in the frequency and the time domain; laser switched collisions - a diagrammatical approach; polarization of atomic fluorescence excited by molecular photodissociation; multiphoton selective excitation; on the role of chaotic dynamics with many basins of attraction; predissociation in a strong electromagnetic field; theory of double resonance; and coherent excitation of polyatomic molecules up to highly excited vibrational states by laser light.